Li Bo-Quan, Xia Zi-Jing, Zhang Bingsen, Tang Cheng, Wang Hao-Fan, Zhang Qiang
Department of Chemical Engineering, Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Tsinghua University, Beijing, 100084, China.
Shenyang National Laboratory for Material Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, China.
Nat Commun. 2017 Oct 16;8(1):934. doi: 10.1038/s41467-017-01053-x.
Water oxidation represents the core process of many sustainable energy systems, such as fuel cells, rechargeable metal-air batteries, and water splitting. Material surface defects with high-energy hanging bonds possess superb intrinsic reactivity, whose actual performance is limited by the dimension and conductivity of the electrocatalyst. Herein we propose a surface defect-rich perovskite electrocatalyst through a p-block metal regulation concept to achieve high performance for oxygen evolution. As a typical p-metal, Sn dissolves from the solid phase from model SnNiFe perovskite nanodots, resulting in abundant surface defects with superior water oxidation performance. An oxygen pool model and a fusion-evolution mechanism are therefore proposed for the in-depth understanding of p-block metal regulation and the oxygen evolution reaction. The energy chemistry unveiled herein provides insights into water oxidation and helps to tackle critical issues in multi-electron oxygen electrocatalysis.Electrocatalysts that possess high densities of surface defects show great promise for efficient water oxidation. Here the authors demonstrate that regulating the p-block metal content in perovskite nanodots imparts these materials with abundant surface defects and excellent electrocatalytic activity.
水氧化是许多可持续能源系统的核心过程，如燃料电池、可充电金属空气电池和水分解。具有高能悬挂键的材料表面缺陷具有出色的本征反应活性，但其实际性能受到电催化剂尺寸和导电性的限制。在此，我们通过p区金属调控概念提出了一种富含表面缺陷的钙钛矿电催化剂，以实现高性能的析氧反应。作为典型的p区金属，Sn从模型SnNiFe钙钛矿纳米点的固相中溶解出来，产生大量具有优异水氧化性能的表面缺陷。因此，提出了一个氧池模型和一个融合演化机制，以深入理解p区金属调控和析氧反应。本文揭示的能量化学为水氧化提供了见解，并有助于解决多电子氧电催化中的关键问题。具有高密度表面缺陷的电催化剂在高效水氧化方面显示出巨大潜力。在此，作者证明了调节钙钛矿纳米点中的p区金属含量可使这些材料具有丰富的表面缺陷和优异的电催化活性。
