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工程化沼渣衍生生物炭介导过一硫酸盐活化用于可持续废水修复中去除土霉素。

Engineered digestate-derived biochar mediated peroxymonosulfate activation for oxytetracycline removal in sustainable wastewater remediation.

机构信息

Department of Biology, Hong Kong Baptist University, Hong Kong, China.

State Key Laboratory of Environmental and Biological Analysis, Hong Kong Baptist University, Hong Kong, China.

出版信息

Environ Pollut. 2024 Nov 1;360:124640. doi: 10.1016/j.envpol.2024.124640. Epub 2024 Jul 30.

Abstract

Nowadays, biochar is extensively used in wastewater remediation with the aim of achieving water security and circularity with minimal impacts on ecosystems and the environment. In this study, digestate biochar was prepared and modified using different methods and then employed as a peroxymonosulfate (PMS) activator to oxidize oxytetracycline, a model antibiotic pollutant in wastewater. The optimal biochar catalyst was characterized, spin trapping tests were carried out to confirm the dominant catalytic mechanism, and in silico toxicity prediction was conducted based on structure-activity relationships. Assessment of the catalytic performance of the pristine and engineered biochar showed that nitrogen doping increased oxytetracycline degradation efficiency by 1.92-fold (i.e., 100% oxytetracycline degradation with the engineered biochar compared to 52% with pristine biochar), while pyrrolic nitrogen was identified as a major PMS activation site. It was discovered that several parameters, such as catalyst dose, pH, PMS concentration, and competing ions, affected oxytetracycline degradation efficiencies. Additionally, the toxicity of the degradation intermediate was studied. Scavenger trapping tests showed that O and SO• were the most prevalent species during oxytetracycline degradation in the system, with four possible degradation pathways proposed, including secondary alcohol oxidation, hydroxylation, dehydration, and deamidation. Overall, it is anticipated that this study would contribute to our understanding of metal-free biochar activation of PMS as an attractive treatment scheme for antibiotic-polluted water.

摘要

如今,生物炭被广泛应用于废水修复中,旨在实现水安全和循环利用,同时对生态系统和环境的影响最小。在这项研究中,使用不同的方法制备和修饰了消化生物炭,然后将其用作过一硫酸盐 (PMS) 的激活剂来氧化废水模型抗生素污染物土霉素。对最佳生物炭催化剂进行了表征,通过自旋捕获试验证实了主要的催化机制,并基于构效关系进行了计算机毒性预测。对原始和工程生物炭的催化性能评估表明,氮掺杂将土霉素的降解效率提高了 1.92 倍(即工程生物炭的土霉素降解率为 100%,而原始生物炭的降解率为 52%),而吡咯氮被确定为主要的 PMS 活化位点。研究发现,催化剂剂量、pH 值、PMS 浓度和竞争离子等几个参数影响土霉素的降解效率。此外,还研究了降解中间产物的毒性。清除剂捕获试验表明,在该体系中土霉素降解过程中,O 和 SO•是最常见的物种,提出了四条可能的降解途径,包括仲醇氧化、羟化、脱水和脱酰胺。总的来说,预计这项研究将有助于我们理解无金属生物炭激活过一硫酸盐作为一种有吸引力的抗生素污染水处理方案。

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