Boosted persulfate activation by hierarchically porous carbonaceous materials: Pivotal role of pore structure and electron-accepting capacity

被引：15

作者：

Tang, Xiaodan ^{[1
]}

Ma, Shuanglong ^{[1
]}

Xu, Shengjun ^{[2
]}

Pei, Chenhao ^{[1
]}

Dong, Tingting ^{[1
]}

Yang, Qiuyun ^{[3
]}

Huang, Yan ^{[1
]}

Wang, Jingzhen ^{[1
]}

Gao, Boqiang ^{[1
]}

Hua, Dangling ^{[1
]}

Dang, Bingjun ^{[4
]}

Zhan, Sihui ^{[5
]}

机构：

[1] Henan Agr Univ, Coll Resources & Environm Sci, Zhengzhou 450002, Peoples R China

[2] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, 18 Shuangqing Rd, Beijing 100085, Peoples R China

[3] Henan Agr Univ, Coll Agron, Zhengzhou 450002, Peoples R China

[4] Henan Agr Univ, Coll Tobacco Sci, Zhengzhou 450002, Peoples R China

[5] Nankai Univ, Coll Environm Sci & Engn, Key Lab Pollut Proc & Environm Criteria, Minist Educ, Tianjin 300071, Peoples R China

来源：

CHEMICAL ENGINEERING JOURNAL | 2023年 / 471卷

基金：

中国国家自然科学基金;

关键词：

Porous carbonaceous materials; Defect; Electron-accepting capacity; Reactive complexes; OXIDATION; DEGRADATION; POLLUTANTS; CATALYSTS;

D O I：

10.1016/j.cej.2023.144765

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

Porous carbonaceous materials (CMs) have been praised as superior candidates in activating persulfate for antibiotic wastewater decontamination. Whereas, as one of the frequently reported nonradical pathways, the formation mechanism of the reactive complexes and their correlation with physicochemical properties of CMs have not been comprehensively unveiled. Herein, a series of carbonaceous materials (CMs) with different specific surface area (SSA) and defect structures were fabricated by using KCl, MgCl2, KHCO3 and K2C2O4 as porogenic agents to activate peroxydisulfate (PDS) for sulfadiazine (SDZ) degradation. Results showed that the total pore volume of CMs exhibited a good linearity with degradation rate, attributing to the combined effect of SSA, defect degree and oxygen-containing functional groups according to multiple regression model. The reactive complexes (CM/PDS*) were proved as the foremost active species for SDZ oxidation via a suite of solid evidences. Compared with that after PS addition, the current direction was reversed after SDZ addition in i-t curves shedding light on the sharp enhanced potential of CM/PDS* and much low potential of SDZ. Furthermore, the inner-sphere CM/ PDS* originating from the formation of new covalent bonds between CMs and PDS was inferred due to the poor dependence between electron-donating capacity and SDZ degradation result. The CM/PDS* with considerably higher potential can extract electron from SDZ based on the excellent positive relationship between electronaccepting capacity of CMs and SDZ degradation effect. This study advances the mechanistic comprehension of nonradical PDS activation, and provides a multiple regression model to predict degradation effects of carbon materials.

引用

页数：11