二维金属偶氮盐框架用于高效二氧化碳光还原

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中文摘要：由可见光驱动的将CO2转化为高附加值燃料是一种清洁可再生的技术,有助于控制全球变暖和应对能源短缺.近年来,二维的金属偶氮盐框架(2D MAFs)因其特定的电子传输路径、高度暴露的表面活性位点及可调节的吸光能力,在CO2光还原研究中备受关注.然而,对其在该领域的研究仍处于初级阶段.本文设计了一种新型二维MAFs(compound 1),通过四-(4-四唑基苯基)乙烯(H4TTPE)与钴的自组装实现了对CO2的光还原.作为对比,通过类似的合成过程构建了具有三维结构的compound 2.非均相光催化实验结果显示,2D compound 1的光还原性能明显优于3D compound 2,在相同条件下,其CO产率高达11.56 mmol g-1 h-1,是compound 2(1.94 mmol g-1 h-1)的6倍.这一性能优势源于compound 1独特的二维结构,其不仅具有有利于CO2还原的能级,还能在整个CO2光还原过程中促进电子-空穴高效分离.本工作为设计适用于高效CO2光还原的2D MAFs光催化剂指引了方向.

外文标题：2D metal azolate framework for efficient CO2 photoreduction

外文摘要：Visible-light-driven conversion of CO2 into value-added fuel is a clean and renewable technology to retard global warming and address energy shortages.Two-dimen-sional metal-azolate frameworks(2D MAFs)have recently received tremendous attention as CO2 photoreduction-related catalysts due to their specific electron transport pathways,highly exposed surface-active sites,and tailorable light-absorption abilities.However,the research on 2D MAFs for efficient CO2 photoconversion is still at the early stage.Herein,a novel 2D MAFs(compound 1)was designed by self-assembly of tetra-(4-tetrazole-phenyl)ethylene(H4TTPE)and cobalt for CO2 photoreduction.As a comparison,three-di-mensional(3D)compound 2 was also constructed using a si-milar synthesis process.The experimental results of heterogeneous photocatalysis show that the photoreduction performance of 2D compound 1 is obviously better than that of 3D compound 2,exhibiting an extremely high CO pro-duction rate(11.56 mmol g-1 h-1)in 3 h,which is 6.0-fold higher than that of compound 2(1.94 mmol g-1 h-1)under the same conditions.This performance advantage stems from the unique 2D structure of compound 1,which not only possesses an energy level conducive to CO2 reduction but also facilitates efficient electron-hole separation throughout the CO2 photo-reduction process.This work paves the way for the design of 2D MAFs photocatalysts tailored for efficient CO2 photo-conversion.

外文关键词：

metal-azolate frameworkstwo-dimensional struc-tureCO2 photoreduction

作者：

谷建霞、王龄欣、韩旭、贺敬婷、由思琦、董曼、单国刚、何丹凤、周付江、孙春义、苏忠民

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作者单位：

Department of Chemistry,Xinzhou Normal University,Xinzhou 034000,China

National & Local United Engineering Laboratory for Power Batteries,Key Laboratory of Polyoxometalate Science of Ministry of Education,Department of Chemistry,Northeast Normal University,Changchun 130024,China

School of Chemical and Environmental Engineering,Changchun University of Science and Technology,Changchun 130022,China

College of Science,Qiongtai Normal University,Haikou 571100,China

National&Local United Engineering Laboratory for Power Batteries,Key Laboratory of Polyoxometalate Science of Ministry of Education,Department of Chemistry,Northeast Normal University,Changchun 130024,China

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关键词：

metal-azolate frameworks two-dimensional struc-ture CO2 photoreduction

基金：

National Natural Science Foundation of China(NSFC)National Natural Science Foundation of China(NSFC)National Natural Science Foundation of China(NSFC)Outstanding Young Technology Talent Foundation of Jilin ProvinceFundamental Research Funds for the Central UniversitiesNatural Science Foundation of Hainan ProvinceFoundation of Xinzhou Teachers UniversityScience and Technology Innovation Project of Higher Education in Shanxi ProvinceYouth Science Research Project of Shanxi Province

项目编号：

22371033221750332226602820230508108RC2412019FZ007823MS0622021KY072021L450202103021223362

出版年：

2024

DOI：

10.1007/s40843-024-2996-2

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(8)