Mechanism of Molecular Oxygen Activation Mediated by Hydroxyl Groups on the Surface of Red Clay

Qing Du, Huibin Niu, Yan Xu, Jing Zhang, Xing Lan,Yingping Huang,Yunzhi Tan, Xiaoting Chen,Yanfen Fang

CHEMICAL JOURNAL OF CHINESE UNIVERSITIES-CHINESE(2024)

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摘要
The activation mechanism of molecular oxygen(O2? by surface hydroxyl groups(Me-OH? Me=Al? Si? Fe?of natural clay minerals is still unclear. In this study? red clay(R-Clay? was heat-treated at varying temperatures in N2 to adjust the number and shape of Me-OH sites on its surface? thus activating O2 to different degrees for tetracy ?cline(TC? degradation in water. As the temperature increased? the kaolin structure in R-Clay was gradually destroyed? and the Fe2O3 structure became more prominent. Among them? Me-OH on the surface of red clay (R-Clay400? exists in the form of Al-Al-OH and Al-Si-OH? which efficiently degraded(86.36%? and mineralized TC(40%?6 h?. Under visible light irradiation? both oxygen atoms and TC molecules on R-Clay400 Si-O-Al can be used as electron donors to transfer photogenerated electrons(e-? to O2 adsorbed on the surface of R-Clay400 to form superoxide radical(center dot O2-? and singlet oxygen(1O2?? thus achieving efficient degradation of TC. Here? the surface Me-OH? used as the Bronsted site? adsorbs O2 by hydrogen bond? which promotes electron transfer rather than traditional electron donor. This study further clarified the activation mechanism of clay minerals to O2 and promoted the development of related research fields of mineral-based materials.
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关键词
Heat treatment,Red clay,Surface hydroxyl group,Molecular oxygen activation mechanism,Degradation
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