嵌入二维方形四氟四氰基对苯二醌二甲烷单层的过渡金属作为一类用于氮还原反应的新型电催化剂。
Transition Metals Embedded Two-Dimensional Square Tetrafluorotetracyanoquinodimethane Monolayers as a Class of Novel Electrocatalysts for Nitrogen Reduction Reaction.
作者信息
Lv Sheng-Yao, Li Guoliang, Yang Li-Ming
机构信息
Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica; Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education; Hubei Key Laboratory of Materials Chemistry and Service Failure; Hubei Engineering Research Center for Biomaterials and Medical Protective Materials; School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, China.
Key Laboratory of Theoretical Chemistry of Environment, Ministry of Education; Center for Computational Quantum Chemistry, School of Chemistry, South China Normal University, Guangzhou 510006, China.
出版信息
ACS Appl Mater Interfaces. 2022 Jun 8;14(22):25317-25325. doi: 10.1021/acsami.2c02677. Epub 2022 May 24.
The combination of transition metal (TM) atoms and high electron affinity organic framework tetrafluorotetracyanoquinodimethanes (FTCNQs) makes the TM-embedded two-dimensional (2D) square FTCNQ monolayers (TM-sFTCNQ) possible to have excellent characteristics of single-atom catalysts and 2D materials. For the first time, the TM-sFTCNQ monolayers have been considered for application in the electrocatalytic nitrogen reduction reaction (eNRR) field. Through high-throughput screening, the catalytic performance of 30 TM-sFTCNQ (TM = 3d∼5d TMs) monolayers for eNRR was comprehensively evaluated. The Mo-, Nb-, and Tc-sFTCNQ catalysts stand out with the onset potentials of -0.18, -0.44, and -0.54 V, respectively, through the optimal reaction paths. Our work will provide guidance for the green and sustainable development of electrocatalytic nitrogen fixation.
过渡金属（TM）原子与高电子亲和性有机骨架四氟四氰基对苯二醌二甲烷（FTCNQs）的结合，使得嵌入TM的二维（2D）方形FTCNQ单层（TM-sFTCNQ）有可能具备单原子催化剂和二维材料的优异特性。首次考虑将TM-sFTCNQ单层应用于电催化氮还原反应（eNRR）领域。通过高通量筛选，全面评估了30种TM-sFTCNQ（TM = 3d∼5d过渡金属）单层对eNRR的催化性能。通过最优反应路径，Mo-sFTCNQ、Nb-sFTCNQ和Tc-sFTCNQ催化剂分别以-0.18、-0.44和-0.54 V的起始电位脱颖而出。我们的工作将为电催化固氮的绿色可持续发展提供指导。
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