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Ce 掺杂 BiMoO 中形成的受阻路易斯对:一种促进 HO 高效利用用于类 Fenton 光降解的通用策略。

Frustrated Lewis pairs created by Ce-doped BiMoO: A universal strategy to promote efficient utilization of HO for Fenton-like photodegradation.

机构信息

Key Laboratory of Crop Physiology, Ecology and Genetic Breeding, Ministry of Education, Key Laboratory of Chemical Utilization of Plant Resources of Nanchang, College of Chemistry and Materials, Jiangxi Agricultural University, Nanchang, 330045, PR China.

Key Laboratory of Crop Physiology, Ecology and Genetic Breeding, Ministry of Education, Key Laboratory of Chemical Utilization of Plant Resources of Nanchang, College of Chemistry and Materials, Jiangxi Agricultural University, Nanchang, 330045, PR China.

出版信息

Chemosphere. 2024 May;356:141952. doi: 10.1016/j.chemosphere.2024.141952. Epub 2024 Apr 8.

Abstract

Photo-Fenton-like technology based on HO is considered as an ideal strategy to generate reactive oxygen species (ROS) for antibiotic degradation, but O overflow in the process severely limits the utilization efficiency of HO. Herein, we fabricate BiMoO (BMO) photocatalyst modified with Frustrated Lewis pairs (FLPs) as a Fenton catalyst model for enhancing reuse of spilled O. The FLPs created by the introduction of cerium and oxygen vacancy were found to contribute to regulate the electronic structure of BMO and further improve the acidic and basic properties of photocatalyst surface. More importantly, the frustrated acid and base sites can enhance the HO and O interfacial adsorption process and provide an Ce-O-O active site on the surface of Ce-BMO nanosheets, which can promote O/•O/O/HO redox cycles to achieve high HO utilization efficiency. Specifically, in the experiment using tetracycline as a photocatalytic degradation object, the degradation activity of Ce-BMO was 2.15 times higher than that of BMO pure phase. Quenching experiments and EPR assays also confirmed that O and •O were the dominant oxidative species. This study systematically reveals the design of Fenton photocatalytic active sites at the atomic scale and provides new insights into constructing FLPs photocatalysts with high HO utilization efficiency.

摘要

基于 HO 的光芬顿技术被认为是生成用于抗生素降解的活性氧 (ROS) 的理想策略,但该过程中 O 的溢出严重限制了 HO 的利用效率。在此,我们制备了负载受阻路易斯对 (FLPs) 的 BiMoO (BMO) 光催化剂作为 Fenton 催化剂模型,以提高溢出 O 的再利用效率。研究发现,通过引入铈和氧空位形成的 FLPs 有助于调节 BMO 的电子结构,并进一步改善光催化剂表面的酸碱性。更重要的是,受阻酸和碱位可以增强 HO 和 O 的界面吸附过程,并在 Ce-BMO 纳米片表面提供 Ce-O-O 活性位,从而促进 O/•O/O/HO 氧化还原循环,实现高 HO 利用效率。具体来说,在以四环素作为光催化降解对象的实验中,Ce-BMO 的降解活性比纯相 BMO 高 2.15 倍。猝灭实验和 EPR 分析也证实了 O 和 •O 是主要的氧化物种。本研究系统地揭示了原子尺度上 Fenton 光催化活性位的设计,并为构建具有高 HO 利用效率的 FLPs 光催化剂提供了新的思路。

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