成果归属作者：

姚俊

成果归属机构：

水资源与环境学院

作者：

Chen, Zhihui ; Yao, Jun ; Knudsen, Tatjana Solevic ; Li, Hao ; Liu, Bang ; Ma, Bo ; Pang, Wancheng

单位：

Hunan Inst Technol, Sch Chem & Environm Engn, Res Ctr Environm Pollut Control Technol, 18 Henghua Rd, Hengyang 421002, Peoples R China;China Univ Geosci Beijing, Res Ctr Environm Sci & Engn, Sch Water Resources & Environm, 29 Xueyuan Rd, Beijing 100083, Peoples R China;Univ Belgrade, Dept Chem, Inst Chem Technol & Met, Njegoseva 12, Belgrade 11000, Serbia

关键词：

DEGRADATION; NANOPARTICLES; TOXICITY; WATER; TRANSFORMATION; CONTAMINANTS

摘要：

Residual organic flotation reagents in mineral processing wastewater (MPW) can pose environmental hazards and hinder the sustainable development of the mining industry. Laccase as a versatile biocatalyst can eliminate various recalcitrant contaminants from the environment, but its potential applications for the removal and detoxification of organic flotation reagents have until now been overlooked. Herein, the influence of super- paramagnetic immobilized laccase (SPM-IMLac) on the enzymatic removal of salicylhydroxamic acid (SHA), a typical mineral flotation reagent, as well as the mechanism of this process have been explored for the first time. The results indicated that SPM-IMLac can effectively remove SHA over a broad pH range and this process follows the pseudo-first-order reaction kinetics. A methodology which combined high resolution mass spectrometry (HRMS) and a solid phase extraction (SPE) technique revealed that SPM-IMLac could catalyze a single-electron oxidation of SHA to generate self/cross-oligomers via radical-driven C-C and/or C-O-C covalent coupling pathways. The Vibrio fischeri bioluminescence inhibition assay and a total organic carbon (TOC) analysis corroborated that the SHA transformation was accompanied by detoxification and by a reduction in TOC of the reaction solution, the extent of which correlated with the extent of the oxidative coupling. Moreover, SPM-IMLac could be easily recovered and reused, while keeping its high removal efficiency of SHA in the actual MPW matrices. This study not only provides fascinating insights into the transformation mechanisms and environmental fate of SHA mediated by SPM-IMLac, but it also exploits a viable and sustainable approach for the remediation of organic flotation reagents-contaminated MPW.

基金：

National Natural Science Foundation of China [42230716]; Major National R & D Projects for Chinese Ministry of Science and Technology [2023YFC3707600]; Project 111 [B21017]; Ministry of Science, Technological Development and Innovation of the Republic of Serbia [451-03-66/2024-03/200026]; International Joint Scientific and Technical Collaboration between the People's Republic of China [4-18]

语种：

英文

DOI：

10.1016/j.cej.2024.157012

来源：

CHEMICAL ENGINEERING JOURNAL,2024():.

出版日期：

2024-11-15

提交日期：

2024-11-19

引用参考：

Chen, Zhihui; Yao, Jun; Knudsen, Tatjana Solevic; Li, Hao; Liu, Bang; Ma, Bo; Pang, Wancheng. Application of a laccase-catalyzed oxidative coupling for the removal and detoxification of typical flotation reagent salicylhydroxamic acid[J]. CHEMICAL ENGINEERING JOURNAL,2024():.