Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2023-04-22 , DOI: 10.1016/j.jhazmat.2023.131471 Zhengfang Zhang 1 , Yang Liu 1 , Ying Zhang 1 , Ruohan Li 1 , Yuntao Guan 1
In this study, a novel carbon-based material (Fe-N-PGWBC) utilizing the garden waste, melamine and FeSO4 as the precursor was successfully synthesized, efficiently activating peroxydisulfate (PDS) to degrade tetrabromobisphenol A (TBBPA). Under typical conditions (Fe-N-PGWBC dose of 100 mg·L−1, PDS of 0.2 mM and TBBPA of 10 mg·L−1), Fe-N-PGWBC/PDS system could achieve over 99% TBBPA removal (including adsorption and degradation) within 60 min, and the corresponding rate constant ks was 0.0724 min−1, which was almost 40.2 times higher than that of the pristine biochar. The extraction experiments implied that the excellent adsorption performance of Fe-N-PGWBC did not hinder the degradation of TBBPA. Abundant active sites (rich oxygen-containing functional groups, Fe-O and Fe3C) of Fe-N-PGWBC could effectively promote PDS decomposition to produce reactive oxygen species. The probe-based kinetic modelling methods verified that approximately 87.6% TBBPA was degraded by SO4·-, 12.2% TBBPA was degraded by 1O2, and 0.2% TBBPA was degraded by ·OH. Furthermore, based on the calculation of density functional theory and identification of products, TBBPA was mainly involved in three transformation pathways including hydroxylation, debromination and β-scission process. The study proposed a facile resource approach of garden waste and provided deeper understanding for the TBBPA degradation mechanisms in heterogeneous system.
中文翻译:
活性过硫酸盐通过碳基材料高效降解四溴双酚 A:掺杂 N 和 Fe 的协同机制
在这项研究中,成功地合成了一种以花园垃圾、三聚氰胺和 FeSO 4为前体的新型碳基材料 (Fe-N-PGWBC) ,可有效激活过二硫酸盐 (PDS) 以降解四溴双酚 A (TBBPA)。在典型条件下(Fe-N-PGWBC 剂量为 100 mg·L -1,PDS 为 0.2 mM 和 TBBPA 为 10 mg·L -1),Fe-N-PGWBC/PDS 系统可实现超过 99% 的 TBBPA 去除(包括吸附和降解)在60 min内,对应的速率常数k s为0.0724 min −1,几乎是原始生物炭的 40.2 倍。萃取实验表明,Fe-N-PGWBC 优异的吸附性能不会阻碍 TBBPA 的降解。Fe-N-PGWBC丰富的活性位点(丰富的含氧官能团、Fe-O和Fe 3 C)可有效促进PDS分解产生活性氧。基于探针的动力学建模方法证实,大约 87.6% 的 TBBPA 被 SO 4 ·-降解,12.2% 的 TBBPA 被1 O 2降解,0.2% 的 TBBPA 被·降解哦。此外,基于密度泛函理论计算和产物鉴定,TBBPA主要参与羟基化、脱溴化和β-裂解过程三个转化途径。该研究提出了一种简便的花园废弃物资源化方法,并为异质系统中 TBBPA 的降解机制提供了更深入的理解。