{"title":"Fabrication of Boron modified bi-functional air diffusion electrode for ciprofloxacin Degradation: In-situ H2O2 generation and self-activation","authors":"Hengrui Zhang, Bairun Chen, Jing Li, Xinran Song, Jiaxin Zhai, Wen Liu, Shuyan Kong, Xuan Xing","doi":"10.1016/j.cej.2024.156427","DOIUrl":null,"url":null,"abstract":"In order to improve H<sub>2</sub>O<sub>2</sub> in-<em>situ</em> generation in electrochemical system, a boron (B) modified air diffusion electrode (B@ADE) was fabricated in the present study. Carbon black (CB) doped by B was deposited on ADE surface as catalytic layer. Performance of B@ADE with different B/C mass ratios has been investigated and 0.3 was identified as the optimal one·H<sub>2</sub>O<sub>2</sub> yield can be achieved 204.85 mg L<sup>-1</sup> within 45 min at 0.3-B@ADE, which was 1.51 times for that of ADE. Meanwhile, H<sub>2</sub>O<sub>2</sub> self-activation on B@ADE surface was observed and effects of different operating parameters on <sup>•</sup>OH formation have been analyzed. XPS analyzation demonstrated that BC<sub>2</sub>O, BC<sub>2</sub>O and C = O/O-C = O were related to H<sub>2</sub>O<sub>2</sub> generation. DFT calculation revealed that BCO<sub>2</sub> was benefit for O<sub>2</sub> adsorption, while BC<sub>2</sub>O promoted *OOH desorption with lower free energy barriers for H<sub>2</sub>O<sub>2</sub> and <sup>•</sup>OH generation. Quenching experiments for ciprofloxacin (CIP) demonstrated that <sup>•</sup>OH, O•-2 and <sup>1</sup>O<sub>2</sub> were co-existed in the system with their contribution quantified. Four possible degradation pathways were proposed through active sites identification by DFT calculation and intermediates detection by HPLC-MS/MS. Bio-toxicity analyzation results showed that the toxicity of most intermediates was lowered than CIP. These results proved that electrochemical oxidation system with B@ADE enhanced in-<em>situ</em> H<sub>2</sub>O<sub>2</sub> generation and self-activation, with great potential for practical application.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":null,"pages":null},"PeriodicalIF":13.3000,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2024.156427","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
In order to improve H2O2 in-situ generation in electrochemical system, a boron (B) modified air diffusion electrode (B@ADE) was fabricated in the present study. Carbon black (CB) doped by B was deposited on ADE surface as catalytic layer. Performance of B@ADE with different B/C mass ratios has been investigated and 0.3 was identified as the optimal one·H2O2 yield can be achieved 204.85 mg L-1 within 45 min at 0.3-B@ADE, which was 1.51 times for that of ADE. Meanwhile, H2O2 self-activation on B@ADE surface was observed and effects of different operating parameters on •OH formation have been analyzed. XPS analyzation demonstrated that BC2O, BC2O and C = O/O-C = O were related to H2O2 generation. DFT calculation revealed that BCO2 was benefit for O2 adsorption, while BC2O promoted *OOH desorption with lower free energy barriers for H2O2 and •OH generation. Quenching experiments for ciprofloxacin (CIP) demonstrated that •OH, O•-2 and 1O2 were co-existed in the system with their contribution quantified. Four possible degradation pathways were proposed through active sites identification by DFT calculation and intermediates detection by HPLC-MS/MS. Bio-toxicity analyzation results showed that the toxicity of most intermediates was lowered than CIP. These results proved that electrochemical oxidation system with B@ADE enhanced in-situ H2O2 generation and self-activation, with great potential for practical application.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.