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可见光下通过加速电子转移增强 CuFeO/生物炭催化剂上四环素的非均相类 Fenton 光降解。

Enhanced heterogeneous photo-Fenton-like degradation of tetracycline over CuFeO/biochar catalyst through accelerating electron transfer under visible light.

机构信息

Key Lab of Marine Environment and Ecology, Ministry of Education, Ocean University of China, Qingdao, 266100, China; Qingdao Engineering Research Center for Rural Environment, College of Resources and Environment, Qingdao Agricultural University, Qingdao, 266109, China.

Key Lab of Marine Environment and Ecology, Ministry of Education, Ocean University of China, Qingdao, 266100, China.

出版信息

J Environ Manage. 2021 May 1;285:112093. doi: 10.1016/j.jenvman.2021.112093. Epub 2021 Feb 16.

Abstract

The visible-light induced heterogeneous photo-Fenton-like (HPF-like) process is regarded as a promising technique for organic pollutants degradation due to its efficient utilization of solar energy and high HO activation activity. This study prepared the CuFeO/biochar catalysts via hydrothermal technique at no extra reductant and systematically investigated their band structure and photoelectric properties. The dispersed distribution of CuFeO particles in CuFeO/biochar composites narrowed bandgap of CuFeO and promoted electron transport of CuFeO. Compared with CuFeO, the CuFeO/biochar containing 1.0 g biochar in the preparation (CuFeO/biochar-1.0) possessed higher carrier density and longer photoelectron lifetime, which is beneficial to higher catalytic performance. The apparent rate constant for tetracycline as target pollutant degradation by CuFeO/biochar-1.0 was 2.0 times higher than that by CuFeO. The acquired optimum conditions for tetracycline degradation were 220 mg L CuFeO/BC-1.0, 22 mM HO and pH 6.4 using response surface methodology. The quenching experiments and ESR analysis revealed that OH was the predominant active species, and photoelectron and O were auxiliary species. The photoelectron could promote in-situ recycling of Cu to Cu and Fe to Fe, which significantly improved HO activation by CuFeO. The possible pathway of tetracycline was proposed according to intermediates identified by HPLC/MS. The toxicity analysis demonstrated that the overall toxicity of the identified intermediates was reduced in HPF-like system.

摘要

可见光诱导非均相类芬顿(HPF-like)过程因其能有效利用太阳能和高 HO 激活活性而被认为是一种有前途的有机污染物降解技术。本研究通过水热技术制备了 CuFeO/生物炭催化剂,无需额外的还原剂,并系统地研究了它们的能带结构和光电性能。CuFeO 颗粒在 CuFeO/生物炭复合材料中的分散分布缩小了 CuFeO 的带隙,促进了 CuFeO 的电子输运。与 CuFeO 相比,在制备过程中含有 1.0 g 生物炭的 CuFeO/生物炭复合材料(CuFeO/生物炭-1.0)具有更高的载流子密度和更长的光电子寿命,这有利于更高的催化性能。以四环素为目标污染物,CuFeO/生物炭-1.0 的表观降解速率常数是 CuFeO 的 2.0 倍。使用响应面法获得的四环素降解最佳条件为 220 mg·L CuFeO/BC-1.0、22 mM HO 和 pH 6.4。猝灭实验和 ESR 分析表明,OH 是主要的活性物质,光电子和 O 是辅助物质。光电子可以促进 Cu 的原位循环再生为 Cu 和 Fe 的原位循环再生,从而显著提高了 CuFeO 对 HO 的激活。根据高效液相色谱/质谱法鉴定的中间产物提出了四环素的可能降解途径。毒性分析表明,在 HPF-like 体系中,鉴定出的中间产物的整体毒性降低。

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