Jingwei Wang, Lejuan Cai, Zhipeng Yu, Hao Tan, Xinyi Xiang, Kaiyang Xu, Yang Chao, Sitaramanjaneya Mouli Thalluri, Fei Lin, Haoliang Huang, Chenyue Zhang, Yang Zhao, Wenlong Wang, Lifeng Liu
Proton exchange membrane water electrolysis (PEMWE) is considered a promising technology for green hydrogen production in combination with renewable energy. However, the high cost and particularly the scarcity of iridium (Ir) for use as oxygen evolution reaction (OER) catalysts in the anode severely impede large-scale deployment of PEMWE. Herein, we report the synthesis of oxygen-defective ruthenium oxide (HP-RuOx), which can serve as a cost-effective alternative to Ir-based catalysts, showing outstanding electrocatalytic performance for acidic OER. HP-RuOx was obtained through a sol-gel process using hexamethylenetetramine (HMTA) and polyvinylpyrrolidone (PVP) as co-surfactants. The defect-rich nature of HP-RuOx proves to be effective in enhancing the catalytic activity toward acidic OER. Specifically, HP-RuOx exhibits an overpotential of only 237 mV at a current density of 10 mA cm-2 in 0.05 M H2SO4, outperforming commercial RuO2 and other RuOx control catalysts. Both in-situ differential electrochemical mass spectrometry (DEMS) studies and theoretical calculations reveal that the OER occurring on HP-RuOx proceeds predominantly through the absorbate evolution mechanism (AEM) and the lattice oxygen barely participates in the OER. Consequently, the defect-rich HP-RuOx demonstrates good electrocatalytic stability in 0.05 M H2SO4, with only 90 mV potential increase after 140 hours of OER at 100 mA cm-2. Furthermore, the performance of HP-RuOx is also evaluated in membrane electrode assemblies (MEAs), which can reach 1 A cm-2 at 1.60 V at 60 ℃ and stably operate at 0.5 A cm-2 for 230 hours with minimal degradation, showing substantial potential for use as efficient and durable OER catalysts in PEMWE.
质子交换膜水电解法（PEMWE）被认为是一种结合可再生能源进行绿色制氢的前景广阔的技术。然而，用于阳极氧进化反应（OER）催化剂的铱（Ir）的高成本和稀缺性严重阻碍了 PEMWE 的大规模应用。在此，我们报告了氧缺陷氧化钌（HP-RuOx）的合成过程，它可以作为铱基催化剂的一种具有成本效益的替代品，在酸性 OER 中显示出卓越的电催化性能。HP-RuOx 是以六亚甲基四胺（HMTA）和聚乙烯吡咯烷酮（PVP）为辅助表面活性剂，通过溶胶-凝胶工艺获得的。事实证明，HP-RuOx 的富缺陷特性可有效提高其对酸性 OER 的催化活性。具体来说，在 0.05 M H2SO4 中，当电流密度为 10 mA cm-2 时，HP-RuOx 的过电位仅为 237 mV，优于商用 RuO2 和其他 RuOx 控制催化剂。原位差分电化学质谱（DEMS）研究和理论计算均表明，HP-RuOx 上发生的 OER 主要通过吸收演化机制（AEM）进行，晶格氧几乎不参与 OER。因此，富含缺陷的 HP-RuOx 在 0.05 M H2SO4 中表现出良好的电催化稳定性，在 100 mA cm-2 的条件下进行 140 小时的 OER 后，电位仅增加 90 mV。此外，还在膜电极组件（MEA）中对 HP-RuOx 的性能进行了评估，结果表明，在 60 ℃、1.60 V 的条件下，HP-RuOx 可达到 1 A cm-2，并可在 0.5 A cm-2 的条件下稳定运行 230 小时，且降解极小。
{"title":"Oxygen-defective ruthenium oxide as an efficient and durable electrocatalyst for acidic oxygen evolution reaction","authors":"Jingwei Wang, Lejuan Cai, Zhipeng Yu, Hao Tan, Xinyi Xiang, Kaiyang Xu, Yang Chao, Sitaramanjaneya Mouli Thalluri, Fei Lin, Haoliang Huang, Chenyue Zhang, Yang Zhao, Wenlong Wang, Lifeng Liu","doi":"10.1039/d4ta06592a","DOIUrl":"https://doi.org/10.1039/d4ta06592a","url":null,"abstract":"Proton exchange membrane water electrolysis (PEMWE) is considered a promising technology for green hydrogen production in combination with renewable energy. However, the high cost and particularly the scarcity of iridium (Ir) for use as oxygen evolution reaction (OER) catalysts in the anode severely impede large-scale deployment of PEMWE. Herein, we report the synthesis of oxygen-defective ruthenium oxide (HP-RuOx), which can serve as a cost-effective alternative to Ir-based catalysts, showing outstanding electrocatalytic performance for acidic OER. HP-RuOx was obtained through a sol-gel process using hexamethylenetetramine (HMTA) and polyvinylpyrrolidone (PVP) as co-surfactants. The defect-rich nature of HP-RuOx proves to be effective in enhancing the catalytic activity toward acidic OER. Specifically, HP-RuOx exhibits an overpotential of only 237 mV at a current density of 10 mA cm-2 in 0.05 M H2SO4, outperforming commercial RuO2 and other RuOx control catalysts. Both in-situ differential electrochemical mass spectrometry (DEMS) studies and theoretical calculations reveal that the OER occurring on HP-RuOx proceeds predominantly through the absorbate evolution mechanism (AEM) and the lattice oxygen barely participates in the OER. Consequently, the defect-rich HP-RuOx demonstrates good electrocatalytic stability in 0.05 M H2SO4, with only 90 mV potential increase after 140 hours of OER at 100 mA cm-2. Furthermore, the performance of HP-RuOx is also evaluated in membrane electrode assemblies (MEAs), which can reach 1 A cm-2 at 1.60 V at 60 ℃ and stably operate at 0.5 A cm-2 for 230 hours with minimal degradation, showing substantial potential for use as efficient and durable OER catalysts in PEMWE.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"22 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600084","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}
Retraction of ‘Thermally reduced graphene oxide/polymelamine formaldehyde nanocomposite as a high specific capacitance electrochemical supercapacitor electrode’ by Ali A. Ensafi et al., J. Mater. Chem. A, 2018, 6, 6045–6053, https://doi.org/10.1039/C7TA10825G.
撤回 Ali A. Ensafi 等人撰写的 "作为高比电容电化学超级电容器电极的热还原氧化石墨烯/聚甲醛胺纳米复合材料"，J. Mater.Chem.a，2018，6，6045-6053，https://doi.org/10.1039/C7TA10825G。
{"title":"Retraction: Thermally reduced graphene oxide/polymelamine formaldehyde nanocomposite as a high specific capacitance electrochemical supercapacitor electrode","authors":"Ali A. Ensafi, Hossein A. Alinajafi, B. Rezaei","doi":"10.1039/d4ta90211d","DOIUrl":"https://doi.org/10.1039/d4ta90211d","url":null,"abstract":"Retraction of ‘Thermally reduced graphene oxide/polymelamine formaldehyde nanocomposite as a high specific capacitance electrochemical supercapacitor electrode’ by Ali A. Ensafi <em>et al.</em>, <em>J. Mater. Chem. A</em>, 2018, <strong>6</strong>, 6045–6053, https://doi.org/10.1039/C7TA10825G.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"80 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600073","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}
Xinyu Cheng, Yuke Wang, Jia Lu, Wangqi Dai, Huanhao Lei, Jinning Zuo, Hong Li, Zhengwen Fu
Lithium-rich materials (LRM), which hold promise as high-energy-density cathodes, face challenges due to irreversible oxygen evolution. This leads to rapid capacity decay and structural instability. In this work, a regulated oxygen redox reaction is achieved by constructing an ultrathin and uniform Al2O3-doped ZnO (AZO) layer on LRM (AZO–LRM). The AZO coating layer serves as a charge carrier layer that can generate an internal electric field, thereby suppressing the migration of anions. A space charge layer is formed at the interface between AZO and LRM due to electron transfer, significantly reducing the non-bonding orbital energy and restraining oxidation of surface oxygen in LRM. Benefiting from regulated oxygen redox, AZO–LRM shows reduced phase degradation and fewer side reactions, resulting in a thinner, improved cathode electrolyte interphase (CEI) and more complete layered structure, significantly enhancing Li-ion diffusion and reducing impedance. Consequently, AZO–LRM retains 91% of its capacity after 200 cycles and shows a 145 mA h g−1 capacity at a 5C rate. This work provides a universal and low-cost solution to oxygen evolution in LRM, offering a promising approach to overcome practical application challenges and highlighting the potential of doped oxides in high-voltage cathode materials.
{"title":"Regulating oxygen redox reactions in lithium-rich materials via an Al2O3-doped ZnO layer for enhanced stability and performance","authors":"Xinyu Cheng, Yuke Wang, Jia Lu, Wangqi Dai, Huanhao Lei, Jinning Zuo, Hong Li, Zhengwen Fu","doi":"10.1039/d4ta06843b","DOIUrl":"https://doi.org/10.1039/d4ta06843b","url":null,"abstract":"Lithium-rich materials (LRM), which hold promise as high-energy-density cathodes, face challenges due to irreversible oxygen evolution. This leads to rapid capacity decay and structural instability. In this work, a regulated oxygen redox reaction is achieved by constructing an ultrathin and uniform Al<small><sub>2</sub></small>O<small><sub>3</sub></small>-doped ZnO (AZO) layer on LRM (AZO–LRM). The AZO coating layer serves as a charge carrier layer that can generate an internal electric field, thereby suppressing the migration of anions. A space charge layer is formed at the interface between AZO and LRM due to electron transfer, significantly reducing the non-bonding orbital energy and restraining oxidation of surface oxygen in LRM. Benefiting from regulated oxygen redox, AZO–LRM shows reduced phase degradation and fewer side reactions, resulting in a thinner, improved cathode electrolyte interphase (CEI) and more complete layered structure, significantly enhancing Li-ion diffusion and reducing impedance. Consequently, AZO–LRM retains 91% of its capacity after 200 cycles and shows a 145 mA h g<small><sup>−1</sup></small> capacity at a 5C rate. This work provides a universal and low-cost solution to oxygen evolution in LRM, offering a promising approach to overcome practical application challenges and highlighting the potential of doped oxides in high-voltage cathode materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"61 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600076","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}
This research explores the intricacies of oxygen exchange kinetics in Pr4Ni3O10+δ (PNO), aiming to assess its potential as a viable cathode material for solid oxide fuel cell applications. Utilizing a multifaceted approach, advanced techniques such as electrical conductivity relaxation, pulse isotopic exchange, and oxygen permeation are employed. A comparative analysis with other promising cathode materials, specifically La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF6428), reveals PNO superior performance. At 650 °C, PNO demonstrates an order of magnitude higher chemical diffusion exchange coefficient, Dchem, than LSCF6428, and its surface exchange coefficient, kchem, surpasses LSCF6428 by one and a half orders of magnitude. Long-term stability assessment through 1000 h electrical conductivity relaxation testing at 700 °C confirms PNO consistent performance. Oxygen permeation studies reveal an inverse correlation between membrane thickness and permeation rate. Notably, PNO demonstrates an impressive two-fold higher oxygen flux compared to LSCF6428. Furthermore, PNO maintains stable oxygen permeation over 1000 h at 700 °C, contrasting with an observed 11% degradation in LSCF6428. X-ray diffraction and scanning electron microscopy analyses corroborate PNO stability, while secondary phase formation observed in LSCF6428 contributes to its degradation. The pulse isotopic exchange measurements conducted on the fractionated powder of PNO within the temperature range of 350-450 °C provide valuable insights into the surface exchange mechanism. These measurements reveal that at highest oxygen partial pressure (pO2) values covered by the experiments, the relative rates of dissociative adsorption, ℜads, and oxygen incorporation, ℜinc, engage in competitive oxygen exchange dynamics. Conversely, at the lower pO2 values, oxygen exchange is predominantly limited by ℜads.
{"title":"Enhanced oxygen exchange kinetics and long-term stability of Ruddlesden-Popper phase Pr4Ni3O10+δ cathode for solid oxide fuel cells","authors":"Saim Saher, Affaq Qamar, Chou Yong Tan, Singh Ramesh, Walied Alfraidi","doi":"10.1039/d4ta01845a","DOIUrl":"https://doi.org/10.1039/d4ta01845a","url":null,"abstract":"This research explores the intricacies of oxygen exchange kinetics in Pr4Ni3O10+δ (PNO), aiming to assess its potential as a viable cathode material for solid oxide fuel cell applications. Utilizing a multifaceted approach, advanced techniques such as electrical conductivity relaxation, pulse isotopic exchange, and oxygen permeation are employed. A comparative analysis with other promising cathode materials, specifically La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF6428), reveals PNO superior performance. At 650 °C, PNO demonstrates an order of magnitude higher chemical diffusion exchange coefficient, Dchem, than LSCF6428, and its surface exchange coefficient, kchem, surpasses LSCF6428 by one and a half orders of magnitude. Long-term stability assessment through 1000 h electrical conductivity relaxation testing at 700 °C confirms PNO consistent performance. Oxygen permeation studies reveal an inverse correlation between membrane thickness and permeation rate. Notably, PNO demonstrates an impressive two-fold higher oxygen flux compared to LSCF6428. Furthermore, PNO maintains stable oxygen permeation over 1000 h at 700 °C, contrasting with an observed 11% degradation in LSCF6428. X-ray diffraction and scanning electron microscopy analyses corroborate PNO stability, while secondary phase formation observed in LSCF6428 contributes to its degradation. The pulse isotopic exchange measurements conducted on the fractionated powder of PNO within the temperature range of 350-450 °C provide valuable insights into the surface exchange mechanism. These measurements reveal that at highest oxygen partial pressure (pO2) values covered by the experiments, the relative rates of dissociative adsorption, ℜads, and oxygen incorporation, ℜinc, engage in competitive oxygen exchange dynamics. Conversely, at the lower pO2 values, oxygen exchange is predominantly limited by ℜads.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"67 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600082","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}
Febri Baskoro, Santosh U. Sharma, Andre Lammiduk Lubis, Hung-Ju Yen
Lithium-ion batteries stand at the forefront of energy storage technologies, facilitating the transition towards sustainable and electrified systems. To meet the increasing demands for energy density, safety, and longevity, the development of high-performance electrode materials is paramount. Although inorganic materials have been dominated in the current lithium-ion battery cathodes, the widely utilized inorganic cathode materials suffer from drawbacks such as limited capacity, high energy consumption during production, safety hazards associated with toxic metals (Li, Co, Mn, Ni), and high raw material costs due to the limited or localized resource distributions. Alternatively, polymeric materials have been seen and considered as a promising candidate to replace conventional inorganic materials, due to their advantages such as abundance and environmentally friendly resources, structural diversity, ease of functionalization, fabrication, and recycling, high capacity and rate capability, and excellent flexibility. This review article explores the strategic design principles underlying the synthesis and optimization of p-type polymeric electrode materials for next-generation 4.0 V-class batteries. Through a comprehensive analysis of recent advancements, morphology control, and interface engineering, this review elucidates the key strategies employed to achieve high-energy-density electrodes. Additionally, this review discusses the fundamental mechanisms governing the electrochemical performance of p-type polymeric electrodes and highlights emerging trends and future directions in the field. By integrating insights from materials science, electrochemistry, and engineering, this paper provides a roadmap for the rational design and development of p-type polymeric electrode materials towards the realization of high-performance 4.0 V-class lithium-ion batteries.
锂离子电池处于储能技术的最前沿，有助于向可持续和电气化系统过渡。为了满足对能量密度、安全性和寿命日益增长的需求，开发高性能电极材料至关重要。虽然目前的锂离子电池正极材料以无机材料为主，但广泛使用的无机正极材料存在容量有限、生产过程中能耗高、有毒金属（锂、钴、锰、镍）带来的安全隐患以及因资源分布有限或局部分布而导致的原材料成本高昂等缺点。另外，高分子材料具有资源丰富、环境友好、结构多样、易于功能化、制造和回收、容量大、速率高、灵活性强等优点，因此被视为替代传统无机材料的理想候选材料。这篇综述文章探讨了用于下一代 4.0 V 级电池的 p 型聚合物电极材料的合成和优化所依据的战略设计原则。通过对最新进展、形态控制和界面工程的全面分析，本综述阐明了实现高能量密度电极的关键策略。此外，本综述还讨论了制约 p 型聚合物电极电化学性能的基本机制，并重点介绍了该领域的新兴趋势和未来发展方向。通过整合材料科学、电化学和工程学的观点，本文为合理设计和开发对型聚合物电极材料，实现高性能 4.0 V 级锂离子电池提供了路线图。
{"title":"Recent Advances p-type Polymeric Electrode Materials towards High-Voltage 4.0 V-class Organic Lithium-ion Batteries","authors":"Febri Baskoro, Santosh U. Sharma, Andre Lammiduk Lubis, Hung-Ju Yen","doi":"10.1039/d4ta06028h","DOIUrl":"https://doi.org/10.1039/d4ta06028h","url":null,"abstract":"Lithium-ion batteries stand at the forefront of energy storage technologies, facilitating the transition towards sustainable and electrified systems. To meet the increasing demands for energy density, safety, and longevity, the development of high-performance electrode materials is paramount. Although inorganic materials have been dominated in the current lithium-ion battery cathodes, the widely utilized inorganic cathode materials suffer from drawbacks such as limited capacity, high energy consumption during production, safety hazards associated with toxic metals (Li, Co, Mn, Ni), and high raw material costs due to the limited or localized resource distributions. Alternatively, polymeric materials have been seen and considered as a promising candidate to replace conventional inorganic materials, due to their advantages such as abundance and environmentally friendly resources, structural diversity, ease of functionalization, fabrication, and recycling, high capacity and rate capability, and excellent flexibility. This review article explores the strategic design principles underlying the synthesis and optimization of p-type polymeric electrode materials for next-generation 4.0 V-class batteries. Through a comprehensive analysis of recent advancements, morphology control, and interface engineering, this review elucidates the key strategies employed to achieve high-energy-density electrodes. Additionally, this review discusses the fundamental mechanisms governing the electrochemical performance of p-type polymeric electrodes and highlights emerging trends and future directions in the field. By integrating insights from materials science, electrochemistry, and engineering, this paper provides a roadmap for the rational design and development of p-type polymeric electrode materials towards the realization of high-performance 4.0 V-class lithium-ion batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"36 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600079","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}
Flexible electrode materials have gained significant breakthroughs recently due to their freestanding nature and long-term stability. The integration of MXene into carbon nanofiber leads to improved conductivity and stability. Herein, we employed an electrospinning technique to prepare self-standing MXene (Ti3C2Tx) carbon nanofiber (MX-CNF), onto which a one-dimensional π–d conjugated conductive metal–organic framework (c-MOF) is uniformly coated, exhibiting outstanding properties. The enhanced specific capacitance and conductivity is due to π–d mode of electron transfer in c-MOF on MX-CNF leads to improved conductivity. The obtained composite material achieved a specific capacitance of 1076 F g−1 with an excellent rate capability and superior cycling retention of 86.4% after 15 000 cycles owing to its self-standing nature and ultra-stability. The electrode materials show better conductivity, hydrophilicity, and flexibility. A fabricated flexible asymmetric energy storage device achieved an energy density of 45.7 W h kg−1 with outstanding cycling stability. The flexible device was tested for different bending angles, maintaining its flexibility and ensuring no deformation occurred. The CV curves retains its orignal shapes at different bending angles. This work offers a new avenue for utilizing 1D conductive MOF on 2D material-based conductive nanofibers for flexible energy storage systems.
柔性电极材料因其独立特性和长期稳定性而在近期取得了重大突破。将 MXene 融入碳纳米纤维可提高导电性和稳定性。在此，我们采用电纺丝技术制备了自立MXene（Ti3C2Tx）碳纳米纤维（MX-CNF），并在其上均匀涂覆了一维π-d共轭导电金属有机框架（c-MOF），显示出卓越的性能。比电容和电导率的提高是由于 MX-CNF 上的 c-MOF 中的π-d 电子传递模式提高了电导率。所获得的复合材料的比电容达到了 1076 F g-1，具有出色的速率能力，由于其自立性质和超稳定性，在 15 000 次循环后，循环保持率高达 86.4%。电极材料具有更好的导电性、亲水性和柔韧性。制备的柔性非对称储能装置的能量密度达到 45.7 W h kg-1，并具有出色的循环稳定性。对柔性装置进行了不同弯曲角度的测试，测试结果表明，该装置保持了柔性，没有发生变形。在不同的弯曲角度下，CV 曲线都保持了原来的形状。这项工作为在基于二维材料的导电纳米纤维上利用一维导电 MOF 实现柔性储能系统提供了一条新途径。
{"title":"A π–d conjugated metal–organic framework decorated on a MXene-carbon nanofiber as a self-standing electrode for flexible supercapacitors","authors":"Zahir Abbas, Shaikh M. Mobin","doi":"10.1039/d4ta06232a","DOIUrl":"https://doi.org/10.1039/d4ta06232a","url":null,"abstract":"Flexible electrode materials have gained significant breakthroughs recently due to their freestanding nature and long-term stability. The integration of MXene into carbon nanofiber leads to improved conductivity and stability. Herein, we employed an electrospinning technique to prepare self-standing MXene (Ti<small><sub>3</sub></small>C<small><sub>2</sub></small>T<small><sub><em>x</em></sub></small>) carbon nanofiber (MX-CNF), onto which a one-dimensional π–d conjugated conductive metal–organic framework (c-MOF) is uniformly coated, exhibiting outstanding properties. The enhanced specific capacitance and conductivity is due to π–d mode of electron transfer in c-MOF on MX-CNF leads to improved conductivity. The obtained composite material achieved a specific capacitance of 1076 F g<small><sup>−1</sup></small> with an excellent rate capability and superior cycling retention of 86.4% after 15 000 cycles owing to its self-standing nature and ultra-stability. The electrode materials show better conductivity, hydrophilicity, and flexibility. A fabricated flexible asymmetric energy storage device achieved an energy density of 45.7 W h kg<small><sup>−1</sup></small> with outstanding cycling stability. The flexible device was tested for different bending angles, maintaining its flexibility and ensuring no deformation occurred. The CV curves retains its orignal shapes at different bending angles. This work offers a new avenue for utilizing 1D conductive MOF on 2D material-based conductive nanofibers for flexible energy storage systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"17 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600077","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}
MXenes and metal-organic frameworks (MOFs) are emerging as promising materials for integration into paper-based sensors (PSs), offering unique properties that can enhance sensor performance in various applications. MXenes, with their high conductivity and large surface area, and MOFs, known for their tunable porosity and chemical functionalities, bring distinct advantages to PSs. By leveraging the exceptional properties of MXenes and MOFs, researchers can develop PSs with improved sensitivity, selectivity, and stability, paving the way for advanced sensing platforms with diverse capabilities in environmental monitoring, healthcare diagnostics, and beyond. However, challenges are still existed in incorporating MXenes and MOFs into PSs, including sensitivity, stability, interference, and scalability. Addressing these challenges is crucial for optimizing sensor performance and reliability. Herein, recent developments pertaining to the applications of MXenes and MOFs in PSs are deliberated, focusing on challenges and future perspectives. By examining the unique properties of these materials, exploring innovative sensor designs, and discussing potential solutions to current challenges, this review seeks to pave the way for the development of next-generation PSs with enhanced sensitivity, selectivity, and reliability.
{"title":"Advancing Paper-Based Sensors with MXenes and MOFs: Exploring the Cutting-Edge Innovations","authors":"Sepehr Larijani, Atefeh Zarepour, Arezoo Khosravi, Siavash Iravani, Mahnaz Eskandari, Ali Zarrabi","doi":"10.1039/d4ta06561a","DOIUrl":"https://doi.org/10.1039/d4ta06561a","url":null,"abstract":"MXenes and metal-organic frameworks (MOFs) are emerging as promising materials for integration into paper-based sensors (PSs), offering unique properties that can enhance sensor performance in various applications. MXenes, with their high conductivity and large surface area, and MOFs, known for their tunable porosity and chemical functionalities, bring distinct advantages to PSs. By leveraging the exceptional properties of MXenes and MOFs, researchers can develop PSs with improved sensitivity, selectivity, and stability, paving the way for advanced sensing platforms with diverse capabilities in environmental monitoring, healthcare diagnostics, and beyond. However, challenges are still existed in incorporating MXenes and MOFs into PSs, including sensitivity, stability, interference, and scalability. Addressing these challenges is crucial for optimizing sensor performance and reliability. Herein, recent developments pertaining to the applications of MXenes and MOFs in PSs are deliberated, focusing on challenges and future perspectives. By examining the unique properties of these materials, exploring innovative sensor designs, and discussing potential solutions to current challenges, this review seeks to pave the way for the development of next-generation PSs with enhanced sensitivity, selectivity, and reliability.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"19 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600072","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}
Yi Ma, Luming Li, Jialing Tang, Zongkun Hu, Yong Zhang, Ning Jian, Huan Ge, Jun Zhao, Andreu Cabot, Junshan Li
Plastics have become an integral part of modern society due to their excellent mechanical properties, lightweight, chemical stability and low cost. However, their continuous production and use worldwide have resulted in a major environmental problem. In this context, the green degradation and upcycling of waste plastics using electrochemical oxidation present a promising solution. To make this solution practical, the development of cost-effective catalysts optimized for this reaction is essential. In this study, we propose a new catalyst for the electrocatalytic reforming of ethylene glycol (EG) derived from polyethylene terephthalate (PET) to formic acid. The catalyst comprises layered Ni-Co9S8 nanosheet arrays (NSAs) grown on nickel foam (NF) via hydrothermal method. Under EG oxidation reaction (EGOR) conditions, the Ni-Co9S8 NSAs/NF catalyst achieves Faraday efficiencies (FEs) of up to 92%. Additionally, the direct use of commercial PET plastic powder hydrolysate still enables FEs to formate to exceed 90%. These outstanding results are rationalized using density functional theory (DFT) calculations providing insights into the role of the different elements in the EGOR reaction.
{"title":"Electrochemical PET recycling to formate through ethylene glycol oxidation on Ni-Co-S nanosheet arrays","authors":"Yi Ma, Luming Li, Jialing Tang, Zongkun Hu, Yong Zhang, Ning Jian, Huan Ge, Jun Zhao, Andreu Cabot, Junshan Li","doi":"10.1039/d4ta07156e","DOIUrl":"https://doi.org/10.1039/d4ta07156e","url":null,"abstract":"Plastics have become an integral part of modern society due to their excellent mechanical properties, lightweight, chemical stability and low cost. However, their continuous production and use worldwide have resulted in a major environmental problem. In this context, the green degradation and upcycling of waste plastics using electrochemical oxidation present a promising solution. To make this solution practical, the development of cost-effective catalysts optimized for this reaction is essential. In this study, we propose a new catalyst for the electrocatalytic reforming of ethylene glycol (EG) derived from polyethylene terephthalate (PET) to formic acid. The catalyst comprises layered Ni-Co9S8 nanosheet arrays (NSAs) grown on nickel foam (NF) via hydrothermal method. Under EG oxidation reaction (EGOR) conditions, the Ni-Co9S8 NSAs/NF catalyst achieves Faraday efficiencies (FEs) of up to 92%. Additionally, the direct use of commercial PET plastic powder hydrolysate still enables FEs to formate to exceed 90%. These outstanding results are rationalized using density functional theory (DFT) calculations providing insights into the role of the different elements in the EGOR reaction.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"2 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600069","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}
N-ethylcarbazole (NEC) hydrogen storage has garnered significant attention owing to its large-scale safe storage of hydrogen superiority. However, the sluggish hydrogenation kinetics in NEC are extremely dependent on catalysts with superior catalytic activity and high selectivity. Numerous researches have demonstrated noble metal catalysts present the best catalytic performance in NEC hydrogen storage, but their high cost impedes widespread commercial applications. In contrast, non-noble metal catalysts effectively address the high-cost issue associated with noble metal catalysts. Furthermore, by optimizing the structural design of the catalysts and increasing the density of active sites, their catalytic performance can be significantly enhanced. This approach achieves a better balance between cost-effectiveness and catalytic efficiency. Therefore, this review first summarizes the synthetic methods and typical structures of NEC hydrogenation non-noble metal catalysts. Subsequently, the recent advances and catalytic mechanisms regarding non-noble metal catalysts for hydrogenation are discussed in detail. Finally, through in-depth analysis of potential problems and active exploration of future prospects, we can better guide the relevant research and application work in the future to continuously reach new heights.
N-乙基咔唑（NEC）储氢因其大规模安全储氢的优越性而备受关注。然而，NEC 中缓慢的氢化动力学极其依赖于具有卓越催化活性和高选择性的催化剂。大量研究表明，贵金属催化剂在 NEC 储氢中具有最佳的催化性能，但其高昂的成本阻碍了其广泛的商业应用。相比之下，非贵金属催化剂能有效解决贵金属催化剂的高成本问题。此外，通过优化催化剂的结构设计和增加活性位点密度，可以显著提高催化性能。这种方法在成本效益和催化效率之间实现了更好的平衡。因此，本综述首先总结了 NEC 加氢非贵金属催化剂的合成方法和典型结构。随后，详细讨论了非贵金属加氢催化剂的最新研究进展和催化机理。最后，通过对潜在问题的深入分析和对未来前景的积极探索，我们可以更好地指导今后的相关研究和应用工作，不断达到新的高度。
{"title":"Recent Advances on Non-noble Metal Catalysts toward N-ethylcarbazole Hydrogen Storage","authors":"Hansai Wu, junming Zhang, Zicong Wang, Xianglong Kong, Gaofu Li, Ying Zhao, Piaoping Yang, Zhiliang Liu","doi":"10.1039/d4ta06468b","DOIUrl":"https://doi.org/10.1039/d4ta06468b","url":null,"abstract":"N-ethylcarbazole (NEC) hydrogen storage has garnered significant attention owing to its large-scale safe storage of hydrogen superiority. However, the sluggish hydrogenation kinetics in NEC are extremely dependent on catalysts with superior catalytic activity and high selectivity. Numerous researches have demonstrated noble metal catalysts present the best catalytic performance in NEC hydrogen storage, but their high cost impedes widespread commercial applications. In contrast, non-noble metal catalysts effectively address the high-cost issue associated with noble metal catalysts. Furthermore, by optimizing the structural design of the catalysts and increasing the density of active sites, their catalytic performance can be significantly enhanced. This approach achieves a better balance between cost-effectiveness and catalytic efficiency. Therefore, this review first summarizes the synthetic methods and typical structures of NEC hydrogenation non-noble metal catalysts. Subsequently, the recent advances and catalytic mechanisms regarding non-noble metal catalysts for hydrogenation are discussed in detail. Finally, through in-depth analysis of potential problems and active exploration of future prospects, we can better guide the relevant research and application work in the future to continuously reach new heights.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"51 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600083","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}
Na3V2(PO4)3 (NVP) is recognized as one of the most promising NASICON-type cathodes for sodium-ion storage. Enhancing electronic conductivity and further ensuring long-term structural stability when activating the high-voltage V⁴⁺/V⁵⁺ redox reaction is crucial for the practical application of NVP cathodes. In this study, a high-entropy NVP with carbon coating (Na3V1.5(CrMnFeMgAl)0.5(PO4)3@C, HE-NVMP@C) has been designed and synthesized. Due to the enhanced electronic/ionic conductivity facilitated by the carbon coating and lattice distortion from the high-entropy effect, the HE-NVMP@C exhibits improved high-rate performance. Additionally, benefiting from the collaboration between the doped heteroatoms, the HE-NVMP@C can effectively activate V3+/V4+/V5+ redox reactions within the 2.5-4.3 V voltage window while maintaining excellent structural stability over extended cycles. This work provides an efficient approach to enhance the electrochemical performances of NASICON-type cathodes for sodium-ion batteries.
{"title":"Synergetic Effects from a High-Entropy NASICON-type Cathode for Advanced Sodium-Ion Batteries","authors":"Shouyue Wang, Taiding Xu, Huitao Leng, Shengyu Liang, Wei Zhang, Yuheng Jin, Jingxia Qiu, Sheng Li","doi":"10.1039/d4ta06950a","DOIUrl":"https://doi.org/10.1039/d4ta06950a","url":null,"abstract":"Na3V2(PO4)3 (NVP) is recognized as one of the most promising NASICON-type cathodes for sodium-ion storage. Enhancing electronic conductivity and further ensuring long-term structural stability when activating the high-voltage V⁴⁺/V⁵⁺ redox reaction is crucial for the practical application of NVP cathodes. In this study, a high-entropy NVP with carbon coating (Na3V1.5(CrMnFeMgAl)0.5(PO4)3@C, HE-NVMP@C) has been designed and synthesized. Due to the enhanced electronic/ionic conductivity facilitated by the carbon coating and lattice distortion from the high-entropy effect, the HE-NVMP@C exhibits improved high-rate performance. Additionally, benefiting from the collaboration between the doped heteroatoms, the HE-NVMP@C can effectively activate V3+/V4+/V5+ redox reactions within the 2.5-4.3 V voltage window while maintaining excellent structural stability over extended cycles. This work provides an efficient approach to enhance the electrochemical performances of NASICON-type cathodes for sodium-ion batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"25 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600064","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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