Composition Engineering Opens an Avenue Toward Efficient and Sustainable Nitrogen Fixation

作     者：Xiaolin Wang Liming Yang Xiaolin Wang;Liming Yang

作者机构：Key Laboratory of Material Chemistry for Energy Conversion and StorageMinistry of EducationWuhan 430074China Hubei Key Laboratory of Materials Chemistry and Service FailureWuhan 430074China Hubei Key Laboratory of Bioinorganic Chemistry and Materia MedicaWuhan 430074China Hubei Engineering Research Center for Biomaterials and Medical Protective MaterialsWuhan 430074China School of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China 

出 版 物：《Energy & Environmental Materials》 (能源与环境材料（英文）)

年 卷 期：2024年第7卷第1期

页      面：313-325页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：support from the National Natural Science Foundation of China(22073033,21873032,21673087,21903032) startup fund(2006013118 and 3004013105)from Huazhong University of Science and Technology the Fundamental Research Funds for the Central Universities(2019kfyRCPY116) the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003) 

主　　题：composition engineering strategy diatomic catalysts electrocatalytic nitrogen reduction reaction first-principles calculations graphdiyne hierarchical high-throughput screening synergistic effects 

摘      要：In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active sites as exemplified by diatomic metals anchored graphdiyne via the combination of hierarchical high-throughput screening,first-principles calculations,and molecular dynamics *** 43 highly efficient catalysts feature ultralow onset potentials(|U_(onset)|≤0.40 V)with Rh-Hf and Rh-Ta showing negligible onset potentials of 0 and-0.04 V,*** high catalytic activities of Rh-Hf and Rh-Ta can be ascribed to the synergistic *** forming heteronuclears,the combinations of relatively weak(such as Rh)and relatively strong(such as Hf or Ta)components usually lead to the optimal strengths of adsorption Gibbs free energies of reaction *** origin can be ascribed to the mediate d-band centers of Rh-Hf and Rh-Ta,which lead to the optimal adsorption strengths of intermediates,thereby bringing the high catalytic *** work provides a new and general strategy toward the architecture of highly efficient catalysts not only for electrocatalytic nitrogen reduction reaction(eNRR)but also for other important *** expect that our work will boost both experimental and theoretical efforts in this direction.