催化作用
光催化
金属有机骨架
膜
化学工程
传质
扩散
人工光合作用
材料科学
分子
化学
金属
纳米技术
物理化学
吸附
有机化学
热力学
工程类
物理
生物化学
色谱法
作者
Yuchen Hao,Liwei Chen,Jiani Li,Guanlong Yu,Xin Su,Shu Miao,Qinghua Zhang,Wenyan Gao,Siwu Li,Zhengkun Yu,Lin Gu,Xiao Feng,Anxiang Yin,Rui Si,Yawen Zhang,Bo Wang,Chun‐Hua Yan
标识
DOI:10.1038/s41467-021-22991-7
摘要
Abstract The demand for sustainable energy has motivated the development of artificial photosynthesis. Yet the catalyst and reaction interface designs for directly fixing permanent gases (e.g. CO 2 , O 2 , N 2 ) into liquid fuels are still challenged by slow mass transfer and sluggish catalytic kinetics at the gas-liquid-solid boundary. Here, we report that gas-permeable metal-organic framework (MOF) membranes can modify the electronic structures and catalytic properties of metal single-atoms (SAs) to promote the diffusion, activation, and reduction of gas molecules (e.g. CO 2, O 2 ) and produce liquid fuels under visible light and mild conditions. With Ir SAs as active centers, the defect-engineered MOF (e.g. activated NH 2 -UiO-66) particles can reduce CO 2 to HCOOH with an apparent quantum efficiency (AQE) of 2.51% at 420 nm on the gas-liquid-solid reaction interface. With promoted gas diffusion at the porous gas-solid interfaces, the gas-permeable SA/MOF membranes can directly convert humid CO 2 gas into HCOOH with a near-unity selectivity and a significantly increased AQE of 15.76% at 420 nm. A similar strategy can be applied to the photocatalytic O 2 -to-H 2 O 2 conversions, suggesting the wide applicability of our catalyst and reaction interface designs.
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