复旦大学张立武团队报道了微滴气液界面显著加速光催化CO₂还原。相关研究成果发表在2023年5月5日出版的国际学术期刊《德国应用化学》。

太阳能驱动的CO₂还原反应（CO₂RR）在很大程度上受到缓慢的传质和光生载流子快速组合的限制。

该文中，研究人员发现微滴提供的丰富气液界面处的光催化CO₂RR效率比相应的体相反应高两个数量级。即使在没有牺牲剂的情况下，微滴介导的WO₃·0.33H2O上HCOOH的产率也达到2536μmol h^-1g^-1（相对于体相中的13μmol h^-1g^-1），这显著优于先前报道的体相反应条件下的光催化CO₂RR。除了将CO₂有效地输送到微滴内的光催化剂表面外，还揭示了微滴气液界面处的强电场本质上促进了光生电子-空穴对的分离。

该项研究深入了解了微滴气液界面促进的超快反应动力学，并为解决光催化CO2还原为燃料的低效率问题提供了一种新的方法。

附：英文原文

Title: Significant Acceleration of Photocatalytic CO2 Reduction at the Gas-Liquid Interface of Microdroplets

Author: Qiuyue Ge, Yangyang Liu, Kejian Li, Lifang Xie, Xuejun Ruan, Wei Wang, Longqian Wang, Tao Wang, Wenbo You, Liwu Zhang

Issue&Volume: 2023-05-05

Abstract: Solar-driven CO2 reduction reaction (CO2RR) is largely constrained by the sluggish mass transfer and fast combination of photogenerated charge carriers. Herein, we find that the photocatalytic CO2RR efficiency at the abundant gas-liquid interface provided by microdroplets is two orders of magnitude higher than that of the corresponding bulk phase reaction. Even in the absence of sacrificial agents, the production rates of HCOOH over WO3·0.33H2O mediated by microdroplets reaches 2536 μmol h-1g-1 (vs. 13 μmol h-1g-1 in bulk phase), which is significantly superior to the previously reported photocatalytic CO2RR in bulk phase reaction condition. Beyond the efficient delivery of CO2 to photocatalyst surfaces within microdroplets, we reveal that the strong electric field at the gas-liquid interface of microdroplets essentially promotes the separation of photogenerated electron-hole pairs.  This study provides a deep understanding of ultrafast reaction kinetics promoted by the gas-liquid interface of microdroplets and a novel way of addressing the low efficiency of photocatalytic CO2 reduction to fuel.

DOI: 10.1002/anie.202304189

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202304189