Boosting electron transport in CoFe2O4/Fe2O3 heterojunction with iron-oxygen bridges for enhanced photo-Fenton degradation of emerging contaminants

IF 5.4 3区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Fengting Geng , Kechao Wang , Yingsheng Yang , Xiaoli Wang , Haixiang Han , Junjie Tian , Shujuan Zhuang , Wenyuan Han , Longlong Geng
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引用次数: 0

Abstract

Photo-assisted Fenton-like catalysis is regarded as a green and sustainable route for degrading and mineralizing emerging contaminants in water. In this work, novel CoFe2O4/Fe2O3 heterojunction (CFO/FO) with iron-oxygen bridges were successfully constructed via a temperature controled in-situ pyrolysis using bimetallic MOF as precursors. Interestingly, the iron-oxygen bridges endowed CFO/FO with atomically aligned interface, thus suppressing carrier recombination during photo-Fenton degradation of emerging contaminants. Under visible-light-irradiation, CFO/FO achieves 99.6 % tetracycline (TC) degradation within 25 min, achieving a rate constant (0.163 min−1) 6.3 times and 3.1 times higher than that of bare FO and CFO. Additionally, CFO/FO exhibits remarkable versatility across a wide pH range, various water sources, diverse pollutants, and achieved high efficiency in continuous pollutant degradation for over 2000 min with negligible metal leaching. The combined DFT simulations and characterizations confirmed the key role of iron-oxygen bridges by providing efficient transmission channel for photoinduced charges, thereby contributing abundant photogenerated holes and promoting the cycle of dual-metal redox couples (Co3+/Co2+ and Fe3+/Fe2+), which synergistically promote the generation of oxygen-containing radicals and the complete degradation of pollutants. This study advances charge transfer boosting through interfacial bridges construction in heterojunctions, and offer paradigm for development of robust catalysts for sustainable water purification.

Abstract Image

铁氧桥增强CoFe2O4/Fe2O3异质结中的电子传递,增强新污染物的光- fenton降解
光辅助类芬顿催化被认为是一种绿色和可持续的降解和矿化水中新兴污染物的途径。本文以双金属MOF为前驱体,通过控温原位热解成功构建了具有铁氧桥的新型CoFe2O4/Fe2O3异质结(CFO/FO)。有趣的是,铁氧桥赋予CFO/FO原子排列的界面,从而抑制了光- fenton降解新污染物过程中的载流子重组。在可见光照射下,CFO/FO在25 min内达到99.6%的四环素(TC)降解,其降解速率常数(0.163 min−1)分别是裸FO和CFO的6.3倍和3.1倍。此外,CFO/FO在广泛的pH范围、不同的水源、不同的污染物中表现出显著的多功能性,并且在超过2000分钟的连续污染物降解中实现了高效率,金属浸出可以忽略不计。结合DFT模拟和表征证实了铁氧桥的关键作用,它为光诱导电荷提供了有效的传输通道,从而提供了丰富的光生空穴,促进了双金属氧化还原对(Co3+/Co2+和Fe3+/Fe2+)的循环,协同促进了含氧自由基的产生和污染物的完全降解。本研究通过异质结界面桥的构建促进了电荷转移,为可持续水净化催化剂的开发提供了范例。
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
Inorganic Chemistry Communications
Inorganic Chemistry Communications 化学-无机化学与核化学
CiteScore
5.50
自引率
7.90%
发文量
1013
审稿时长
53 days
期刊介绍: Launched in January 1998, Inorganic Chemistry Communications is an international journal dedicated to the rapid publication of short communications in the major areas of inorganic, organometallic and supramolecular chemistry. Topics include synthetic and reaction chemistry, kinetics and mechanisms of reactions, bioinorganic chemistry, photochemistry and the use of metal and organometallic compounds in stoichiometric and catalytic synthesis or organic compounds.
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