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157. Volcano relationship of electron polarization degree in core-shelled Ni@C catalysts and catalytic activity for HOR, ACS Catalysis, 2025, 15, 4110-4120.
2024-12-20 09:29  

Jing Liu, Wanqing Yu, Mengdi Wang, Jie Gao, Xuejing Cui, Luhua Jiang*

College of Materials Science & Engineering, Qingdao University of Science & Technology, Qingdao, 266042, P.R. China

Abstract:

Tuning metal - support interaction by encapsulating metal nanoparticles within carbon shells has emerged as a strategy to enhance alkaline hydrogen oxidation reaction (HOR) catalysts. However, the precise impact of the carbon shell on catalytic activity remains to be fully understood, yet is crucial to guide the rational design of core - shell structured catalysts. In this study, with a sequence of well - designed Ni catalysts coated by heteroatom - doped carbon layers (including Ni@BNC, Ni@SNC and Ni@NC), we discover a volcano - type relationship between the electron polarization degree and the HOR activity. Experimental and theoretical analyses show heteroatom doping adjusts the carbon layer’s electron - withdrawing ability, modulating the Ni core’s d - band center and hydrogen binding energy (HBE). Additionally, heteroatom doping shifts the potential of zero charge (PZC) negatively and enhances hydrogen bond connectivity, facilitating hydroxyl ion transfer. As a result, Ni@BNC achieves optimal HBE and enhanced water adsorption, placing it at the volcano summit for HOR activity. This study establishes a delicate volcano - relationship between the electron polarization degree and the HOR activity of core - shelled catalysts, by shedding lights on the underlying determining factors, both the d - band center of metals and the surface PZC, related tightly with the HBE and hydrogen bond connectivity/water adsorption.

https://doi.org/10.1021/acscatal.5c00053




附件【2025-6-LiuJ-ACS Catal-1.pdf已下载
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姜鲁华 教授
中科院百人

泰山学者特聘教授

德国洪堡学者

     能源短缺和环境污染是当今世界面临的两大难题,研究团队围绕洁净高效新型电能源技术,聚焦电能源相关的纳米材料和电催化应用基础研究。团队已发表SCI收录论文近200篇,申请发明专利80余件。纳米材料与电催化团队负责人姜鲁华教授连续多年入选Elsevier 能源领域/材料领域“中国高被引学者”和“全球前2%顶尖科学家”榜单。主持科技部、国家基金委、山东省科技厅等省部级以上项目20余项。研究成果曾获国家自然科学二等奖、辽宁省自然科学一等奖、国防技术发明二等奖、大连市技术发明一等奖、山东省自然科学学术创新奖等多个奖项。团队教师兼任 Chemical Engineering JournalNano Materials ScineceJournal of Electrochemistry 等多个期刊的编委/编辑。团队多名研究生获得国家奖学金和各类奖助学金以及研究生创新研究计划支持,培养的本科生多人获得大学生创新研究计划支持。

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