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
谷建霞 1王龄欣 2韩旭 3贺敬婷 2由思琦 4董曼 4单国刚 4何丹凤 5周付江 5孙春义 4苏忠民2
作者信息
- 1. 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
- 2. School of Chemical and Environmental Engineering,Changchun University of Science and Technology,Changchun 130022,China
- 3. College of Science,Qiongtai Normal University,Haikou 571100,China;School of Chemical and Environmental Engineering,Changchun University of Science and Technology,Changchun 130022,China
- 4. 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
- 5. College of Science,Qiongtai Normal University,Haikou 571100,China
- 折叠
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.
Abstract
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.
关键词
metal-azolate frameworks/two-dimensional struc-ture/CO2 photoreductionKey words
metal-azolate frameworks/two-dimensional struc-ture/CO2 photoreduction引用本文复制引用
基金项目
National Natural Science Foundation of China(NSFC)(22371033)
National Natural Science Foundation of China(NSFC)(22175033)
National Natural Science Foundation of China(NSFC)(22266028)
Outstanding Young Technology Talent Foundation of Jilin Province(20230508108RC)
Fundamental Research Funds for the Central Universities(2412019FZ007)
Natural Science Foundation of Hainan Province(823MS062)
Foundation of Xinzhou Teachers University(2021KY07)
Science and Technology Innovation Project of Higher Education in Shanxi Province(2021L450)
Youth Science Research Project of Shanxi Province(202103021223362)
出版年
2024
NETL
NSTL
万方数据