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工程化锰掺杂钼酸镍多孔纳米片的电子结构和氧空位用于高效析氧反应

Engineering electronic structures and oxygen vacancies of manganese-doped nickel molybdate porous nanosheets for efficient oxygen evolution reaction.

作者信息

Miao Fang, Cui Peng, Gu Tao, Sun Bo, Yan Zhijie

机构信息

College of Materials Science and Engineering, North University of China, Taiyuan, 030051, China; Defense Innovation Institute, Academy of Military Science, Beijing 100071, China; Shanxi Key Laboratory of Advanced Metal Materials for Special Environments, North University of China, Taiyuan 030051, China.

School of Materials Science and Engineering, Southeast University, Nanjing, 211189, China.

出版信息

J Colloid Interface Sci. 2024 Dec 15;676:680-690. doi: 10.1016/j.jcis.2024.07.118. Epub 2024 Jul 15.

Abstract

The design strategy of designing effective local electronic structures of active sites to improve the oxygen evolution reaction (OER) performance is the key to the success of sustainable alkaline water electrolysis processes. Herein, a series of manganese-doped nickel molybdate porous nanosheets with rich oxygen vacancies on the nickel foam (Mn-NiMoO/NF PNSs) synthesized by the facile hydrothermal and following annealing routes are used as high-efficiency and robust catalysts towards OER. By virtue of unique nanosheets architectures, more exposed active site, rich oxygen vacancies, tailored electronic structures, and improved electrical conductivity induced by Mn incorporation, as predicted, the optimized Mn-NiMoO/NF PNSs catalyst exhibits superior the OER performance with a low overpotential of 211 mV at 10 mA‧cm, a small Tafel slope of 41.7 mV‧dec, and an excellent stability for 100 h operated at 100 mA‧cm in 1.0 M KOH electrolyte. The in-situ Raman measurements reveal the surface dynamic reconstruction. Besides, the results of density functional theory (DFT) calculations unveil the reaction mechanism. This study provides an effective design strategy via Mn incorporation to synergistically engineer electronic structures and oxygen vacancies of metal oxides for efficiently boosting the OER performance.

摘要

设计活性位点的有效局部电子结构以提高析氧反应(OER)性能的策略是可持续碱性水电解过程成功的关键。在此,通过简便的水热法和后续退火路线合成的一系列在泡沫镍上具有丰富氧空位的锰掺杂钼酸镍多孔纳米片(Mn-NiMoO/NF PNSs)被用作高效且稳健的OER催化剂。凭借独特的纳米片结构、更多暴露的活性位点、丰富的氧空位、定制的电子结构以及因锰掺入而提高的电导率,如预期的那样,优化后的Mn-NiMoO/NF PNSs催化剂展现出优异的OER性能,在10 mA‧cm⁻²时过电位低至211 mV,塔菲尔斜率为41.7 mV‧dec⁻¹,并且在1.0 M KOH电解液中以100 mA‧cm⁻²运行100小时具有出色的稳定性。原位拉曼测量揭示了表面动态重构。此外,密度泛函理论(DFT)计算结果揭示了反应机理。本研究通过锰掺入提供了一种有效的设计策略,以协同调控金属氧化物的电子结构和氧空位,从而有效提升OER性能。

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