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Non-radical oxidation by N,S,P co-doped biochar for persulfate activation: Different roles of exogenous P/S doping, and electron transfer path
Journal of Cleaner Production ( IF 9.7 ) Pub Date : 2022-09-07 , DOI: 10.1016/j.jclepro.2022.133995
Jiangfang Yu , Lin Tang , Ya Pang , Yaoyu Zhou , Haopeng Feng , Xiaoya Ren , Jing Tang , Jiajia Wang , Lifei Deng , Binbin Shao

Despite many studies on single doping (especially N, S) to improve the catalytic performance of biochar in persulfate-based oxidation process (PS-AOP), the investigations of co-doping with multiple heteroatoms for biochar are relatively few. Herein, choosing shrimp shell biochar (NSC-bio, natural N,S co-doped) as research object with exogenous P/S doping, N,S co-doped and N,S,P co-doped biochars were prepared and applied in PS-AOP, respectively. Exogenous S doping (NSC–S-bio) showed a negative effect with the decreased removal efficiency from 88.7% to 45.7%. Quantitative structure-activity relationships analysis showed that, the decreased kobs (0.0692–0.0171 min−1) of NSC-S-bio was linearly related to the decreased Qe (229.0–158.7 mg/g), where the increased electrostatic repulsion during the key catalytic zone by S doping was the key factor. As for NSC-P-bio, a positive effect could be observed (98.9% removal). The increased kobs (0.0692–0.1299 min−1) showed high linear fitting toward P content and specific surface area (449.4–971.6 m2/g) but low fitting degree toward Qe. Further electrochemical characterization revealed that, the increased surface catalytic sites and enhanced electronic conductivity endowed NSC-P-bio improved catalytic performance, which achieved rapid activation of PDS via non-radical electron transfer path and showed selectively toward substrate with electron-donating groups. This study provides new insight for the construction of efficient co-doped biochar catalysts in PS-AOP.



中文翻译:

N,S,P共掺杂生物炭的非自由基氧化活化过硫酸盐:外源P/S掺杂的不同作用,以及电子转移路径

尽管对单一掺杂(尤其是 N、S)以提高生物炭在过硫酸盐氧化过程(PS-AOP)中的催化性能进行了许多研究,但对生物炭的多个杂原子共掺杂的研究相对较少。在此,选择虾壳生物炭(NSC-bio,天然N,S共掺杂)作为研究对象,外源P/S掺杂,制备了N,S共掺杂和N,S,P共掺杂生物炭并应用于PS-AOP,分别。外源 S 掺杂 (NSC-S-bio) 显示出负面影响,去除效率从 88.7% 降低到 45.7%。定量构效关系分析表明,NSC-S-bio的k obs (0.0692-0.0171 min -1 )降低与Qe降低呈线性相关。(229.0-158.7 mg/g),其中 S 掺杂在关键催化区增加的静电排斥是关键因素。至于 NSC-P-bio,可以观察到积极的效果(去除 98.9%)。增加的k obs (0.0692–0.1299 min -1 ) 显示出对 P 含量和比表面积 (449.4–971.6 m 2 /g) 的高线性拟合,但对Qe的拟合度低. 进一步的电化学表征表明,增加的表面催化位点和增强的电子电导率赋予 NSC-P-bio 更好的催化性能,通过非自由基电子转移路径实现 PDS 的快速活化,并显示出对具有给电子基团的底物的选择性。该研究为在 PS-AOP 中构建高效的共掺杂生物炭催化剂提供了新的思路。

更新日期:2022-09-07
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