journal article·2021-03-04

Two-Dimensional Carbonitride MXenes as an Efficient Electrocatalyst for Hydrogen Evolution

Bo Wei, Zhongheng Fu, Dominik Legut, Timothy C. Germann, Qianfan Zhang, Shiyu Du, Haijun Zhang, Joseph S. Francisco, Ruifeng Zhang

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Abstract

Owing to their excellent thermostability, superior electrical conductivity, and tunable surface chemistry, two-dimensional transition-metal carbides, nitrides, and carbonitrides (MXenes) are highly desirable as potential electrocatalysts for the hydrogen evolution reaction (HER). However, while nearly 30 MXenes have already been synthesized, less carbonitride MXenes were experimentally reported so far, yet their potential promising electrochemical properties are greatly expected. Here, we explored the thermodynamically favorable configurations of Mo 2 (CN)T x (T = F, OH, and O) with a mixture of functional groups under various electrochemical environments. It is revealed that the O*/OH*-terminated Mo-based carbonitride MXenes exhibit the most stable state under ambient conditions. By exploring the catalytic performance of HER for various Mo 2 (C x N 1– x )T 2 at different ratios of C and N atoms, we found that three optimal C/N ratios with 0.5 ML O* and 0.5 ML OH* showed good catalytic activity of HER, comparable to Pt metals. Further investigations of strain-tunable HER of the cofunctionalized Mo 2 (C x N 1– x )OOH suggest that the biaxial strain may effectively modify the Δ G H* of HER, which can be ascribed to the asymmetrical surface topology and charge polarization. These results provide not only a strategy to synthesize carbonitride MXenes with various surface functionalizations but also a feasible solution to design by chemical doping and strain engineering.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: MXene and MAX Phase Materials · Electrocatalysts for Energy Conversion · Advanced Photocatalysis Techniques

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Materials Science and Engineering, Beihang University, Beijing 100191, P. R. China

Center for Integrated Computational Materials Engineering (International Research Institute for Multidisciplinary Science) and Key Laboratory of High-Temperature Structural Materials & Coatings Technology (Ministry of Industry and Information Technology), Beihang University, Beijing 100191, P. R. China

IT4Innovations, VSB-Technical University of Ostrava, 17.listopadu 2172/15, CZ-70800 Ostrava, Czech Republic

Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States

Engineering Laboratory of Specialty Fibers and Nuclear Energy Materials, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, Zhejiang 315201, P. R. China

National United Engineering Laboratory for Biomedical Material Modification, Dezhou, Shandong 251100, China

Department of Vascular & Intervention, Tenth Peoples’ Hospital of Tongji University, Shanghai 200072, China

Department of Earth and Environmental Science and Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States

Funding

Ministry of Education of the People's Republic of China · Ministry of Science and Technology of the People's Republic of China · European Regional Development Fund · National Natural Science Foundation of China · Ministry of Education, Youth and Sports of the Czech Republic · National Thousand Young Talents Program of China

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