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通过聚苯胺电子桥增强界面电子转移以调控动态重构并实现高性能水氧化。

Enhancing interfacial electron transfer through PANI electron bridge for tailoring dynamic reconstruction and achieving high-performance water oxidation.

作者信息

Xu Hui, Yang Lida, Jin Lei, Liu Yang, Wang Kun, Chen Jie, He Guangyu, Chen Haiqun

机构信息

Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Changzhou University, Changzhou, Jiangsu Province 213164, China.

Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Changzhou University, Changzhou, Jiangsu Province 213164, China.

出版信息

J Colloid Interface Sci. 2025 Jan;677(Pt A):158-166. doi: 10.1016/j.jcis.2024.07.224. Epub 2024 Jul 30.

Abstract

Tailoring the dynamic reconstruction of transition metal compounds into highly active oxyhydroxides through surface electron state modification is crucial for advancing water oxidation, yet remains a formidable challenge. In this study, a unique polyaniline (PANI) electron bridge was integrated into the metal-organic frameworks (MOFs)/layer double hydroxides (LDHs) heterojunction to expedite electron transfer from MOFs to LDHs, facilitating electron accumulation at the metal sites within MOF and electron-deficient LDHs. This configuration promotes the surface dynamic reconstruction of LDHs into highly active oxyhydroxides while safeguarding the MOF from corrosion in harsh environments over extended periods. The optimized electronic structure modification of both MOFs and LDHs enhances reaction kinetics. The superior MIL-88B(Fe)@PANI@NiCo LDH catalyst achieved 10 mA∙cm at an overpotential of 202 mV and demonstrated stable operation for 120 h at this current density. This research introduces an innovative approach for guiding electron transfer and dynamic catalyst reconstruction by constructing a PANI electron bridge, potentially paving the way for more efficient catalytic systems.

摘要

通过表面电子态修饰将过渡金属化合物动态重构为高活性羟基氧化物对于推进水氧化反应至关重要,但仍然是一项艰巨的挑战。在本研究中,一种独特的聚苯胺(PANI)电子桥被整合到金属有机框架(MOFs)/层状双氢氧化物(LDHs)异质结中,以加速电子从MOFs向LDHs的转移,促进电子在MOF内的金属位点和缺电子的LDHs处积累。这种结构促进了LDHs向高活性羟基氧化物的表面动态重构,同时在长时间的恶劣环境中保护MOF不被腐蚀。对MOFs和LDHs的优化电子结构修饰增强了反应动力学。优化后的MIL-88B(Fe)@PANI@NiCo LDH催化剂在202 mV的过电位下实现了10 mA∙cm的电流密度,并在此电流密度下稳定运行120 h。本研究通过构建PANI电子桥引入了一种指导电子转移和动态催化剂重构的创新方法,可能为更高效的催化系统铺平道路。

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