氮掺杂碳上单原子锌:CO2固定和转化的高效稳定催化剂

doi:10.1016/S1872-2067(19)63316-4

催化学报 ›› 2019, Vol. 40 ›› Issue (11): 1679-1685.DOI: 10.1016/S1872-2067(19)63316-4

氮掺杂碳上单原子锌:CO₂固定和转化的高效稳定催化剂

Xinjiang Cui^a, Xingchao Dai^b, Annette-Enrica Surkus^a, Kathrin Junge^a, Carsten Kreyenschulte^a, Giovanni Agostini^a, Nils Rockstroh^a, Matthias Beller^a

a 莱布尼茨催化研究所, 罗斯托克 18059, 德国;
b 中国科学院兰州化学物理研究所绿色化学与催化中心, 羰基合成与选择氧化国家重点实验室, 甘肃兰州 730000, 中国

收稿日期:2019-01-21 修回日期:2019-01-27 出版日期:2019-11-18 发布日期:2019-09-06
通讯作者: Matthias Beller
基金资助:
国家重点研发计划（2017YFA0403103）；梅克伦堡-西波美拉尼亚州和德国联邦教育和研究部项目资助

Zinc single atoms on N-doped carbon: An efficient and stable catalyst for CO₂ fixation and conversion

Xinjiang Cui^a, Xingchao Dai^b, Annette-Enrica Surkus^a, Kathrin Junge^a, Carsten Kreyenschulte^a, Giovanni Agostini^a, Nils Rockstroh^a, Matthias Beller^a

a Leibniz-Institut für Katalyse e.V. Albert-Einstein-Str. 29a, 18059 Rostock, Germany;
b State Key Laboratory for Oxo Synthesis and Selective Oxidation, Centre for Green Chemistry and Catalysis, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, Gansu, China

Received:2019-01-21 Revised:2019-01-27 Online:2019-11-18 Published:2019-09-06
Contact: Matthias Beller
Supported by:
This work was supported by the National Key R&D Program of China (2017YFA0403103), the state of Mecklenburg-Vorpommern and the Bundesministerium für Bildung und Forschung.

摘要/Abstract

摘要： 环氧化合物与CO₂环加成反应是环状碳酸酯合成和CO₂利用的一种直接的原子经济方法，目前主要采用均相金属络合物催化此类转化反应.本文报道了一种新型多相Zn基催化剂，它可方便地通过热解活性炭负载的邻菲啰啉络合Zn（OAc）₂而得到.详细的结构表征证实该材料中存在单原子Zn活性位.与Zn基纳米粒子催化剂相比，本文制备的单原子Zn催化剂在环氧化物环加成反应中表现出更高的活性和稳定性.采用该优化的催化剂成功地以高产率得到了一系列碳酸酯，该催化剂具有较好的基团容忍性.

关键词: 多相催化, 单原子催化剂, 锌, 二氧化碳, 环加成, 碳酸酯

Abstract: The cycloaddition of epoxides and carbon dioxide represents a straightforward and atom-efficient method for synthesis of cyclic carbonates and utilization of CO₂. So far, homogeneous metal complexes have been mainly applied for such transformations. Here, we describe the synthesis of novel heterogeneous Zn-based catalysts, which were conveniently prepared by pyrolysis of an active-carbon-supported phenanthroline-ligated Zn(OAc)₂ complex. Detail structural characterizations proved the existence of single zinc sites in the active material. Compared to a Zn-based nanoparticle (Zn-NP) catalyst, the resulting single metal atom catalyst (SAC) displayed improved activity and stability for the cycloaddition of epoxides. By applying the optimal catalyst, a variety of carbonates were successfully obtained in high yields with good functional group tolerance.

Key words: Heterogeneous catalysis, Single atom catalyst, Zinc, Carbon dioxide, Cycloaddition, Carbonate

Xinjiang Cui, Xingchao Dai, Annette-Enrica Surkus, Kathrin Junge, Carsten Kreyenschulte, Giovanni Agostini, Nils Rockstroh, Matthias Beller. 氮掺杂碳上单原子锌:CO₂固定和转化的高效稳定催化剂[J]. 催化学报, 2019, 40(11): 1679-1685.

Xinjiang Cui, Xingchao Dai, Annette-Enrica Surkus, Kathrin Junge, Carsten Kreyenschulte, Giovanni Agostini, Nils Rockstroh, Matthias Beller. Zinc single atoms on N-doped carbon: An efficient and stable catalyst for CO₂ fixation and conversion[J]. Chinese Journal of Catalysis, 2019, 40(11): 1679-1685.

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氮掺杂碳上单原子锌:CO₂固定和转化的高效稳定催化剂

Zinc single atoms on N-doped carbon: An efficient and stable catalyst for CO₂ fixation and conversion

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