Strong Oxide-Support Interaction over IrO(2) /V(2) O(5) for Efficient pH-Universal Water Splitting.
Strong Oxide-Support Interaction over IrO(2) /V(2) O(5) for Efficient pH-Universal Water Splitting.
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强氧化物 — 支持 IrO2/V2O5 相互作用，实现高效 pH — 通用水分解
DOI：
10.1002/advs.202104636
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发表时间：
2022-04
期刊：
影响因子：
15.1
通讯作者：
Wang, Yong
中科院分区：
文献类型：
--
作者：
Zheng, Xiaozhong;Qin, Minkai;Ma, Shuangxiu;Chen, Yuzhuo;Ning, Honghui;Yang, Rui;Mao, Shanjun;Wang, Yong
关键词：
构建强氧化物-载体相互作用（SOSI）对于调节负载型催化剂的原子构型和电子结构是引人注目的。本文中，超细氧化铱纳米团簇（约1 nm）通过SOSI锚定在氧化钒载体（IrO 2/V2 O 5）上。发现具有独特扭曲IrO 2结构的原样催化剂可显著提高pH-通用析氧反应（OER）的性能。根据实验结果和理论计算，IrO 2/V2 O 5中具有柔性氧化还原态的IrO 2活性中心作为亲电中心，平衡了氧代-中间体的吸附，有效促进了O-O耦合过程，最终推动了水氧化的快速周转.结果，IrO 2/V2 O 5不仅在10 mA cm-2时表现出超低过电位（266 mV，pH = 0; 329 mV，pH = 7; 283 mV，pH = 14），而且在宽pH范围内具有高性能的整体水电解，电位仅为1.50 V（pH = 0），10 mA cm−2时为1.65 V（pH = 7）或1.49 V（pH = 14）。此外，SOSI可以同时保护扭曲的活性中心，从而显着提高催化稳定性，使其成为开发高性能催化体系的一种有前途的策略。在这里，通过强氧化物-载体相互作用（SOSI）成功制备了高分散的IrO 2/V2 O 5催化剂，IrO 2/V2 O 5中具有灵活氧化还原态的扭曲IrO 2活性中心作为亲电中心，平衡了氧代中间体的吸附，有效地推动了水氧化的快速周转，最终实现了在宽pH范围内的高性能水裂解。
Constructing strong oxide‐support interaction (SOSI) is compelling for modulating the atomic configurations and electronic structures of supported catalysts. Herein, ultrafine iridium oxide nanoclusters (≈1 nm) are anchored on vanadium oxide support (IrO2/V2O5) via SOSI. The as made catalyst, with a unique distorted IrO2 structure, is discovered to significantly boost the performance for pH‐universal oxygen evolution reaction (OER). Based on experimental results and theoretical calculations, the distorted IrO2 active sites with flexible redox states in IrO2/V2O5 server as electrophilic centers balance the adsorption of oxo‐intermediates and effectively facilitate the process of O—O coupling, eventually propelling the fast turnover of water oxidation. As a result, IrO2/V2O5 demonstrates not only ultralow overpotentials at 10 mA cm−2 (266 mV, pH = 0; 329 mV, pH = 7; 283 mV, pH = 14) for OER, but also high‐performance overall water electrolysis over a broad pH range, with a potential of mere 1.50 V (pH = 0), 1.65 V (pH = 7) or 1.49 V (pH = 14) at 10 mA cm−2. In addition, SOSI can simultaneously secure the distorted active sites and thus remarkably improving the catalytic stability, making it a promising strategy to develop high‐performance catalytic systems. Here, highly dispersed IrO2/V2O5 catalyst is successfully manufactured via strong oxide‐support interaction (SOSI), the distorted IrO2 active sites with flexible redox states in IrO2/V2O5 server as electrophilic centers to balance the adsorption of oxo‐intermediates and effectively propel the fast turnover of water oxidation, eventually achieving high‐performance water splitting in a wide pH range.
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