二维金属偶氮盐框架用于高效二氧化碳光还原  

2D metal azolate framework for efficient CO2 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 Jianxia Gu;Lingxin Wang;Xu Han;Jingting He;Siqi You;Man Dong;Guogang Shan;Danfeng He;Fujiang Zhou;Chunyi Sun;Zhongmin Su(Department of Chemistry,Xinzhou Normal University,Xinzhou 034000,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;School of Chemical and Environmental Engineering,Changchun University of Science and Technology,Changchun 130022,China)

机构地区：[1]Department of Chemistry,Xinzhou Normal University,Xinzhou 034000,China [2]College of Science,Qiongtai Normal University,Haikou 571100,China [3]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 [4]School of Chemical and Environmental Engineering,Changchun University of Science and Technology,Changchun 130022,China

出　　处：《Science China Materials》2024年第8期2637-2644,共8页中国科学（材料科学）（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(NSFC)(22371033,22175033,and 22266028);the Outstanding Young Technology Talent Foundation of Jilin Province(20230508108RC);the Fundamental Research Funds for the Central Universities(2412019FZ007);the Natural Science Foundation of Hainan Province(823MS062);the Foundation of Xinzhou Teachers University(2021KY07);the Science and Technology Innovation Project of Higher Education in Shanxi Province(2021L450);the Youth Science Research Project of Shanxi Province(202103021223362)。

摘　　要：由可见光驱动的将CO_(2)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CO_(2)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(H;4;TTPE)与钴的自组装实现了对CO_(2)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CO_(2)还原的能级,还能在整个CO_(2)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CO_(2)光还原的2D MAFs光催化剂指引了方向.Visible-light-driven conversion of CO_(2)into value-added fuel is a clean and renewable technology to retard global warming and address energy shortages.Two-dimensional metal-azolate frameworks(2D MAFs)have recently received tremendous attention as CO_(2)photoreduction-related catalysts due to their specific electron transport pathways,highly exposed surface-active sites,and tailorable lightabsorption abilities.However,the research on 2D MAFs for efficient CO_(2)photoconversion is still at the early stage.Herein,a novel 2D MAFs(compound 1)was designed by selfassembly of tetra-(4-tetrazole-phenyl)ethylene(H4TTPE)and cobalt for CO_(2)photoreduction.As a comparison,three-dimensional(3D)compound 2 was also constructed using a similar 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 production 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 CO_(2)reduction but also facilitates efficient electron-hole separation throughout the CO_(2)photoreduction process.This work paves the way for the design of 2D MAFs photocatalysts tailored for efficient CO_(2)photoconversion.

关 键 词：光还原 表面活性位 能源短缺 二维结构 二氧化碳 三维结构 传输路径 全球变暖 

分 类 号：X701[环境科学与工程—环境工程] O643.36[理学—物理化学] O644.1[理学—化学]