应用于氧还原反应的非贵金属原子分散级金属-氮-碳催化剂的设计  

Atomically Dispersed Metal-Nitrogen-Carbon Catalysts for Oxygen Reduction Reaction

作　　者：徐斯然 阴恒铂 薛冬萍 夏会聪 赵舒琰 闫文付[2] 木士春[3] 张佳楠[1] XU Siran;YIN Hengbo;XUE Dongping;XIA Huicong;ZHAO Shuyan;YAN Wenfu;MU Shichun;ZHANG Jianan(College of Materials Science and Engineering,Zhengzhou University,Zhengzhou 450001,China;State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,College of Chemistry,Jilin University,Changchun 130012,China;State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China)

机构地区：[1]郑州大学材料科学与工程学院,郑州450001 [2]吉林大学化学学院,无机合成与制备化学国家重点实验室,长春130012 [3]武汉理工大学材料复合新技术国家重点实验室,武汉430070

出　　处：《高等学校化学学报》2022年第5期42-61,共20页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:21875221);郑州大学青年创新人才团队支持计划专项(批准号:32320275)资助。

摘　　要：为了进一步实现质子交换膜燃料电池(PEMFC)能量转化技术的大规模开发和应用,提高催化剂的成本效益是先决条件.目前,与铂族等贵金属基催化剂相比,原子分散的金属-氮-碳(M-N-C)催化剂也在提高活性位点密度、原子利用率和催化活性等方面表现出巨大的潜力,是最有望代替铂基催化剂的首选材料.在原子分散M-N-C催化剂的制备过程中,获得活性位点均匀分散且结构体系最优化是挑战性问题.基于此,我们重点研究了各种有利于原子分散的M-N-C催化剂的制备方法,以及不同催化剂中原子的化学环境调控对催化位点的影响.本文从M-N-C催化剂的合成与表征、反应机理、密度泛函理论计算等方面进行了深入的探讨,着重讨论了双金属位点、原子簇结构和杂原子对催化位点的化学环境调控.最后,提出了原子分散M-N-C催化剂大规模应用存在的问题及进一步优化的发展方向.To further accelerate the large-scale development and application of proton exchange membrane fuel cell(PEMFC)energy conversion technology,improving the cost-effectiveness of the catalyst is a prerequisite. Currently,atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts also take tremendous potential in terms of increased active site density,atomic utilization and catalytic activity compared to noble metal-based catalysts such as platinumbased catalysts,and are the most promising candidate of platinum-based catalysts. During the preparation of atomically dispersed M-N-C catalysts,the contribution of the uniform dispersion and the optimal structural system of all active sites are the challenge issues. On this basis,we focused on the preparation of various M-N-C catalysts with favorable atomic dispersion and the effect of chemical environment modulation of atoms in different catalysts on the catalytic sites. Herein,we provide an in-depth discussion on the synthesis and characterization of M-N-C catalysts,reaction mechanism,and density functional theory calculations,focusing on the regulation of the chemical environment of catalytic sites by bimetallic sites,atomic cluster structure and heteroatoms. Finally,the problems of the large-scale application of atomically dispersed M-N-C catalysts and the development directions for further optimization are presented.

关 键 词：金属-氮-碳 原子分散 双金属位点 原子簇结构 杂原子 

分 类 号：O611[理学—无机化学]