Optimization of CO2 Mass Transfer and Modulation of Reaction Kinetics for Efficient CO2 Conversion via a Three‐Phase Photocatalytic Flow System

IF 18.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Hui Fu, Yuli Lei, Qianqian Zhang, Yuanyuan Liu, Zhaoke Zheng, Hefeng Cheng, Baibiao Huang, Haibo Ma, Peng Wang
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Abstract

The design of a photocatalytic system with conducive CO2 mass transfer, reaction kinetics, and product venting is crucial for achieving stable and efficient photocatalytic CO2 reduction reaction (CO2RR). Herein, a three‐phase photocatalytic flow system is developed to optimize the CO2 mass transfer and modulate the reaction kinetics, and prepare single‐atom‐based photocatalyst to boost the performance of CO2RR. Kinetic calculations present that the flow system optimizes the first‐order reaction of the conventional non‐flow system to zero‐order reaction, which facilitates the efficient and long‐lasting photocatalytic CO2RR. Ab initio quantum chemical simulations of both the ground and excited states reveal that the enhanced performance stems from charge transfer photoexcitation associated with the doped single Co atom, which facilitates proton adsorption, reduces the energy barrier, and promotes C–OH bond cleavage. Taking advantage of the three‐phase flow system and single‐atom catalyst, the CO generation rate increases to 2.35 µmol h−1 with a selectivity of 97.8%. This work opens a new avenue for the rational design of high‐efficiency CO2 conversion systems and holds promise for other photocatalytic applications.
通过三相光催化流动系统优化CO2传质及高效CO2转化反应动力学
设计一个有利于CO2传质、反应动力学和产物排气的光催化体系是实现稳定、高效的光催化CO2还原反应(CO2RR)的关键。为了优化CO2传质和调节反应动力学,设计了一种三相光催化流体系,制备了单原子基光催化剂,提高了CO2RR的性能。动力学计算表明,流动体系将常规非流动体系的一级反应优化为零级反应,有利于高效、持久的光催化CO2RR。基态和激发态的从头算量子化学模拟表明,性能的增强源于掺杂单Co原子的电荷转移光激发,这有利于质子吸附,降低能量势垒,促进C-OH键的裂解。采用三相流体系和单原子催化剂,CO的生成速率提高到2.35µmol h−1,选择性为97.8%。这项工作为合理设计高效的二氧化碳转化系统开辟了新的途径,并为其他光催化应用带来了希望。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
期刊介绍: Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.
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