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.
作者
陈敏
吴嗣怡
钟豪杰
胡嘉欢
付永前
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)
出处
《分子催化(中英文)》
北大核心
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)。
关键词
光催化
二氧化碳
催化剂
MOFS
甲酸
photocatalysis
carbon dioxide
catalyst
MOFs
formic acid
作者简介
陈敏(2003-),女,本科生,研究方向为生物材料,E-mail:2580302800@qq.com;通信联系人:孙小龙,E-mail:sunxiaolong198901@163.com.
