生物炭负载γ-MnO_(2)纳米复合材料活化过一硫酸盐降解对氯苯酚的性能及机理  

Performance and mechanism of biochar doped γ-MnO_(2) nanocomposite activated peroxymonsulfate on 4-Chlorophenol degradation

作　　者：姚宏嘉 陈星 张玉[2] 刘彤 崔康平 陈长斌[3] 徐正江[3] YAO Hongjia;CHEN Xing;ZHANG Yu;LIU Tong;CUI Kangping;CHEN Changbin;XU Zhengjiang(School of Resources and Environmental Engineering,Hefei University of Technology,Hefei 230009,PR China;School of Materials Science and Engineering,Hefei University of Technology,Hefei 230009,China;Anqing Shuguang Chemical Co.Ltd.,Anqing246003,China)

机构地区：[1]合肥工业大学资源与环境工程学院,合肥230009 [2]合肥工业大学材料科学与工程学院,合肥230009 [3]安徽省安庆市曙光化工股份有限公司,安庆246003

出　　处：《环境工程学报》2022年第6期1833-1844,共12页Chinese Journal of Environmental Engineering

基　　金：国家重点研发计划(2019YFC0408500);安徽省科技重大专项(201903a07020009,202003a07020004);合肥市自主创新政策“借转补”项目(J2020K07)。

摘　　要：采用水热法合成了4种不同晶相结构MnO_(2)及生物炭负载γ-MnO_(2)复合纳米材料,并对其活化过硫酸盐(PMS)降解4-CP的性能进行了研究。采用XRD、SEM、EDS以及XRF等手段对不同复合纳米材料进行了表征分析,发现仅有γ-MnO_(2)成功负载到生物炭材料表面形成γ-MnO_(2)@BC复合纳米材料。在优化条件下,γ-MnO_(2)@BC活化PMS体系能在20 min内将10 mg·L^(-1)对氯苯酚完全降解。γ-MnO_(2)@BC对H_(2)PO_(4)^(-)之外的阴离子均表现出较强的抗干扰性。采用自由基捕获及电子自旋共振波谱(ESR)、X射线光电子能谱(XPS)等手段研究了该复合纳米材料活化PMS降解污染物的机理。结果表明,γ-MnO_(2)@BC活化PMS产生的活性氧物种为单线态氧,并发现Mn(III)与Mn(IV)的比值是影响不同晶相二氧化锰催化性能的主要因素。Four kinds of MnO_(2) with different crystal phase structure and biochar supported γ-MnO_(2)nanocomposites were synthesized by hydrothermal method,and their performance on activating peroxymonsulfate(PMS) and degrading 4-CP was studied.XRD,SEM,EDS and XRF were used to characterize different nano-composite materials.It was found that only γ-MnO_(2) was successfully loaded on the surface of biochar to form γ-MnO_(2)@BC.Under the optimum conditions,10 mg·L^(-1) 4-chlorophenol could be completely degraded by γ-MnO_(2)@BC activated PMS in 20 min.γ-MnO_(2)@BC showed the strong anti-interference against anions except for H_(2)PO_(4)^(-).Finally,the mechanism of reactive oxygen species(ROS) generated by γ-MnO_(2)@BC activated PMS was studied by means of free radical capture,electron spin resonance spectroscopy(ESR) and Xray energy spectroscopy(XPS).The results showed that the ROS produced by γ-MnO_(2)@BC activated PMS was singlet oxygen.It is found that the ratio of Mn(III) to Mn(IV) was the main factor affecting the catalytic performance of MnO_(2) with different crystalline phases.

关 键 词：MnO_(2) 晶相 生物炭 过一硫酸盐 对氯苯酚降解 

分 类 号：X703.1[环境科学与工程—环境工程]