Holey Graphene-Supported Single Metal Atoms as Highly Efficient Electrocatalysts

多孔石墨烯支撑的单金属原子作为高效电催化剂

• 批准号: 1800580
• 负责人: Xiangfeng Duan
• 金额: $ 37.5万
• 依托单位: University of California-Los Angeles
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2022-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1800580&HistoricalAwards=false
• 关键词: Holey; Graphene; Supported; Single; Metal

Electricity can provide the needed energy for chemical reactions such as the splitting of water into hydrogen and oxygen. Electrocatalysts are materials that are often needed for efficient and cost-effective electricity-driven, chemical reactions. Single atom catalysts (SACs) are composed of single, isolated metal atoms held on solid base (support). Supported electrocatalysts have potentially high reaction speeds, and tunable behavior, high durability, and recyclability. However, SACs are usually produced using high temperature processes that lead to complex and difficult to characterize structures. In this project, Dr. Xiangfeng Duan and his team at University of California, Los Angeles are developing a general approach for the preparation of single metal atoms supported on graphine with well-defined and systematically-tunable structures. The team uses advanced X-ray analyses and electron microscopy imaging approaches to unambiguously identify the arrangement of the single metal atoms, and matches the structures with reactivities to determine the best catalysts. The goal of this research is to define design criteria for the next generation of highly efficient electrocatalysts that could be used in mobile electronics, transportation, and renewable energy. SACs can combine the merits of both homogeneous catalysts (e.g., highly uniform active sites, tunable coordination environment and maximized atom utilization efficiency) and traditional heterogeneous catalysts (e.g., high durability, easy separation from the product, excellent recyclability, and easy integration with electrodes for electrocatalysis). In this project, Dr. Xiangfeng Duan is developing a general approach to prepare a series of single metal atoms embedded in two-dimensional graphene lattices with well-defined atomistic structure and systematically tunable metal centers (e.g., Fe, Co, Ni, Cu, Ru, Pd, Pt), then evaluating their catalytic properties towards various electrochemical processes. The team uses extended X-ray absorption fine structure (EXAFS) and X-ray absorption near-edge structure (XANES) analyses as well as high resolution transmission electron microscopy imaging approaches to unambiguously identify the local coordination configuration of the single metal atoms. These are further correlated with electrocatalytic activities through both experimental and theoretical studies to establish the structure-property relationship. The general synthesis of a series of single metal sites supported by highly crystalline graphene can allow unambiguous structural identification and systematic catalytic investigations (both experimentally and theoretically). The goal is to establish structure-property correlation and thus define the critical steps toward the rational design of SACs with tailored activity, selectivity and stability.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

电可以为化学反应提供所需的能量，例如将水分解成氢气和氧气。电催化剂是高效且经济高效的电力驱动化学反应通常所需的材料。单原子催化剂 (SAC) 由固定在固体基底（载体）上的单个孤立金属原子组成。 负载型电催化剂具有潜在的高反应速度、可调行为、高耐用性和可回收性。然而，SAC 通常是使用高温工艺生产的，这会导致结构复杂且难以表征。 在这个项目中，加州大学洛杉矶分校的段向峰博士和他的团队正在开发一种通用方法，用于制备石墨烯上支撑的具有明确和系统可调结构的单金属原子。该团队使用先进的 X 射线分析和电子显微镜成像方法来明确识别单个金属原子的排列，并将结构与反应性相匹配，以确定最佳催化剂。 这项研究的目标是确定可用于移动电子、交通和可再生能源的下一代高效电催化剂的设计标准。 SAC可以结合均相催化剂（例如高度均匀的活性位点、可调节的配位环境和最大化的原子利用效率）和传统的多相催化剂（例如高耐久性、易于从产品中分离、优异的可回收性以及易于与电极集成）的优点用于电催化）。在这个项目中，段向峰博士正在开发一种通用方法来制备嵌入二维石墨烯晶格中的一系列单金属原子，这些单金属原子具有明确的原子结构和系统可调的金属中心（例如Fe、Co、Ni、Cu、 Ru、Pd、Pt），然后评估它们对各种电化学过程的催化性能。该团队使用扩展X射线吸收精细结构（EXAFS）和X射线吸收近边缘结构（XANES）分析以及高分辨率透射电子显微镜成像方法来明确识别单个金属原子的局部配位构型。 通过实验和理论研究，这些与电催化活性进一步相关，以建立结构-性能关系。由高度结晶石墨烯支撑的一系列单金属位点的一般合成可以实现明确的结构识别和系统的催化研究（实验和理论上）。目标是建立结构-性能相关性，从而确定合理设计具有定制活性、选择性和稳定性的 SAC 的关键步骤。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力优点和稳定性进行评估，被认为值得支持。更广泛的影响审查标准。

项目成果

Ultra-high Areal Capacity Realized in Three-Dimensional Holey Graphene/SnO2 Composite Anodes

三维多孔石墨烯/SnO2复合阳极实现超高面积容量

• DOI: 10.1016/j.isci.2019.08.025
• 发表时间: 2019-08-20
• 期刊: iScience
• 影响因子: 5.8
• 作者: Junfei Liang;Hongtao Sun;Zipeng Zhao;Yiliu Wang;Zhiying Feng;Jian Zhu;Lin Guo;Yu Huang;X. Du
• 通讯作者: X. Du

The role of alkali metal cations and platinum-surface hydroxyl in the alkaline hydrogen evolution reaction

碱金属阳离子和铂表面羟基在碱性析氢反应中的作用

• DOI: 10.1038/s41929-022-00851-x
• 发表时间: 2022-10-01
• 期刊: Nature Catalysis
• 影响因子: 37.8
• 作者: Aamir Hassan Shah;Zisheng Zhang;Zhihong Huang;Siwei Wang;Guang;Chengzhang Wan;A. Ale;rova;rova;Yu Huang;X. Duan
• 通讯作者: X. Duan

Noble Metal Based Electrocatalysts for Alcohol Oxidation Reactions in Alkaline Media

用于碱性介质中醇氧化反应的贵金属基电催化剂

• DOI: 10.1002/adfm.202106401
• 发表时间: 2022-01-22
• 期刊: Advanced Functional Materials
• 影响因子: 19
• 作者: Xiaoyang Fu;Chengzhang Wan;Yu Huang;X. Duan
• 通讯作者: X. Duan

Determining the hydronium pKα at platinum surfaces and the effect on pH-dependent hydrogen evolution reaction kinetics

确定铂表面的水合氢 pKα 以及对 pH 依赖性析氢反应动力学的影响

• DOI: 10.1073/pnas.2208187119
• 发表时间: 2022-09-27
• 期刊: Proceedings of the National Academy of Sciences of the United States of America
• 影响因子: 11.1
• 作者: Guang;T. Cheng;Aamir Hassan Shah;Chengzhang Wan;Zhihong Huang;Siwei Wang;Tianle Leng;Yu Huang;W. Goddard;X. Duan
• 通讯作者: X. Duan

Single Atoms at Crystal Ladder Steps

水晶阶梯上的单原子

• DOI: 10.1016/j.chempr.2020.11.015
• 发表时间: 2020-12-01
• 期刊: Chem
• 影响因子: 23.5
• 作者: Chengzhang Wan;X. Duan
• 通讯作者: X. Duan