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 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.

Authors:

Shi, Rui ^[1]; Tian, Chengcheng ^[2]; Zhu, Xiang  ^[3];

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• Search DOE PAGES for ORCID "0000-0002-3973-4998"
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Peng, Cheng-Yun ^[1]; Mei, Bingbao ^[4]; He, Lin  ^[5];

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Du, Xian-Long ^[4]; Jiang, Zheng ^[4]; Chen, Yong  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-6689-8923"
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Dai, Sheng  ^[2]

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• Search DOE PAGES for ORCID "0000-0002-8046-3931"
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+ Show Author Affiliations

1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, HKU-CAS Joint Laboratory on New Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190
2. Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, USA
3. Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, USA, State Key Laboratory for Oxo Synthesis and Selective Oxidation
4. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
5. State Key Laboratory for Oxo Synthesis and Selective Oxidation, Suzhou Research Institute of Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou, China

Publication Date:

2019-02-27

Research Org.:

Oak Ridge National Laboratory (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); Strategic Priority Research Program of the Chinese Academy of Sciences; National Natural Science Foundation of China (NSFC); 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:

Published Article

Journal Name:

Chemical Science

Additional Journal Information:

Journal Name: Chemical Science Journal Volume: 10 Journal Issue: 9; Journal ID: ISSN 2041-6520

Publisher:

Royal Society of Chemistry (RSC)

Country of Publication:

United Kingdom

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY