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Origin of the Enhanced Reusability and Electron Transfer of the Carbon-Coated Mn3O4 Nanocube for Persulfate Activation
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-12-03 , DOI: 10.1021/acscatal.0c04049 Yani Liu 1, 2 , Jun Luo 1, 2 , Lin Tang 1, 2 , Chengyang Feng 1, 2 , Jiajia Wang 1, 2 , Yaocheng Deng 3 , Haoyu Liu 1 , Jiangfang Yu 1 , Haopeng Feng 1 , Jingjing Wang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-12-03 , DOI: 10.1021/acscatal.0c04049 Yani Liu 1, 2 , Jun Luo 1, 2 , Lin Tang 1, 2 , Chengyang Feng 1, 2 , Jiajia Wang 1, 2 , Yaocheng Deng 3 , Haoyu Liu 1 , Jiangfang Yu 1 , Haopeng Feng 1 , Jingjing Wang 1
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Manganese oxides and carbon materials are both desirable catalysts for persulfate (PS) advanced oxidation processes in environmental remediation. Nevertheless, manganese oxides suffer from low reusability while carbon materials face the problem of limited catalytic efficiency. For the purpose of making full use of the advantages of the two materials as well as avoiding their shortcomings, carbon-coated Mn3O4 composites (Mn3O4/C) with a regular nanocube structure were designed to activate PS for the removal of organics, and the catalytic processes were deeply investigated. The catalyst prepared at 400 °C with a precursor ratio (glucose/KMnO4) of 0.5 exhibited the best catalytic performance along with satisfactory reusability owing to the protection of the outer carbon layer. According to experimental results and density functional theory calculation, there were van der Waals interaction and a part of the strong attraction between the interface of PS and Mn3O4/C, which could be enhanced by inner Mn3O4 and thus promoted the electron transfer between PS and carbon shell, and the defective edges of the carbon layer with hydroxyl (C–OH) groups could act as active sites for PS activation. Radical (SO4•–, •OH) and nonradical (1O2) oxidation processes both participated in the degradation of 2,4-dichlorophenol, in which •OH was dominating. This study not only proposed a promising catalyst for the degradation of pollutants but also expanded research ideas for future PS activation mechanism studies by integrating the experiment and simulation.
中文翻译：
碳包覆的Mn 3 O 4纳米立方体过硫酸盐活化作用增强的可重用性和电子转移的起源
锰氧化物和碳材料都是环境修复中过硫酸盐（PS）先进氧化工艺的理想催化剂。然而，锰氧化物的可重复使用性低，而碳材料面临催化效率有限的问题。为了充分利用两种材料的优点并避免它们的缺点，设计了具有规则纳米立方体结构的碳包覆Mn 3 O 4复合材料（Mn 3 O 4 / C）来活化PS以去除对有机物的催化过程进行了深入研究。在400°C下以前体比（葡萄糖/ KMnO 4由于保护了外部碳层，0.5的α）表现出最佳的催化性能以及令人满意的可重复使用性。根据实验结果和密度泛函理论计算，PS和Mn 3 O 4 / C的界面之间存在范德华相互作用和部分强吸引力，这可以通过内部Mn 3 O 4增强，从而促进。 PS和碳壳之间的电子转移以及带有羟基（C-OH）的碳层的缺陷边缘可能充当PS活化的活性位点。自由基（SO 4 •–，• OH）和非自由基（1 O 2）氧化过程均参与了2，4-二氯苯酚的降解，其中• OH为主导。这项研究不仅为污染物的降解提出了有希望的催化剂，而且通过结合实验和模拟，为今后的PS活化机理研究扩展了研究思路。
更新日期：2020-12-18
中文翻译：
碳包覆的Mn 3 O 4纳米立方体过硫酸盐活化作用增强的可重用性和电子转移的起源
锰氧化物和碳材料都是环境修复中过硫酸盐（PS）先进氧化工艺的理想催化剂。然而，锰氧化物的可重复使用性低，而碳材料面临催化效率有限的问题。为了充分利用两种材料的优点并避免它们的缺点，设计了具有规则纳米立方体结构的碳包覆Mn 3 O 4复合材料（Mn 3 O 4 / C）来活化PS以去除对有机物的催化过程进行了深入研究。在400°C下以前体比（葡萄糖/ KMnO 4由于保护了外部碳层，0.5的α）表现出最佳的催化性能以及令人满意的可重复使用性。根据实验结果和密度泛函理论计算，PS和Mn 3 O 4 / C的界面之间存在范德华相互作用和部分强吸引力，这可以通过内部Mn 3 O 4增强，从而促进。 PS和碳壳之间的电子转移以及带有羟基（C-OH）的碳层的缺陷边缘可能充当PS活化的活性位点。自由基（SO 4 •–，• OH）和非自由基（1 O 2）氧化过程均参与了2，4-二氯苯酚的降解，其中• OH为主导。这项研究不仅为污染物的降解提出了有希望的催化剂，而且通过结合实验和模拟，为今后的PS活化机理研究扩展了研究思路。
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