Mo-doped boron nitride monolayer as a promising single-atom electrocatalyst for CO2 conversion

Beilstein Journal of Nanotechnology

Weihua Wang^2¹  Gangqiang Qin^1²  Lixiang Sun^3³  Qianyi Cui^1⁴ 

[1] College of Chemistry and Materials Science, Ludong University, Yantai 264025, China^3;School of Chemistry and Chemical Engineering, Qufu Normal University, Qufu, Shandong, 273165, China^2;School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology, Brisbane, QLD 4001, Australia more less^4;State Key Laboratory of Radiation Medicine and Protection, Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, School for Radiological and Interdisciplinary Sciences, Soochow University, Suzhou 215123, China^1

关键词: boron nitride monolayer;    CO2 conversion;    density functional theory;    single-atom electrocatalyst;   

DOI  :  10.3762/bjnano.10.55

学科分类：地球科学(综合)

来源: Beilstein - Institut zur Foerderung der Chemischen Wissenschaften

【 摘 要 】

The design of new, efficient catalysts for the conversion of CO₂ to useful fuels under mild conditions is urgent in order to reduce greenhouse gas emissions and alleviate the energy crisis. In this work, a series of transition metals (TMs), including Sc to Zn, Mo, Ru, Rh, Pd and Ag, supported on a boron nitride (BN) monolayer with boron vacancies, were investigated as electrocatalysts for the CO₂ reduction reaction (CRR) using comprehensive density functional theory (DFT) calculations. The results demonstrate that a single-Mo-atom-doped boron nitride (Mo-doped BN) monolayer possesses excellent performance for converting CO₂ to CH₄ with a relatively low limiting potential of −0.45 V, which is lower than most catalysts for the selective production of CH₄ as found in both theoretical and experimental studies. In addition, the formation of OCHO on the Mo-doped BN monolayer in the early hydrogenation steps is found to be spontaneous, which is distinct from the conventional catalysts. Mo, as a non-noble element, presents excellent catalytic performance with coordination to the BN monolayer, and is thus a promising transition metal for catalyzing CRR. This work not only provides insight into the mechanism of CRR on the single-atom catalyst (Mo-doped BN monolayer) at the atomic level, but also offers guidance in the search for appropriate earth-abundant TMs as electrochemical catalysts for the efficient conversion of CO₂ to useful fuels under ambient conditions.

【 授权许可】

CC BY