Ru3@Mo2C02 MXene single-cluster catalyst for highly efficient N2-to-NH3 conversion

扫码查看

原文链接

万方数据

外文摘要：Single-cluster catalysts(SCCs)representing structurally well-defined metal clusters anchored on support tend to exhibit tunable catalytic performance for complex redox reactions in heterogeneous catalysis.Here we report a theoretical study on an SCC of Ru3@Mo2CO2 MXene for N2-to-NH3 thermal conversion.Our results show that Ru3@Mo2CO2 can effectively activate N2 and promotes its conversion to NH3 through an association mechanism,in which the rate-determining step of NH2*+H*→ NH3*has a low energy barrier of 1.29 eV.Notably,with the assistance of Mo2CO2 support,the positively charged Ru3 cluster active site can effectively adsorb and activate N2,leading to 0.74|e|charge transfer from Ru3@Mo2CO2 to the adsorbed N2.The supported Ru3 also acts as an electron reservoir to regulate the charge transfer for various intermediate steps of ammonia synthesis.Microkinetic analysis shows that the turnover frequency of the N2-to-NH3 conversion on Ru3@Mo2CO2 is as high as 1.45 × 10-2 s-1 site-1 at a selected thermodynamic condition of 48 bar and 700 K,the performance of which even surpasses that of the Ru B5 site and Fe3/θ-Al2O3(010)reported before.Our work provides a theoretical understanding of the high stability and catalytic mechanism of Ru3@Mo2CO2 and guidance for further designing and fabricating MXene-based metal SCCs for ammonia synthesis under mild conditions.

外文关键词：

N2 reduction reactionsingle-cluster catalystRu3@Mo2CO2DFTab initio molecular dynamics simulation

作者：

Cong Zhang、Ze-Hui Wang、Haiyan Wang、Jin-Xia Liang、Chun Zhu、Jun Li

展开 >

作者单位：

School of Chemistry and Chemical Engineering,Guizhou University,Guiyang 550025,China

Shaanxi Key Laboratory of Catalysis,Institute of Theoretical and Computational Chemistry,School of Chemistry and Environment Science,Shaanxi University of Technology,Hanzhong 723000,China

Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry,Southern University of Science and Technology,Shenzhen 518055,China

Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education,Tsinghua University,Beijing 100084,China

Fundamental Science Center of Rare Earths,Ganjiang Innovation Academy,Chinese Academy of Sciences,Ganzhou 341000,China

展开 >

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNSFC Center for Single-Atom CatalysisNational Key R&D ProjectNatural Science Special Foundation of Guizhou University

项目编号：

NSFC22363001219630052176300622250710677223881022022YFA1503900202140

出版年：

2024

DOI：

10.1093/nsr/nwae251

国家科学评论(英文版)

CSTPCD

ISSN：

年,卷(期)：2024.11(9)