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Title: Achieving an exceptionally high loading of isolated cobalt single atoms on a porous carbon matrix for efficient visible-light-driven photocatalytic hydrogen production

Abstract

Single-atom catalysts (SACs) have shown great potential in a wide variety of chemical reactions and become the most active new frontier in catalysis due to the maximum efficiency of metal atom use. The key obstacle in preparing SAs lies in the development of appropriate supports that can avoid aggregation or sintering during synthetic procedures. As such, achieving high loadings of isolated SAs is nontrivial and challenging. Conventional methods usually afford the formation of SAs with extremely low loadings (less than 1.5 wt%). In this work, a new in situ preparation strategy that enables the synthesis of isolated cobalt (Co) SAs with an exceptionally high metal loading, up to 5.9 wt%, is developed. The approach is based on a simple one-step pyrolysis of a nitrogen-enriched molecular carbon precursor (1,4,5,8,9,12-hexaazatriphenylene hexacarbonitrile) and CoCl 2. Furthermore, due to the successful electron transfer from carbon nitride to the isolated Co SAs, we demonstrate a high-performance photocatalytic H 2 production using Co SAs as a co-catalyst, and the evolution rate is measured to be 1180 μmol g -1 h -1. We anticipate that this new study will inspire the discovery of more isolated SACs with high metal loadings, evidently advancing the development of this emergingmore » type of advanced catalysts.« less

Authors:
 [1];  [2]; ORCiD logo [3];  [1];  [4]; ORCiD logo [5];  [4];  [4]; ORCiD logo [1]; ORCiD logo [2]
  1. Chinese Academy of Sciences (CAS), Beijing (China). Key Lab. of Photochemical Conversion and Optoelectronic Materials. HKU-CAS Joint Lab. on New Materials. Technical Inst. of Physics and Chemistry
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Chinese Academy of Sciences (CAS), Lanzhou (China). State Key Lab. for Oxo Synthesis and Selective Oxidation. Suzhou Research Inst. of Lanzhou Inst. of Chemical Physics; Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry
  4. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Synchrotron Radiation Facility. Shanghai Inst. of Applied Physics
  5. Chinese Academy of Sciences (CAS), Lanzhou (China). State Key Lab. for Oxo Synthesis and Selective Oxidation. Suzhou Research Inst. of Lanzhou Inst. of Chemical Physics
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China); Chinese Academy of Sciences (CAS), Lanzhou (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Strategic Priority Research Program of the Chinese Academy of Sciences; National Natural Science Foundation of China (NNSFC); Foundation Research Project of Jiangsu Province (China)
OSTI Identifier:
1493936
Alternate Identifier(s):
OSTI ID: 1511923
Grant/Contract Number:  
AC05-00OR22725; XDB17000000; 21773275; 91645118; BK20171242
Resource Type:
Journal Article: Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 10; Journal Issue: 9; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English

Citation Formats

Shi, Rui, Tian, Chengcheng, Zhu, Xiang, Peng, Cheng-Yun, Mei, Bingbao, He, Lin, Du, Xian-Long, Jiang, Zheng, Chen, Yong, and Dai, Sheng. Achieving an exceptionally high loading of isolated cobalt single atoms on a porous carbon matrix for efficient visible-light-driven photocatalytic hydrogen production. United States: N. p., 2019. Web. doi:10.1039/c8sc05540h.
Shi, Rui, Tian, Chengcheng, Zhu, Xiang, Peng, Cheng-Yun, Mei, Bingbao, He, Lin, Du, Xian-Long, Jiang, Zheng, Chen, Yong, & Dai, Sheng. Achieving an exceptionally high loading of isolated cobalt single atoms on a porous carbon matrix for efficient visible-light-driven photocatalytic hydrogen production. United States. doi:10.1039/c8sc05540h.
Shi, Rui, Tian, Chengcheng, Zhu, Xiang, Peng, Cheng-Yun, Mei, Bingbao, He, Lin, Du, Xian-Long, Jiang, Zheng, Chen, Yong, and Dai, Sheng. Wed . "Achieving an exceptionally high loading of isolated cobalt single atoms on a porous carbon matrix for efficient visible-light-driven photocatalytic hydrogen production". United States. doi:10.1039/c8sc05540h.
@article{osti_1493936,
title = {Achieving an exceptionally high loading of isolated cobalt single atoms on a porous carbon matrix for efficient visible-light-driven photocatalytic hydrogen production},
author = {Shi, Rui and Tian, Chengcheng and Zhu, Xiang and Peng, Cheng-Yun and Mei, Bingbao and He, Lin and Du, Xian-Long and Jiang, Zheng and Chen, Yong and Dai, Sheng},
abstractNote = {Single-atom catalysts (SACs) have shown great potential in a wide variety of chemical reactions and become the most active new frontier in catalysis due to the maximum efficiency of metal atom use. The key obstacle in preparing SAs lies in the development of appropriate supports that can avoid aggregation or sintering during synthetic procedures. As such, achieving high loadings of isolated SAs is nontrivial and challenging. Conventional methods usually afford the formation of SAs with extremely low loadings (less than 1.5 wt%). In this work, a new in situ preparation strategy that enables the synthesis of isolated cobalt (Co) SAs with an exceptionally high metal loading, up to 5.9 wt%, is developed. The approach is based on a simple one-step pyrolysis of a nitrogen-enriched molecular carbon precursor (1,4,5,8,9,12-hexaazatriphenylene hexacarbonitrile) and CoCl2. Furthermore, due to the successful electron transfer from carbon nitride to the isolated Co SAs, we demonstrate a high-performance photocatalytic H2 production using Co SAs as a co-catalyst, and the evolution rate is measured to be 1180 μmol g-1 h-1. We anticipate that this new study will inspire the discovery of more isolated SACs with high metal loadings, evidently advancing the development of this emerging type of advanced catalysts.},
doi = {10.1039/c8sc05540h},
journal = {Chemical Science},
issn = {2041-6520},
number = 9,
volume = 10,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1039/c8sc05540h

Figures / Tables:

Scheme 1 Scheme 1: Synthesis route and proposed structure for isolated Co single atoms.

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.