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Photoinduction of Cu Single Atoms Decorated on UiO-66-NH2 for Enhanced Photocatalytic Reduction of CO2 to Liquid Fuels
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-10-29 , DOI: 10.1021/jacs.0c09599
Gang Wang 1 , Chun-Ting He 2 , Rong Huang 1 , Junjie Mao 1 , Dingsheng Wang 3 , Yadong Li 3
Affiliation  

Photocatalytic reduction of CO2 to value-added fuels is a promising route to reduce global warming and enhance energy supply. However, poor selectivity and low efficiency of catalysts are usually the limiting factor of their applicability. Herein, a photoinduction method was developed to achieve the formation of Cu single atoms on a UiO-66-NH2 support (Cu SAs/UiO-66-NH2) that could significantly boost the photoreduction of CO2 to liquid fuels. Notably, the developed Cu SAs/UiO-66-NH2 achieved the solar-driven conversion of CO2 to methanol and ethanol with an evolution rate of 5.33 and 4.22 μmol h-1 g-1, respectively. These yields were much higher than those of pristine UiO-66-NH2 and Cu nanoparticles/UiO-66-NH2 composites. Theoretical calculations revealed that the introduction of the Cu SAs on the UiO-66-NH2 greatly facilitates the conversion of CO2 to CHO* and CO* intermediates, leading to excellent selectivity toward methanol and ethanol. This study provides new insights for designing high-performance catalyst for photocatalytic reduction of CO2 at the atomic scale.

中文翻译:

在 UiO-66-NH2 上装饰的 Cu 单原子的光诱导增强 CO2 光催化还原为液体燃料

将二氧化碳光催化还原为增值燃料是减少全球变暖和增加能源供应的有前途的途径。然而,催化剂的选择性差和效率低通常是其适用性的限制因素。在此,开发了一种光诱导方法来实现在 UiO-66-NH2 载体(Cu SAs/UiO-66-NH2)上形成 Cu 单原子,该方法可以显着促进 CO2 光还原为液体燃料。值得注意的是,所开发的 Cu SAs/UiO-66-NH2 实现了太阳能驱动的 CO2 向甲醇和乙醇的转化,其演化速率分别为 5.33 和 4.22 μmol h-1 g-1。这些产率远高于原始 UiO-66-NH2 和 Cu 纳米颗粒/UiO-66-NH2 复合材料的产率。理论计算表明,在 UiO-66-NH2 上引入 Cu SA 极大地促进了 CO2 向 CHO* 和 CO* 中间体的转化,从而对甲醇和乙醇具有出色的选择性。该研究为设计用于在原子尺度上光催化还原 CO2 的高性能催化剂提供了新的见解。
更新日期:2020-10-29
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