In Situ Anchoring Massive Isolated Pt Atoms at Cationic Vacancies of α-NixFe1-x(OH)2 to Regulate the Electronic Structure for Overall Water Splitting
In Situ Anchoring Massive Isolated Pt Atoms at Cationic Vacancies of α-NixFe1-x(OH)2 to Regulate the Electronic Structure for Overall Water Splitting
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DOI：
10.1002/adfm.202203342
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发表时间：
2022-05-16
影响因子：
19
通讯作者：
Zhou, Zhen
中科院分区：
文献类型：
--
作者：
Wang, Liming;Zhang, Lili;Zhou, Zhen
合理的单原子催化剂的设计和制备为显着提高电催化裂解水的活性提供了一种很有前途的策略。尤其是锚定在阳离子空位上的单原子可以提高催化剂的稳定性，改善反应动力学。在本工作中，通过用H_2PtCl6氧化Fe2+的方法，在层状的α-Ni2/3Fe1/3(OH)(2)上负载了铂单原子，具体地说，铂原子固定在原位产生的铁阳离子空位上，得到了稳定的铂单原子在α-Ni2/3Fe1/3(OH)(2)表面，最大负载量约为6.15wt%。铂单原子不仅可以作为析氢反应的活性中心，还可以调节NiFe氢氧化物的电子结构，激活与铂相邻的Ni原子进行析氧反应。因此，用这种双功能催化剂组装的裂水电解槽，比分别以RuO2和20wt%的铂/C催化剂为阳极和阴极的电解槽具有更小的过电位，并能有效地将太阳能转化为氢。结果表明，单原子铂催化剂具有成本低、负载量大、制备工艺简单等特点，具有实际应用价值。
Rational design and preparation of single-atom catalysts provide a promising strategy to significantly improve the electrocatalytic activity for water splitting. In particular, single atoms anchored at cationic vacancies can enhance the stability of the catalysts and improve reaction kinetics. In this work, Pt single atoms are loaded at layered alpha-Ni2/3Fe1/3(OH)(2) by oxidizing Fe2+ with H2PtCl6, and specifically, Pt atoms are anchored at in situ generated iron cationic vacancies during the process, resulting in stabilized Pt single atoms in the surface of alpha-Ni2/3Fe1/3(OH)(2) with the maximum loading of approximate to 6.15 wt%. The Pt single atoms not only act as active sites for hydrogen evolution reaction but also regulate the electronic structure of NiFe hydroxides and activate Ni atoms adjacent to Pt for oxygen evolution reaction. Therefore, the water-splitting electrolyzer assembled with such a bifunctional catalyst shows a smaller overpotential than that with RuO2 and 20 wt% Pt/C catalysts as the anode and cathode, respectively, and efficient solar-to-hydrogen conversion. The results demonstrate the practical application of single-atom Pt catalysts with low cost, large loading, and facile preparation route.