Loading Nickel Atoms on GDY for Efficient CO2 Fixation and Conversion

doi:10.1007/s40242-021-1387-9

高等学校化学研究 ›› 2022, Vol. 38 ›› Issue (1): 92-98.doi: 10.1007/s40242-021-1387-9

Loading Nickel Atoms on GDY for Efficient CO₂ Fixation and Conversion

ZHENG Zhiqiang¹, HE Feng^2,3, XUE Yurui^1,2, LI Yuliang^1,2,3

1. Science Center for Material Creation and Energy Conversion, School of Chemistry and Chemical Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University, Jinan 250100, P. R. China;
2. Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China;
3. University of Chinese Academy of Sciences, Beijing 100049, P. R. China

收稿日期:2021-09-24 修回日期:2021-10-21 出版日期:2022-02-01 发布日期:2021-10-25
通讯作者: XUE Yurui, LI Yuliang E-mail:yrxue@sdu.edu.cn;ylli@iccas.ac.cn
基金资助:
This work was supported by the National Key Research and Development Project of China(No.2018YFA0703501), the National Natural Science Foundation of China(Nos.21790050, 21790051, 22021002), and the Key Program of the Chinese Academy of Sciences(No.QYZDY-SSW-SLH015).

Loading Nickel Atoms on GDY for Efficient CO₂ Fixation and Conversion

ZHENG Zhiqiang¹, HE Feng^2,3, XUE Yurui^1,2, LI Yuliang^1,2,3

1. Science Center for Material Creation and Energy Conversion, School of Chemistry and Chemical Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University, Jinan 250100, P. R. China;
2. Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China;
3. University of Chinese Academy of Sciences, Beijing 100049, P. R. China

Received:2021-09-24 Revised:2021-10-21 Online:2022-02-01 Published:2021-10-25
Contact: XUE Yurui, LI Yuliang E-mail:yrxue@sdu.edu.cn;ylli@iccas.ac.cn
Supported by:
This work was supported by the National Key Research and Development Project of China(No.2018YFA0703501), the National Natural Science Foundation of China(Nos.21790050, 21790051, 22021002), and the Key Program of the Chinese Academy of Sciences(No.QYZDY-SSW-SLH015).

摘要/Abstract

摘要： Carbon dioxide(CO₂) is an important and valuable C1 resource for the synthesis of numerous of value-added products. However, efficient fixation and conversion of CO₂ into organic carbonates under mild conditions remain great challenges. Herein, graphdiyne(GDY)-based nickel atomic catalysts(Ni⁰/GDYs) were synthesized through a facile in-situ reduction method. Experimental results showed that the obtained Ni⁰/GDY had outstanding catalytic performances for converting CO₂ into cyclic carbonates with a high reaction conversion(99%) and reaction selectivity(ca. 100%) at 80℃ and under 1 atm(1 atm=101325 Pa). Specially, the activation energy (E_a) value for the Ni⁰/GDY is 37.05 kJ/mol, lower than those of reported catalysts. The reaction mechanism was next carefully analyzed by using density functional theory(DFT) calculations. Such an excellent catalytic property could be mainly attributed to the high dispersion of active sites on the Ni⁰/GDY, and the unique incomplete charge transfer properties of GDY-based zero-valent metallic catalysts.

关键词: Graphdiyne, Atomic catalyst, Atomic catalysis, CO₂ fixation, CO₂ conversion

Abstract: Carbon dioxide(CO₂) is an important and valuable C1 resource for the synthesis of numerous of value-added products. However, efficient fixation and conversion of CO₂ into organic carbonates under mild conditions remain great challenges. Herein, graphdiyne(GDY)-based nickel atomic catalysts(Ni⁰/GDYs) were synthesized through a facile in-situ reduction method. Experimental results showed that the obtained Ni⁰/GDY had outstanding catalytic performances for converting CO₂ into cyclic carbonates with a high reaction conversion(99%) and reaction selectivity(ca. 100%) at 80℃ and under 1 atm(1 atm=101325 Pa). Specially, the activation energy (E_a) value for the Ni⁰/GDY is 37.05 kJ/mol, lower than those of reported catalysts. The reaction mechanism was next carefully analyzed by using density functional theory(DFT) calculations. Such an excellent catalytic property could be mainly attributed to the high dispersion of active sites on the Ni⁰/GDY, and the unique incomplete charge transfer properties of GDY-based zero-valent metallic catalysts.

Key words: Graphdiyne, Atomic catalyst, Atomic catalysis, CO₂ fixation, CO₂ conversion

ZHENG Zhiqiang, HE Feng, XUE Yurui, LI Yuliang. Loading Nickel Atoms on GDY for Efficient CO₂ Fixation and Conversion[J]. 高等学校化学研究, 2022, 38(1): 92-98.

ZHENG Zhiqiang, HE Feng, XUE Yurui, LI Yuliang. Loading Nickel Atoms on GDY for Efficient CO₂ Fixation and Conversion[J]. Chemical Research in Chinese Universities, 2022, 38(1): 92-98.

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Loading Nickel Atoms on GDY for Efficient CO₂ Fixation and Conversion

Loading Nickel Atoms on GDY for Efficient CO₂ Fixation and Conversion

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