Oxygen-tolerant photocatalytic conversion of simulated flue gas to ethylene

IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Chem Pub Date : 2025-05-08 Epub Date: 2025-03-05 DOI:10.1016/j.chempr.2024.102391
Qiong Liu , Hui Cheng , Ching Kit Tommy Wun , Tianxiang Chen , Tsz Woon Benedict Lo , Fuxian Wang
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Abstract

Photocatalytic reduction of CO2 in flue gas faces significant challenges due to the low CO2 concentration and the presence of oxygen (O2), which induces competitive oxygen reduction reactions, as well as the sluggish kinetics and complex product separation of oxidation half-reactions. Herein, we developed a dual copper (Cu)/platinum (Pt) atom on carbon nitride (CN-CuPt) photocatalyst, achieving synergistic ethylene production through low CO2 concentration (i.e., 12% CO2) reduction coupled with isopropanol oxidation to acetone for the first example. A benchmark photocatalytic ethylene yield of 778.6 μmolh−1gcat−1 with a high selectivity of 87.0% is obtained, outperforming all the state-of-the-art CO2 photocatalysts. What’s more, the CN-CuPt exhibits high oxygen tolerance, and more than 90% of its performance is retained under the interference of 5% oxygen due to oxygen inhibition by Cu species. Our strategy of regulating adsorption sites shows great potential for designing catalysts for practical photocatalytic reduction of flue gas.

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模拟烟气耐氧光催化转化为乙烯
由于低CO2浓度和氧气(O2)的存在导致竞争性氧还原反应,以及氧化半反应动力学缓慢和产物分离复杂,因此在烟气中光催化还原CO2面临重大挑战。在此,我们开发了一种双铜(Cu)/铂(Pt)原子氮化碳(CN-CuPt)光催化剂,通过低CO2浓度(即12% CO2)还原以及异丙醇氧化成丙酮来实现协同乙烯生产。光催化乙烯的收率为778.6 μmolh - 1gcat - 1,选择性高达87.0%,优于现有的CO2光催化剂。此外,CN-CuPt具有较高的氧耐受性,由于Cu的阻氧作用,在5%氧的干扰下仍能保持90%以上的性能。我们的调节吸附位点的策略显示出设计用于实际光催化还原烟气的催化剂的巨大潜力。
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来源期刊
Chem
Chem Environmental Science-Environmental Chemistry
CiteScore
32.40
自引率
1.30%
发文量
281
期刊介绍: Chem, affiliated with Cell as its sister journal, serves as a platform for groundbreaking research and illustrates how fundamental inquiries in chemistry and its related fields can contribute to addressing future global challenges. It was established in 2016, and is currently edited by Robert Eagling.
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