Sun Dengrong, Fu Yanghe, Liu Wenjun, Ye Lin, Wang Dengke, Yang Lin, Fu Xianzhi, Li Zhaohui
Research Institute of Photocatalysis, Fujian Provincial Key Laboratory of Photocatalysis, State Key Laboratory Breeding Base, College of Chemistry and Chemical Engineering, Fuzhou University, Fuzhou 350002 (P. R. China).
Chemistry. 2013 Oct 11;19(42):14279-85. doi: 10.1002/chem.201301728. Epub 2013 Sep 3.
Metal-organic framework (MOF) NH2 -Uio-66(Zr) exhibits photocatalytic activity for CO2 reduction in the presence of triethanolamine as sacrificial agent under visible-light irradiation. Photoinduced electron transfer from the excited 2-aminoterephthalate (ATA) to Zr oxo clusters in NH2 -Uio-66(Zr) was for the first time revealed by photoluminescence studies. Generation of Zr(III) and its involvement in photocatalytic CO2 reduction was confirmed by ESR analysis. Moreover, NH2 -Uio-66(Zr) with mixed ATA and 2,5-diaminoterephthalate (DTA) ligands was prepared and shown to exhibit higher performance for photocatalytic CO2 reduction due to its enhanced light adsorption and increased adsorption of CO2 . This study provides a better understanding of photocatalytic CO2 reduction over MOF-based photocatalysts and also demonstrates the great potential of using MOFs as highly stable, molecularly tunable, and recyclable photocatalysts in CO2 reduction.
金属有机框架（MOF）NH2 -Uio-66(Zr)在可见光照射下，以三乙醇胺作为牺牲剂时，表现出光催化还原二氧化碳的活性。光致发光研究首次揭示了光激发下2-氨基对苯二甲酸（ATA）向NH2 -Uio-66(Zr)中的Zr氧簇的电子转移。电子顺磁共振（ESR）分析证实了Zr(III)的生成及其在光催化还原二氧化碳中的作用。此外，制备了具有混合ATA和2,5-二氨基对苯二甲酸（DTA）配体的NH2 -Uio-66(Zr)，由于其增强的光吸附和对二氧化碳吸附的增加，该材料表现出更高的光催化还原二氧化碳性能。这项研究有助于更好地理解基于MOF的光催化剂对二氧化碳的光催化还原作用，同时也证明了MOF作为高稳定性、分子可调控且可回收的光催化剂在二氧化碳还原中的巨大潜力。
