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

Shi, Rui; Tian, Chengcheng; Zhu, Xiang; Peng, Cheng-Yun; Mei, Bingbao; He, Lin; Du, Xian-Long; Jiang, Zheng; Chen, Yong; Dai, Sheng

doi:10.1039/C8SC05540H

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

Journal Article · Wed Feb 27 00:00:00 EST 2019 · Chemical Science

DOI:https://doi.org/10.1039/C8SC05540H· OSTI ID:1493936

Shi, Rui ^[1]; Tian, Chengcheng ^[2];

^[3]; Peng, Cheng-Yun ^[1]; Mei, Bingbao ^[4];

^[5]; Du, Xian-Long ^[4]; Jiang, Zheng ^[4];

^[1];

^[2]

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
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, USA
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, USA, State Key Laboratory for Oxo Synthesis and Selective Oxidation
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
State Key Laboratory for Oxo Synthesis and Selective Oxidation, Suzhou Research Institute of Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou, China

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.

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Research Organization:: 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 Organization:: 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)

Grant/Contract Number:: AC05-00OR22725; XDB17000000; 21773275; 91645118; BK20171242

OSTI ID:: 1493936

Alternate ID(s):: OSTI ID: 1511923

Journal Information:: Chemical Science, Journal Name: Chemical Science Vol. 10 Journal Issue: 9; ISSN 2041-6520

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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Cited by: 44 works

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