High-efficiency photodriven coupling of CO2 and various epoxides via a multi-shelled hollow ZIF/MXene derived composite with low activation energy†

IF 6.1 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Yang Wang, Meili Ding, Xiaotong Fu and Jianfeng Yao
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Abstract

Photo-induced coupling of carbon dioxide (CO2) and various epoxides is a promising pathway for synthesizing value-added chemicals but the process is hampered by the high activation energy, poor light absorption, and fast recombination of charge carriers. Herein, cobalt nanoparticles encapsulated in N-doped hierarchically porous carbon/TiO2/MXene (CoNHPC/TM) composites were synthesized by pyrolysis, employing a multilayer ZIF-8@ZIF-67@ZIF-8@ZIF-67 (4L-ZIF)/MXene hybrid as a precursor. During thermolysis, 4L-ZIF was transformed into CoNHPC with a multi-shell hollow structure, while TiO2 nanoparticles formed in situ on the MXene surface. This unique structure induces multiple reflections of internal light, thus increasing the efficiency of light energy harvesting and photothermal conversion, and improving mass diffusion and the separation efficiency of photogenerated carriers. Consequently, a 96% yield for cyclic carbonate was achieved by optimal CoNHPC/TM-8 under irradiation with full spectrum light at 350 mW cm−2 for 6 h. Additionally, its high catalytic efficiency was maintained even under simulated flue gas conditions. Further investigations revealed a decrease in the activation energy and a synergistic photocatalytic–photothermal effect in the reaction systems with CoNHPC/TM-8. Our research provides inspiration for the rational design of MOF-based photocatalysts with desirable practical applicability for enhancing CO2 transformation.

Abstract Image

利用低活化能的多壳中空ZIF/MXene衍生复合材料实现CO2与多种环氧化物的高效光驱动耦合
光诱导二氧化碳(CO2)转化是一种有前途的可持续合成增值化学品的途径,但该过程通常受到高活化能、低光收集能力和电荷载流子快速重组的阻碍。本文以多层ZIF-8@ZIF-67@ZIF-8@ZIF-67 (4L-ZIF)/MXene杂化物为前驱体,采用高温热解法制备了包裹在n掺杂分层多孔碳/TiO2/MXene (CoNHPC/TM)复合材料中的钴纳米颗粒。在热解过程中,多层4L-ZIF固体转化为具有多壳中空结构的CoNHPC,而TiO2纳米颗粒在MXene表面原位形成。这种独特的结构诱导了内部光的多次反射,从而提高了光能收集和光热转换的效率,并显著提高了光生载流子的质量扩散和分离效率。因此,最佳的CoNHPC/TM-8 (4L-ZIF与MXene的初始质量比为8:1)在350 mW/cm2的全光谱光照射6小时下,循环碳化物的收率达到96%。此外,即使在模拟烟气条件下,其催化效率也保持较高。进一步的研究表明,在与CoNHPC/TM-8的反应体系中,活化能降低,并具有协同光催化-光热效应。我们的研究为合理设计mof基光催化剂提供了灵感,这些催化剂在促进CO2转化方面具有良好的实用性。
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来源期刊
Inorganic Chemistry Frontiers
Inorganic Chemistry Frontiers CHEMISTRY, INORGANIC & NUCLEAR-
CiteScore
10.40
自引率
7.10%
发文量
587
审稿时长
1.2 months
期刊介绍: The international, high quality journal for interdisciplinary research between inorganic chemistry and related subjects
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