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Nano Research 2023, 16(7): 9039-9049 https://doi.org/10.1007/s12274-023-5681-3
Research Article | Issue | Published: 29 April 2023

Manipulating micro-electric field and coordination-saturated site configuration boosted activity and safety of frustrated single-atom Cu/O Lewis pair for acetylene hydrochlorination

Show Author's Information Junchen Peng1,§,  Dandan Dong1,§,  Zongyuan Wang1,§,  Hong Yang2,  Dongyang Qiao1,  Qinqin Wang1,  Wei Sun1,  Minmin Liu1,  Jiajun Wang3,  Mingyuan Zhu4( ),  Bin Dai1( ),  Fei He5( ),  Chaofeng Huang1( )
School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi University, Shihezi 832000, China
School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, China
School of Materials Science and Engineering, Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education, Tianjin University, Tianjin 300072, China
College of Chemistry & Chemical Engineering, Yantai University, Yantai 264010, China
School of Material Science and Engineering, University of Jinan, Jinan 250022, China

§ Junchen Peng, Dandan Dong, and Zongyuan Wang contributed equally to this work.

Keywords:
electric field, acetylene hydrochlorination, Lewis pair, site configuration, single-atom Cu
Topics:
Catalysis
Cite this article:
Peng J, Dong D, Wang Z, et al. Manipulating micro-electric field and coordination-saturated site configuration boosted activity and safety of frustrated single-atom Cu/O Lewis pair for acetylene hydrochlorination. Nano Research, 2023, 16(7): 9039-9049. https://doi.org/10.1007/s12274-023-5681-3
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Abstract Full text Electronic supplementary material About this article

Simultaneously boosting acetylene hydrochlorination activity and avoiding formation of explosive copper acetylide over Cu-based catalyst, which represented a promising alternative to Hg-based and noble metal catalysts, remained challenging. Herein, we fabricated a frustrated single-atom Cu/O Lewis pair catalyst (Cu/O-FLP) by coupling epoxide group (C–O–C) with atom-dispersed Cu-cis-N2C2Cl center to address this challenge. The basic epoxy site modulated the electron-deficient state of Lewis-acidic Cu center and paired with the Cu-cis-N2C2Cl moiety to preferentially break HCl into different electronegative Cu–Clδ− and C–O–Hδ+ intermediates, which further induced both an extra localized electric field to polarize acetylene and a upshift of the d-band center of catalyst, thereby promoting adsorption and enrichment of acetylene by enhancing the dipolar interaction between acetylene and active intermediates. Moreover, the generated Cu–Clδ− and C–O–Hδ+ drastically reduced the energy barrier of rate-limiting step and made vinyl chloride easier to desorb from the Lewis-basic oxygen-atom site rather than traditional Lewis-acidic Cu center. These superiorities ensured a higher activity of Cu/O-FLP compared with its counterparts. Meanwhile, preferential dissociation of HCl endowed single-atom Cu with the coordination-saturated configuration, which impeded formation of explosive copper acetylide by avoiding the direct interaction between Cu and acetylene, ensuring the intrinsic safety during catalysis.


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Abstract
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Electronic supplementary material
About this article

Manipulating micro-electric field and coordination-saturated site configuration boosted activity and safety of frustrated single-atom Cu/O Lewis pair for acetylene hydrochlorination

Show Author's information Junchen Peng1,§, Dandan Dong1,§, Zongyuan Wang1,§, Hong Yang2, Dongyang Qiao1, Qinqin Wang1, Wei Sun1, Minmin Liu1, Jiajun Wang3, Mingyuan Zhu4( ), Bin Dai1( ), Fei He5( ), Chaofeng Huang1( )
School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi University, Shihezi 832000, China
School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, China
School of Materials Science and Engineering, Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education, Tianjin University, Tianjin 300072, China
College of Chemistry & Chemical Engineering, Yantai University, Yantai 264010, China
School of Material Science and Engineering, University of Jinan, Jinan 250022, China

§ Junchen Peng, Dandan Dong, and Zongyuan Wang contributed equally to this work.

Abstract

Simultaneously boosting acetylene hydrochlorination activity and avoiding formation of explosive copper acetylide over Cu-based catalyst, which represented a promising alternative to Hg-based and noble metal catalysts, remained challenging. Herein, we fabricated a frustrated single-atom Cu/O Lewis pair catalyst (Cu/O-FLP) by coupling epoxide group (C–O–C) with atom-dispersed Cu-cis-N2C2Cl center to address this challenge. The basic epoxy site modulated the electron-deficient state of Lewis-acidic Cu center and paired with the Cu-cis-N2C2Cl moiety to preferentially break HCl into different electronegative Cu–Clδ− and C–O–Hδ+ intermediates, which further induced both an extra localized electric field to polarize acetylene and a upshift of the d-band center of catalyst, thereby promoting adsorption and enrichment of acetylene by enhancing the dipolar interaction between acetylene and active intermediates. Moreover, the generated Cu–Clδ− and C–O–Hδ+ drastically reduced the energy barrier of rate-limiting step and made vinyl chloride easier to desorb from the Lewis-basic oxygen-atom site rather than traditional Lewis-acidic Cu center. These superiorities ensured a higher activity of Cu/O-FLP compared with its counterparts. Meanwhile, preferential dissociation of HCl endowed single-atom Cu with the coordination-saturated configuration, which impeded formation of explosive copper acetylide by avoiding the direct interaction between Cu and acetylene, ensuring the intrinsic safety during catalysis.

Keywords: electric field, acetylene hydrochlorination, Lewis pair, site configuration, single-atom Cu

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Acknowledgements

Publication history

Received: 04 February 2023
Revised: 16 March 2023
Accepted: 20 March 2023
Published: 29 April 2023
Issue date: July 2023

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© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 22062021), the Science and Technology Project of Xinjiang Bingtuan supported by Central government (No. 2022BC001), the Opening Project of Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan (No. KF2019010), the Start-Up Foundation for high-level professionals of Shihezi University (No. RCZK201932), and the research project of Shihezi University (No. CXFZ202205).

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