Waste Eggshell-derived N, P, S Tri-doped Core-shell Catalysts for Efficient Fenton-like Catalysis

Waste Eggshell-derived N, P, S Tri-doped Core-shell Catalysts for Efficient Fenton-like Catalysis
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废蛋壳衍生的 N、P、S 三掺杂核壳催化剂用于高效类芬顿催化

DOI:
10.1016/j.cej.2022.135879
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发表时间:
2022-03
影响因子:
15.1
通讯作者:
Dihua Wang
Dihua Wang
中科院分区:
工程技术1区
文献类型:
--
作者:
Yongsong Ma;Xianglin Liu;Mengyi Tang;Kaifa Du;Huayi Yin;Xuhui Mao;Dihua Wang

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杂原子掺杂碳材料已被证明是一种有效的催化剂,用于有机污染物的修复。采用熔盐电解法(MSE)将废蛋壳和Co 3 O 4转化为N,P,S三掺杂核壳催化剂(Co@NPSC),实现废蛋壳的高附加值转化。令人印象深刻的是,Co@NPSC/过氧单硫酸盐(PMS)系统在0.001 g L-1的低催化剂剂量下,对磺胺甲恶唑(SMX)的降解表现出83.86 min-1的超高转换频率(TOF)值。随后,密度泛函理论(DFT)模拟阐明了催化氧化的协同本质(即,Co@NPSC催化剂降低了PMS分子在其表面的吸附能,降低了PMS分子本身的功函数,增加了PMS分子的O O键长度,有利于PMS活化的电子转移。此外,理论预测和急性毒性试验结果表明,SMX的降解相当于解毒。本工作为废蛋壳的再利用和杂原子掺杂核壳催化剂的设计提供了新的思路。
Heteroatom-doped carbon materials have been proved as potent catalysts for the remediation of organic contaminants. Herein, molten salt electrolysis (MSE) was employed to convert waste eggshell and Co3O4into N, P, S tri-doped core–shell catalyst (Co@NPSC), achieving the conversion of waste eggshell into value-added materials. Impressively, Co@NPSC/peroxymonosulfate (PMS) system exhibited an exceptional ultra-high turnover frequency (TOF) value of 83.86 min−1for sulfamethoxazole (SMX) degradation with a low catalyst dosage of 0.001 g L–1. Subsequently, density functional theory (DFT) simulation clarified the synergistic essences of catalytic oxidation (i.e., the Co@NPSC catalyst reduced the adsorption energy of PMS molecular on its surface, reduced itself work function, enhanced the length of the O-O bond (IO-O) of PMS molecule, and facilitated electron transfer for PMS activation). In addition, both theoretical predictions and acute toxicity assay results indicated that the degradation of SMX equals detoxification. This work provides a new insight into the reutilization of waste eggshell and the design of heteroatom-doped core–shell catalysts.
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