Hongda Zhang , Yunzhe Zhao , Chenxu Wang , Baolin Liu , Yong Yu
{"title":"氮化硼负载钴混合氧化物和硼空位活化过一硫酸盐,超快去除地表水中的药物","authors":"Hongda Zhang , Yunzhe Zhao , Chenxu Wang , Baolin Liu , Yong Yu","doi":"10.1016/j.jece.2024.114241","DOIUrl":null,"url":null,"abstract":"<div><div>The mediation of vacancy in catalysts is crucial for the enhancement of oxidant activation. Here the boron nitride loaded with Co mixed oxides (Co<sub>2</sub>O<sub>3</sub>-CoO) and boron vacancy (B<sub>v</sub>) catalyst (Co/BN-X) was prepared to degrade sulfamethoxazole (SMX) by activating peroxymonosulfate (PMS). Under dark condition, Co/BN-3+PMS system can completely remove SMX in surface water within 15 min, and its removal efficiency constant (0.5154 min<sup>−1</sup>) was 4.0 and 6.7 times greater than those of Co/BN-2+PMS (0.1284 min<sup>−1</sup>) and Co/BN-1+PMS (0.0771 min<sup>−1</sup>), respectively. The system showed excellent performance in different influencing factors and cyclic experiments, and exhibited good practical application potential in secondary effluent. Electron paramagnetic resonance, radical quenching and electrochemical tests certified that singlet oxygen (<sup>1</sup>O<sub>2</sub>) was the major active species, followed by •O<sub>2</sub><sup>–</sup>, and SO<sub>4</sub><sup>•–</sup>, further elaborating the activation pathway of PMS in Co/BN-3+PMS system. The density functional theory (DFT) calculations confirmed that CoO and PMS-O<sub>2</sub> sites were the main reaction sites, and the existence of B<sub>v</sub> reduced the adsorption energy of Co/BN-3 for PMS. This work reveals the synergistic effect between Co oxide sites and B<sub>v</sub> on the catalyst surface and offers a potential modification method to accelerate Fenton-like reaction.</div></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":"12 6","pages":"Article 114241"},"PeriodicalIF":7.4000,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Activation of peroxymonosulfate by boron nitride loaded with Co mixed oxides and boron vacancy for ultrafast removal of drugs in surface water\",\"authors\":\"Hongda Zhang , Yunzhe Zhao , Chenxu Wang , Baolin Liu , Yong Yu\",\"doi\":\"10.1016/j.jece.2024.114241\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The mediation of vacancy in catalysts is crucial for the enhancement of oxidant activation. Here the boron nitride loaded with Co mixed oxides (Co<sub>2</sub>O<sub>3</sub>-CoO) and boron vacancy (B<sub>v</sub>) catalyst (Co/BN-X) was prepared to degrade sulfamethoxazole (SMX) by activating peroxymonosulfate (PMS). Under dark condition, Co/BN-3+PMS system can completely remove SMX in surface water within 15 min, and its removal efficiency constant (0.5154 min<sup>−1</sup>) was 4.0 and 6.7 times greater than those of Co/BN-2+PMS (0.1284 min<sup>−1</sup>) and Co/BN-1+PMS (0.0771 min<sup>−1</sup>), respectively. The system showed excellent performance in different influencing factors and cyclic experiments, and exhibited good practical application potential in secondary effluent. Electron paramagnetic resonance, radical quenching and electrochemical tests certified that singlet oxygen (<sup>1</sup>O<sub>2</sub>) was the major active species, followed by •O<sub>2</sub><sup>–</sup>, and SO<sub>4</sub><sup>•–</sup>, further elaborating the activation pathway of PMS in Co/BN-3+PMS system. The density functional theory (DFT) calculations confirmed that CoO and PMS-O<sub>2</sub> sites were the main reaction sites, and the existence of B<sub>v</sub> reduced the adsorption energy of Co/BN-3 for PMS. This work reveals the synergistic effect between Co oxide sites and B<sub>v</sub> on the catalyst surface and offers a potential modification method to accelerate Fenton-like reaction.</div></div>\",\"PeriodicalId\":15759,\"journal\":{\"name\":\"Journal of Environmental Chemical Engineering\",\"volume\":\"12 6\",\"pages\":\"Article 114241\"},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2024-09-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Chemical Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2213343724023728\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343724023728","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Activation of peroxymonosulfate by boron nitride loaded with Co mixed oxides and boron vacancy for ultrafast removal of drugs in surface water
The mediation of vacancy in catalysts is crucial for the enhancement of oxidant activation. Here the boron nitride loaded with Co mixed oxides (Co2O3-CoO) and boron vacancy (Bv) catalyst (Co/BN-X) was prepared to degrade sulfamethoxazole (SMX) by activating peroxymonosulfate (PMS). Under dark condition, Co/BN-3+PMS system can completely remove SMX in surface water within 15 min, and its removal efficiency constant (0.5154 min−1) was 4.0 and 6.7 times greater than those of Co/BN-2+PMS (0.1284 min−1) and Co/BN-1+PMS (0.0771 min−1), respectively. The system showed excellent performance in different influencing factors and cyclic experiments, and exhibited good practical application potential in secondary effluent. Electron paramagnetic resonance, radical quenching and electrochemical tests certified that singlet oxygen (1O2) was the major active species, followed by •O2–, and SO4•–, further elaborating the activation pathway of PMS in Co/BN-3+PMS system. The density functional theory (DFT) calculations confirmed that CoO and PMS-O2 sites were the main reaction sites, and the existence of Bv reduced the adsorption energy of Co/BN-3 for PMS. This work reveals the synergistic effect between Co oxide sites and Bv on the catalyst surface and offers a potential modification method to accelerate Fenton-like reaction.
期刊介绍:
The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.