材料科学
光催化
尼亚尔
光化学
催化作用
氢氧化物
无机化学
金属间化合物
有机化学
化学
合金
复合材料
作者
Chenjun Ning,Jiangrong Yang,Sha Bai,Guangbo Chen,Guihao Liu,Tianyang Shen,Lirong Zheng,Simin Xu,Xianggui Kong,Bin Liu,Yufei Zhao,Yu‐Fei Song
标识
DOI:10.1002/adfm.202300365
摘要
Abstract Photocatalytic CO 2 reduction (CO 2 PR) into multi‐carbon products (especially C 2 H 4 ) is a highly attractive route for global carbon cycle, however, which is seriously limited by sluggish C‐C coupling kinetics and competitive hydrogen evolution reaction (HER) and so on. Herein, the fabrication of a novel supramolecular assembly of NiAl‐Fe‐TCPP is reported by intercalating iron porphyrin (Fe‐TCPP) into NiAl‐layered double hydroxide (NiAl‐LDH), and the resultant NiAl‐Fe‐TCPP exhibit superior catalytic performance on CO 2 PR to C 2 H 4 under visible light irradiation in presence of photosensitizer. A high C 2 H 4 selectivity up to 93.4% in the carbon‐containing products with the production rate as high as 24.7 µmol h −1 can be achieved over NiAl‐Fe‐TCPP. The ex/in situ X–ray absorption spectoscopy (XAS) indicates that the electron transfer between NiAl‐LDH and Fe‐TCPP can promote the generation of low‐valence of Fe sites, resulting in the efficient production of C 2 H 4 . The spin‐polarized density functional theory (DFT) calculations find that the synergistic mechanism that CO 2 molecules are activated to CO on NiAl‐LDH and then spilled to Fe‐TCPP and coupled to COCHO # , which is further reduced to C 2 H 4 , are feasible in the perspective of Gibbs free energy. Moreover, the strong host‐guest interactions between NiAl‐LDH and Fe‐TCPP lead to the promoted photocatalytic activity and superior cycle stability.
科研通智能强力驱动
Strongly Powered by AbleSci AI