Frenkel-defected monolayer MoS2 catalysts for efficient hydrogen evolution

Jie Xu; Gonglei Shao; Xuan Tang; Fang Lv; Haiyan Xiang; Changfei Jing; Song Liu; Sheng Dai; Yanguang Li; Jun Luo; Zhen Zhou

doi:10.1038/s41467-022-29929-7

Frenkel-defected monolayer MoS₂ catalysts for efficient hydrogen evolution

Nat Commun. 2022 Apr 22;13(1):2193. doi: 10.1038/s41467-022-29929-7.

Authors

Jie Xu^#¹, Gonglei Shao^#^{2

3}, Xuan Tang^#⁴, Fang Lv¹, Haiyan Xiang², Changfei Jing⁵, Song Liu⁶, Sheng Dai⁷, Yanguang Li⁸, Jun Luo⁹, Zhen Zhou³

Affiliations

¹ Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, 215123, Suzhou, China.
² State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, 410082, Changsha, Hunan, China.
³ Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of Education, School of Chemical Engineering, Zhengzhou University, 450001, Zhengzhou, China.
⁴ Feringa Nobel Prize Scientist Joint Research Centre, School of Chemistry and Molecular Engineering, East China University of Science & Technology, 200237, Shanghai, China.
⁵ School of Materials Science and Engineering, Tianjin Key Lab of Photoelectric Materials & Devices, Tianjin University of Technology, 300384, Tianjin, China.
⁶ State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, 410082, Changsha, Hunan, China. liusong@hnu.edu.cn.
⁷ Feringa Nobel Prize Scientist Joint Research Centre, School of Chemistry and Molecular Engineering, East China University of Science & Technology, 200237, Shanghai, China. shengdai@ecust.edu.cn.
⁸ Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, 215123, Suzhou, China. yanguang@suda.edu.cn.
⁹ School of Materials Science and Engineering, Tianjin Key Lab of Photoelectric Materials & Devices, Tianjin University of Technology, 300384, Tianjin, China. jluo@tjut.edu.cn.

^# Contributed equally.

Abstract

Defect engineering is an effective strategy to improve the activity of two-dimensional molybdenum disulfide base planes toward electrocatalytic hydrogen evolution reaction. Here, we report a Frenkel-defected monolayer MoS₂ catalyst, in which a fraction of Mo atoms in MoS₂ spontaneously leave their places in the lattice, creating vacancies and becoming interstitials by lodging in nearby locations. Unique charge distributions are introduced in the MoS₂ surface planes, and those interstitial Mo atoms are more conducive to H adsorption, thus greatly promoting the HER activity of monolayer MoS₂ base planes. At the current density of 10 mA cm^-2, the optimal Frenkel-defected monolayer MoS₂ exhibits a lower overpotential (164 mV) than either pristine monolayer MoS₂ surface plane (358 mV) or Pt-single-atom doped MoS₂ (211 mV). This work provides insights into the structure-property relationship of point-defected MoS₂ and highlights the advantages of Frenkel defects in tuning the catalytic performance of MoS₂ materials.