“碳中和”专刊系列文章（四）｜在光催化剂表面构筑外来的氧空位作为CO2和光生电子捕获中心提高光催化CO2还原活性

Constructing extrinsic oxygen vacancy on the surface of photocatalyst as CO₂ and electrons reservoirs to improve photocatalytic CO₂ reduction activity

Zaiyong Jiang, Hao Li, Zhimin Yuan, Zheng Wang, Maohong Fan*, Wenkang Miao^*, Hong He*

https://doi.org/10.1016/j.jes.2023.03.027

在光催化剂表面构建自身氧空位是一种有效的提高光催化CO₂还原活性的方法。然而，一些催化剂具有优异的稳定性，这使得它们很难在其表面构建自身氧空位。为在稳定光催化剂表面实现氧空位的利用，本文提出了在其表面构建外来氧空位的新思路。本文选择稳定的TiO₂纳米片作为研究对象，采用简单的吸附-沉积法在其表面均匀沉积BiOCl量子点。发现当光催化剂进行光催化CO₂还原时，BiOCl量子点能够同时自转化为具有许多氧空位的缺陷BiOCl。这些外来的氧空位可以作为“CO₂和光生电子的捕获中心（类似储存库）”，改善稳定性较好的TiO₂对CO₂的捕获与活化能力，加速光生电子与空穴的分离；因此，与纯TiO₂和BiOCl相比，构建外来氧空位后的TiO₂光催化CO₂还原能力明显增强，并对其作用机制、影响因素和反应路径等进行了全面而深入的探索。本研究不仅扩展了对设计氧空位提高光催化剂CO₂还原活性的基本原理理解，也为稳定催化剂外来氧空位的设计和构筑提供了重要的理论参考。

为在稳定光催化剂表面实现氧空位的利用，本文提出了在其表面构建外来氧空位的新思路，为稳定催化剂外来氧空位的设计和构筑提供了重要的理论参考。

Constructing own oxygen vacancies in the photocatalysts is a very promising method to improve their photocatalytic CO₂ reduction activity. However, some catalysts have excellent stabilities, making it difficult for them to construct their own oxygen vacancies. To simplify the above difficulty of stable photocatalysts, constructing extrinsic oxygen vacancies on their surface as a novel idea is proposed. Here, a stable TiO₂ nanosheet is chosen as a research object, we uniformly deposited BiOCl quantum dots on their surface via a simple adsorption-deposition method. It is found that BiOCl quantum dots are able to simultaneously self-transform into defective BiOCl with many oxygen vacancies when the photocatalyst is performed photocatalytic CO₂ reduction. These extrinsic oxygen vacancies can act as “CO₂ and photo-generated electrons reservoirs” to improve CO₂ capture and accelerate the separation of photogenerated electrons and holes. For the above reasons, the modified TiO₂ showed obvious enhancement of photocatalytic CO₂ reduction compared to pristine TiO₂ and BiOCl. This work may open a new avenue to broaden the use of oxygen vacancies in the process of photocatalytic CO₂ reduction.

第一作者

姜在勇，潍坊学院教授，主要从事光催化、光热催化CO₂为有机碳源的研究，以第一及通讯作者在Angew. Chem. Int. Ed.（2篇）、Chem Catalysis、Advanced Science、Appl. Catal. B: Environ. （5篇）、Chem. Eng. J.（2篇）、Environmental Science and Ecotechnology、Green Energy & Environment等期刊发表SCI论文30篇，1区论文16篇，授权发明专利10项。获山东省自然科学二等奖、山东省优秀博士学位论文、最美教师、潍院好人等。

通讯作者

贺泓，中国工程院院士，中国科学院生态环境研究中心研究员，区域大气环境研究卓越创新中心首席科学家。主要研究方向为环境催化和非均相大气化学过程，系统研究大气复合污染形成机理、环境催化反应体系设计和大气污染物催化净化新原理、新方法及其应用，取得了柴油车排放污染控制、室内空气净化和大气灰霾成因与控制研究方面的系列成果。发表学术论文600余篇，SCI总被引39600余次。获授权发明专利70余项，多项专利技术转让企业实施应用。现任Environmental Science & Technology、Journal of Environmental Sciences和《环境科学》副主编以及Applied Catalysis B: Environmental 等多个国际、国内期刊编委。

https://www.sciencedirect.com/science/article/abs/pii/S1001074223001419

Zaiyong Jiang, Hao Li, Zhimin Yuan, Zheng Wang, Maohong Fan,Wenkang Miao, Hong He, 2024. Constructing extrinsic oxygen vacancy on the surface of photocatalyst as CO₂ and electrons reservoirs to improve photocatalytic CO₂ reduction activity. J. Environ. Sci. 140, 37-45.