清华大学Yadong Li小组近日取得一项新成果。他们通过在UiO-66-NH₂基底上引入单个铜原子，显著提升了光催化还原二氧化碳生成液体燃料的表现。 相关论文发表在2020年10月29日的《美国化学会志》上。

研究人员开发了一种光诱导的方法来实现在UiO-66-NH₂基底上单个铜原子的形成(Cu SAs/UiO-66-NH₂)，可以显著提升光还原二氧化碳产生液体燃料的过程。值得注意的是，开发的Cu SAs/UiO-66-NH₂实现了太阳能转换二氧化碳到甲醇和乙醇，其转化速率分别为5.33和4.22 μmol h ^-1 g ^-1。这些产率远高于那些原始的UiO-66-NH₂和铜纳米粒子/ UiO-66-NH₂复合材料。

理论计算表明，在UiO-66-NH₂上引入铜单原子大大促进二氧化碳转换成CHO*和CO*中间体，导致生成甲醇和乙醇的优秀选择性。这项研究为设计高性能的催化剂在原子尺度光催化还原二氧化碳提供了新的见解。

据介绍，光催化还原二氧化碳产生价值提升的燃料是一种很有前景的途径，用来缓解全球变暖及提高能源供应。然而，催化剂的选择性差和效率低是它们实用性的限制因素。

附：英文原文

Title: Photoinduction of Cu Single Atoms Decorated on UiO-66-NH2 for Enhanced Photocatalytic Reduction of CO2 to Liquid Fuels

Author: Gang Wang, Chun-Ting He, Rong Huang, Junjie Mao, Dingsheng Wang, Yadong Li

Issue&Volume: October 29, 2020

Abstract: 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.

DOI: 10.1021/jacs.0c09599

Source: https://pubs.acs.org/doi/10.1021/jacs.0c09599