Transforming CO2 into Sulfur-Doped Carbon As a High-Efficiency Persulfate Catalyst for the Degradation of 2,4-Dichlorphenol: Influential Factors, Activation Mechanism, and Regeneration of Catalyst,ACS ES&T Water

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Transforming CO2 into Sulfur-Doped Carbon As a High-Efficiency Persulfate Catalyst for the Degradation of 2,4-Dichlorphenol: Influential Factors, Activation Mechanism, and Regeneration of Catalyst
ACS ES&T Water ( IF 4.8 ) Pub Date : 2021-07-21 , DOI: 10.1021/acsestwater.1c00112
Yongsong Ma ₁ , Yuxing Gu ₁ , Da Jiang ₁ , Xuhui Mao ₁ , Dihua Wang _{1,

2}

Affiliation

The burning of fossil fuels leads to the emission of large amounts of CO₂ into the air, and how to deal with the increasingly generated CO₂ has been a great challenge. In an effort to convert the low-value CO₂ into valuable material, this work proposed sulfur-doped CO₂ converted carbon (S-EC) by molten salt carbon capture electrochemical transformation (MSCC-ET) as a persulfate (PS) activator for 2,4-dichlorophenol (2,4-DCP) removal. The catalytic performance of CO₂ converted carbon (EC) was dramatically enhanced by sulfur modification. The most efficient dosage of S-EC was 50 mg L^–1; the most efficient dosage of PS was 5:1 M for PS/2,4-DCP, and the efficient pH range was 3.0–9.0. The results of radical quenching experiments and electron paramagnetic resonance spectroscopy further confirmed the novel nonradical process in a S-EC/PS system. Furthermore, the novel nonradical activation mechanism of S-EC on PS was further identified on the basis of the results of density functional theory (DFT) calculations and polarization curves. In addition, the degradation intermediates such as 4-chlorophenol, 2-chlorophenol, 2-chlorohydroquinone, and some carboxylic acids were identified by gas chromatography–mass spectrometry (GC–MS), and the possible degradation pathways were summarized. Remarkably, the molten salt redox-sulfidation method can completely restore the catalytic performance of used S-EC for PS. This work extends the application of EC materials for environmental remediation.

中文翻译：

将 CO2 转化为掺硫碳作为高效过硫酸盐催化剂降解 2,4-二氯苯酚：影响因素、活化机制和催化剂再生

化石燃料的燃烧导致大量CO ₂排放到空气中，如何处理日益增多的CO ₂成为一个巨大的挑战。为了将低价值的 CO ₂转化为有价值的材料，这项工作提出了通过熔盐碳捕获电化学转化 (MSCC-ET) 作为过硫酸盐 (PS) 活化剂的硫掺杂 CO ₂转化碳 (S-EC) 2,4-二氯苯酚（2,4-DCP）去除。CO ₂转化碳（EC）的催化性能通过硫改性显着提高。S-EC 的最有效剂量为 50 mg L ^–1; 对于 PS/2,4-DCP，PS 的最有效剂量为 5:1 M，有效 pH 范围为 3.0-9.0。自由基猝灭实验和电子顺磁共振光谱的结果进一步证实了 S-EC/PS 系统中的新型非自由基过程。此外，基于密度泛函理论（DFT）计算和极化曲线的结果，进一步确定了 S-EC 对 PS 的新型非自由基激活机制。此外，4-氯苯酚、2-氯苯酚、2-氯氢醌和一些羧酸等降解中间体通过气相色谱-质谱联用（GC-MS）进行了鉴定，并总结了可能的降解途径。值得注意的是，熔盐氧化还原硫化法可以完全恢复使用过的S-EC对PS的催化性能。

更新日期：2021-08-13

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