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在过一硫酸盐激活中,具有空间受限 Co 物种的纳米反应器中 N 掺杂碳壳和空心结构的关键作用:阻碍金属浸出和增强催化稳定性。

Pivotal roles of N-doped carbon shell and hollow structure in nanoreactor with spatial confined Co species in peroxymonosulfate activation: Obstructing metal leaching and enhancing catalytic stability.

机构信息

State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China; Yibin Institute of Industrial Technology, Sichuan University, Yibin, China.

State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Water Safety and Water Pollution Control Engineering Technology Research Center in Sichuan Province, Haitian Water Group, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China; Yibin Institute of Industrial Technology, Sichuan University, Yibin, China.

出版信息

J Hazard Mater. 2022 Apr 5;427:128204. doi: 10.1016/j.jhazmat.2021.128204. Epub 2022 Jan 4.

Abstract

Metal leaching and catalytic stability are the key issues in Fenton-like reaction. Herein, a hollow yolk-shell nanoreactor (HYSCN) with shell confined Co species was fabricated for peroxymonosulfate (PMS) activation to degrade carbamazepine (CBZ). The uniform Co nanoparticles were completely anchored in a hollow void, further confined by a porous N-doped carbon shell. The unique construction significantly reduces Co species leaching in PMS activation and enhances catalytic stability. Co leaching came from HYSCN dropped by almost fourfold compared to CN-8 without shell confined (0.403 mg/L to 0.120 mg/L). The catalytic stability is also greatly improved, confirming the dominant role of heterogeneous catalysis in the HYSCN/PMS system. HYSCN exhibits excellent catalytic performance compared to a solid structure (SCSCN), demonstrating the significance of hollow structures. Mechanism study found that HO, SO and O induced in HYSCN/PMS system and the relative contributions were distinguished and quantified by stoichiometric methods. The UPLC-Q-TOF-MS/MS was used to identify the CBZ degraded intermediate products and the possible degradation pathway was proposed. This study will provide theoretical guidance for reducing metal leaching and improving catalytic stability in the PMS activation.

摘要

金属浸出和催化稳定性是类芬顿反应中的关键问题。本文制备了一种具有壳层限域 Co 物种的中空蛋黄壳纳米反应器 (HYSCN),用于过一硫酸盐 (PMS) 活化以降解卡马西平 (CBZ)。均匀的 Co 纳米颗粒完全锚定在中空空隙中,进一步被多孔氮掺杂碳壳限制。独特的结构显著减少了 PMS 活化过程中 Co 物种的浸出,并提高了催化稳定性。与没有壳层限域的 CN-8 相比,HYSCN 中 Co 的浸出量减少了近四倍(从 0.403mg/L 降至 0.120mg/L)。催化稳定性也得到了极大的提高,这证实了非均相催化在 HYSCN/PMS 体系中的主导作用。与固体结构 (SCSCN) 相比,HYSCN 表现出优异的催化性能,证明了中空结构的重要性。通过化学计量法研究发现,在 HYSCN/PMS 体系中诱导生成了 HO、SO 和 O,并且区分和量化了它们的相对贡献。使用 UPLC-Q-TOF-MS/MS 鉴定了 CBZ 降解的中间产物,并提出了可能的降解途径。本研究将为减少 PMS 活化过程中的金属浸出和提高催化稳定性提供理论指导。

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