基于MOFs的新型催化剂光催化转化CO_(2)制备甲酸  

Novel Catalyst Based on MOFs for Photocatalytic Conversion of CO_(2)to Formic Acid

作　　者：陈敏 吴嗣怡 钟豪杰 胡嘉欢 付永前[1,2] 孙小龙 CHEN Min;WU Siyi;ZHONG Haojie;HU Jiahuan;FU Yongqian;SUN Xiaolong(School of Life Sciences,Taizhou University,Taizhou 318000,China;Taizhou Key Laboratory of Biomass Functional Materials Development and Application,Taizhou University,Taizhou 318000,China)

机构地区：[1]台州学院生命科学学院,浙江台州318000 [2]台州学院台州市生物质功能材料开发与应用重点实验室,浙江台州318000

出　　处：《分子催化(中英文)》2025年第2期120-128,I0001,I0002,共11页Journal of Molecular Catalysis(China)

基　　金：全国大学生创新创业项目(202310350025);浙江省新苗项目(2024R435A006);台州市科技计划项目(23gyb07)。

摘　　要：当今世界,全球气候变暖、能源短缺等问题都与二氧化碳息息相关.金属-有机框架(Metal-Organic Frameworks,MOFs)材料具有高孔隙、大比表面积、丰富的活性位点等结构优势,在光催化转化CO_(2)过程具有重要优势.通过金属有机框架制备了一种新型光催化剂(TCPP-C_(3)N_(4)/PEI/Rh@ZIF-8)和酶催化剂(FDH@ZIF-8),分别负载了Rh配合物偶联到TCPP修饰的g-C_(3)N_(4)光催化剂(TEOA为电子供体)和甲酸脱氢酶(FDH),利用烟酰胺腺嘌呤二核苷酸(NADH)的再生催化转化CO_(2),在合成体系中光催化生成969.42μmol·L^(-1)甲酸.在游离FDH与未连接PEI的光催化剂对比研究发现FDH@ZIF-8系统中生成的甲酸(969.42μmol·L^(-1))略高于游离FDH和未连接PEI的甲酸(934.78μmol·L^(-1)和793.48μmol·L^(-1)),但稳定性与耐受性都有较大提高.因此,该工作为探讨开发新型催化剂光催化转化CO_(2)高效合成甲酸提供了思路.In today's world,global warming,energy shortage and other problems are closely related to carbon dioxide.Metal-organic frameworks(MOFs)materials have structural advantages such as high porosity,large specific surface area and abundant active sites,and have important advantages in the photocatalytic CO_(2)conversion process.A new type of photocatalyst(TCPP-C_3N_4/PEI/Rh@ZIF-8)and enzyme catalyst(FDH@ZIF-8)were prepared by MOFs.The Rh-complex was coupled to TCPP-modified g-C_3N_(4)photocatalyst(TEOA as electron donor)and formate dehydrogenase(FDH),respectively.The CO_(2)was converted by the regeneration of nicotinamide adenine dinucleotide(NADH),and 969.42μmol·L^(-1)formic acid was formed in the synthesis system.In the comparison of photocatalysts with free FDH and unconnected PEI,969.42μmol·L^(-1)formic acid produced in FDH@ZIF-8 system is slightly higher than that produced by free FDH and unconnected PEI(934.78μmol·L^(-1)and 793.48μmol·L^(-1)),but the stability and tolerance are greatly improved.Therefore,this work provides a way to explore the development of new catalysts for photocatalytic conversion of CO_(2)to efficiently synthesize formic acid.

关 键 词：光催化 二氧化碳 催化剂 MOFS 甲酸 

分 类 号：O643.36[理学—物理化学]