Cobalt/nitrogen co-carved carbon nanorod for efficient Fenton-like reaction:Degradation efficacy,reaction mechanism and singlet oxygen generation  

作　　者：Meng Li Ke Zheng Yu-Ting Jin Zhao-Xin Zhang Ji-Liang Cheng Long-Wei Huang Ce-Hui Mo Shao-Qi Zhou 

机构地区：[1]Guangdong Provincial Research Center for Environment Pollution Control and Remediation Materials,College of Life Science and Technology,Jinan University,Guangzhou 510632,China [2]College of Environment and Energy,Guangzhou Higher Education Mega Centre,South China University of Technology,Guangzhou 510006,China [3]Department of Chemical and Biological Engineering,The Hong Kong University of Science and Technology,Clear Water Bay,Kowloon,Hong Kong SAR,China [4]School of Civil Engineering and Transportation,South China University of Technology,Guangzhou 510640,China [5]Thrust of Sustainable Energy&Environment,The Hong Kong University of Science and Technology,Guangzhou 511458,China [6]College of Resources and Environmental Engineering,Guizhou University,Guiyang 550025,China

出　　处：《Journal of Materials Science & Technology》2023年第6期67-78,共12页材料科学技术（英文版）

基　　金：This work was financially supported from the Key Program of National Natural Science Foundation of China(No.42030713);the National Natural Science Foundation of China(No.42007358);the Guangdong Basic and Applied Basic Research Foundation(Nos.2020A1515110518 and2021A1515110369);the Hongkong Schol-arship Program(No.XJ2020059);the China Postdoctoral Sci-ence Foundation(No.2019M663382);the Ministry of Science and Technology of China for State Key Research and Development Project(No.2016YFC0400702);the YoungInnovativeTalent Project of Guangdong Provincial Department of Education(No.2019GKQNCX056).The authors would like to thank Shiyanjia Lab(www.shiyanjia.com)for the GC-MS measurements.

摘　　要：The Fenton-like process shows promising potential to generate reactive oxygen species for the reme-diation of increasingly environmental pollutants.However,the slow development of high-activity cata-lysts with strong stability and low leaching of metal ions has greatly inhibited scale-up application of this technology.Here,cobalt(Co)/nitrogen(N)atom co-curved carbon nanorod(CoNC)containing highly uniform CoN_(x)active sites is developed as a Fenton-like catalyst for the effective catalytic oxidation of various organics via peroxymonosulfate(PMS)activation with high stability.As confirmed by the exper-imental results,singlet oxygen(^(1)O_(2))is the dominant active species for the degradation of the organ-ics,with a proportion of 100%.Furthermore,density functional theory calculations indicate that CoN_(2)C_(2)is the most effective ligand structure with more negative adsorption energy for PMS and the shortest length Co-O bond,while the most reasonable generation pathway for^(1)O_(2)was CoN_(2)C_(2)-PMS→CoN_(2)C_(2)-OH∗→2O∗→^(1)O_(2).Further studies demonstrate that the electron can be transferred from the highest occupied molecular orbitals of the organics to the lowest unoccupied molecular orbitals of the PMS via CoN_(2)C_(2)action.In addition,the CoNC presents strong resistance to inorganic ions and natural organic matter in the Fenton-like catalysis process.The presence of CoN_(2)C_(2)active centre can significantly shorten the migration distance of the^(1)O_(2)generated from PMS activation,which further enhances the Fenton-like catalytic activity in terms of mineralising various organic contaminants with high efficiency over a wide pH range.

关 键 词：Non-radical pathway Singlet oxygen Co/N co-carved carbon nanorod Fenton-like catalysis 

分 类 号：TQ116.2[化学工程—无机化工] O643.36[理学—物理化学] TB383.1[理学—化学]