摘要
通过对非均相复合催化剂进行合理的电子结构调控,可有效促进界面电荷分离和转移,进而提升催化剂的性能。近年来,以生物炭(BC)基材料活化过氧乙酸[CH3C(O)OOH,PAA]的非均相高级氧化工艺因能产生多种活性氧物种(ROS)而备受关注。采用一种简易的共沉淀法合成了Co(OH)2纳米颗粒修饰的生物炭材料(h-Co/BC),并将其应用于活化PAA降解水中的典型抗生素四环素(TC)。实验结果表明h-Co/BC在pH=7条件下,7 min内可实现对初始浓度为10µmol/L的TC的完全降解去除。自由基猝灭实验和电子顺磁共振(EPR)分析表明,该非均相体系中主要的ROS为烷氧基自由基,包括CH3COO·、CH3COOO·、·OH和1O_(2)。材料表征结合密度泛函理论计算表明,Co(OH)2纳米颗粒成功地负载于生物炭上,Co 3d带中心更靠近费米能级,利于电子的定向迁移,进而被PAA捕获,随后PAA裂解生成ROS。该研究可为非均相PAA高级氧化技术中功能材料的研发提供新的理念。
Reasonable regulation of electronic structures of heterogeneous composite catalysts can enhance the charge separation and transfer at the interface of materials,thus further promoting the catalytic performance of cata-lysts.Recently,peracetic acid[CH3C(O)OOH,PAA]based on heterogeneous advanced oxidation process with bio-char(BC)materials has attacked much interests due to various reactive oxygen species(ROS)generated in the pro-cess.In this study,biochar modified with Co(OH)2 nanoparticles(h-Co/BC)was successfully synthesized by a simple co-precipitation method,which was applied to activate PAA for tetracycline(TC)degradation.The results showed that h-Co/BC could completely degrade TC with an initial concentration of 10µmol/L within 7 min at pH 7.The scavenger quenching tests and electron paramagnetic resonance(EPR)analysis further indicated that the produced primary ROS were alkoxy radical,which mainly including CH3COO·,CH3COOO·,·OH and 1O_(2).In addition,materi-als characterizations combined with density functional theory calculation showed that biochar was successfully modi-fied with Co(OH)2 nanoparticles.Thus,the Co 3d-band in h-Co/BC was closer to Fermi level compared with that in pure Co(OH)2,benefiting to directional electron transfer,which could then be easily captured by PAA for cleavage to ROS.This study provided a new method for synthesis of functional materials applied in PAA-based AOPs.
作者
孙丰宾
杨旭东
李璠
乔林
刘文
SUN Fengbin;YANG Xudong;LI Fan;QIAO Lin;LIU Wen(Institute of Urban Meteorology,CMA,Beijing 100089,China;Institute of Atmospheric Physics,Chinese Academy of Sciences,Beijing 100029,China;The Key Laboratory of Water and Sediment Sciences,Ministry of Education,College of Environmental Sciences and Engineering,Peking University,Beijing 100871,China;State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems,Peking University,Beijing 100871,China)
出处
《工业水处理》
CAS
CSCD
北大核心
2024年第6期78-87,共10页
Industrial Water Treatment
基金
国家自然科学基金项目(52270053)
国家重点研发计划青年科学家项目(2021YFA1202500)
北京市自然科学基金项目(8232035)
北京市科技新星计划交叉合作课题(20220484215)。
关键词
生物炭
氢氧化钴
过氧乙酸
抗生素
密度泛函理论计算
biochar
cobalt hydroxide
peracetic acid
antibiotics
density functional theory calculation
