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二硫化钼共催化增强基于纳米零价铁的类芬顿反应过程:性能与机制。

Molybdenum disulfide co-catalysis boosting nanoscale zero-valent iron based Fenton-like process: Performance and mechanism.

机构信息

College of Environmental Science and Engineering, Central South University of Forestry and Technology, Changsha, 410004, China.

College of Environmental Science and Engineering, Central South University of Forestry and Technology, Changsha, 410004, China.

出版信息

Environ Res. 2023 Jun 15;227:115752. doi: 10.1016/j.envres.2023.115752. Epub 2023 Mar 24.

Abstract

The conventional Fenton process has the drawbacks of low efficiency of Fe/Fe conversion, low utilization of HO, and narrow range of pH. In this paper, molybdenum sulfide (MoS) was used as a co-catalyst to boost the nanoscale zero-valent iron (nZVI) based heterogeneous Fenton-like process for the degradation of Rhodamine B (RhB). The catalytic performance, influences of parameters, degradation mechanism, and toxicity of intermediates were explored. Compared with the conventional like-Fenton process, the existence of MoS accelerated the decomposition of HO and the RhB degradation rate constant of MoS/nZVI/HO reached more than six times that of nZVI/HO. In addition, the effective pH range of MoS/nZVI/HO was broadened to 9.0 with 84.9% of RhB being removed within 15 min. The co-catalytic system of MoS and nZVI was stable and had high reusability according to the results of four consecutive runs. Quenching tests and electron paramagnetic resonance (EPR) demonstrated that hydroxyl radical (·OH), superoxide anions (·O), and singlet oxygen (O) were all involved in MoS/nZVI/HO. Compared with nZVI/HO system, MoS not only increased the corrosion of nZVI but also accelerated the conversion of Fe/Fe. ECOSAR analysis suggested that the overall acute and chronic toxicity of the degradation products decreased after treatment. Hence, this MoS co-catalytic nZVI based Fenton-like process can be used as a promising alternative for the treatment of organic wastewater.

摘要

传统的芬顿工艺存在 Fe/Fe 转化率低、HO 利用率低、pH 范围窄等缺点。本文采用硫化钼(MoS)作为共催化剂,以提高基于纳米零价铁(nZVI)的类芬顿非均相反应体系对罗丹明 B(RhB)的降解性能。探讨了催化剂的催化性能、影响因素、降解机制和中间产物的毒性。与传统的类芬顿工艺相比,MoS 的存在加速了 HO 的分解,MoS/nZVI/HO 的 RhB 降解速率常数是 nZVI/HO 的 6 倍以上。此外,MoS/nZVI/HO 的有效 pH 范围拓宽至 9.0,15 min 内 RhB 的去除率达到 84.9%。根据连续 4 次运行的结果,MoS 和 nZVI 的共催化体系稳定且具有较高的可重复使用性。猝灭实验和电子顺磁共振(EPR)表明,羟基自由基(·OH)、超氧阴离子自由基(·O)和单线态氧(O)均参与了 MoS/nZVI/HO 反应。与 nZVI/HO 体系相比,MoS 不仅加速了 nZVI 的腐蚀,还促进了 Fe/Fe 的转化。ECOSAR 分析表明,处理后降解产物的整体急性和慢性毒性降低。因此,这种 MoS 共催化 nZVI 基类芬顿反应可以作为处理有机废水的一种有前途的替代方法。

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