In Situ Pyrolysis of ZIF-67 to Construct Co₂N_0.67@ZIF-67 for Photocatalytic CO₂ Cycloaddition Reaction.

IF 4.3 2区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

Inorganic Chemistry Pub Date : 2024-08-05 Epub Date: 2024-07-26 DOI:10.1021/acs.inorgchem.4c02504

Lingjing Jiang, Dengqi Wu, Zishan Huang, Fengfeng Chen, Kai Chen, Aziz Bakhtiyarovich Ibragimov, Junkuo Gao

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引用次数: 0

Abstract

The development of heterogeneous catalysts with abundant active sites is pivotal for enhancing the efficiency of photothermal CO₂ conversion. Herein, we report the construction of Co₂N_0.67@ZIF-67 through the in situ pyrolysis of ZIF-67 under low-temperature pyrolysis conditions. During the pyrolysis process, the crystal structure of ZIF-67 is predominantly preserved concurrently with the formation of Co₂N_0.67 nanoparticles (NPs) within the ZIF-67 pores. The optimal catalyst Co₂N_0.67@ZIF-67(450,2) not only possesses high photothermal efficiency but also can efficiently activate CO₂. Benefiting from these characteristics, Co₂N_0.67@ZIF-67(450,2) exhibited significant catalytic activity in the photocatalytic cycloaddition of CO₂ and epichlorohydrin. The yield of (chloromethyl)ethylene carbonate reached 95%, which is more than 4 times higher than that of ZIF-67 under visible light irradiation (300 W·m² Xe lamp, 3 h). This study could offer an alternative approach to enhance the photocatalytic activity of MOFs through low-temperature pyrolysis.

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原位热解 ZIF-67 以构建用于光催化 CO2 环加成反应的 Co2N0.67@ZIF-67。

开发具有丰富活性位点的异质催化剂对于提高光热转化二氧化碳的效率至关重要。在此，我们报告了在低温热解条件下通过原位热解 ZIF-67 构建 Co2N0.67@ZIF-67 的过程。在热解过程中，ZIF-67 的晶体结构得以保留，同时 Co2N0.67 纳米颗粒（NPs）在 ZIF-67 孔隙中形成。最佳催化剂 Co2N0.67@ZIF-67(450,2)不仅具有很高的光热效率，还能有效活化二氧化碳。利用这些特点，Co2N0.67@ZIF-67(450,2)在 CO2 和环氧氯丙烷的光催化环加成反应中表现出显著的催化活性。在可见光（300 W-m2 Xe 灯，3 h）照射下，（氯甲基）碳酸乙烯酯的产率达到 95%，是 ZIF-67 的 4 倍多。这项研究为通过低温热解提高 MOFs 的光催化活性提供了另一种方法。

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来源期刊

Inorganic Chemistry 化学-无机化学与核化学

CiteScore

7.60

自引率

13.00%

发文量

1960

审稿时长

1.9 months

期刊介绍： Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.