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Developing a stable and high-performance W-CoMnP electrocatalyst by mitigating the Jahn-Teller effect through W doping strategy
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作者 bohan an Xin Li +6 位作者 Weilong Liu Jipeng Dong Ruichao Bian Luyao Zhang Ning Li Yangqin Gao Lei Ge 《Chinese Journal of Catalysis》 2025年第7期264-278,共15页
Manganese-based materials are influenced by the Jahn-Teller effect,causing the spontaneous dismutation of Mn^(3+)(2Mn^(3+)→Mn^(2+)+Mn^(4+))and the dissolution of Mn^(2+),which often results in diminished activity.Thi... Manganese-based materials are influenced by the Jahn-Teller effect,causing the spontaneous dismutation of Mn^(3+)(2Mn^(3+)→Mn^(2+)+Mn^(4+))and the dissolution of Mn^(2+),which often results in diminished activity.This study uniquely employs a W doping strategy to suppress this effect.Externally,a simple template-free method was initially used to prepare cobalt-and manganese-based precursors,followed by a W doping process during the synthesis of transition bimetallic phosphides.Ultimately,W-doped bimetallic phosphides(W-CoMnP)were obtained.The W-CoMnP material demonstrates excellent HER and OER performance with low overpotentials of 95 mV(η_(₁₀)HER)and 225 mV(η_(₅₀)OER),and can achieve overall water splitting at a voltage of 1.52 V while maintaining stable cycling for 24 h.To enable commercial application,W-CoMnP was incorporated into an anion exchange membrane(AEM)electrolysis water device,demonstrating continuous and stable hydrogen production under ambient temperature conditions.This study offers a promising strategy for the future development of catalysts for AEM electrolysis water devices. 展开更多
关键词 Bimetallic phosphide Density functional theory calculation Jiang-Taylor effect W doping Anion exchange membrane water electrolysis device
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Atomic orbitals modulated dual functional bimetallic phosphides derived from MOF on MOF structure for boosting high efficient overall water splitting 被引量:1
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作者 bohan an Weilong Liu +3 位作者 Jipeng Dong Ning Li Yangqin Gao Lei Ge 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第10期113-125,共13页
The electronic modulation characteristics of efficient metal phosphide electrocatalysts can be utilized to tune the performance of oxygen evolution reaction(OER).However,improving the overall water splitting performan... The electronic modulation characteristics of efficient metal phosphide electrocatalysts can be utilized to tune the performance of oxygen evolution reaction(OER).However,improving the overall water splitting performance remains a challenging task.By building metal organic framework(MOF)on MOF heterostructures,an efficient strategy for controlling the electrical structure of MOFs was presented in this study.ZIF-67 was in-situ synthesized on MIL-88(Fe)using a two-step self-assembly method,followed by low-temperature phosphorization to ultimately synthesize FeP-CoP_(3)bimetallic phosphides.By combining atomic orbital theory and theoretical calculations(density functional theory),the results reveal the successful modulation of electronic orbitals in FeP-CoP_(3)bimetallic phosphides,which are synthesized from MOF on MOF structure.The synergistic impact of the metal center Co species and the phase conjugation of both kinds of MOFs are responsible for this regulatory phenomenon.Therefore,the catalyst demonstrates excellent properties,demonstrating HER 81 mV(η10)in a 1.0 mol L^(−1)KOH solution and OER 239 mV(η50)low overpotentials.The FeP-CoP_(3)linked dual electrode alkaline batteries,which are bifunctional electrocatalysts,have a good electrocatalytic ability and may last for 50 h.They require just 1.49 V(η50)for total water breakdown.Through this technique,the electrical structure of electrocatalysts may be altered to increase catalytic activity. 展开更多
关键词 Transition metal phosphides MOF on MOF Atomic orbital theory Density functional theory calculation
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过渡金属硫化物相关电催化剂的设计与应用研究 被引量:6
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作者 苏慧 姜静 +4 位作者 宋少佳 安博涵 李宁 高旸钦 戈磊 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2023年第1期7-49,共43页
自从国际社会提出“碳达峰、碳中和”目标以来,人们越来越意识到节约资源、保护环境、开发新能源的必要性.氢能(H_(2))作为最具竞争力的清洁能源之一,引起了研究人员的广泛关注.电化学全解水被认为是一种利用风能和太阳能产生氢气的有... 自从国际社会提出“碳达峰、碳中和”目标以来,人们越来越意识到节约资源、保护环境、开发新能源的必要性.氢能(H_(2))作为最具竞争力的清洁能源之一,引起了研究人员的广泛关注.电化学全解水被认为是一种利用风能和太阳能产生氢气的有效技术,其主要由两个半反应组成:析氧反应(OER)和析氢反应(HER).然而,在实际工业化生产过程中阳极反应动力学OER慢,能量转换效率低,阴极反应稳定性差,导致经济效益不理想,因此,急需开发和探索耐久高效的电催化剂.过渡金属硫化物因具有独特的结构特征、丰富的活性位点和可调控的电子性质和组成,而被广泛用于电化学全解水制氢.本文综述了过渡金属硫化物的合成方法,一般包括:水热(溶剂热)法、电化学沉积法、液相剥离法、化学气相沉积法和球磨法,并概述了不同方法的基本概念、合成步骤以及优缺点.总结了近年用于电催化领域中典型单一硫化物(包括MoS_(2),WS_(2),Co3S_(4),Ni_(3)S_(2)等)材料的合成方法和机理,明确了S元素在整个电催化过程中的重要作用.针对单一硫化物稳定性差、活性位点少、电化学活性不高的缺点,详细总结了双金属、多金属以及单原子、双原子硫化物的催化机理和催化性能.当采用复合、引入缺陷、空缺和形态调节等手段修饰时,能够有效调控金属硫化物的电子结构,增加活性位点数量,优化反应中间体的吸附能,降低OER过程的能垒,从而使多金属硫化物具有优异的电化学性能.最后,通过一些典型的研究结果揭示了过渡金属硫化物在水分子分裂过程中的结构特性变化原理,特别是对于多金属硫化物,活性位点可以是金属阳离子,而其他金属的引入将在一定程度上改变活性中心附近的电子结构和配位环境,进而改善材料的催化性能.尽管过渡金属硫化物在电催化领域的应用研究取得了一系列进展,但仍存在诸多挑战,距实际应用仍有较大差距.需要综合考虑经济、高性能、稳定性和环境友好等因素进行过渡金属硫化物催化材料的设计、制备和性能调控,并为大规模应用提供基础.同时,深入探索电催化机理有利于设计高效电催化剂和推动电催化领域的持续发展.综上,本文为新型电催化材料的制备和电催化全解水机理的深入研究提供一定的参考. 展开更多
关键词 过渡金属硫化物 析氢反应 析氧反应 全解水 电催化
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