中国科学院过程工程研究所Dan Wang团队的最新研究制备了具有无定型晶态外壳的异相空心多层结构，可用于CO₂的连续光还原。这一研究成果于2022年10月11日发表在国际顶尖学术期刊《德国应用化学》上。

在该研究中，团队制备了具有空间有序异壳结构的中空多壳结构基（HoMS）微反应器，实现了CO₂→CH₄的两步光致还原作用。该结构内部的多个CeO₂壳增加了活性催化位点的数量，以确保有效的第一步反应生成CO，同时丰富了局部CO浓度。第二步CO→CH₄反应是由邻近的最外层壳中的非晶态TiO₂（A-TiO₂）复合材料诱导的，从而通过一个CeO₂@CeO₂/A-TiO₂ HoMS实现了CO₂向CH₄的转化。这项对微反应器的深入研究为设计可高效连续催化、具有时空有序壳层的基于HoMS的微反应器，提供了成分、结构和界面的指导。

据了解，构建具有串联活性位点的多级别精细纳米/微反应器，是设计可实现CO2减少这一诱人而具有挑战性目标的光催化反应器的有前景的策略。

附：英文原文

Title: Heterogeneous Hollow Multi-Shelled Structures with Amorphous-Crystalline Outer-Shells for Sequentially Photoreduction of CO2

Author: Yanze Wei, Feifei You, Decai Zhao, Jiawei Wan, Lin Gu, Dan Wang

Issue&Volume: 2022-10-11

Abstract: Constructing delicate nano-/microreactors with tandem active sites in hierarchical architectures is a promising strategy for designing photocatalysts to realize the challenging but attractive CO  2    reduction. Herein, hollow multi-shell structure (HoMS) based microreactors with spatial ordered hetero-shells are fabricated, which achieve two-step CO  2   -to-CH  4  photoreduction. The multiple inner CeO  2  shells increase the number of active catalytic sites to ensure efficient first-step reaction for generating CO, along with enriching the local CO concentration. The second-step CO-to-CH  4   reaction is consequently induced by amorphous TiO  2   (A-TiO  2  ) composites on the adjacent outer-most shell, thus realizing the CO  2   -to-CH  4   conversion capability using one CeO  2   @CeO  2   /A-TiO  2   HoMS. In-depth explorations in the microreactors provide compositional, structural, and interfacial guidance for engineering HoMS-based microreactors with temporally–spatially ordered shells toward efficient tandem catalysis.

DOI: 10.1002/anie.202212049

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202212049