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用于碱性析氢反应的氮掺杂碳杂化钴钼磷化物纳米片包裹氧化钼纳米棒的缺陷工程

Defect engineering with N-doped carbon hybrid cobalt-molybdenum phosphide nanosheets wrapped molybdenum oxide nanorods for alkaline hydrogen evolution reaction.

作者信息

Zheng Yunhua, Hu Huiting, Qian Long, Zhu Yao, Rong Jian, Zhang Tao, Yang Dongya, Qiu Fengxian

机构信息

School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China.

School of Environmental and Safety Engineering, Changzhou University, Changzhou 213164, China.

出版信息

J Colloid Interface Sci. 2023 Dec 15;652(Pt B):1803-1811. doi: 10.1016/j.jcis.2023.09.017. Epub 2023 Sep 5.

DOI:10.1016/j.jcis.2023.09.017
PMID:37683408
Abstract

Regulating the electrocatalytic hydrogen evolution reaction (HER) performance through defect engineering of the surface of the catalysts is an effective pathway. Herein, cobalt-molybdenum phosphide (CoMoP) nanosheets wrapped molybdenum oxide (MoO) core-shell nanorods (MoO@CoMoP), as alkaline electrocatalysts with ligand-derived N-doped carbon hybrid and oxygen-vacancies, were synthesized via solvothermal approaches and followed by phosphorization. As expected, the MoO@MoCoP affords efficient HER with a low overpotential (η) of 84.2 ± 0.4 mV at 10 mA cm. After phosphorization, not only the MoCoP active species are incorporated into the catalyst, but also the defects sites are achieved. Impressively, the metal-ligand-derived MoCoP are distributed uniformly in the N-doped carbon hybrid matrix, exhibiting well-exposed active sites. Benefiting from the synergy effect of MoCoP active species and oxygen-vacancy, the MoO@MoCoP showed increased conductivity and stability, which can deliver a current density of 10 mA cm over 40 h. MoO@MoCoP exhibits an optimal electronic structure on the surface by charge redistribution at the interface, thereby optimizing the hydrogen adsorption energy and accelerating the hydrogen evolution kinetics. This work paves the way for the design of transition metal electrocatalysts with desirable properties through a promising strategy in the field of energy conversion.

摘要

通过催化剂表面的缺陷工程来调控电催化析氢反应(HER)性能是一条有效途径。在此,通过溶剂热法合成了包裹有氧化钼(MoO)核壳纳米棒(MoO@CoMoP)的磷化钴钼(CoMoP)纳米片,其作为具有配体衍生的氮掺杂碳杂化物和氧空位的碱性电催化剂,随后进行了磷化处理。正如预期的那样,MoO@MoCoP在10 mA cm时具有84.2±0.4 mV的低过电位(η),能高效催化析氢反应。磷化处理后,不仅将MoCoP活性物种引入到催化剂中,还形成了缺陷位点。令人印象深刻的是,金属 - 配体衍生的MoCoP均匀分布在氮掺杂碳杂化基质中,展现出充分暴露的活性位点。受益于MoCoP活性物种与氧空位的协同效应,MoO@MoCoP表现出更高的导电性和稳定性,能够在40小时内提供10 mA cm的电流密度。MoO@MoCoP通过界面处的电荷重新分布在表面呈现出最佳电子结构,从而优化了氢吸附能并加速了析氢动力学。这项工作通过能量转换领域一种有前景的策略,为设计具有理想性能的过渡金属电催化剂铺平了道路。

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