Single Atom-Modified Hybrid Transition Metal Carbides as Efficient Hydrogen Evolution Reaction Catalysts

被引:79
作者
Gu, Yitao [1 ,2 ,3 ]
Wei, Bo [1 ,2 ,3 ]
Legut, Dominik [4 ]
Fu, Zhongheng [1 ,2 ,3 ]
Du, Shiyu [5 ]
Zhang, Haijun [6 ,7 ]
Francisco, Joseph S. [8 ,9 ]
Zhang, Ruifeng [1 ,2 ,3 ]
机构
[1] Beihang Univ, Sch Mat Sci & Engn, Beijing 100191, Peoples R China
[2] Beihang Univ, Ctr Integrated Computat Mat Engn, Int Res Inst Multidisciplinary Sci, Minist Ind & Informat Technol, Beijing 100191, Peoples R China
[3] Beihang Univ, Key Lab High Temp Struct Mat & Coatings Technol, Minist Ind & Informat Technol, Beijing 100191, Peoples R China
[4] VSB Tech Univ Ostrava, IT4Innovat, 17 Listopadu 2172-15, CZ-70800 Ostrava, Czech Republic
[5] Chinese Acad Sci, Engn Lab Specialty Fibers & Nucl Energy Mat, Ningbo Inst Mat Technol & Engn, Ningbo 315201, Zhejiang, Peoples R China
[6] Natl United Engn Lab Biomed Mat Modificat, Dezhou 251100, Shandong, Peoples R China
[7] Tongji Univ, Tenth Peoples Hosp, Dept Vasc & Intervent, Shanghai 200072, Peoples R China
[8] Univ Penn, Dept Earth & Environm Sci, Philadelphia, PA 19104 USA
[9] Univ Penn, Dept Chem, Philadelphia, PA 19104 USA
基金
中国国家自然科学基金;
关键词
density functional theory; hydrogen evolution; MXenes; single-atom catalysts; HIGHLY-ACTIVE CATALYSTS; MOLYBDENUM CARBIDE; OXYGEN REDUCTION; MXENE; FUNCTIONALIZATION; ADSORPTION; MECHANISM; GRAPHENE; PHASE; LAYER;
D O I
10.1002/adfm.202104285
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
2D transition metal carbides and nitrides (MXenes) are promising hydrogen evolution reaction (HER) catalysts owing to their metallic conductivity, abundant surface active sites, and high specific surface area. The introduction of a single transition metal atom (TM) at the surface is a good way to improve the HER performance of MXenes. However, the effect of TM on MXenes in previous theoretical studies focused on pure functional groups, and ignored the hybrid-functionalized ones, which are mostly observed in experiments. Herein, the HER performance of four O/F ratios stable hybrids MXenes, Ti2CTx (T = -O, -F), is explored. Ti2CO1.33F0.67 exhibits superior HER catalytic activity, comparable to that of platinum metals. Further combinatorial screening of approximate to 200 TMs based on Ti2CTx structures suggests that Rh, Ti, Ir, and Pt are optimal TM candidates that enhance the sensitivity to strain modulation and reduce the activation barrier for hydrogen generation. A descriptor psi is used to quantify HER performance and reveals the role of the electron filling of TM to the antibonding orbitals. These findings propose feasible candidates with high HER performance through single-atom modification for hybrid-functional MXenes, and a useful descriptor to screen for MXenes with desirable catalytic properties.
引用
收藏
页数:11
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