Rational Design of Graphene-Supported Single-Atom Catalysts for Electroreduction of Nitrogen

Min Yan; Lakshitha Jasin Arachchige; Ani Dong; Xiao Li Zhang; Zhongxu Dai; Chenghua Sun

doi:10.1021/acs.inorgchem.1c02946

Rational Design of Graphene-Supported Single-Atom Catalysts for Electroreduction of Nitrogen

Inorg Chem. 2021 Dec 6;60(23):18314-18324. doi: 10.1021/acs.inorgchem.1c02946. Epub 2021 Nov 17.

Authors

Min Yan¹, Lakshitha Jasin Arachchige^{2

3}, Ani Dong⁴, Xiao Li Zhang⁵, Zhongxu Dai⁶, Chenghua Sun^{2

3}

Affiliations

¹ Science & Technology Innovation Institute, Dongguan University of Technology, Dongguan 523808, China.
² School of Chemical Engineering and Energy Technology, Dongguan University of Technology, Dongguan 523808, China.
³ Department of Chemistry and Biotechnology and Center for Translational Atomaterials, Swinburne University of Technology, Hawthorn, Victoria 3122, Australia.
⁴ Department of Computer and Information Science, City College of Dongguan University of Technology, Dongguan 523419, China.
⁵ State Centre for International Cooperation on Designer Low-Carbon & Environmental Materials, School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China.
⁶ College of Materials and Chemical Engineering, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang 443002, China.

PMID: 34787407
DOI: 10.1021/acs.inorgchem.1c02946

Abstract

Critically, the central metal atoms along with their coordination environment play a significant role in the catalytic performance of single-atom catalysts (SACs). Herein, 12 single Fe, Mo, and Ru atoms supported on defective graphene are theoretically deigned for investigation of their structural and electronic properties and catalytic nitrogen reduction reaction (NRR) performance using first-principles calculations. Our results reveal that graphene with vacancies can be an ideal anchoring site for stabilizing isolated metal atoms owing to the strong metal-support interaction, forming stable TMC_x or TMN_x active centers (x = 3 or 4). Six SACs are screened as promising NRR catalyst candidates with excellent activity and selectivity during NRR, and RuN₃ is identified as the optimal one with an overpotential of ≥0.10 V via the distal mechanism.