Engineering the electron localization of metal sites on nanosheets assembled periodic macropores for CO2 photoreduction
Year: 2024
Type: article
Abstract: Photocatalytic conversion of CO2 into syngas is highly appealing, yet still suffers from the undesirable product yield due to the sluggish carrier transfer and the uncontrollable affinity between catalytic sites and intermediates. Here we report the fabrication of Co sites with tunable electron localization capability on two dimensional (2D) nanosheets assembled three dimensional (3D) ordered macroporous framework (3DOM-NS). The as-prepared Co-based 3DOM-NS catalysts exhibit attractive photocatalytic performances toward CO2 reduction, among which the cobalt sulfide one (3DOM Co-SNS) shows the highest syngas generation rate up to 347.3 μmol h−1 under the irradiation of visible light and delivers a remarkable catalytic activity (1150.7 μmol h−1) in a flow reaction system under natural sunlight. Mechanism studies reveal that the high electron localization of metal sites in 3DOM Co-SNS strengthens the interaction between Co and HCOO* via the orbital interactions of dyz/dxz-p and s-s, thus facilitating the cleaving process of C-O bond. Additionally, the ordered macroporous framework with nanosheet subunits elevates the transfer efficiency of photoexcited electrons, which contributes to its high activity. Efficient photocatalytic conversion of CO2 into syngas is a promising but challenging technology. Here, the authors report a phase transformation method to produce Co sites with tunable electron localization on multi-dimensional architecture framework that can improve the syngas evolution kinetics.
Source: Nature Communications
Authors: Wenyuan Lyu, Yang Liu, Datong Chen, Fengliang Wang, Yingwei Li
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $6,790
Funders: National Natural Science Foundation of China, China Postdoctoral Science Foundation, Natural Science Foundation of Guangdong Province, State Key Laboratory of Pulp and Paper Engineering, Fundamental Research Funds for the Central Universities, Basic and Applied Basic Research Foundation of Guangdong Province
Awards: G1197288352, G1343567502, G196906030, G2056755392, G2175268510, G352717400, G3580910146, G3677923084, G450522368, G4539161472, G4686007098, G5049568817, G5634135377, G5967657561, G6353200517, G6457381068, G669941323, G6725202966, G6903804668, G7335439668, G7560627288, G8262475474, G8343759103
OpenAlex ID: W4405017985
