确定 Fe 作为 OER 活性位点和用于整体水分解的超低成本双功能电催化剂,Small

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确定 Fe 作为 OER 活性位点和用于整体水分解的超低成本双功能电催化剂
Small ( IF 13.0 ) Pub Date : 2023-05-05 , DOI: 10.1002/smll.202301715
Bo Li _{1,

2,

3,

4} , Jun Zhao _{2,

3} , Yishang Wu ₅ , Guobin Zhang _{1,

2,

3,

4} , Haikun Wu ₆ , Fucong Lyu _{1,

4,

7} , Jun He ₈ , Jun Fan _{2,

3} , Jian Lu _{1,

3,

4,

7} , Yang Yang Li _{1,

2,

3,

4,

7}

Affiliation

Hong Kong Branch of National Precious Metals Material Engineering Research Centre, City University of Hong Kong, Hong Kong, 999077, China.
Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Hong Kong, 999077, China.
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, 999077, China.
Department of Mechanical Engineering, Greater Bay Joint Division, Shenyang National Laboratory for Materials Science, City University of Hong Kong, Hong Kong, 999077, China.
Department of Chemistry, University of Science and Technology of China, Hefei, 230026, China.
Department of Chemistry, City University of Hong Kong, Hong Kong, 999077, China.
Centre for Advanced Structural Materials, City University of Hong Kong Shenzhen Research Institute, Greater Bay Joint Division, Shenyang National Laboratory for Materials Science, 8 Yuexing 1st Road, Shenzhen Hi-Tech Industrial Park, Nanshan District, Shenzhen, 518057, China.
School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, China.

基于Fe和其他过渡金属的电催化剂被认为是加速析氧反应（OER）最有希望的候选者，而Fe是否是OER的催化活性位点仍存在争议。在此，一元 Fe 基和二元 FeNi 基催化剂 FeOOH 和 FeNi(OH) _x是通过自重构产生的。前者是双相FeOOH，具有丰富的氧空位（V _O）和混合价态，在迄今为止报道的所有一元铁氧化物和氢氧化物基粉末催化剂中具有最高的OER性能，负载Fe可以催化积极参与开放教育资源 (OER)。对于二元催化剂，FeNi(OH) _x的制备具有以下特点：1) 等摩尔含量的 Fe 和 Ni 以及 2) 富含 V2O _，这两者对于实现丰富的稳定反应中心至关重要 (  Fe  OOH  Ni ）以获得高 OER 性能。发现 Fe 在 *OOH 过程中被氧化为 3.5+，因此，Fe 被确定为这种新型层状双氢氧化物 (LDH) 结构中的活性位点，其中 Fe:Ni = 1:1。此外，最大化的催化中心使FeNi(OH) _x @NF（泡沫镍）成为用于整体水分解的低成本双功能电极，具有可与基于贵金属的商业电极相媲美的优异性能，克服了商业化的主要障碍双功能电极：成本高昂。

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Identifying Fe as OER Active Sites and Ultralow-Cost Bifunctional Electrocatalysts for Overall Water Splitting

Electrocatalysts based on Fe and other transition metals are regarded as most promising candidates for accelerating the oxygen evolution reaction (OER), whereas whether Fe is the catalytic active site for OER is still under debate. Here, unary Fe- and binary FeNi- based catalysts, FeOOH and FeNi(OH)_x, are produced by self-reconstruction. The former is a dual-phased FeOOH, possessing abundant oxygen vacancies (V_O) and mixed-valence states, delivering the highest OER performance among all the unary iron oxides- and hydroxides- based powder catalysts reported to date, supporting Fe can be catalytically active for OER. As to binary catalyst, FeNi(OH)_x is fabricated featuring 1) an equal molar content of Fe and Ni and 2) rich V_O, both of which are found essential to enable abundant stabilized reactive centers (FeOOHNi) for high OER performance. Fe is found to be oxidized to 3.5+ during the *OOH process, thus, Fe is identified to be the active site in this new layered double hydroxide (LDH) structure with Fe:Ni = 1:1. Furthermore, the maximized catalytic centers enable FeNi(OH)_x@NF (nickel foam) as low-cost bifunctional electrodes for overall water-splitting, delivering excellent performance comparable to commercial electrodes based on precious metals, which overcomes a major obstacle to the commercialization of bifunctional electrodes: prohibitive cost.

更新日期：2023-05-05

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