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利用离子浸出效应在具有自优化行为的混合纳米复合材料上实现高析氧性能。

Utilizing ion leaching effects for achieving high oxygen-evolving performance on hybrid nanocomposite with self-optimized behaviors.

作者信息

Guan Daqin, Ryu Gihun, Hu Zhiwei, Zhou Jing, Dong Chung-Li, Huang Yu-Cheng, Zhang Kaifeng, Zhong Yijun, Komarek Alexander C, Zhu Ming, Wu Xinhao, Pao Chih-Wen, Chang Chung-Kai, Lin Hong-Ji, Chen Chien-Te, Zhou Wei, Shao Zongping

机构信息

State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, 211800, China.

Max-Planck-Institute for Chemical Physics of Solids, Nöthnitzer Str. 40, Dresden, 01187, Germany.

出版信息

Nat Commun. 2020 Jul 6;11(1):3376. doi: 10.1038/s41467-020-17108-5.

Abstract

Ion leaching from pure-phase oxygen-evolving electrocatalysts generally exists, leading to the collapse and loss of catalyst crystalline matrix. Here, different from previous design methodologies of pure-phase perovskites, we introduce soluble BaCl and SrCl into perovskites through a self-assembly process aimed at simultaneously tuning dual cation/anion leaching effects and optimizing ion match in perovskites to protect the crystalline matrix. As a proof-of-concept, self-assembled hybrid BaSrCoFeO (BSCF) nanocomposite (with BaCl and SrCl) exhibits the low overpotential of 260 mV at 10 mA cm in 0.1 M KOH. Multiple operando spectroscopic techniques reveal that the pre-leaching of soluble compounds lowers the difference of interfacial ion concentrations and thus endows the host phase in hybrid BSCF with abundant time and space to form stable edge/face-sharing surface structures. These self-optimized crystalline structures show stable lattice oxygen active sites and short reaction pathways between Co-Co/Fe metal active sites to trigger favorable adsorption of OH species.

摘要

从纯相析氧电催化剂中离子浸出普遍存在,这会导致催化剂晶体基质的坍塌和损失。在此,与之前纯相钙钛矿的设计方法不同,我们通过自组装过程将可溶性BaCl和SrCl引入钙钛矿中,旨在同时调节双阳离子/阴离子浸出效应并优化钙钛矿中的离子匹配,以保护晶体基质。作为概念验证,自组装的混合BaSrCoFeO(BSCF)纳米复合材料(含有BaCl和SrCl)在0.1 M KOH中,在10 mA cm时表现出260 mV的低过电位。多种原位光谱技术表明,可溶性化合物的预浸出降低了界面离子浓度的差异,从而赋予混合BSCF中的主体相充足的时间和空间来形成稳定的边/面共享表面结构。这些自优化的晶体结构显示出稳定的晶格氧活性位点以及Co-Co/Fe金属活性位点之间的短反应路径,以触发对OH物种的有利吸附。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d848/7338502/11a41c29a9aa/41467_2020_17108_Fig1_HTML.jpg

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