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Nanomaterials for Ion Battery Applications
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Nanomaterials for Ion Battery Applications

A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Energy and Catalysis".

Deadline for manuscript submissions: closed (31 March 2022) | Viewed by 40833

Printed Edition Available!
A printed edition of this Special Issue is available here.

Special Issue Editor

Dr. Jaehyun Hur

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Guest Editor
Department of Chemical and Biological Engineering, Gachon University, Seongnam, Republic of Korea
Interests: nanoparticles; quantum dots; polymers; carbon-based materials; metal oxide materials; transition metal chalcogenides; 2D materials; nanostructures; alloys; hybrid materials
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Rechargeable batteries, ranging from small portable devices to large energy storage systems, have emerged as indispensable electrochemical devices in our daily lives. The three primary components of rechargeable cells are the positive and negative electrodes and the electrolytes. Nanotechnologies are positioned to play a critical role in significantly improving battery performance. The rational design of various nanomaterials has been a major research theme in the process of developing high-performance batteries. Although nanomaterials may face a higher risk of unwanted secondary reactions than bulk materials, a suitable material design can overcome this issue while providing beneficial opportunities. For example, suitably designed nanomaterials may provide a significant increase in the effective surface area of electrodes, thereby increasing the energy storage. Moreover, the judicious design of nanoarchitecture can boost the diffusion of ions into the electrodes, resulting in the enhancement of the electrochemical reaction kinetics.

Among various types of rechargeable batteries, Li-ion batteries are presently regarded as market-leading technologies thanks to their many beneficial features. However, Li-ion batteries still have limitations to be overcome, and thus there is ongoing research into several different types of potential next-generation batteries.

This Special Issue of Nanomaterials will cover the advancements in recent nanotechnologies and nanomaterials for various ion batteries (Li-ion batteries, sodium-ion batteries, Li–sulfur batteries, multivalent ion batteries, aqueous batteries, etc.). The development of new functional nanomaterials, as important components in these batteries, is the central topic to be discussed in this Special Issue.

Dr. Jaehyun Hur
Guest Editor

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Nanomaterials is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

  • nanostructured cathodes or anodes
  • functional nanomaterials
  • synthesis of electrode materials
  • hybrid nanomaterials
  • advanced electrolytes
  • characterizations

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Published Papers (12 papers)

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Editorial

Jump to: Research, Review

3 pages, 178 KiB  
Editorial
Nanomaterials for Ion Battery Applications
by Jaehyun Hur
Nanomaterials 2022, 12(13), 2293; https://doi.org/10.3390/nano12132293 - 4 Jul 2022
Cited by 4 | Viewed by 2035
Abstract
Nanomaterials offer opportunities to improve battery performance in terms of energy density and electrochemical reaction kinetics owing to a significant increase in the effective surface area of electrodes and reduced ion diffusion pathways [...] Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)

Research

Jump to: Editorial, Review

13 pages, 4612 KiB  
Article
In Situ Growth of W2C/WS2 with Carbon-Nanotube Networks for Lithium-Ion Storage
by Thang Phan Nguyen and Il Tae Kim
Nanomaterials 2022, 12(6), 1003; https://doi.org/10.3390/nano12061003 - 18 Mar 2022
Cited by 11 | Viewed by 2450
Abstract
The combination of W2C and WS2 has emerged as a promising anode material for lithium-ion batteries. W2C possesses high conductivity but the W2C/WS2-alloy nanoflowers show unstable performance because of the lack of [...] Read more.
The combination of W2C and WS2 has emerged as a promising anode material for lithium-ion batteries. W2C possesses high conductivity but the W2C/WS2-alloy nanoflowers show unstable performance because of the lack of contact with the leaves of the nanoflower. In this study, carbon nanotubes (CNTs) were employed as conductive networks for in situ growth of W2C/WS2 alloys. The analysis of X-ray diffraction patterns and scanning/transmission electron microscopy showed that the presence of CNTs affected the growth of the alloys, encouraging the formation of a stacking layer with a lattice spacing of ~7.2 Å. Therefore, this self-adjustment in the structure facilitated the insertion/desertion of lithium ions into the active materials. The bare W2C/WS2-alloy anode showed inferior performance, with a capacity retention of ~300 mAh g−1 after 100 cycles. In contrast, the WCNT01 anode delivered a highly stable capacity of ~650 mAh g−1 after 100 cycles. The calculation based on impedance spectra suggested that the presence of CNTs improved the lithium-ion diffusion coefficient to 50 times that of bare nanoflowers. These results suggest the effectiveness of small quantities of CNTs on the in situ growth of sulfides/carbide alloys: CNTs create networks for the insertion/desertion of lithium ions and improve the cyclic performance of metal-sulfide-based lithium-ion batteries. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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Graphical abstract

Graphical abstract
Full article ">Figure 1
<p>FESEM images of (<b>a</b>) <span class="html-italic">W</span><sub>2</sub><span class="html-italic">C</span>/<span class="html-italic">WS</span><sub>2</sub> (<b>b</b>) WCNT01, (<b>c</b>) WCNT02, and (<b>d</b>) WCNT03 samples.</p> Full article ">Figure 2
<p>(<b>a</b>) XRD patterns of <span class="html-italic">W</span><sub>2</sub><span class="html-italic">C</span>/<span class="html-italic">WS</span><sub>2</sub> and WCNT01/02/03; (<b>b</b>) TEM images and (<b>c</b>,<b>d</b>) high-resolution TEM (HR-TEM) images of WCNT01.</p> Full article ">Figure 3
<p>(<b>a</b>) Raman spectra of bare <span class="html-italic">W</span><sub>2</sub><span class="html-italic">C</span>/<span class="html-italic">WS</span><sub>2</sub> and WCNT01 samples. High-resolution XPS spectra of (<b>b</b>) W 4f, (<b>c</b>) S 2p, and (<b>d</b>) C 1s of WCNT01 sample.</p> Full article ">Figure 4
<p>Cyclic voltammograms of the (<b>a</b>) <span class="html-italic">W</span><sub>2</sub><span class="html-italic">C</span>/<span class="html-italic">WS</span><sub>2</sub>, (<b>b</b>) WCNT01, (<b>c</b>) WCNT02, and (<b>d</b>) WCNT03 anodes.</p> Full article ">Figure 5
<p>Initial voltage profiles of the (<b>a</b>) <span class="html-italic">W</span><sub>2</sub><span class="html-italic">C</span>/<span class="html-italic">WS</span><sub>2</sub> alloys, (<b>b</b>) WCNT01, (<b>c</b>) WCNT02, and (<b>d</b>) WCNT03 anodes.</p> Full article ">Figure 6
<p>Cyclic performance of the (<b>a</b>) <span class="html-italic">W</span><sub>2</sub><span class="html-italic">C</span>/<span class="html-italic">WS</span><sub>2</sub> alloys, (<b>b</b>) WCNT01, (<b>c</b>) WCNT02, and (<b>d</b>) WCNT03 anodes under the current rate of 0.1 A g<sup>−1</sup>.</p> Full article ">Figure 7
<p>(<b>a</b>) Nyquist plots and (<b>b</b>) <span class="html-italic">Z</span>′ vs. <math display="inline"><semantics> <mrow> <msup> <mi>ω</mi> <mrow> <mo>−</mo> <mn>1</mn> <mo>/</mo> <mn>2</mn> </mrow> </msup> </mrow> </semantics></math> plots of the bare <span class="html-italic">W</span><sub>2</sub><span class="html-italic">C</span>/<span class="html-italic">WS</span><sub>2</sub> alloys and WCNT01/02/03 anodes.</p> Full article ">
17 pages, 5973 KiB  
Article
The Effects of the Binder and Buffering Matrix on InSb-Based Anodes for High-Performance Rechargeable Li-Ion Batteries
by Vo Pham Hoang Huy, Il Tae Kim and Jaehyun Hur
Nanomaterials 2021, 11(12), 3420; https://doi.org/10.3390/nano11123420 - 17 Dec 2021
Cited by 9 | Viewed by 3033
Abstract
C-decorated intermetallic InSb (InSb–C) was developed as a novel high-performance anode material for lithium-ion batteries (LIBs). InSb nanoparticles synthesized via a mechanochemical reaction were characterized using X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and [...] Read more.
C-decorated intermetallic InSb (InSb–C) was developed as a novel high-performance anode material for lithium-ion batteries (LIBs). InSb nanoparticles synthesized via a mechanochemical reaction were characterized using X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and energy-dispersive X-ray spectroscopy (EDX). The effects of the binder and buffering matrix on the active InSb were investigated. Poly(acrylic acid) (PAA) was found to significantly improve the cycling stability owing to its strong hydrogen bonding. The addition of amorphous C to InSb further enhanced mechanical stability and electronic conductivity. As a result, InSb–C demonstrated good electrochemical Li-ion storage performance: a high reversible specific capacity (878 mAh·g−1 at 100 mA·g−1 after 140 cycles) and good rate capability (capacity retention of 98% at 10 A·g−1 as compared to 0.1 A·g−1). The effects of PAA and C were comprehensively studied using cyclic voltammetry, differential capacity plots, ex-situ SEM, and electrochemical impedance spectroscopy (EIS). In addition, the electrochemical reaction mechanism of InSb was revealed using ex-situ XRD. InSb–C exhibited a better performance than many recently reported Sb-based electrodes; thus, it can be considered as a potential anode material in LIBs. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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Graphical abstract

Graphical abstract
Full article ">Figure 1
<p>(<b>a</b>) XRD pattern (inset: crystalline structure), (<b>b</b>) SEM image, (<b>c</b>) particle size distribution, and (<b>d</b>) EDX spectrum of the as-synthesized InSb powder. XPS profiles of (<b>e</b>) In 3d, and (<b>f</b>) Sb 3d for the InSb powder.</p> Full article ">Figure 2
<p>Electrochemical performance of the InSb electrode. (<b>a</b>) GCD voltage profiles of InSb_PAA at a current density of 100 mA·g<sup>−1</sup>. Cyclic performance of the InSb_PAA and InSb_PVDF at a current density of (<b>b</b>) 100 and (<b>c</b>) 500 mA·g<sup>−1</sup>. (<b>d</b>) CV curves of InSb_PAA.</p> Full article ">Figure 3
<p>Comparison of the InSb_PAA and InSb_PVDF electrodes before and after 20 cycles. Cross-sectional images of (<b>a</b>) pristine InSb_PAA, (<b>b</b>,<b>c</b>) InSb_PAA after 20 cycles at different magnifications, (<b>d</b>) pristine InSb_PVDF, and (<b>e</b>,<b>f</b>) InSb_PVDF after 20 cycles at different magnifications. The dashed yellow lines in (<b>b</b>,<b>e</b>) indicate the boundary between electrode and Cu collector.</p> Full article ">Figure 4
<p>(<b>a</b>) XRD patterns collected at selected potential states in the initial lithiation/delithiation process. (<b>b</b>) Schematic of the electrochemical reaction mechanism of the InSb_PAA electrode during cycling.</p> Full article ">Figure 5
<p>(<b>a</b>) XRD pattern, (<b>b</b>) SEM image, (<b>c</b>) HRTEM image, and (<b>d</b>) EDX elemental maps of In, Sb, O, and C of InSb–C.</p> Full article ">Figure 6
<p>Electrochemical performance of the half-cells. (<b>a</b>) GCD profiles of InSb-C_PAA at a current density of 100 mA·g<sup>−1</sup>, cyclic performance of InSb-C_PAA at (<b>b</b>) 100 mA·g<sup>−1</sup> and (<b>c</b>) 500 mA·g<sup>−1</sup>, (<b>d</b>) CV curves of InSb-C_PAA, (<b>e</b>) rate capabilities of the composites, and (<b>f</b>) capacity retention of the composites at different current densities.</p> Full article ">Figure 7
<p>(<b>a</b>) The equivalent circuit. Nyquist plots after 1, 5, and 20 cycles for (<b>b</b>) InSb_PAA, (<b>c</b>) InSb_PVDF, and (<b>d</b>) InSb–C_PAA.</p> Full article ">Figure 8
<p>Illustration of the InSb–C_PAA reaction mechanism.</p> Full article ">
14 pages, 5490 KiB  
Article
Microwave-Assisted Rapid Synthesis of NH4V4O10 Layered Oxide: A High Energy Cathode for Aqueous Rechargeable Zinc Ion Batteries
by Seokhun Kim, Vaiyapuri Soundharrajan, Sungjin Kim, Balaji Sambandam, Vinod Mathew, Jang-Yeon Hwang and Jaekook Kim
Nanomaterials 2021, 11(8), 1905; https://doi.org/10.3390/nano11081905 - 24 Jul 2021
Cited by 17 | Viewed by 4343
Abstract
Aqueous rechargeable zinc ion batteries (ARZIBs) have gained wide interest in recent years as prospective high power and high energy devices to meet the ever-rising commercial needs for large-scale eco-friendly energy storage applications. The advancement in the development of electrodes, especially cathodes for [...] Read more.
Aqueous rechargeable zinc ion batteries (ARZIBs) have gained wide interest in recent years as prospective high power and high energy devices to meet the ever-rising commercial needs for large-scale eco-friendly energy storage applications. The advancement in the development of electrodes, especially cathodes for ARZIB, is faced with hurdles related to the shortage of host materials that support divalent zinc storage. Even the existing materials, mostly based on transition metal compounds, have limitations of poor electrochemical stability, low specific capacity, and hence apparently low specific energies. Herein, NH4V4O10 (NHVO), a layered oxide electrode material with a uniquely mixed morphology of plate and belt-like particles is synthesized by a microwave method utilizing a short reaction time (~0.5 h) for use as a high energy cathode for ARZIB applications. The remarkable electrochemical reversibility of Zn2+/H+ intercalation in this layered electrode contributes to impressive specific capacity (417 mAh g?1 at 0.25 A g?1) and high rate performance (170 mAh g?1 at 6.4 A g?1) with almost 100% Coulombic efficiencies. Further, a very high specific energy of 306 Wh Kg?1 at a specific power of 72 W Kg?1 was achieved by the ARZIB using the present NHVO cathode. The present study thus facilitates the opportunity for developing high energy ARZIB electrodes even under short reaction time to explore potential materials for safe and sustainable green energy storage devices. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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Graphical abstract

Graphical abstract
Full article ">Figure 1
<p>(<b>a</b>) Powder XRD pattern of NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub> (NHVO) cathode prepared by a microwave reaction, (<b>b</b>) Low and (<b>c</b>) high magnification FE-SEM images of the NHVO electrode.</p> Full article ">Figure 2
<p>(<b>a</b>) Low and (<b>b</b>) high resolution TEM images and (<b>c</b>) corresponding SAED pattern of the prepared NHVO electrode. (<b>d</b>–<b>h</b>) FE-TEM and elemental mapping images recorded from the area shown in (<b>b</b>). The colored regions correspond to specific elements.</p> Full article ">Figure 3
<p>(<b>a</b>) DLS result for the prepared NHVO (<b>b</b>) N<sub>2</sub> adsorption/desorption plot and (<b>c</b>) corresponding pore-size distribution plot for the prepared NHVO sample.</p> Full article ">Figure 4
<p>(<b>a</b>) The initial five CV profiles of NHVO electrode in ARZIBs, (<b>b</b>) Galvanostatic discharge/charge profiles at 250 mA g<sup>−1</sup> current density for initial two cycles and (<b>c</b>) corresponding cyclability configuration of NHVO at the same applied current density.</p> Full article ">Figure 5
<p>(<b>a</b>) Cycle lifespan of the NHVO electrode under prolonged cycling of 1500 cycles at 2.5 A g<sup>−1</sup> (<b>b</b>) Rate performance at different progressively varying (increasing and decreasing alternatively) current densities for the NHVO cathode for ARZIB applications. (<b>c</b>) Galvanostatic discharge/charge profiles corresponding to one set of progressively increasing current density from 100 mA g<sup>−1</sup> to 6.4 A g<sup>−1</sup>.</p> Full article ">Figure 6
<p>Ex-situ XRD patterns of the NHVO electrode recovered at different conditions.</p> Full article ">Figure 7
<p>(<b>a</b>) Ragone plot for the present NHVO along with reported vanadium-based cathode materials for ARZIBs. (<b>b</b>) CV curves at various scan rates between 0.1 and 0.5 mV s<sup>−1</sup>. (<b>c</b>) Surface-controlled capacitive contribution (shaded area) to the overall charge storage at 0.1 mV s<sup>–1</sup>. (<b>d</b>) Ratio of surface-controlled and diffusion-induced contribution to the charge capacity depicted at different scan rates.</p> Full article ">
16 pages, 6590 KiB  
Article
Graphene Nanosheet-Wrapped Mesoporous La0.8Ce0.2Fe0.5Mn0.5O3 Perovskite Oxide Composite for Improved Oxygen Reaction Electro-Kinetics and Li-O2 Battery Application
by Chelladurai Karuppiah, Chao-Nan Wei, Natarajan Karikalan, Zong-Han Wu, Balamurugan Thirumalraj, Li-Fan Hsu, Srinivasan Alagar, Shakkthivel Piraman, Tai-Feng Hung, Ying-Jeng Jame Li and Chun-Chen Yang
Nanomaterials 2021, 11(4), 1025; https://doi.org/10.3390/nano11041025 - 16 Apr 2021
Cited by 12 | Viewed by 3071
Abstract
A novel design and synthesis methodology is the most important consideration in the development of a superior electrocatalyst for improving the kinetics of oxygen electrode reactions, such as the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) in Li-O2 battery [...] Read more.
A novel design and synthesis methodology is the most important consideration in the development of a superior electrocatalyst for improving the kinetics of oxygen electrode reactions, such as the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) in Li-O2 battery application. Herein, we demonstrate a glycine-assisted hydrothermal and probe sonication method for the synthesis of a mesoporous spherical La0.8Ce0.2Fe0.5Mn0.5O3 perovskite particle and embedded graphene nanosheet (LCFM(8255)-gly/GNS) composite and evaluate its bifunctional ORR/OER kinetics in Li-O2 battery application. The physicochemical characterization confirms that the as-formed LCFM(8255)-gly perovskite catalyst has a highly crystalline structure and mesoporous morphology with a large specific surface area. The LCFM(8255)-gly/GNS composite hybrid structure exhibits an improved onset potential and high current density toward ORR/OER in both aqueous and non-aqueous electrolytes. The LCFM(8255)-gly/GNS composite cathode (ca. 8475 mAh g?1) delivers a higher discharge capacity than the La0.5Ce0.5Fe0.5Mn0.5O3-gly/GNS cathode (ca. 5796 mAh g?1) in a Li-O2 battery at a current density of 100 mA g?1. Our results revealed that the composite’s high electrochemical activity comes from the synergism of highly abundant oxygen vacancies and redox-active sites due to the Ce and Fe dopant in LaMnO3 and the excellent charge transfer characteristics of the graphene materials. The as-developed cathode catalyst performed appreciable cycle stability up to 55 cycles at a limited capacity of 1000 mAh g?1 based on conventional glass fiber separators. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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Figure 1

Figure 1
<p>SEM images of (<b>A</b>) LCFM(5555)-no gly, (<b>B</b>) LCFM(5555)-gly and (<b>C</b>) LCFM(8255)-gly. (<b>D</b>) XRD patterns of (<b>a</b>) LCFM(5555)-no gly, (<b>b</b>) LCFM(5555)-gly and (<b>c</b>) LCFM(8255)-gly.</p> Full article ">Figure 2
<p>(<b>A</b>–<b>C</b>) N<sub>2</sub> adsorption–desorption and (<b>D</b>–<b>F</b>) pore-size distribution curves of LCFM(5555)-no gly, LCFM(5555)-gly and LCFM(8255)-gly catalyst samples.</p> Full article ">Figure 3
<p>(<b>A</b>). XPS survey for elements present in LCFM(8255)-gly, deconvoluted XPS curves of (<b>B</b>) La 3d, (<b>C</b>) Ce 3d, (<b>D</b>) Fe 2p, (<b>E</b>) Mn 2p and (<b>F</b>) O 1s peak in LCFM(8255)-gly sample.</p> Full article ">Figure 4
<p>(<b>A</b>,<b>B</b>) TEM images of LCFM(8255)-gly and (<b>C</b>,<b>D</b>) LCFM(8255)-gly/GNS composite. (<b>E</b>) XRD patterns and (<b>F</b>) micro-Raman spectra of (<b>a</b>) LCFM(8255)-gly, (<b>b</b>) GNS and (<b>c</b>) LCFM(8255)-gly/GNS composite.</p> Full article ">Figure 5
<p>(<b>A</b>). CVs and (<b>B</b>). LSVs for ORR kinetics at various electrodes recorded in O<sub>2</sub>-saturated 0.1 M KOH; Scan rate: 20 mV s<sup>−1</sup>; Rotation speed: 1600 rpm for LSV measurements. (<b>C</b>). LSVs of RDE measurements using LCFM(8255)-gly/GNS composite electrode at various rotation speeds from 400 to 2500 rpm in O<sub>2</sub>-saturated 0.1 M KOH; Scan rate: 20 mV s<sup>−1</sup>, (<b>D</b>). Koutecky–Levich plot of j<sup>−1</sup> vs. ω<sup>−1/2</sup>.</p> Full article ">Figure 6
<p>(<b>A</b>). LSVs for ORR and OER kinetics at various electrodes recorded in O<sub>2</sub>-saturated 0.1 M KOH; Scan rate: 20 mV s<sup>−1</sup>; Rotation speed: 1600 rpm, (<b>B</b>). CVs for ORR and OER kinetics using (<b>a</b>) GNS, (<b>b</b>) LCFM(5555)-gly/GNS and (<b>c</b>) LCFM(8255)-gly/GNS-based Li-O<sub>2</sub> cells in 1 M LiTFSI-TEGDME + 0.5 M LiI at a scan rate of 1 mV s<sup>−1</sup>, (<b>C</b>). EIS data for electron transfer properties of (<b>a</b>) GNS, (<b>b</b>) LCFM(5555)-gly/GNS and (<b>c</b>) LCFM(8255)-gly/GNS-based Li-O<sub>2</sub> cells.</p> Full article ">Figure 7
<p>(<b>A</b>) Initial discharge curves of (<b>a</b>) GNS, (<b>b</b>) LCFM(5555)-gly/GNS and (<b>c</b>) LCFM(8255)-gly/GNS-based Li-O<sub>2</sub> cells at a current density of 100 mA g<sup>−1</sup>. Discharge–charge curves of (<b>a</b>) GNS, (<b>b</b>) LCFM(5555)-gly/GNS and (<b>c</b>) LCFM(8255)-gly/GNS-based Li-O<sub>2</sub> cells for (<b>B</b>) overpotential difference and (<b>C</b>–<b>E</b>) cycling stability analysis. (<b>F</b>) Cycle life of (<b>a</b>) GNS, (<b>b</b>) LCFM(5555)-gly/GNS and (<b>c</b>) LCFM(8255)-gly/GNS-based Li-O<sub>2</sub> cells. Current density: 100 mA g<sup>−1</sup>; Limited discharge capacity: 1000 mAh g<sup>−1</sup>; Electrolyte: 1 M LiTFSI-TEGDME + 0.5 M LiI.</p> Full article ">Scheme 1
<p>(<b>i</b>) Schematic for the synthesis of LCFM(8255)-gly perovskites. (<b>ii</b>) Schematic for the synthesis of LCFM(8255)-gly/GNS composite.</p> Full article ">
9 pages, 4521 KiB  
Article
A Facile Chemical Method Enabling Uniform Zn Deposition for Improved Aqueous Zn-Ion Batteries
by Congcong Liu, Qiongqiong Lu, Ahmad Omar and Daria Mikhailova
Nanomaterials 2021, 11(3), 764; https://doi.org/10.3390/nano11030764 - 18 Mar 2021
Cited by 28 | Viewed by 4818
Abstract
Rechargeable aqueous Zn-ion batteries (ZIBs) have gained great attention due to their high safety and the natural abundance of Zn. Unfortunately, the Zn metal anode suffers from dendrite growth due to nonuniform deposition during the plating/stripping process, leading to a sudden failure of [...] Read more.
Rechargeable aqueous Zn-ion batteries (ZIBs) have gained great attention due to their high safety and the natural abundance of Zn. Unfortunately, the Zn metal anode suffers from dendrite growth due to nonuniform deposition during the plating/stripping process, leading to a sudden failure of the batteries. Herein, Cu coated Zn (Cu–Zn) was prepared by a facile pretreatment method using CuSO4 aqueous solution. The Cu coating transformed into an alloy interfacial layer with a high affinity for Zn, which acted as a nucleation site to guide the uniform Zn nucleation and plating. As a result, Cu–Zn demonstrated a cycling life of up to 1600 h in the symmetric cells and endowed a stable cycling performance with a capacity of 207 mAh g?1 even after 1000 cycles in the full cells coupled with a V2O5-based cathode. This work provides a simple and effective strategy to enable uniform Zn deposition for improved ZIBs. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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Figure 1

Figure 1
<p>SEM images and optical images (insets) of (<b>a</b>) bare Zn foil and (<b>b</b>) Cu–Zn foil, (<b>c</b>) cross-section SEM images of Cu–Zn foil, (<b>d</b>) high resolution Cu 2p XP spectrum measured on Cu–Zn foil.</p> Full article ">Figure 2
<p>(<b>a</b>) SEM image and (<b>b</b>,<b>c</b>) the corresponding elemental mappings of Cu–Zn.</p> Full article ">Figure 3
<p>Long-term galvanostatic discharge/charge profiles of symmetric cells with bare Zn and Cu–Zn at current density of (<b>a</b>) 0.2 mA cm<sup>−2</sup>, (<b>b</b>) 0.5 mA cm<sup>−2</sup>, and (<b>c</b>) 1 mA cm<sup>−2</sup>.</p> Full article ">Figure 4
<p>(<b>a</b>) The voltage-time curves during Zn nucleation and deposition on Zn and Cu–Zn at 1 mA cm<sup>−2</sup>, SEM images of (<b>b</b>) Zn and (<b>c</b>) Cu–Zn after Zn-depositing with a capacity of 2 mAh cm<sup>−2</sup> at current density of 1 mA cm<sup>−2</sup>.</p> Full article ">Figure 5
<p>SEM images of (<b>a</b>) Zn and (<b>b</b>) Cu–Zn after 30 cycles at a current density of 5 mA cm<sup>−2</sup> with a capacity of 1 mAh cm<sup>−2</sup>.</p> Full article ">Figure 6
<p>(<b>a</b>) SEM image and (<b>b</b>,<b>c</b>) corresponding elemental mappings of Cu–Zn after 50 cycles at current density of 5 mA cm<sup>−2</sup> with a capacity of 1 mAh cm<sup>−2</sup>.</p> Full article ">Figure 7
<p>XRD pattern of Cu–Zn (<b>a</b>) after 1 cycle and (<b>b</b>) after 100 cycles at current density of 5 mA cm<sup>−2</sup> with a capacity of 1 mAh cm<sup>−2</sup>. ★ represents the XRD peak of CuZn<sub>5</sub>.</p> Full article ">Figure 8
<p>(<b>a</b>) Rate performance of V<sub>2</sub>O<sub>5</sub>-PEDOT//Zn and V<sub>2</sub>O<sub>5</sub>-PEDOT//Cu-Zn, (<b>b</b>) charge/discharge curves of V<sub>2</sub>O<sub>5</sub>-PEDOT//Cu–Zn at different current densities, (<b>c</b>) cycling performance of V<sub>2</sub>O<sub>5</sub>-PEDOT//Zn and V<sub>2</sub>O<sub>5</sub>-PEDOT//Cu–Zn at a current density of 5 A∙g<sup>−1</sup>.</p> Full article ">
13 pages, 4220 KiB  
Article
Ag Nanoparticle-Decorated MoS2 Nanosheets for Enhancing Electrochemical Performance in Lithium Storage
by Thang Phan Nguyen and Il Tae Kim
Nanomaterials 2021, 11(3), 626; https://doi.org/10.3390/nano11030626 - 3 Mar 2021
Cited by 26 | Viewed by 3944
Abstract
Metallic phase 1T MoS2 is a well-known potential anode for enhancing the electrochemical performance of lithium-ion batteries owing to its mechanical/chemical stability and high conductivity. However, during the lithiation/delithiation process, MoS2 nanosheets (NSs) tend to restack to form bulky structures that [...] Read more.
Metallic phase 1T MoS2 is a well-known potential anode for enhancing the electrochemical performance of lithium-ion batteries owing to its mechanical/chemical stability and high conductivity. However, during the lithiation/delithiation process, MoS2 nanosheets (NSs) tend to restack to form bulky structures that deteriorate the cycling performance of bare MoS2 anodes. In this study, we prepared Ag nanoparticle (NP)-decorated 1T MoS2 NSs via a liquid exfoliation method with lithium intercalation and simple reduction of AgNO3 in NaBH4. Ag NPs were uniformly distributed on the MoS2 surface with the assistance of 3-mercapto propionic acid. Ag NPs with the size of a few nanometers enhanced the conductivity of the MoS2 NS and improved the electrochemical performance of the MoS2 anode. Specifically, the anode designated as Ag3@MoS2 (prepared with AgNO3 and MoS2 in a weight ratio of 1:10) exhibited the best cycling performance and delivered a reversible specific capacity of 510 mAh·g?1 (approximately 73% of the initial capacity) after 100 cycles. Moreover, the rate performance of this sample had a remarkable recovery capacity of ~100% when the current decreased from 1 to 0.1 A·g?1. The results indicate that the Ag nanoparticle-decorated 1T MoS2 can be employed as a high-rate capacity anode in lithium-ion storage applications. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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Figure 1
<p>(<b>a</b>,<b>b</b>) Scanning electron microscopy (SEM) images of MoS<sub>2</sub> nanosheets (NSs); (<b>c</b>) illustration of Ag-decorated MoS<sub>2</sub> NS; SEM images of (<b>d</b>) Ag1@MoS<sub>2</sub>, (<b>e</b>) Ag2@MoS<sub>2</sub>, and (<b>f</b>) Ag3@MoS<sub>2</sub> NSs.</p> Full article ">Figure 2
<p>X-ray diffraction patterns of bulk MoS<sub>2</sub>, Li<sub>x</sub>MoS<sub>2</sub>, and Ag3@MoS<sub>2</sub> materials.</p> Full article ">Figure 3
<p>(<b>a</b>,<b>b</b>) Transmission electron microscopy (TEM) image and element mapping images of Ag3@MoS<sub>2</sub> materials; (<b>c</b>,<b>f</b>) TEM, high-resolution TEM (HRTEM) with inset selected area electron diffraction (SAED) pattern of MoS<sub>2</sub> NS; (<b>d</b>,<b>e</b>) TEM, HRTEM with inset SAED pattern of Ag3@MoS<sub>2</sub> materials.</p> Full article ">Figure 4
<p>Cyclic voltammetry (CV) profiles of (<b>a</b>) MoS<sub>2</sub> NSs, (<b>b</b>) Ag1@MoS<sub>2</sub>, (<b>c</b>) Ag2@MoS<sub>2</sub> and (<b>d</b>) Ag3@MoS<sub>2</sub> anodes, over the initial three cycles.</p> Full article ">Figure 5
<p>Initial voltage profiles of (<b>a</b>) MoS<sub>2</sub> NSs, (<b>b</b>) Ag1@MoS<sub>2</sub>, (<b>c</b>) Ag2@MoS<sub>2,</sub> and (<b>d</b>) Ag3@MoS<sub>2</sub> anodes.</p> Full article ">Figure 6
<p>Cyclic performance of (<b>a</b>) MoS<sub>2</sub> NSs, (<b>b</b>) Ag1@MoS<sub>2</sub>, (<b>c</b>) Ag2@MoS<sub>2</sub>, and (<b>d</b>) Ag3@MoS<sub>2</sub> anodes.</p> Full article ">Figure 7
<p>Rate performance of (<b>a</b>) MoS<sub>2</sub> NSs, (<b>b</b>) Ag1@MoS<sub>2</sub>, (<b>c</b>) Ag3@MoS<sub>2</sub>, and (<b>d</b>) Nyquist plots of MoS<sub>2</sub> without/with Ag-decorated anodes.</p> Full article ">
13 pages, 3496 KiB  
Article
Self-Assembled Few-Layered MoS2 on SnO2 Anode for Enhancing Lithium-Ion Storage
by Thang Phan Nguyen and Il Tae Kim
Nanomaterials 2020, 10(12), 2558; https://doi.org/10.3390/nano10122558 - 20 Dec 2020
Cited by 21 | Viewed by 3538
Abstract
SnO2 nanoparticles (NPs) have been used as reversible high-capacity anode materials in lithium-ion batteries, with reversible capacities reaching 740 mAh·g−1. However, large SnO2 NPs do not perform well in charge–discharge cycling. In this work, we report the incorporation of [...] Read more.
SnO2 nanoparticles (NPs) have been used as reversible high-capacity anode materials in lithium-ion batteries, with reversible capacities reaching 740 mAh·g−1. However, large SnO2 NPs do not perform well in charge–discharge cycling. In this work, we report the incorporation of MoS2 nanosheet (NS) layers with SnO2 NPs. SnO2 NPs of ~5 nm in diameter synthesized by a facile hydrothermal precipitation method. Meanwhile, MoS2 NSs of a few hundreds of nanometers to a few micrometers in lateral size were produced by top-down chemical exfoliation. The self-assembly of the MoS2 NS layer on the gas–liquid interface was first demonstrated to achieve up to 80% coverage of the SnO2 NP anode surface. The electrochemical properties of the pure SnO2 NPs and MoS2-covered SnO2 NP anodes were investigated. The results showed that the SnO2 electrode with a single-layer MoS2 NS film exhibited better electrochemical performance than the pure SnO2 anode in lithium storage applications. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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<p>Illustration and photographs of self-assembled MoS<sub>2</sub> nanosheet (NS) on Cu substrate.</p> Full article ">Figure 2
<p>Scanning electron microscope (SEM) images of (<b>a</b>,<b>b</b>) SnO<sub>2</sub> nanoparticle (NP) powder, (<b>c</b>,<b>d</b>) single-layer MoS<sub>2</sub> NS thin film on Cu electrode, and (<b>e</b>,<b>f</b>) M1SnO<sub>2</sub> anode.</p> Full article ">Figure 3
<p>X-ray diffraction (XRD) patterns of (<b>a</b>) SnO<sub>2</sub> NPs and M3SnO<sub>2</sub> anode and (<b>b</b>) lithium-ion intercalated and exfoliated MoS<sub>2</sub> nanosheet.</p> Full article ">Figure 4
<p>(<b>a</b>) Transmission electron microscope (TEM) image of SnO<sub>2</sub> NP; energy-dispersive X-ray spectroscopy (EDS) mapping of the elements (<b>b</b>) O and (<b>c</b>) Sn; (<b>d</b>) high-resolution TEM (HRTEM) image of SnO<sub>2</sub> NP with inset selected-area electron diffraction (SAED) pattern; (<b>e</b>) exfoliated MoS<sub>2</sub> NS with inset SAED pattern.</p> Full article ">Figure 5
<p>Cyclic voltammetry (CV) profiles of (<b>a</b>) SnO<sub>2</sub> NS and (<b>b</b>–<b>d</b>) M1/M2/M3SnO<sub>2</sub> anodes over three cycles.</p> Full article ">Figure 6
<p>Galvanostatic charge–discharge profiles of (<b>a</b>) SnO<sub>2</sub> NS and (<b>b</b>–<b>d</b>) M1/M2/M3SnO<sub>2</sub> anodes for the initial three cycles.</p> Full article ">Figure 7
<p>Cyclic performances and Nyquist plots of (<b>a</b>) SnO<sub>2</sub> NPs and (<b>b</b>–<b>d</b>) M1/M2/M3SnO<sub>2</sub> anodes.</p> Full article ">Figure 8
<p>Rate cycling performance of (<b>a</b>) bare SnO<sub>2</sub> electrode and (<b>b</b>) M1SnO<sub>2</sub> electrode at different current rates.</p> Full article ">Figure 9
<p>SEM images of (<b>a</b>,<b>d</b>) SnO<sub>2</sub> electrode, (<b>b</b>,<b>e</b>) M1SnO<sub>2</sub> electrode and (<b>c</b>,<b>f</b>) M3SnO<sub>2</sub> electrode after 10 cycles at different magnifications.</p> Full article ">

Review

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32 pages, 10640 KiB  
Review
Zn Metal Anodes for Zn-Ion Batteries in Mild Aqueous Electrolytes: Challenges and Strategies
by Vo Pham Hoang Huy, Luong Trung Hieu and Jaehyun Hur
Nanomaterials 2021, 11(10), 2746; https://doi.org/10.3390/nano11102746 - 17 Oct 2021
Cited by 47 | Viewed by 7756
Abstract
Over the past few years, rechargeable aqueous Zn-ion batteries have garnered significant interest as potential alternatives for lithium-ion batteries because of their low cost, high theoretical capacity, low redox potential, and environmentally friendliness. However, several constraints associated with Zn metal anodes, such as [...] Read more.
Over the past few years, rechargeable aqueous Zn-ion batteries have garnered significant interest as potential alternatives for lithium-ion batteries because of their low cost, high theoretical capacity, low redox potential, and environmentally friendliness. However, several constraints associated with Zn metal anodes, such as the growth of Zn dendrites, occurrence of side reactions, and hydrogen evolution during repeated stripping/plating processes result in poor cycling life and low Coulombic efficiency, which severely impede further advancements in this technology. Despite recent efforts and impressive breakthroughs, the origin of these fundamental obstacles remains unclear and no successful strategy that can address these issues has been developed yet to realize the practical applications of rechargeable aqueous Zn-ion batteries. In this review, we have discussed various issues associated with the use of Zn metal anodes in mildly acidic aqueous electrolytes. Various strategies, including the shielding of the Zn surface, regulating the Zn deposition behavior, creating a uniform electric field, and controlling the surface energy of Zn metal anodes to repress the growth of Zn dendrites and the occurrence of side reactions, proposed to overcome the limitations of Zn metal anodes have also been discussed. Finally, the future perspectives of Zn anodes and possible design strategies for developing highly stable Zn anodes in mildly acidic aqueous environments have been discussed. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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<p>Major limitations of Zn metal anodes for battery applications.</p> Full article ">Figure 2
<p>(<b>a</b>) Brief summary of recent reviews on Zn metal anodes for AZIBs [<a href="#B45-nanomaterials-11-02746" class="html-bibr">45</a>,<a href="#B50-nanomaterials-11-02746" class="html-bibr">50</a>,<a href="#B51-nanomaterials-11-02746" class="html-bibr">51</a>,<a href="#B52-nanomaterials-11-02746" class="html-bibr">52</a>,<a href="#B53-nanomaterials-11-02746" class="html-bibr">53</a>,<a href="#B54-nanomaterials-11-02746" class="html-bibr">54</a>,<a href="#B55-nanomaterials-11-02746" class="html-bibr">55</a>,<a href="#B56-nanomaterials-11-02746" class="html-bibr">56</a>,<a href="#B57-nanomaterials-11-02746" class="html-bibr">57</a>,<a href="#B58-nanomaterials-11-02746" class="html-bibr">58</a>,<a href="#B59-nanomaterials-11-02746" class="html-bibr">59</a>,<a href="#B60-nanomaterials-11-02746" class="html-bibr">60</a>,<a href="#B61-nanomaterials-11-02746" class="html-bibr">61</a>,<a href="#B62-nanomaterials-11-02746" class="html-bibr">62</a>,<a href="#B63-nanomaterials-11-02746" class="html-bibr">63</a>,<a href="#B64-nanomaterials-11-02746" class="html-bibr">64</a>], (<b>b</b>) a typical full cell battery configuration of AZIBs in a mildly acidic aqueous electrolyte. (<b>c</b>) The number of publications on AZIBs from 2010 to 2021 (search from Google Scholar; search time: 7 September 2021).</p> Full article ">Figure 3
<p>(<b>a</b>) Gravimetric capacity, volumetric capacity, and price of typical metal anodes. Reprinted with permission from Liang et al. [<a href="#B58-nanomaterials-11-02746" class="html-bibr">58</a>]. Copyright 2021 Wiley-VCH GmbH. (<b>b</b>) Pourbaix diagram of water. Reprinted with permission from Zeng et al. [<a href="#B75-nanomaterials-11-02746" class="html-bibr">75</a>]. Copyright 2019 Elsevier B.V. (<b>c</b>) Pourbaix diagram of the Zn/H<sub>2</sub>O system with HER overpotential considerations. Reprinted with permission from Wippermann et al. [<a href="#B76-nanomaterials-11-02746" class="html-bibr">76</a>]. Copyright 1990 Elsevier Ltd.</p> Full article ">Figure 4
<p>Schematic illustration of the phenomena observed on Zn electrodes in (<b>a</b>) alkaline and (<b>b</b>) mild aqueous electrolytes.</p> Full article ">Figure 5
<p>Components of the AZIB in coin cell assembly.</p> Full article ">Figure 6
<p>Cycling performance of Zn/Zn symmetric cells tested at (<b>a</b>) 2 mA cm<sup>−2</sup> and 2 mAh cm<sup>−2</sup>, (<b>b</b>) 5 mA cm<sup>−2</sup> and 5 mAh cm<sup>−2</sup>, (<b>c</b>) cycling performance at 0.3 A g<sup>−1</sup>. Reprinted with permission from Zhen et al. [<a href="#B83-nanomaterials-11-02746" class="html-bibr">83</a>]. (<b>d</b>) The standard potentials of redox couple in some reported cathode materials in ZIB systems. Reprinted with permission from [<a href="#B84-nanomaterials-11-02746" class="html-bibr">84</a>]. Copyright 2021 Wiley-VCH GmbH.</p> Full article ">Figure 7
<p>(<b>a</b>) Energy barrier for the Zn nucleation process, (<b>b</b>) voltage profile during Zn deposition. Reprinted with permission from Pei et al. [<a href="#B87-nanomaterials-11-02746" class="html-bibr">87</a>]. Copyright 2017 American Chemical Society. Simulation of (<b>c</b>) electric field and (<b>d</b>) ion distribution on the Zn anode surface under different dendrite formation conditions: flat surface, small dendritic seeds, and large dendritic seeds. Reprinted with permission from [<a href="#B90-nanomaterials-11-02746" class="html-bibr">90</a>]. Copyright 2019 WILEY-VCH Verlag GmbH&amp;Co. KgaA, Weinheim.</p> Full article ">Figure 8
<p>SEM images of (<b>a</b>,<b>b</b>) a fresh filter paper, and (<b>c</b>,<b>d</b>) a cycled bare Zn foil. The pores in filter papers act as “highways” for electrolyte transport, like the (<b>e</b>) pores in water-permeable bricks. Reprinted with permission from [<a href="#B92-nanomaterials-11-02746" class="html-bibr">92</a>]. Copyright 2018 WILEY-VCH Verlag GmbH&amp;Co. KgaA, Weinheim.</p> Full article ">Figure 9
<p>SEM images of a Zn electrode (<b>a</b>) before and (<b>b</b>) after 30 days of operation, (<b>c</b>) Chemical corrosion of the Zn metal electrode in a ZnSO<sub>4</sub> electrolyte. (<b>d</b>) cross-section SEM and EDS elemental mapping results of the electrode operated for 30 days. Reprinted with permission from Cai et al. [<a href="#B101-nanomaterials-11-02746" class="html-bibr">101</a>]. Copyright 2020 Elsevier B.V.</p> Full article ">Figure 10
<p>Modification strategies for enhancing the electrochemical performance of Zn metal anodes.</p> Full article ">Figure 11
<p>Schematic illustration of the ALD process; (<b>a</b>) the substrate surface is naturally functionalized or treated to be functionalized; (<b>b</b>) precursor A reacts with the surface after being pulsed; (<b>c</b>) an inert carrier gas is used to remove the excess precursor and by-products; (<b>d</b>) the surface reacts with the pulsed precursor B; (<b>e</b>) the inert carrier gas is used to remove excess precursor and byproducts; (<b>f</b>) repeat steps 2–5 until the desired material thickness is achieved. Reprinted with permission from Johnson et al. [<a href="#B114-nanomaterials-11-02746" class="html-bibr">114</a>]. Copyright 2014 Elsevier Ltd.</p> Full article ">Figure 12
<p>(<b>a</b>) Schematic illustration of Zn corrosion and H<sub>2</sub> evolution under repeated plating/stripping cycles, (<b>b</b>) stable deposition/stripping process with a thin layer of TiO<sub>2</sub> coated on the Zn anode, (<b>c</b>) symmetric cell performances of pristine Zn and TiO<sub>2</sub>@Zn, (<b>d</b>,<b>e</b>) ex-situ SEM images of the (<b>d</b>) TiO<sub>2</sub>@Zn and (<b>e</b>) pristine Zn anodes, (<b>f</b>) full cell performances of ALD TiO<sub>2</sub>@Zn-MnO<sub>2</sub> and Zn-MnO<sub>2</sub> at 100 mA g<sup>−1</sup>, (<b>g</b>) CEs of the ALD TiO<sub>2</sub>@Zn-MnO<sub>2</sub> and Zn-MnO<sub>2</sub> full cells at 100 mA g<sup>−1</sup>. Reprinted with permission from [<a href="#B116-nanomaterials-11-02746" class="html-bibr">116</a>]. Copyright 2018 WILEY-VCH Verlag GmbH&amp;Co. KgaA, Weinheim.</p> Full article ">Figure 13
<p>(<b>a</b>) Schematic illustration of the fabrication of the Cu-Zn electrode. (<b>b</b>) linear polarization curve of the Cu/Zn electrode in a 3 M ZnSO<sub>4</sub> electrolyte. Reprinted with permission from Cai et al. [<a href="#B101-nanomaterials-11-02746" class="html-bibr">101</a>]. Copyright 2020 Elsevier B.V. (<b>c</b>) Photographs depicting the preparation of the Zn/rGO. Zn plate (<b>d</b>) before and (<b>e</b>) after coating the rGO film. Reprinted with permission from Xia et al. [<a href="#B119-nanomaterials-11-02746" class="html-bibr">119</a>]. Copyright 2019 Elsevier B.V.</p> Full article ">Figure 14
<p>Schematics for the stripping/plating processes of (<b>a</b>) bare Zn and (<b>b</b>) ZrO<sub>2</sub>-coated Zn. Voltage profiles of bare Zn and ZrO<sub>2</sub>-coated Zn in a symmetric cell at (<b>c</b>) 0.25 mA cm<sup>−2</sup> for 0.125 mAh cm<sup>−2</sup> and (<b>d</b>) 5 mA cm<sup>−2</sup> for 1 mAh cm<sup>−2</sup>. Reprinted with permission from Liang et al. [<a href="#B121-nanomaterials-11-02746" class="html-bibr">121</a>]. Copyright 2020 WILEY-VCH Verlag GmbH&amp;Co. KgaA, Weinheim.</p> Full article ">Figure 15
<p>(<b>a</b>) Schematic illustration of morphology evolution for bare and nano-CaCO<sub>3</sub>-coated Zn foils during Zn stripping/plating cycling, (<b>b</b>) charge-discharge profiles and (<b>c</b>) full cell performance of nano-CaCO<sub>3</sub>-coated Zn foil and bare Zn foil. Reprinted with permission from [<a href="#B92-nanomaterials-11-02746" class="html-bibr">92</a>]. Copyright 2018 WILEY-VCH Verlag GmbH&amp;Co. KgaA, Weinheim.</p> Full article ">Figure 16
<p>(<b>a</b>) Schematic illustration of the β- and α-PVDF coating processes, (<b>b</b>) long-term profiles of β-PVDF@Zn (red), α-PVDF@Zn (blue), and bare Zn (black) with symmetrical cells at a current density of (<b>b</b>) 0.25–0.05 mAh cm<sup>−2</sup>, (<b>c</b>) 1.5–0.3 mAh cm<sup>−2</sup>. Reprinted with permission from Hieu et al. [<a href="#B123-nanomaterials-11-02746" class="html-bibr">123</a>]. Copyright 2021 Elsevier B.V.</p> Full article ">Figure 17
<p>Schematic of Zn ion transport during Zn stripping/plating for (<b>a</b>) bare Zn, and (<b>b</b>) BTO@ Zn foil. Cyclic performances of the symmetric cells with Zn and BTO@Zn at (<b>c</b>) 1 mA cm<sup>−2</sup> (1 mAh cm<sup>−2</sup>), and (<b>d</b>) 5 mA cm<sup>−2</sup> (2.5 mAh cm<sup>−2</sup>). Reprinted with permission from [<a href="#B125-nanomaterials-11-02746" class="html-bibr">125</a>].</p> Full article ">Figure 18
<p>(<b>a</b>) Schematic illustration of Zn deposition on CM@CuO and CM. SEM images of CM@CuO@Zn with the capacities of (<b>b</b>) 1 and (<b>c</b>) 5 mAh cm<sup>−2</sup>. SEM images of CM@Zn with the capacities of (<b>d</b>) 1 and (<b>e</b>) 5 mAh cm<sup>−2</sup>. Reprinted with permission from [<a href="#B126-nanomaterials-11-02746" class="html-bibr">126</a>]. Copyright 2020 Wiley-VCH GmbH.</p> Full article ">
25 pages, 2219 KiB  
Review
Review of ZnO Binary and Ternary Composite Anodes for Lithium-Ion Batteries
by Vu Khac Hoang Bui, Tuyet Nhung Pham, Jaehyun Hur and Young-Chul Lee
Nanomaterials 2021, 11(8), 2001; https://doi.org/10.3390/nano11082001 - 4 Aug 2021
Cited by 26 | Viewed by 5257
Abstract
To enhance the performance of lithium-ion batteries, zinc oxide (ZnO) has generated interest as an anode candidate owing to its high theoretical capacity. However, because of its limitations such as its slow chemical reaction kinetics, intense capacity fading on potential cycling, and low [...] Read more.
To enhance the performance of lithium-ion batteries, zinc oxide (ZnO) has generated interest as an anode candidate owing to its high theoretical capacity. However, because of its limitations such as its slow chemical reaction kinetics, intense capacity fading on potential cycling, and low rate capability, composite anodes of ZnO and other materials are manufactured. In this study, we introduce binary and ternary composites of ZnO with other metal oxides (MOs) and carbon-based materials. Most ZnO-based composite anodes exhibit a higher specific capacity, rate performance, and cycling stability than a single ZnO anode. The synergistic effects between ZnO and the other MOs or carbon-based materials can explain the superior electrochemical characteristics of these ZnO-based composites. This review also discusses some of their current limitations. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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<p>Published articles/patents related to MOs and their composites for LIB applications. Data collected from Google Scholar (<a href="https://scholar.google.com" target="_blank">https://scholar.google.com</a>) (accessed on 15 June 2021) database with keyword: “Metal oxide lithium-ion batteries”.</p> Full article ">Figure 2
<p>Synthesis of intermixed (<b>a</b>) and nanolaminated (<b>b</b>) ZnO–SnO<sub>2</sub> composite films by ALD. Reprinted with permission from [<a href="#B6-nanomaterials-11-02001" class="html-bibr">6</a>]. Copyright 2019, Elsevier.</p> Full article ">Figure 3
<p>Scheme of ZZFO and ZFO synthesis process. Reprinted with permission from [<a href="#B71-nanomaterials-11-02001" class="html-bibr">71</a>]. Copyright 2015, John Wiley and Sons.</p> Full article ">Figure 4
<p>Scheme of synthesis of ZnO/NC-Z NRDs and N-doped carbon nanotubes. Reprinted with permission from [<a href="#B29-nanomaterials-11-02001" class="html-bibr">29</a>]. Copyright 2017, Elsevier.</p> Full article ">Figure 5
<p>Folding process of FGCZ composite. Reprinted with permission from [<a href="#B133-nanomaterials-11-02001" class="html-bibr">133</a>]. Copyright 2019, Elsevier.</p> Full article ">Figure 6
<p>Scheme of preparation of ZnO/ZnCo<sub>2</sub>O<sub>4</sub>/C composite. Reprinted with permission from [<a href="#B28-nanomaterials-11-02001" class="html-bibr">28</a>]. Copyright 2015, American Chemical Society.</p> Full article ">Figure 7
<p>Scheme of synthesis process of ZZFO-C and ZZFO. Reprinted with permission from [<a href="#B142-nanomaterials-11-02001" class="html-bibr">142</a>]. Copyright 2017, Elsevier.</p> Full article ">
30 pages, 7929 KiB  
Review
Recent Advances in Transition Metal Dichalcogenide Cathode Materials for Aqueous Rechargeable Multivalent Metal-Ion Batteries
by Vo Pham Hoang Huy, Yong Nam Ahn and Jaehyun Hur
Nanomaterials 2021, 11(6), 1517; https://doi.org/10.3390/nano11061517 - 8 Jun 2021
Cited by 36 | Viewed by 8396
Abstract
The generation of renewable energy is a promising solution to counter the rapid increase in energy consumption. Nevertheless, the availability of renewable resources (e.g., wind, solar, and tidal) is non-continuous and temporary in nature, posing new demands for the production of next-generation large-scale [...] Read more.
The generation of renewable energy is a promising solution to counter the rapid increase in energy consumption. Nevertheless, the availability of renewable resources (e.g., wind, solar, and tidal) is non-continuous and temporary in nature, posing new demands for the production of next-generation large-scale energy storage devices. Because of their low cost, highly abundant raw materials, high safety, and environmental friendliness, aqueous rechargeable multivalent metal-ion batteries (AMMIBs) have recently garnered immense attention. However, several challenges hamper the development of AMMIBs, including their narrow electrochemical stability, poor ion diffusion kinetics, and electrode instability. Transition metal dichalcogenides (TMDs) have been extensively investigated for applications in energy storage devices because of their distinct chemical and physical properties. The wide interlayer distance of layered TMDs is an appealing property for ion diffusion and intercalation. This review focuses on the most recent advances in TMDs as cathode materials for aqueous rechargeable batteries based on multivalent charge carriers (Zn2+, Mg2+, and Al3+). Through this review, the key aspects of TMD materials for high-performance AMMIBs are highlighted. Furthermore, additional suggestions and strategies for the development of improved TMDs are discussed to inspire new research directions. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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<p>(<b>a</b>) Brief summary of recent reviews on transition metal dichalcogenides (TMD) materials, (<b>b</b>) Year-wise publication plot for TMD materials including MoS<sub>2</sub>, VS<sub>2</sub>, WS<sub>2</sub>, and TiS<sub>2</sub> in the period of 2010–2020. (searched by Google Scholar, 2 June 2021), (<b>c</b>) The applications of TMDs in the period of 2010–2020.</p> Full article ">Figure 2
<p>(<b>a</b>) TMDs with the MX<sub>2</sub> structure consisting of M from the 16 transition metals indicated by the red dotted box and X from the three halogen elements indicated by the green dotted box, (<b>b</b>) layered structure of MX<sub>2</sub>.</p> Full article ">Figure 3
<p>(<b>a</b>) Polytype structure of TMDs (1T, 2H, and 3R). Reprinted with permission from Coogan et al. [<a href="#B61-nanomaterials-11-01517" class="html-bibr">61</a>] Copyright 2021, Royal Society of Chemistry. (<b>b</b>) Polytype structure of MoS<sub>2</sub>. Reprinted with permission from Song et al. [<a href="#B62-nanomaterials-11-01517" class="html-bibr">62</a>] Copyright 2015, Royal Society of Chemistry.</p> Full article ">Figure 4
<p>Direct bandgap and interlayer distance of various types of TMD.</p> Full article ">Figure 5
<p>(<b>a</b>) Transmission electron microscopy (TEM) image of MoS<sub>2</sub> (left:MoS<sub>2</sub> with oxygen incorporation, right: bulk MoS<sub>2</sub>). (<b>b</b>) cyclic voltammetry curves of MoS<sub>2</sub>-O (pink) and bulk MoS<sub>2</sub> (light blue) at a scan rate of 0.1 mV s<sup>−1</sup>. (<b>c</b>) Rate capability of MoS<sub>2</sub>-O and bulk MoS<sub>2</sub> at various current densities. Reprinted with permission from Liang et al. [<a href="#B77-nanomaterials-11-01517" class="html-bibr">77</a>] Copyright 2019, American Chemical Society. (<b>d</b>) Illustration for the preparation of E-MoS<sub>2</sub>. (<b>e</b>) Rate capability of E-MoS<sub>2</sub> at various current densities. Reprinted with permission from Li et al. [<a href="#B78-nanomaterials-11-01517" class="html-bibr">78</a>] Copyright 2018, Elsevier B.V.</p> Full article ">Figure 6
<p>(<b>a</b>) TEM image of defect-rich MoS<sub>2</sub> nanosheets, (<b>b</b>) cyclic performance of defect-rich MoS<sub>2</sub> nanosheets at 200 mA g<sup>−1</sup>. Reprinted with permission from Xu et al. [<a href="#B79-nanomaterials-11-01517" class="html-bibr">79</a>] Copyright 2018, Elsevier B.V. (<b>c</b>) TEM image of tubular MoS<sub>2</sub>, (<b>d</b>) cyclic performance of tubular MoS<sub>2</sub> at 500 mA g<sup>−1</sup>. Reprinted with permission from Yang et al. [<a href="#B80-nanomaterials-11-01517" class="html-bibr">80</a>] Copyright 2020, ESG Publication.</p> Full article ">Figure 7
<p>(<b>a</b>) TEM image of VS<sub>2</sub> nanosheets, (<b>b</b>) cyclic performance of VS<sub>2</sub> nanosheets at 500 mA g<sup>−1</sup>. Reprinted with permission from He et al. [<a href="#B81-nanomaterials-11-01517" class="html-bibr">81</a>] Copyright 2017,WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim. (<b>c</b>) Rate capability of VS<sub>4</sub>, (<b>d</b>) cyclic performance of VSe<sub>2</sub> nanosheets at 100 and 500 mA g<sup>−1</sup>. Reprinted with permission from Wu et al. [<a href="#B83-nanomaterials-11-01517" class="html-bibr">83</a>] Copyright 2020, Wiley-VCH GmbH.</p> Full article ">Figure 8
<p>(<b>a</b>) TEM image of G-MoS<sub>2</sub> nanosheet, (<b>b</b>) cyclic performance of G-MoS<sub>2</sub> and B-MoS<sub>2</sub> with Mg nanoparticle (N-Mg) and bulk Mg (B-Mg) anodes at 20 mA g<sup>−1</sup>. Reprinted with permission from Liang et al. [<a href="#B88-nanomaterials-11-01517" class="html-bibr">88</a>] Copyright 2011, WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim.(<b>c</b>) TEM image of WSe<sub>2</sub> nanosheets, (<b>d</b>) cyclic performance of WSe<sub>2</sub> nanosheets at 50 mA g<sup>−1</sup>. Reprinted with permission from Xu et al. [<a href="#B93-nanomaterials-11-01517" class="html-bibr">93</a>] Copyright 2020, Elsevier Inc.</p> Full article ">Figure 9
<p>(<b>a</b>) TEM image of freestanding MoS<sub>2</sub>-graphene foam composite with glucose (E-MG), (<b>b</b>) cyclic performance of bulk-MoS<sub>2</sub>, MoS<sub>2</sub>-graphene foam without glucose (MG), and E-MG at 20 mA g<sup>−1</sup>. Reprinted with permission from Fan et al. [<a href="#B104-nanomaterials-11-01517" class="html-bibr">104</a>] Copyright 2017, WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim. (<b>c</b>) Schematic of the MoX<sub>2</sub> structure (X: S, Se) with M1 and M2 site, (<b>d</b>) coulombic efficiency of MoX<sub>2</sub> at 100 mA g<sup>−1</sup>. Reprinted with permission from Divya et al. [<a href="#B106-nanomaterials-11-01517" class="html-bibr">106</a>] Copyright 2020, WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim.</p> Full article ">Figure 10
<p>Cyclic performance of (<b>a</b>) TiS<sub>2</sub> and (<b>b</b>) Cu<sub>0.31</sub>Ti<sub>2</sub>S<sub>4</sub> at room temperature and 50 °C at 5 mA g<sup>−1</sup>. Reprinted with permission from Geng et al. [<a href="#B108-nanomaterials-11-01517" class="html-bibr">108</a>] Copyright 2017, American Chemical Society. (<b>c</b>) Schematic structure of Al insertion sites in Mo<sub>6</sub>S<sub>8</sub>, (<b>d</b>) cyclic performance of Mo<sub>6</sub>S<sub>8</sub>. Reprinted with permission from Geng et al. [<a href="#B109-nanomaterials-11-01517" class="html-bibr">109</a>] Copyright 2015, American Chemical Society.</p> Full article ">Figure 11
<p>(<b>a</b>) Schematic showing the difficulty in the intercalation of Zn hydrates into bulk MoS<sub>2</sub> owing to the large energy barrier between the layers, (<b>b</b>) the expanded interlayer distance that supports the diffusion of Zn<sup>2+</sup>, (<b>c</b>) hydrophobicity control by the Zn–H<sub>2</sub>O–O interaction, (<b>d</b>) theoretical energy barrier between MoS<sub>2</sub> and MoS<sub>2</sub>–O depending on the hydration level of Zn<sup>2+</sup>. Reprinted with permission from Liang et al. [<a href="#B77-nanomaterials-11-01517" class="html-bibr">77</a>] Copyright 2019, American Chemical Society.</p> Full article ">Figure 12
<p>(<b>a</b>) Schematic diagram of the supercritical fluid (SCF) procedure to synthesize TMDs. Reprinted with permission from Truong et al. [<a href="#B90-nanomaterials-11-01517" class="html-bibr">90</a>] Copyright 2017, American Chemical Society.(<b>b</b>) Illustration of two Mg adsorption positions (H and T sites) on MoS<sub>2</sub> nanoribbon:. Reprinted with permission from Yang et al. [<a href="#B87-nanomaterials-11-01517" class="html-bibr">87</a>] Copyright 2012, American Chemical Society.</p> Full article ">Figure 13
<p>(<b>a</b>) Schematic for the synthesis of E-MG. (<b>b</b>) Scanning electron microscopy (SEM) image of free-standing MoS<sub>2</sub>/graphene foam. Reprinted with permission from Fan et al. [<a href="#B104-nanomaterials-11-01517" class="html-bibr">104</a>] Copyright 2017, WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim. (<b>c</b>) The atomic structure with the expanded interlayer distance of MoS<sub>2</sub>. Reprinted with permission from Li et al. [<a href="#B78-nanomaterials-11-01517" class="html-bibr">78</a>] Copyright 2018, Elsevier B.V.</p> Full article ">Figure 14
<p>(<b>a</b>) Schematic of a rechargeable MoS<sub>2</sub> cathode with different phases (1T- and 2H-MoS<sub>2</sub>). (<b>b</b>) The adsorption sites and diffusion pathway of Zn<sup>2+</sup> (left:2H phase MoS<sub>2</sub>and right: 1T phase MoS<sub>2</sub>). (<b>c</b>) Calculation of Zn<sup>2+</sup> diffusion energy barrier on the1T and 2H phases. Reprinted with permission from Liu et al. [<a href="#B75-nanomaterials-11-01517" class="html-bibr">75</a>] Copyright 2020, Elsevier B.V.</p> Full article ">
38 pages, 13056 KiB  
Review
Inorganic Fillers in Composite Gel Polymer Electrolytes for High-Performance Lithium and Non-Lithium Polymer Batteries
by Vo Pham Hoang Huy, Seongjoon So and Jaehyun Hur
Nanomaterials 2021, 11(3), 614; https://doi.org/10.3390/nano11030614 - 1 Mar 2021
Cited by 66 | Viewed by 12139
Abstract
Among the various types of polymer electrolytes, gel polymer electrolytes have been considered as promising electrolytes for high-performance lithium and non-lithium batteries. The introduction of inorganic fillers into the polymer-salt system of gel polymer electrolytes has emerged as an effective strategy to achieve [...] Read more.
Among the various types of polymer electrolytes, gel polymer electrolytes have been considered as promising electrolytes for high-performance lithium and non-lithium batteries. The introduction of inorganic fillers into the polymer-salt system of gel polymer electrolytes has emerged as an effective strategy to achieve high ionic conductivity and excellent interfacial contact with the electrode. In this review, the detailed roles of inorganic fillers in composite gel polymer electrolytes are presented based on their physical and electrochemical properties in lithium and non-lithium polymer batteries. First, we summarize the historical developments of gel polymer electrolytes. Then, a list of detailed fillers applied in gel polymer electrolytes is presented. Possible mechanisms of conductivity enhancement by the addition of inorganic fillers are discussed for each inorganic filler. Subsequently, inorganic filler/polymer composite electrolytes studied for use in various battery systems, including Li-, Na-, Mg-, and Zn-ion batteries, are discussed. Finally, the future perspectives and requirements of the current composite gel polymer electrolyte technologies are highlighted. Full article
(This article belongs to the Special Issue Nanomaterials for Ion Battery Applications)
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Graphical abstract

Graphical abstract
Full article ">Figure 1
<p>Advantages and disadvantages of solid polymer electrolytes (SPEs), liquid electrolytes (LEs), and gel polymer electrolytes (GPEs).</p> Full article ">Figure 2
<p>Schematic of a lithium polymer battery based on GPEs.</p> Full article ">Figure 3
<p>Historical overview of the developments of inorganic fillers in GPEs.</p> Full article ">Figure 4
<p>Surface morphology of P poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) with varying TiO<sub>2</sub> (rutile) contents from the upper left to the lower right panel. Reprinted with permission from Kim et al. [<a href="#B74-nanomaterials-11-00614" class="html-bibr">74</a>]. Copyright 2003 Elsevier B.V.</p> Full article ">Figure 5
<p>(<b>a</b>) SEM image of the TiO<sub>2</sub>-SiO<sub>2</sub> hybrid composite, (<b>b</b>) wide angle X-ray spectroscopy of the TiO<sub>2</sub>-SiO<sub>2</sub> hybrid composite, (<b>c</b>) nitrogen adsorption/desorption isotherm and pore size of the TiO<sub>2</sub>-SiO<sub>2</sub> hybrid composite, and (<b>d</b>) SEM image of the surface of the membrane containing the TiO<sub>2</sub>-SiO<sub>2</sub> hybrid composite. Reprinted with permission from Kurc et al. [<a href="#B81-nanomaterials-11-00614" class="html-bibr">81</a>]. Copyright 2014 Elsevier Ltd.</p> Full article ">Figure 6
<p>(<b>a</b>) Schematic of nano-TiO<sub>2</sub>- poly(methyl methacrylate) (PMMA) in N,N-dimethylformamide (DMF) (A: mixture of nano-TiO<sub>2</sub> and PMMA, B: tethered PMMA on Nano-TiO<sub>2</sub>, C: self-assembly of PMMA-tethered Nano-TiO<sub>2</sub>) and (<b>b</b>) photographs of the dispersed NPs in DMF before (top panel) and after (bottom panel) 10 min centrifugation at 10,000 rpm. The same TiO<sub>2</sub> content (5 wt%) was used in each sample: (S1) highly dispersed nano-TiO<sub>2</sub>-PMMA, (S2) nano-TiO<sub>2</sub>-PMMA, and (S3) pristine nano-TiO<sub>2</sub>. (<b>c</b>) SEM images of the GPEs: (S1) pristine PVDF-HFP (“GPE”), (S2) nano-TiO<sub>2</sub>/PVDF-HFP (“CPE”), (S3) nano-TiO<sub>2</sub>-PMMA/PVDF-HFP (“M-CPE”), and (S4) highly dispersed nano-TiO<sub>2</sub>-PMMA/PVDF-HFP (“HM-CPE”). (<b>d</b>) The rate capabilities of the different electrolytes shown in (<b>c</b>). Reprinted with permission from Chen et al. [<a href="#B85-nanomaterials-11-00614" class="html-bibr">85</a>]. Copyright 2013 Elsevier Ltd.</p> Full article ">Figure 7
<p>Thermal behavior of the GPE membranes (<b>a</b>) before and (<b>b</b>) after storing at 130 °C for 1 h, (<b>c</b>) EIS results of the GPE membrane containing varying contents of TiO<sub>2</sub>, and (<b>d</b>) cyclic performance of the LiCoO<sub>2</sub>/Li cells using the GPE at 0.2 C. Reprinted with permission from Chen et al. [<a href="#B88-nanomaterials-11-00614" class="html-bibr">88</a>]. Copyright 2015 Elsevier B.V.</p> Full article ">Figure 8
<p>(<b>a</b>) Separator-supported LE (SLE): limitation in ionic dissociation. (<b>b</b>) GPE- poly(acrylonitrile-co-vinyl acetate) (PAV): a space-charge layer of Li<sup>+</sup> ions is formed due to the PF<sub>6</sub><sup>−</sup> anion absorbed by the nitrile functional groups on the PAV chain. (<b>c</b>) GPE-PAVM:TiO<sub>2</sub>: the 3D percolation pathway is formed by the space-charged layers surrounding the TiO<sub>2</sub> NPs and PAV chain. (<b>d</b>) Nyquist plots of the full cell (graphite-GPE-LFP) and (<b>e</b>) discharge capacity of the full cell at a 20 C-rate over a voltage range of 2.0–3.8 V. Reprinted with permission from Teng et al. [<a href="#B90-nanomaterials-11-00614" class="html-bibr">90</a>]. Copyright 2016 American Chemical Society.</p> Full article ">Figure 9
<p>SEM images of the (<b>a</b>) PVA:NH<sub>4</sub>SCN/DMSO GPE containing (<b>b</b>) 2, (<b>c</b>) 6, and (<b>d</b>) 10 wt% Al<sub>2</sub>O<sub>3</sub> NPs. Reprinted with permission from Rat et al. [<a href="#B97-nanomaterials-11-00614" class="html-bibr">97</a>]. Copyright 2012 Indian Academy of Sciences.</p> Full article ">Figure 10
<p>(<b>a</b>) Schematic of the membrane (Al<sub>2</sub>O<sub>3</sub>/PVFM/Al<sub>2</sub>O<sub>3</sub>). SEM images of the trilayer membrane; (<b>b</b>) cross-sectional image of the trilayer membrane; (<b>c</b>) cross-sectional image of the PVFM membrane; (<b>d</b>) the surface morphology of the Al<sub>2</sub>O<sub>3</sub> coating layer; and (<b>e</b>) the surface morphology of the PVFM-based membrane. Reprinted with permission from Wen et al. [<a href="#B99-nanomaterials-11-00614" class="html-bibr">99</a>]. Copyright 2007 Scientific Research Publishing Inc.</p> Full article ">Figure 11
<p>Morphology of (<b>a</b>,<b>b</b>) pristine GPE and (<b>c</b>,<b>d</b>) Al<sub>2</sub>O<sub>3</sub>-GPE membrane. (<b>e</b>) Initial charge–discharge curves of the Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> (LTO) and LiNi<sub>1/3</sub>Mn<sub>1/3</sub>Co<sub>1/3</sub>O<sub>2</sub> (NMC) half cells and (<b>f</b>) the cyclic performance of the GPE membrane. Reprinted with permission from Kim et al. [<a href="#B100-nanomaterials-11-00614" class="html-bibr">100</a>]. Copyright 2017 Elsevier Ltd.</p> Full article ">Figure 12
<p>(<b>a</b>) Schematic of Na-ion transportation in the Al<sub>2</sub>O<sub>3</sub> nanowire (AN)-GPE. (<b>b</b>,<b>c</b>) Adsorption of ethylene carbonate (EC) and diethylene carbonate (DEC) on the β-Al<sub>2</sub>O<sub>3</sub> (003). (<b>d</b>,<b>e</b>) Cyclic performance of the Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> (NVP)/Na cells using a glass fiber (GF)-LE, GPE, GFs-GPE, and ANs-GPE at 1 C under 25 and 60 °C, respectively. (<b>f</b>) Rate performance of the NVP/Na cells using the different GPEs. Reprinted with permission from Yang et al. [<a href="#B104-nanomaterials-11-00614" class="html-bibr">104</a>]. Copyright 2019 Springer Nature.</p> Full article ">Figure 13
<p>(<b>a</b>) Reaction scheme for the synthesis of the SiO<sub>2</sub>(Li<sup>+</sup>) particles. (<b>b</b>) Charge-discharge curves of the GPE containing 20 wt.% SiO<sub>2</sub>(Li<sup>+</sup>) particles. (<b>c</b>) Discharge capacities of the GPE containing different contents of SiO<sub>2</sub>(Li<sup>+</sup>) particles. Reprinted with permission from Kim et al. [<a href="#B108-nanomaterials-11-00614" class="html-bibr">108</a>]. Copyright 2012 Elsevier B.V.</p> Full article ">Figure 14
<p>SEM images of the GPE membrane: (<b>a</b>) pristine PVDF, (<b>b</b>) PVDF-1% SiO<sub>2</sub>(Li<sup>+</sup>), (<b>c</b>) PVDF-2% SiO<sub>2</sub>(Li<sup>+</sup>), (<b>d</b>) PVDF-5% SiO<sub>2</sub>(Li<sup>+</sup>), and (<b>e</b>) PVDF-10% SiO<sub>2</sub>(Li<sup>+</sup>). Reprinted with permission from Li et al. [<a href="#B109-nanomaterials-11-00614" class="html-bibr">109</a>]. Copyright 2013 Springer Nature.</p> Full article ">Figure 15
<p>Reaction schemes for the synthesis of (<b>a</b>) mesoporous MA-SiO<sub>2</sub> particles and (<b>b</b>) cross-linked composite GPE. (<b>c</b>) Charge-discharge curves of the cell and (<b>d</b>) cyclic performance with different electrolytes at 25 °C. Reprinted with permission from Kim et al. [<a href="#B111-nanomaterials-11-00614" class="html-bibr">111</a>]. Copyright 2016 Springer Nature.</p> Full article ">Figure 16
<p>(<b>a</b>) Schematic of the GPE-sPZ hybrid particles. (<b>b</b>,<b>c</b>) Cyclic performance and Coulombic efficiency of the Li/CPE-sPZ/LiCoO<sub>2</sub> and Li/CPE-sPZ/graphite coin cells at different C-rates at room temperature. Reprinted with permission from Xiao et al [<a href="#B120-nanomaterials-11-00614" class="html-bibr">120</a>]. Copyright 2018 Elsevier B.V.</p> Full article ">Figure 17
<p>The model of the electrolytic conductance on the inorganic filler (SiO<sub>2</sub>) interfaces through the layers of immobile ice layer absorbed on OH-terminated silica surface. Reprinted with permission from Chen et al. [<a href="#B138-nanomaterials-11-00614" class="html-bibr">138</a>]. 2020 Creative Commons Attribution-Noncommercial liscense.</p> Full article ">Figure 18
<p>(<b>a</b>) Schematic illustrations the prevent of lithium dendrite growth by Al<sub>2</sub>O<sub>3</sub>-GPE electrolyte; (<b>b</b>) pristine of lithium anode before cycling in LFP/GPE/Li cell; (<b>c</b>) lithium anode in LFP/GPE/Li cell after 200 cycles at 0.5 C; (<b>d</b>) lithium anode in LFP/Al<sub>2</sub>O<sub>3</sub>-GPE/Li cell after 200 cycles at 0.5 C. Reprinted with permission from Liu et al. [<a href="#B143-nanomaterials-11-00614" class="html-bibr">143</a>]. Copyright 2018. The Chinese Ceramic Society. Production and hosting by Elsevier B.V.</p> Full article ">
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