Aditi De, Pandiarajan Devi, P. Murugan, Subrata Kundu
Electrocatalytic water splitting for the production of green hydrogen addresses current energy crisis and potential energy storage. Herein, we have fabricated a low-cost, highly efficient transition metal-based heterostructure of NiCr-LDH over VS2 using three-dimensional (3D) nickel foam as a substrate. This self-supported NiCr-LDH/VS2/NF heterostructure catalyst works as an excellent bifunctional electrode to catalyze the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) by exhibiting very low overpotential of 209 mV and 116 mV respectively to attain 50 mA/cm2 current density in 1M KOH solution. In addition, NiCr-LDH/VS2/NF shows a cell voltage of 1.545 V to attain 10 mA/cm2 current density and a 40-hour long-term static stability. n-type semiconducting NiCr-LDH and p-type conducting VS2 enhance the electrocatalytic performance by their synergistic effect, change in surface-modified electronic structure, and generation of improved thin-nanosheet-like mesoporous morphology with superhydrophilic surfaces. Density functional theory (DFT) calculations confirm an interesting charge repopulation observation in both the layers of NiCr-LDH and VS2 that increases the overall electrocatalytic reaction performance by electron transfer within the layer (confirmed by charge density and Bader charge analysis). This material holds impressive application potential that can guide the design and screening of efficient earth-abundant bifunctional electrocatalysts.
{"title":"Revolutionizing Water Splitting Performance by Probing the Influence of Electron Transfer in NiCr-LDH/VS2/NF Heterostructure","authors":"Aditi De, Pandiarajan Devi, P. Murugan, Subrata Kundu","doi":"10.1039/d5ta01733e","DOIUrl":"https://doi.org/10.1039/d5ta01733e","url":null,"abstract":"Electrocatalytic water splitting for the production of green hydrogen addresses current energy crisis and potential energy storage. Herein, we have fabricated a low-cost, highly efficient transition metal-based heterostructure of NiCr-LDH over VS2 using three-dimensional (3D) nickel foam as a substrate. This self-supported NiCr-LDH/VS2/NF heterostructure catalyst works as an excellent bifunctional electrode to catalyze the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) by exhibiting very low overpotential of 209 mV and 116 mV respectively to attain 50 mA/cm2 current density in 1M KOH solution. In addition, NiCr-LDH/VS2/NF shows a cell voltage of 1.545 V to attain 10 mA/cm2 current density and a 40-hour long-term static stability. n-type semiconducting NiCr-LDH and p-type conducting VS2 enhance the electrocatalytic performance by their synergistic effect, change in surface-modified electronic structure, and generation of improved thin-nanosheet-like mesoporous morphology with superhydrophilic surfaces. Density functional theory (DFT) calculations confirm an interesting charge repopulation observation in both the layers of NiCr-LDH and VS2 that increases the overall electrocatalytic reaction performance by electron transfer within the layer (confirmed by charge density and Bader charge analysis). This material holds impressive application potential that can guide the design and screening of efficient earth-abundant bifunctional electrocatalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"8 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Samad Yarjan, Rohan B. Ambade, Yawar Abbas, Muhammad Umair Khan, Rui Chang, Yahya Zweiri, Baker Mohammad, Dalaver H. Anjum
The growing demand for low-powered, high-density wearable electronics devices and Internet of Things (IoT) technology requires reliable energy modules. Triboelectric nanogenerators (TENG), as an emerging energy harvesting technology, have the potential to supply power to these IoT devices consistently and low-power consumption devices. Herein this work, we demonstrate the fabrication of a highly efficient triboelectric nanogenerator (TENG) by synthesizing highly pure two-dimensional (2D) hexagonal boron nitride (hBN) flakes as electropositive materials by high-pressure homogenizer (HPH) method, and fluorinated ethylene propylene (FEP) as electronegative materials. The fabricated device exhibits the highly reliable and repeatable open circuit voltage (Voc) ~135 V and short circuit current (Isc) ~ 17.0 µA for the tapping frequency of 5 Hz. Furthermore, the 2D hBN flakes prepared by HPH demonstrated a high-power density of 18 W/cm2, exceeding the previously reported values for hBN-based TENGs. The device can monitor full-range humidity (30 to 100 % RH) and distinguish light and harsh tapping. The HPH-prepared 2D hBN-based TENG powered or operated portable devices like a digital thermometer, stopwatch, and mini-calculator. The HPH-prepared 2D hBN-based TENG device can harvest energy from mechanical input for an energy-efficient lifestyle as it can continuously charge and discharge the capacitor through continuous pressing and releasing by tapping. Thus, HPH-prepared 2D hBN flakes endeavour to create an energy-efficient process to convert mechanical energy into electrical energy, promote sustainability, and advance clean energy technologies.
{"title":"Sustainable High-Pressure Homogenization of Hexagonal Boron Nitride for Triboelectric Nanogenerator: Advancing Self-Powered Environmental Monitoring in Portable Electronics","authors":"Samad Yarjan, Rohan B. Ambade, Yawar Abbas, Muhammad Umair Khan, Rui Chang, Yahya Zweiri, Baker Mohammad, Dalaver H. Anjum","doi":"10.1039/d4ta08698h","DOIUrl":"https://doi.org/10.1039/d4ta08698h","url":null,"abstract":"The growing demand for low-powered, high-density wearable electronics devices and Internet of Things (IoT) technology requires reliable energy modules. Triboelectric nanogenerators (TENG), as an emerging energy harvesting technology, have the potential to supply power to these IoT devices consistently and low-power consumption devices. Herein this work, we demonstrate the fabrication of a highly efficient triboelectric nanogenerator (TENG) by synthesizing highly pure two-dimensional (2D) hexagonal boron nitride (hBN) flakes as electropositive materials by high-pressure homogenizer (HPH) method, and fluorinated ethylene propylene (FEP) as electronegative materials. The fabricated device exhibits the highly reliable and repeatable open circuit voltage (Voc) ~135 V and short circuit current (Isc) ~ 17.0 µA for the tapping frequency of 5 Hz. Furthermore, the 2D hBN flakes prepared by HPH demonstrated a high-power density of 18 W/cm2, exceeding the previously reported values for hBN-based TENGs. The device can monitor full-range humidity (30 to 100 % RH) and distinguish light and harsh tapping. The HPH-prepared 2D hBN-based TENG powered or operated portable devices like a digital thermometer, stopwatch, and mini-calculator. The HPH-prepared 2D hBN-based TENG device can harvest energy from mechanical input for an energy-efficient lifestyle as it can continuously charge and discharge the capacitor through continuous pressing and releasing by tapping. Thus, HPH-prepared 2D hBN flakes endeavour to create an energy-efficient process to convert mechanical energy into electrical energy, promote sustainability, and advance clean energy technologies.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"38 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Simin Zhang, Jiawei Xu, Jiayong Lu, Zhijian Liu, Zechen Xiao, Wei Guo, Mo Zhang, Yan Wan, Yangming Lin
Covalent organic frameworks (COFs), as a class of emerging porous crystalline polymers with high specific surface areas and tunable framework structures, exhibit great potential in oxygen reduction reaction (ORR). Herein, we synthesize a series of benzothiophene-based COFs with varying benzene ring counts in the linkers and employ these materials to unveil the correlation between conjugated structure and the selectivity toward H2O2 electro-synthesis. Experimental results display that the highest H2O2 selectivity (~90%) is offered by the benzothiophene-based COF bearing one benzene ring in the linker, exhibiting a negative correlation with the number of benzene rings in the linker. Theoretical calculations reveal that variations in the number of benzene rings modulated the adsorption strengths and sites of key reaction intermediates, thereby altering 2e- ORR pathway. The decrease in benzene ring count enable the dominant pathway for 2e- ORR become the H2O2 formation through the nucleophilic attack of the active *O2- species, which originates from the electron transfer of 3O2, on the carbon atom near the sulfur atom of the thiophene ring. This work highlights the importance of appropriate linkers and provides valuable insights for devising metal-free COF electrocatalysts.
{"title":"Benzothiophene-Based Covalent Organic Framework for H2O2 Electrosynthesis: The Critical Role of Conjugated Structure","authors":"Simin Zhang, Jiawei Xu, Jiayong Lu, Zhijian Liu, Zechen Xiao, Wei Guo, Mo Zhang, Yan Wan, Yangming Lin","doi":"10.1039/d5ta01794g","DOIUrl":"https://doi.org/10.1039/d5ta01794g","url":null,"abstract":"Covalent organic frameworks (COFs), as a class of emerging porous crystalline polymers with high specific surface areas and tunable framework structures, exhibit great potential in oxygen reduction reaction (ORR). Herein, we synthesize a series of benzothiophene-based COFs with varying benzene ring counts in the linkers and employ these materials to unveil the correlation between conjugated structure and the selectivity toward H2O2 electro-synthesis. Experimental results display that the highest H2O2 selectivity (~90%) is offered by the benzothiophene-based COF bearing one benzene ring in the linker, exhibiting a negative correlation with the number of benzene rings in the linker. Theoretical calculations reveal that variations in the number of benzene rings modulated the adsorption strengths and sites of key reaction intermediates, thereby altering 2e- ORR pathway. The decrease in benzene ring count enable the dominant pathway for 2e- ORR become the H2O2 formation through the nucleophilic attack of the active *O2- species, which originates from the electron transfer of 3O2, on the carbon atom near the sulfur atom of the thiophene ring. This work highlights the importance of appropriate linkers and provides valuable insights for devising metal-free COF electrocatalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"24 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Joel Kingston Ramesh, Sasan Rostami, Jayaprakasan Rajesh, R. Margrate Bhackiyavathi Princess, Radhika Govindaraju, Jinho Kim, Rainer Adelung, Rajkumar Palanisamy, Mozaffar Abdollahifar
ZnMn2O4 (ZMO) has emerged as a promising material for energy storage applications due to its high theoretical capacity, low cost, and environmental friendliness. This review comprehensively explores the structure, synthesis methods, and performance of ZMO in various energy storage systems, including supercapacitors and batteries such as lithium-ion (LIBs), sodium-ion (SIBs) and zinc-ion (ZIBs) batteries, due to exceptional electrochemical properties. The influence of various synthesis techniques on the structural and morphological features of ZMO, which directly impact its electrochemical performance will be discussed. The review also delves into the charge storage mechanism of ZMO in supercapacitors, examining the effects of morphology, composites, and doping on its performance. Additionally, the use of ZMO as an anode material for LIBs and SIBs and its potential as a cathode material in ZIBs are discussed. The review also addresses key challenges and proposes strategies to enhance performance including incorporating conductive materials, synergizing with other materials, and doping. An outlook on the current challenges, future directions, and potential pathways for performance enhancement is also presented
{"title":"ZnMn2O4 Applications in Batteries and Supercapacitors: A Comprehensive Review","authors":"Joel Kingston Ramesh, Sasan Rostami, Jayaprakasan Rajesh, R. Margrate Bhackiyavathi Princess, Radhika Govindaraju, Jinho Kim, Rainer Adelung, Rajkumar Palanisamy, Mozaffar Abdollahifar","doi":"10.1039/d5ta00815h","DOIUrl":"https://doi.org/10.1039/d5ta00815h","url":null,"abstract":"ZnMn2O4 (ZMO) has emerged as a promising material for energy storage applications due to its high theoretical capacity, low cost, and environmental friendliness. This review comprehensively explores the structure, synthesis methods, and performance of ZMO in various energy storage systems, including supercapacitors and batteries such as lithium-ion (LIBs), sodium-ion (SIBs) and zinc-ion (ZIBs) batteries, due to exceptional electrochemical properties. The influence of various synthesis techniques on the structural and morphological features of ZMO, which directly impact its electrochemical performance will be discussed. The review also delves into the charge storage mechanism of ZMO in supercapacitors, examining the effects of morphology, composites, and doping on its performance. Additionally, the use of ZMO as an anode material for LIBs and SIBs and its potential as a cathode material in ZIBs are discussed. The review also addresses key challenges and proposes strategies to enhance performance including incorporating conductive materials, synergizing with other materials, and doping. An outlook on the current challenges, future directions, and potential pathways for performance enhancement is also presented","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"16 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bin Wang, Chao Zhu, Hai Lei, Hanyu Zhou, Wei Sun, Yue Yang, Peng Ge
Attracted by the economic and environmental value, the direct regeneration of spent Ni–Co–Mn oxides has captured plenty of attention. However, considering the low bonding energy of metal–oxygen, F-elements from binders and LiPF6 can be introduced into the bulk phase of regenerated samples, resulting in poor electrochemical properties. Herein, supported by CaO powders, regenerated cathodes were successfully obtained through the formation and removal of CaF2. By tailoring thermal sintering, the as-optimized sample exhibited a smooth surface and an intact morphology/lattice structure. More importantly, benefitting from the formation of oxygen vacancies, a rich oxygen-lattice surface/near-surface was established, exhibiting high stability. As a Li-storage cathode, the as-optimized samples delivered a capacity of 149.7 mA h g−1. The retention ratio remained at approximately 96.3% after 150 loops at 1.0 C. Even at 5.0 C, the capacity reached 134.1 mA h g−1, maintaining ∼84.7% retention after 300 cycles. Detailed kinetic behaviors analysis indicated an improved diffusion coefficient and reduced interfacial resistance, accompanied by a reduction in the voltage gap. Moreover, in situ resistance analysis revealed that stable charge-transfer resistance further alleviated internal stress variation. Thus, this study is expected to illustrate the regeneration process of spent Ni–Co–Mn oxides after the successful removal of F-impurities.
{"title":"Regeneration of spent NCM622: reconstructing the rich lattice oxygen surface for enhanced stability","authors":"Bin Wang, Chao Zhu, Hai Lei, Hanyu Zhou, Wei Sun, Yue Yang, Peng Ge","doi":"10.1039/d5ta00776c","DOIUrl":"https://doi.org/10.1039/d5ta00776c","url":null,"abstract":"Attracted by the economic and environmental value, the direct regeneration of spent Ni–Co–Mn oxides has captured plenty of attention. However, considering the low bonding energy of metal–oxygen, F-elements from binders and LiPF<small><sub>6</sub></small> can be introduced into the bulk phase of regenerated samples, resulting in poor electrochemical properties. Herein, supported by CaO powders, regenerated cathodes were successfully obtained through the formation and removal of CaF<small><sub>2</sub></small>. By tailoring thermal sintering, the as-optimized sample exhibited a smooth surface and an intact morphology/lattice structure. More importantly, benefitting from the formation of oxygen vacancies, a rich oxygen-lattice surface/near-surface was established, exhibiting high stability. As a Li-storage cathode, the as-optimized samples delivered a capacity of 149.7 mA h g<small><sup>−1</sup></small>. The retention ratio remained at approximately 96.3% after 150 loops at 1.0 C. Even at 5.0 C, the capacity reached 134.1 mA h g<small><sup>−1</sup></small>, maintaining ∼84.7% retention after 300 cycles. Detailed kinetic behaviors analysis indicated an improved diffusion coefficient and reduced interfacial resistance, accompanied by a reduction in the voltage gap. Moreover, <em>in situ</em> resistance analysis revealed that stable charge-transfer resistance further alleviated internal stress variation. Thus, this study is expected to illustrate the regeneration process of spent Ni–Co–Mn oxides after the successful removal of F-impurities.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1156 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758615","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A crucial step in the large-scale fabrication of organic photovoltaic (OPV) cells is the coating of the functional layers, which directly influences the efficiency and stability of OPV cells. Among various coating techniques, Meniscus-guided coating (MGC) method has emerged as a promising approach, demonstrating unique advantages in achieving uniform and reproducible films while maintaining high material utilization efficiency. This review specifically focuses on the fluid flow dynamics and drying kinetics involved in the MGC process. We systematically analyse how coating parameters, such as coating speed, solution viscosity, and substrate surface energy, govern the final film morphology and device performance. Understanding these dynamics is essential for optimizing the MGC process and fabricating high-quality OPV cells with consistent performance. Besides, we summarize the recent progress in MGC for OPV cells and highlight the state-of-the-art results. Finally, we propose some forward-looking perspectives on the MGC method, with the aim of promoting the commercialization of OPV technology.
{"title":"Meniscus-Guided Coating for Organic Photovoltaic Cells","authors":"Wenye Xu, Yue Yu, Yong Cui, Jianhui Hou","doi":"10.1039/d5ta01491c","DOIUrl":"https://doi.org/10.1039/d5ta01491c","url":null,"abstract":"A crucial step in the large-scale fabrication of organic photovoltaic (OPV) cells is the coating of the functional layers, which directly influences the efficiency and stability of OPV cells. Among various coating techniques, Meniscus-guided coating (MGC) method has emerged as a promising approach, demonstrating unique advantages in achieving uniform and reproducible films while maintaining high material utilization efficiency. This review specifically focuses on the fluid flow dynamics and drying kinetics involved in the MGC process. We systematically analyse how coating parameters, such as coating speed, solution viscosity, and substrate surface energy, govern the final film morphology and device performance. Understanding these dynamics is essential for optimizing the MGC process and fabricating high-quality OPV cells with consistent performance. Besides, we summarize the recent progress in MGC for OPV cells and highlight the state-of-the-art results. Finally, we propose some forward-looking perspectives on the MGC method, with the aim of promoting the commercialization of OPV technology.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"58 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Christian Heinekamp, Arkendu Roy, Stephanos Karafiludis, Sourabh Kumar, Ana Guilherme Buzanich, Tomasz Maciej Stawski, Aistė Miliūtė, Marcus Florian von der Au, Mike Ahrens, Thomas Braun, Franziska Emmerling
Extended hydrogen initiatives promote the urgency of research on water splitting technologies and therein oxygen evolution reaction catalysts being developed. A route to access a ZrF4 supported high-entropy fluoride catalyst using a facile sol-gel route is presented. The high-entropy character of the catalyst was confirmed by scanning transmission electron microscopy and energy dispersive X-ray spectroscopy (STEM-EDX) as well as inductively coupled plasma-mass spectrometry (ICP-MS). Additional investitions on the local structure were performed using extended X-ray absorption fine structure spectroscopy (EXAFS) and pair distribution function (PDF) analysis. The catalyst shows significant potential for oxygen evolution reaction (OER) in alkaline media with a current density of 100 mA cm-2 at approximately 1.60 V, thus outperforming benchmark materials such as IrO2, despite a significant reduction in electrochemical mass loading. A potential mechanism is suggested based on free energy calculation using DFT calulations.
氢能计划的扩展推动了水分离技术研究的紧迫性，其中氧进化反应催化剂的开发也迫在眉睫。本文介绍了一种利用简便的溶胶-凝胶法获得 ZrF4 支持的高熵氟化物催化剂的途径。该催化剂的高熵特性通过扫描透射电子显微镜和能量色散 X 射线光谱法（STEM-EDX）以及电感耦合等离子体质谱法（ICP-MS）得到了证实。此外，还利用扩展 X 射线吸收精细结构光谱（EXAFS）和对分布函数（PDF）分析对局部结构进行了研究。该催化剂在碱性介质中的氧进化反应（OER）中显示出巨大的潜力，在约 1.60 V 的电压下，电流密度为 100 mA cm-2，因此，尽管电化学质量负荷显著降低，但其性能优于 IrO2 等基准材料。利用 DFT 计算自由能，提出了一种潜在的机理。
{"title":"Zirconium Fluoride-Supported High-Entropy Fluoride: A Catalyst for Enhanced Oxygen Evolution Reaction","authors":"Christian Heinekamp, Arkendu Roy, Stephanos Karafiludis, Sourabh Kumar, Ana Guilherme Buzanich, Tomasz Maciej Stawski, Aistė Miliūtė, Marcus Florian von der Au, Mike Ahrens, Thomas Braun, Franziska Emmerling","doi":"10.1039/d4ta08664c","DOIUrl":"https://doi.org/10.1039/d4ta08664c","url":null,"abstract":"Extended hydrogen initiatives promote the urgency of research on water splitting technologies and therein oxygen evolution reaction catalysts being developed. A route to access a ZrF4 supported high-entropy fluoride catalyst using a facile sol-gel route is presented. The high-entropy character of the catalyst was confirmed by scanning transmission electron microscopy and energy dispersive X-ray spectroscopy (STEM-EDX) as well as inductively coupled plasma-mass spectrometry (ICP-MS). Additional investitions on the local structure were performed using extended X-ray absorption fine structure spectroscopy (EXAFS) and pair distribution function (PDF) analysis. The catalyst shows significant potential for oxygen evolution reaction (OER) in alkaline media with a current density of 100 mA cm-2 at approximately 1.60 V, thus outperforming benchmark materials such as IrO2, despite a significant reduction in electrochemical mass loading. A potential mechanism is suggested based on free energy calculation using DFT calulations.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"58 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
As a unique type of intelligent material, liquid crystal elastomers (LCEs) have numerous valuable advantages and show significant potential for application in the design of flexible actuators. Nevertheless, attaining controllable and precise orientation of LCEs using easily operated methods continues to pose a considerable challenge. In this study, a synchronous differential orientation strategy based on dual dynamic covalent bonds (DCBs) was proposed to solve these problems. Through the integration of dynamic boronic ester bonds and dynamic siloxane bonds into the LCE network, bilayer LCE films that exhibit distinct orientation configurations can be easily fabricated. Meanwhile, the variation in the bond energy between these two chemical bonds provides the ability to control the orientation of each layer separately, resulting in LCE films with adjustable bending angles. Furthermore, the addition of azobenzene to the LCE composition enables the material to undergo reversible bending when illuminated with alternating ultraviolet and visible light, revealing the potential for various actuation capabilities in innovative materials. This approach not only dramatically enhances the self-healing, programming, and recycling of LCEs, but also paves the way for the development of advanced flexible actuators with complex deformation properties, holding substantial potential for applications in robotics, biomedicine, and intelligent devices.
{"title":"Synchronous differential orientation of liquid crystal elastomers based on dual dynamic covalent bonds","authors":"Zhentian Xu, Yangyang Zhu, Yun Ai, Zhongyi Yuan, Chunquan Li, Dan Zhou, Lie Chen","doi":"10.1039/d5ta00568j","DOIUrl":"https://doi.org/10.1039/d5ta00568j","url":null,"abstract":"As a unique type of intelligent material, liquid crystal elastomers (LCEs) have numerous valuable advantages and show significant potential for application in the design of flexible actuators. Nevertheless, attaining controllable and precise orientation of LCEs using easily operated methods continues to pose a considerable challenge. In this study, a synchronous differential orientation strategy based on dual dynamic covalent bonds (DCBs) was proposed to solve these problems. Through the integration of dynamic boronic ester bonds and dynamic siloxane bonds into the LCE network, bilayer LCE films that exhibit distinct orientation configurations can be easily fabricated. Meanwhile, the variation in the bond energy between these two chemical bonds provides the ability to control the orientation of each layer separately, resulting in LCE films with adjustable bending angles. Furthermore, the addition of azobenzene to the LCE composition enables the material to undergo reversible bending when illuminated with alternating ultraviolet and visible light, revealing the potential for various actuation capabilities in innovative materials. This approach not only dramatically enhances the self-healing, programming, and recycling of LCEs, but also paves the way for the development of advanced flexible actuators with complex deformation properties, holding substantial potential for applications in robotics, biomedicine, and intelligent devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"12 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143744785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qihang Wang, Jiqiong Liu, Huichao Lu, Liu Shuo, Liangyu Wang, Chenran Hao, Han Jing, Jun Yang, Yanna NuLi, Jiulin Wang
With the growing concern over increasing energy density, lithium-sulfur batteries have garnered significant interest from researchers. However, the volume expansion of the sulfur cathode, which leads to poor cycling stability at high loadings, poses a major challenge to their practical application. Traditional binders are highly susceptible to cracking and structural collapse as the coating thickness increases. Our study presents a dual-component composite binder (G2CEA) that harmoniously blends rigidity and flexibility, with each component serving a specific function. Guar gum (GG), the rigid component, envelops the SPAN interface and contributes to the formation of the CEI film, ensuring interface stability. Poly(2-Carboxyethyl acrylate) (PCEA), the flexible component, retains adhesion and ductility in the electrolyte, cushioning the volume changes of SPAN particles and maintaining the structural integrity of the electrode. This innovative design endows the G2CEA-based cathode with superior cycling stability (97.6% retention after 164 cycles at 0.1C) under high loadings (7.5 mg cm-²), offering a valuable perspective for the design of practical binders in the future.
{"title":"A Rigid-flexible Binder for Sulfurized Polyacrylonitrile Cathode for Rechargeable Lithium Battery","authors":"Qihang Wang, Jiqiong Liu, Huichao Lu, Liu Shuo, Liangyu Wang, Chenran Hao, Han Jing, Jun Yang, Yanna NuLi, Jiulin Wang","doi":"10.1039/d5ta01612f","DOIUrl":"https://doi.org/10.1039/d5ta01612f","url":null,"abstract":"With the growing concern over increasing energy density, lithium-sulfur batteries have garnered significant interest from researchers. However, the volume expansion of the sulfur cathode, which leads to poor cycling stability at high loadings, poses a major challenge to their practical application. Traditional binders are highly susceptible to cracking and structural collapse as the coating thickness increases. Our study presents a dual-component composite binder (G2CEA) that harmoniously blends rigidity and flexibility, with each component serving a specific function. Guar gum (GG), the rigid component, envelops the SPAN interface and contributes to the formation of the CEI film, ensuring interface stability. Poly(2-Carboxyethyl acrylate) (PCEA), the flexible component, retains adhesion and ductility in the electrolyte, cushioning the volume changes of SPAN particles and maintaining the structural integrity of the electrode. This innovative design endows the G2CEA-based cathode with superior cycling stability (97.6% retention after 164 cycles at 0.1C) under high loadings (7.5 mg cm-²), offering a valuable perspective for the design of practical binders in the future.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"30 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143744791","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lin Sun, Lijun Wang, Yang Liu, Hongyu Wang, Zhong Jin
In contrast to nanosilicon, micron-sized silicon anodes have regained widespread attention due to their high energy density, favorable processability, and reduced side reactions. However, these anodes are plagued by several significant challenges. They undergo substantial volume changes, suffer from sluggish lithium-ion transport kinetics and the loss of electrical contact. In this study, micron-sized porous silicon (pSi) obtained through acid etching of Al60Si40 alloy was utilized as the starting material. A novel approach combining high-energy ball milling and wet chemistry methods was adopted to dope Ge atoms into pSi and modify it with liquid GaInSn metal (LM) alloy (Designated as pSi/Ge@LM). The incorporation of Ge heteroatoms and LM offers multiple benefits. Firstly, it enhances the tap density of pSi. Secondly, it effectively boosts the electron transport performance of the material. Moreover, the excellent metallic properties and liquid fluidity of LM endow it with a unique "self-healing" function. Both the half-cells and full-cells assembled with pSi/Ge@LM electrode demonstrate outstanding electrochemical performance. Specifically, In the half-cells, when cycled at a current density of 1 A g-1 for 400 times, the pSi/Ge@LM electrode retains a remarkably high specific capacity of 1011 mAh g-1. Even at a high current density of 3 A g-1, it still delivers a reversible capacity of over 900 mAh g-1. It is anticipated that this research will offer novel insights and valuable guidance for the development of high-energy-density micron-sized silicon anodes.
{"title":"Synergistic Engineering of Micron-sized Porous Silicon Anodes via Ge Doping and Liquid Metal Alloy Modification for High-energy-density Lithium-ion Batteries","authors":"Lin Sun, Lijun Wang, Yang Liu, Hongyu Wang, Zhong Jin","doi":"10.1039/d5ta00298b","DOIUrl":"https://doi.org/10.1039/d5ta00298b","url":null,"abstract":"In contrast to nanosilicon, micron-sized silicon anodes have regained widespread attention due to their high energy density, favorable processability, and reduced side reactions. However, these anodes are plagued by several significant challenges. They undergo substantial volume changes, suffer from sluggish lithium-ion transport kinetics and the loss of electrical contact. In this study, micron-sized porous silicon (pSi) obtained through acid etching of Al60Si40 alloy was utilized as the starting material. A novel approach combining high-energy ball milling and wet chemistry methods was adopted to dope Ge atoms into pSi and modify it with liquid GaInSn metal (LM) alloy (Designated as pSi/Ge@LM). The incorporation of Ge heteroatoms and LM offers multiple benefits. Firstly, it enhances the tap density of pSi. Secondly, it effectively boosts the electron transport performance of the material. Moreover, the excellent metallic properties and liquid fluidity of LM endow it with a unique \"self-healing\" function. Both the half-cells and full-cells assembled with pSi/Ge@LM electrode demonstrate outstanding electrochemical performance. Specifically, In the half-cells, when cycled at a current density of 1 A g-1 for 400 times, the pSi/Ge@LM electrode retains a remarkably high specific capacity of 1011 mAh g-1. Even at a high current density of 3 A g-1, it still delivers a reversible capacity of over 900 mAh g-1. It is anticipated that this research will offer novel insights and valuable guidance for the development of high-energy-density micron-sized silicon anodes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"12 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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