Heterostructure Engineering of a Reverse Water Gas Shift Photocatalyst

Wang, H (Wang, Hong)^{[ 1 ]} ; Jia, J (Jia, Jia)^{[ 2,3 ]} ; Wang, L (Wang, Lu)^{[ 2,4 ]} ; Butler, K (Butler, Keith)^{[ 5 ]} ; Song, R (Song, Rui)^{[ 2 ]} ; Casillas, G (Casillas, Gilberto)^{[ 6 ]} ; He, L (He, Le)^{[ 4 ]} ; Kherani, NP (Kherani, Nazir P.)^{[ 3 ]} ; Perovic, DD (Perovic, Doug D.)^{[ 3 ]} ; Jing, LQ (Jing, Liqiang)^{[ 7 ]} ; Walsh, A (Walsh, Aron)^{[ 8,9 ]} ; Dittmeyer, R (Dittmeyer, Roland)^{[ 10 ]} ; Ozin, GA (Ozin, Geoffrey A.)^{[ 2 ]}

ADVANCED SCIENCE, 2019, 6(22): 文献号: 1902170

DOI: 10.1002/advs.201902170

摘要

To achieve substantial reductions in CO2 emissions, catalysts for the photoreduction of CO2 into value-added chemicals and fuels will most likely be at the heart of key renewable-energy technologies. Despite tremendous efforts, developing highly active and selective CO2 reduction photocatalysts remains a great challenge. Herein, a metal oxide heterostructure engineering strategy that enables the gas-phase, photocatalytic, heterogeneous hydrogenation of CO2 to CO with high performance metrics (i.e., the conversion rate of CO2 to CO reached as high as 1400 mu mol g cat(-1) h(-1)) is reported. The catalyst is comprised of indium oxide nanocrystals, In2O3-x(OH)(y), nucleated and grown on the surface of niobium pentoxide (Nb2O5) nanorods. The heterostructure between In2O3-x(OH)(y) nanocrystals and the Nb2O5 nanorod support increases the concentration of oxygen vacancies and prolongs excited state (electron and hole) lifetimes. Together, these effects result in a dramatically improved photocatalytic performance compared to the isolated In2O3-x(OH)(y) material. The defect optimized heterostructure exhibits a 44-fold higher conversion rate than pristine In2O3-x(OH)(y). It also exhibits selective conversion of CO2 to CO as well as long-term operational stability.