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Title: Pyrolyzed Triazine-Based Nanoporous Frameworks Enable Electrochemical CO 2 Reduction in Water

Abstract

The first study of rational synthesis of triazine-based nanoporous frameworks as electrocatalysts for CO 2 reduction reaction (CO 2RR) was presented. The resulting optimized framework with rich pyridinic nitrogen-containing sites can selectively reduce CO 2 to CO in water with a high Faradic efficiency of ca. 82% under a moderate overpotential of 560 mV. The key of our success lies in the use of pyridine-based backbones as sacrificial groups inside the triazine framework for in situ generation of CO 2RR-active pyridinic N-doped sites during the high-temperature ZnCl 2-promoted polymerization process. We anticipate that this study may facilitate new possibilities for the development of porous organic polymers for electrochemical conversion of CO 2.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [3]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [4];  [3]; ORCiD logo [2]
  1. 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; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  3. 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
  4. East China Univ. of Science and Technology, Shanghai (China). School of Chemistry and Chemical Engineering
  5. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry
  6. Shanghai Jiao Tong Univ., Shanghai (China). School of Chemistry and Chemical Engineering
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1494879
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 50; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; conjugated triazine frameworks; electrochemical CO2 reduction; high CO Faradic efficiency; porous organic polymers; pyridinic N-doped sites; sacrificial synthesis

Citation Formats

Zhu, Xiang, Tian, Chengcheng, Wu, Haihong, He, Yanyan, He, Lin, Wang, Hai, Zhuang, Xiaodong, Liu, Honglai, Xia, Chungu, and Dai, Sheng. Pyrolyzed Triazine-Based Nanoporous Frameworks Enable Electrochemical CO2 Reduction in Water. United States: N. p., 2018. Web. doi:10.1021/acsami.8b13110.
Zhu, Xiang, Tian, Chengcheng, Wu, Haihong, He, Yanyan, He, Lin, Wang, Hai, Zhuang, Xiaodong, Liu, Honglai, Xia, Chungu, & Dai, Sheng. Pyrolyzed Triazine-Based Nanoporous Frameworks Enable Electrochemical CO2 Reduction in Water. United States. doi:10.1021/acsami.8b13110.
Zhu, Xiang, Tian, Chengcheng, Wu, Haihong, He, Yanyan, He, Lin, Wang, Hai, Zhuang, Xiaodong, Liu, Honglai, Xia, Chungu, and Dai, Sheng. Wed . "Pyrolyzed Triazine-Based Nanoporous Frameworks Enable Electrochemical CO2 Reduction in Water". United States. doi:10.1021/acsami.8b13110.
@article{osti_1494879,
title = {Pyrolyzed Triazine-Based Nanoporous Frameworks Enable Electrochemical CO2 Reduction in Water},
author = {Zhu, Xiang and Tian, Chengcheng and Wu, Haihong and He, Yanyan and He, Lin and Wang, Hai and Zhuang, Xiaodong and Liu, Honglai and Xia, Chungu and Dai, Sheng},
abstractNote = {The first study of rational synthesis of triazine-based nanoporous frameworks as electrocatalysts for CO2 reduction reaction (CO2RR) was presented. The resulting optimized framework with rich pyridinic nitrogen-containing sites can selectively reduce CO2 to CO in water with a high Faradic efficiency of ca. 82% under a moderate overpotential of 560 mV. The key of our success lies in the use of pyridine-based backbones as sacrificial groups inside the triazine framework for in situ generation of CO2RR-active pyridinic N-doped sites during the high-temperature ZnCl2-promoted polymerization process. We anticipate that this study may facilitate new possibilities for the development of porous organic polymers for electrochemical conversion of CO2.},
doi = {10.1021/acsami.8b13110},
journal = {ACS Applied Materials and Interfaces},
issn = {1944-8244},
number = 50,
volume = 10,
place = {United States},
year = {2018},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on November 28, 2019
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