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Integrating single-cobalt-site and electric field of boron nitride in dechlorination electrocatalysts by bioinspired design.
Min, Yuan; Zhou, Xiao; Chen, Jie-Jie; Chen, Wenxing; Zhou, Fangyao; Wang, Zhiyuan; Yang, Jia; Xiong, Can; Wang, Ying; Li, Fengting; Yu, Han-Qing; Wu, Yuen.
Afiliação
  • Min Y; CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, 230026, Hefei, China.
  • Zhou X; Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, 230026, Hefei, China. zhoux08@mail.ustc.edu.cn.
  • Chen JJ; College of Environmental Science and Engineering, Tongji University, 1239 Siping Road, 200092, Shanghai, China. zhoux08@mail.ustc.edu.cn.
  • Chen W; CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, 230026, Hefei, China. chenjiej@ustc.edu.cn.
  • Zhou F; Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, 100081, Beijing, China.
  • Wang Z; Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, 230026, Hefei, China.
  • Yang J; Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, 230026, Hefei, China.
  • Xiong C; Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, 230026, Hefei, China.
  • Wang Y; Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, 230026, Hefei, China.
  • Li F; College of Environmental Science and Engineering, Tongji University, 1239 Siping Road, 200092, Shanghai, China.
  • Yu HQ; College of Environmental Science and Engineering, Tongji University, 1239 Siping Road, 200092, Shanghai, China.
  • Wu Y; CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, 230026, Hefei, China.
Nat Commun ; 12(1): 303, 2021 01 12.
Article em En | MEDLINE | ID: mdl-33436610
The construction of enzyme-inspired artificial catalysts with enzyme-like active sites and microenvironment remains a great challenge. Herein, we report a single-atomic-site Co catalyst supported by carbon doped boron nitride (BCN) with locally polarized B-N bonds (Co SAs/BCN) to simulate the reductive dehalogenases. Density functional theory analysis suggests that the BCN supports, featured with ionic characteristics, provide additional electric field effect compared with graphitic carbon or N-doped carbon (CN), which could facilitate the adsorption of polarized organochlorides. Consistent with the theoretical results, the Co SAs/BCN catalyst delivers a high activity with nearly complete dechlorination (~98%) at a potential of -0.9 V versus Ag/AgCl for chloramphenicol (CAP), showing that the rate constant (k) contributed by unit mass of metal (k/ratio) is 4 and 19 times more active than those of the Co SAs/CN and state-of-the-art Pd/C catalyst, respectively. We show that Co single atoms coupled with BCN host exhibit high stability and selectivity in CAP dechlorination and suppress the competing hydrogen evolution reaction, endowing the Co SAs/BCN as a candidate for sustainable conversion of organic chloride.

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2021 Tipo de documento: Article

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2021 Tipo de documento: Article