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Title: Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis

Abstract

The grand challenge in the development of atomically dispersed metallic catalysts is their low metal-atom loading density, uncontrollable localization and ambiguous interactions with supports, posing difficulty in maximizing their catalytic performance. Here, we achieve an interface catalyst consisting of atomic cobalt array covalently bound to distorted 1T MoS 2 nanosheets (SA Co-D 1T MoS 2). The phase of MoS 2 transforming from 2H to D-1T, induced by strain from lattice mismatch and formation of Co-S covalent bond between Co and MoS 2 during the assembly, is found to be essential to form the highly active single-atom array catalyst. SA Co-D 1T MoS 2 achieves Pt-like activity toward HER and high long-term stability. Active-site blocking experiment together with density functional theory (DFT) calculations reveal that the superior catalytic behaviour is associated with an ensemble effect via the synergy of Co adatom and S of the D-1T MoS 2 support by tuning hydrogen binding mode at the interface.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1];  [3];  [1];  [1];  [2];  [2];  [4];  [2];  [3];  [3];  [1];  [1]; ORCiD logo [3];  [1]; ORCiD logo [5]
  1. Jilin Univ., Changchun (China)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
  3. Peking Univ., Beijing (China)
  4. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Applied Physics, Shanghai Synchrotron Radiation Facility
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1579497
Report Number(s):
BNL-212407-2019-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Qi, Kun, Cui, Xiaoqiang, Gu, Lin, Yu, Shansheng, Fan, Xiaofeng, Luo, Mingchuan, Xu, Shan, Li, Ningbo, Zheng, Lirong, Zhang, Qinghua, Ma, Jingyuan, Gong, Yue, Lv, Fan, Wang, Kai, Huang, Haihua, Zhang, Wei, Guo, Shaojun, Zheng, Weitao, and Liu, Ping. Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis. United States: N. p., 2019. Web. doi:10.1038/s41467-019-12997-7.
Qi, Kun, Cui, Xiaoqiang, Gu, Lin, Yu, Shansheng, Fan, Xiaofeng, Luo, Mingchuan, Xu, Shan, Li, Ningbo, Zheng, Lirong, Zhang, Qinghua, Ma, Jingyuan, Gong, Yue, Lv, Fan, Wang, Kai, Huang, Haihua, Zhang, Wei, Guo, Shaojun, Zheng, Weitao, & Liu, Ping. Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis. United States. doi:10.1038/s41467-019-12997-7.
Qi, Kun, Cui, Xiaoqiang, Gu, Lin, Yu, Shansheng, Fan, Xiaofeng, Luo, Mingchuan, Xu, Shan, Li, Ningbo, Zheng, Lirong, Zhang, Qinghua, Ma, Jingyuan, Gong, Yue, Lv, Fan, Wang, Kai, Huang, Haihua, Zhang, Wei, Guo, Shaojun, Zheng, Weitao, and Liu, Ping. Tue . "Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis". United States. doi:10.1038/s41467-019-12997-7. https://www.osti.gov/servlets/purl/1579497.
@article{osti_1579497,
title = {Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis},
author = {Qi, Kun and Cui, Xiaoqiang and Gu, Lin and Yu, Shansheng and Fan, Xiaofeng and Luo, Mingchuan and Xu, Shan and Li, Ningbo and Zheng, Lirong and Zhang, Qinghua and Ma, Jingyuan and Gong, Yue and Lv, Fan and Wang, Kai and Huang, Haihua and Zhang, Wei and Guo, Shaojun and Zheng, Weitao and Liu, Ping},
abstractNote = {The grand challenge in the development of atomically dispersed metallic catalysts is their low metal-atom loading density, uncontrollable localization and ambiguous interactions with supports, posing difficulty in maximizing their catalytic performance. Here, we achieve an interface catalyst consisting of atomic cobalt array covalently bound to distorted 1T MoS2 nanosheets (SA Co-D 1T MoS2). The phase of MoS2 transforming from 2H to D-1T, induced by strain from lattice mismatch and formation of Co-S covalent bond between Co and MoS2 during the assembly, is found to be essential to form the highly active single-atom array catalyst. SA Co-D 1T MoS2 achieves Pt-like activity toward HER and high long-term stability. Active-site blocking experiment together with density functional theory (DFT) calculations reveal that the superior catalytic behaviour is associated with an ensemble effect via the synergy of Co adatom and S of the D-1T MoS2 support by tuning hydrogen binding mode at the interface.},
doi = {10.1038/s41467-019-12997-7},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {11}
}

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