Ultrafast oxidation of refractory organics via PMS activation by Si-O doped biomimetic montmorillonite: Simultaneous enhanced radical/electron transfer pathways and efficient catalytic membrane system

IF 19.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-03-01 Epub Date: 2023-10-24 DOI:10.1016/j.apcatb.2023.123428

Jiasheng Mao , Kexin Yin , Yang Zhang , Yanan Shang , Qian Li , Yanwei Li , Baoyu Gao , Xing Xu

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引用次数: 0

Abstract

Carbon-based catalysts always rely on graphitized structure, heteroatomic doping, and defect sites as active sites, and still need to solve the problems of low catalytic activity and poor stability. In this work, a Si-O doped carbon-based catalyst with biomimetic montmorillonite (MT) structure (C/Si@MT) was prepared for oxidizing the refractory organic pollutants via peroxymonosulfate (PMS) activation. The C/Si@MT/PMS system exhibited ultrafast oxidation of versatile refractory organics and strong ability to resist interference from environmental matrixes via simultaneously enhancing both radicals and electron transfer process (ETP). The ETP oxidation of versatile pollutants in the C/Si@MT/PMS system were proceeded via the Si-O site as a bridge, with their k_obs data positively correlated to the redox parameters (e.g., falling potential, energy gap between C/Si@MT+PMS* and pollutants). In addition, the inert aluminosilicate was removed in C/Si@MT while retaining the lamellar structure for promoting the continuous oxidation of pollutants with high stability in a catalytic membrane.

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Si-O掺杂仿生蒙脱土PMS活化下难降解有机物的超快氧化:同时增强的自由基/电子转移途径和高效的催化膜系统

碳基催化剂一直依赖石墨化结构、杂原子掺杂、缺陷位点作为活性位点，仍然需要解决催化活性低、稳定性差的问题。本文制备了一种具有仿生蒙脱土(MT)结构的Si-O掺杂碳基催化剂(C/Si@MT)，通过过氧单硫酸盐(PMS)活化来氧化难降解的有机污染物。C/Si@MT/PMS体系通过同时增强自由基和电子转移过程(ETP)，表现出对多种难降解有机物的超快氧化和强抗环境基质干扰的能力。C/Si@MT/PMS系统中多种污染物的ETP氧化通过Si-O位点作为桥梁进行，其kobs数据与氧化还原参数(如下降电位，C/Si@MT+PMS*与污染物之间的能隙)呈正相关。此外，在C/Si@MT中去除了惰性硅酸铝，同时保留了层状结构，促进了污染物在催化膜中的连续氧化，具有较高的稳定性。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.