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| 1 | Recent advances in spinel-type electrocatalysts for bifunctional oxygen reduction and oxygen evolution reactions显示文摘The demand for efficient and environmentally-benign electrocatalysts that help availably harness the renewable energy resources is growing rapidly. In recent years, increasing insights into the design of water electrolysers, fuel cells, and metal–air batteries emerge in response to the need for developing sustainable energy carriers, in which the oxygen evolution reaction and the oxygen reduction reaction play key roles. However, both reactions suffer from sluggish kinetics that restricts the reactivity. Therefore, it is vital to probe into the structure of the catalysts to exploit high-performance bifunctional oxygen electrocatalysts. Spinel-type catalysts are a class of materials with advantages of versatility, low toxicity, low expense, high abundance, flexible ion arrangement, and multivalence structure. In this review, we afford a basic overview of spinel-type materials and then introduce the relevant theoretical principles for electrocatalytic activity, following that we shed light on the structure–property relationship strategies for spinel-type catalysts including electronic structure, microstructure, phase and composition regulation,and coupling with electrically conductive supports. We elaborate the relationship between structure and property, in order to provide some insights into the design of spinel-type bifunctional oxygen electrocatalysts. | Xiao-Meng Liu Xiaoyang Cui Kamran Dastafkan Hao-Fan Wang Cheng Tang Chuan Zhao Aibing Chen Chuanxin He Minghan Han Qiang Zhang | 2021 | Journal of Energy Chemistry2021,30,2: | 7 |
| 2 | 海胆状NiMoO_(4)纳米棒阵列作为高效双功能催化剂用于电催化及光伏驱动尿素电解显示文摘氢能因具有储量丰富、零排放和可再生等优点,受到各国在能源布局过程中的广泛关注.制氢是氢能源开发和利用的重要环节,其中电解水制氢技术可通过低能耗水分解获得氢气,具有很高的社会效益和经济效益.在电解水过程中,由于受析氧反应(OER)的缓慢动力学过程限制,电解水制氢体系在碱性介质中的理论工作电压高达1.23 V,增加了制氢能耗.在使用电化学催化剂的同时采用具有低热力学电势(0.37 V)的尿素氧化反应(UOR)代替OER,可降低制氢过程的能耗.本文采用水热反应结合煅烧反应在泡沫镍上生长了海胆状NiMoO_(4)纳米棒阵列,并将其作为双功能电催化剂,用于阴极析氢和阳极尿素氧化反应.结果表明,200℃煅烧产物(NiMoO_(4)-200/NF)表现出高效的析氢反应(HER)性能,在1.0 mol/L KOH中电流密度为10 mA cm^(-2)时的过电位仅为68 mV.而300℃煅烧产物(NiMoO_(4)-300/NF)表现出优异的析氧反应和尿素氧化反应活性.为了探究NiMoO_(4)纳米棒阵列在不同反应中催化性能差异的原因,通过各种表征手段对催化剂进行了结构及组成的表征.X射线衍射与高分辨透射电镜结果表明,200和300℃下的煅烧产物由NiMoO_(4)与NiMoO_(4)·xH_(2)O组成,而煅烧温度变化引起的电催化活性和选择性的差异则归因于产物不同的晶格氧含量.X射线光电子能谱结果表明,NiMoO_(4)-300/NF比NiMoO_(4)-200/NF含有更多的晶格氧;而对于高价态金属氧化物而言,催化剂中的晶格氧在电氧化过程中可以被激活并直接参与到阳极氧化反应过程,从而有利于析氧反应和尿素氧化反应的进行.另外,以NiMoO_(4)-300/NF和NiMoO_(4)-200/NF作为阳极和阴极组装尿素电解槽,可在1.38 V的电池电压下提供10 mA cm^(–2)的电流密度.将电极与商品太阳能板连接,NiMoO_(4)纳米棒阵列双电极可成功实现光电压驱动的尿素电解和制氢,表明其在太阳能驱动的能量转换方面具有巨大潜力. | 陈晨欣 何苏祺 Kamran Dastafkan 邹泽华 汪庆祥 赵川 | 2022 | Chinese Journal of Catalysis2022,43,5: | 1 |
| 3 | Super-exchange effect induced by early 3d metal doping on NiFe_(2)O_(4)(001)surface for oxygen evolution reaction显示文摘Understanding the intrinsic activity of oxygen evolution reaction(OER) is crucial for catalyst design.To date,different metal-doping strategies have been developed to achieve this,but the involving mechanisms remain unclear.Here,the electronic structure of the transition metal-doped NiFe_(2)O_(4)(001) surface is scrutinized for OER intrinsic activity using density functional theory calculations.Five 3d-orbital filling metals(Ti,V,Cr,Mn,and Co) are introduced as dopants onto A-and B-layers of the NiFe_(2)O_(4)(001) surface,and variation of oxidation states over Fe sites is observed on B-layer.Analyzing the magnetic moment and charge transfer of surface cation sites reveals that the variation of Fe oxidation states originates from the super-exchange effect and is influenced by the t2g-electron configuration of 3d metal dopants.This trend governs the generation of highly-active Fe3+sites on the B-layer,the adsorption strength of OER intermediates,i.e.,*O and*OH,and therefore the intrinsic activity.The finding of super-exchange mechanism induced by 3d early metal doping offers insights into electronic structure tailoring strategies for improving the intrinsic activity of OER electrocatalysts. | Shuhao Wang Xinyan Liu Xiang Chen Kamran Dastafkan Zhong-Heng Fu Xin Tan Qiang Zhang Chuan Zhao | 2023 | Journal of Energy Chemistry2023,,3: | 0 |
| 4 | Common Pitfalls of Reporting Electrocatalysts for Water Splitting显示文摘Rigorous assessment of heterogeneous electrocatalysts for electrochemical water splitting has been a critical issue mainly due to insufficient standard protocols to measure and report experimental data.In this perspective,we highlight some common pitfalls when measuring and reporting electrocatalytic data,which should be avoided to ensure the accuracy and reproducibility and to advance the water splitting field.We advocate to prevent the introduction of artefacts from the counter and reference electrodes,as well as the impurities in the electrolyte when conducting electrocatalyst activity measurements.In addition,we encourage the use of the electrochemically active surface area(ECSA)-normalized current densities to represent the intrinsic activity of the reported catalysts for a better comparison with previously known materials.Suitable ECSA measurement methods should be employed based on the nature of catalysts.Recommendations made in this perspective will hopefully assist in identifying advanced catalysts for water splitting research. | WANG Yuan ARANDIYAN Hamidreza DASTAFKAN Kamran LI Yibing ZHAO Chuan | 2020 | Chemical Research in Chinese Universities2020,36,3: | 0 |