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Experimental and DFT investigation on N-functionalized biochars for enhanced removal of Cr(VI)
Zhao, Nan; Zhao, Chuanfang; Liu, Kunyuan; Zhang, Weihua; Tsang, Daniel C. W.; Yang, Zaikuan; Yang, Xixiang; Yan, Bofang; Morel, Jean Louis; Qiu, Rongliang
AbstractPorous carbons are appealing low-cost and metal-free catalysts in persulfate-based advanced oxidation processes. In this study, a family of porous biochar catalysts (ZnBC) with different porous structures and surface functionalities are synthesized using a chemical activation agent (ZnCl2). The functional biochars are used to activate persulfate for sulfamethoxazole (SMX) degradation. ZnBC-3 with the highest content of ketonic group (C=O, 1.25 at%) exhibits the best oxidation efficiency, attaining a rate constant (k(obs)) of 0.025 min(-1). The correlation coefficient of the density of C=O to k(obs) (R-2 = 0.992) is much higher than the linearity of the organic adsorption capacity to k(obs) (R-2 = 0.694), implying that C=O is the intrinsic active site for persulfate activation. Moreover, the volume of mesopore (R-2 = 0.987), and Zeta potential (R-2 = 0.976) are also positive factors in PS adsorption and catalysis. In the mechanistic study, we identified that singlet oxygen is the primary reactive oxygen species. It can attack the -NH2 group aligned to the benzene ring to form dimer products which could be adsorbed on the biochar surface to reach complete removal of the SMX. The optimal pH range is 4-6 which will minimize the electrostatic repulsion between ZnBCs and the reactants. The SMX degradation in ZnBC/PS system was immune to inorganic anions but would compete with organic impurities in the real wastewater. Finally, the biochar catalysts are filled in hydrogel beads and packed in a flow-through packed-bed column. The continuous system yields a high removal efficiency of over 86% for 8 h without decline, this work provided a simple biochar-based persulfate catalyst for complete antibiotics removal in salty conditions.
KeywordNonradical Porous biochar Persulfate Sulfamethoxazole Singlet oxygen
Document Type期刊论文
Affiliation1.Sun Yat Sen Univ, Sch Environm Sci & Engn, Guangdong Prov Key Lab Environm Pollut Control &, Guangzhou 510275, Peoples R China
2.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China
3.Hong Kong Polytech Univ, Dept Civil & Environm Engn, Hung Hom, Kowloon, Hong Kong, Peoples R China
4.South China Normal Univ, Guangzhou Higher Educ Mega Ctr, Sch Chem,Guangzhou Key Lab Analyt Chem Biomed, Key Lab Theoret Chem Environm,Minist Educ, Guangzhou, Peoples R China
5.Univ Lorraine, Lab Sols & Environm, INRA, 2 Ave Foret Haye BP 20163, F-54505 Vanduvre Les Nancy, France
6.[Qiu, Rongliang
7.South China Agr Univ, Coll Nat Resources & Environm, Guangdong Lab Lingnan Modern Agr, Guangzhou 510642, Peoples R China
Recommended Citation
GB/T 7714
Zhao, Nan,Zhao, Chuanfang,Liu, Kunyuan,et al. Experimental and DFT investigation on N-functionalized biochars for enhanced removal of Cr(VI)[J]. ENVIRONMENTAL POLLUTION,2021,290:-.
APA Zhao, Nan.,Zhao, Chuanfang.,Liu, Kunyuan.,Zhang, Weihua.,Tsang, Daniel C. W..,...&Qiu, Rongliang.(2021).Experimental and DFT investigation on N-functionalized biochars for enhanced removal of Cr(VI).ENVIRONMENTAL POLLUTION,290,-.
MLA Zhao, Nan,et al."Experimental and DFT investigation on N-functionalized biochars for enhanced removal of Cr(VI)".ENVIRONMENTAL POLLUTION 290(2021):-.
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