Mn-Co dual sites relay activation of peroxymonosulfate for accelerated decontamination

IF 21.1 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-08-05 DOI:10.1016/j.apcatb.2023.122656

Yiyuan Yao , Chaohai Wang , Yingpeng Yang, Shuai Zhang, Xin Yan, Chengming Xiao, Yujun Zhou, Zhigao Zhu, Junwen Qi, Xiuyun Sun, Jiansheng Li

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引用次数: 15

Abstract

Dual atomic catalysts are specially designed for relay activation of peroxymonosulfate (PMS). Here, a programmable metal-triazolate framework is utilized as a precursor to introduce the bimetallic sites (containing Mn and Co) for the synthesis of contiguous Mn−N and Co−N sites anchored on nitrogen-doped porous carbon polyhedral (MCNC). Excellent decontamination performance with TOF/PMS = 46.3 L² min⁻¹ g⁻² is observed on the MCNC, which is 1.6 and 1.5 times of single Mn and single Co catalysts. Singlet oxygen quantifying, ¹⁸O isotope labeling, and theoretical simulations jointly unravel that MCNC activates PMS through a unique “relay” mode, where one site interacts with the O atom in PMS, and the other expedites producing ¹O₂ via PMS* activation. This work advances the origin activation of PMS and enhances the removal for the refractory pollutants by rational regulation of dual site synergistic catalyst, which deepens the on-demand design of Fenton-like reaction.

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锰钴双位点中继活化的过氧单硫酸盐加速去污

双原子催化剂是专为过氧单硫酸盐(PMS)的继电活化而设计的。本文利用可编程金属-三氮酸盐框架作为前驱体，引入双金属位点(含Mn和Co)，用于合成锚定在氮掺杂多孔碳多面体(MCNC)上的连续Mn - N和Co - N位点。MCNC的TOF/PMS = 46.3 L2 min−1 g−2，是单一Mn和单一Co催化剂的1.6倍和1.5倍。单重态氧定量、18O同位素标记和理论模拟共同揭示了MCNC通过一种独特的“中继”模式激活PMS，其中一个位点与PMS中的O原子相互作用，另一个位点通过PMS*激活加速产生1O2。本工作通过合理调控双位点协同催化剂，推进了PMS的原点活化，提高了对难降解污染物的去除，深化了类芬顿反应的按需设计。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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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.