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Fe_(2)O_(3)-CuO/rCG催化降解水中苯并三氮唑的效能与机理

Performance and mechanism of catalytic degradation of benzotriazole in water by Fe_(2)O_(3)-CuO/rCG
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摘要 以煤矸石(Coal gangue,CG)为原料,通过煅烧、酸浸和金属改性制备铁铜改性煤矸石(Fe_(2)O_(3)-CuO/rCG),对Fe_(2)O_(3)-CuO/rCG的形貌结构进行了表征分析,并研究了Fe_(2)O_(3)-CuO/rCG/H_(2)O_(2)体系对苯并三氮唑(BTA)的降解效能和作用机理。结果表明:改性后Fe_(2)O_(3)-CuO/rCG比表面积和总孔容均明显增加,Fe_(2)O_(3)与CuO成功填充在材料孔隙内部;Fe_(2)O_(3)-CuO/rCG的最佳制备条件为煅烧温度650℃、煅烧时间3 h、金属离子负载浓度0.07 mol/L;Fe_(2)O_(3)-CuO/rCG/H_(2)O_(2)体系降解BTA的最佳条件为BTA质量浓度30 mg/L、Fe_(2)O_(3)-CuO/rCG投加量2 g/L、H_(2)O_(2)浓度7 mmol/L、温度25℃、转速240 r/min,反应2 h时,体系对BTA降解率最高可达94.86%,TOC与TN去除率分别可达87.69%与84.27%;Fe_(2)O_(3)-CuO/rCG耦合类Fenton体系去除BTA的作用机制主要有吸附和催化降解两种,吸附主要有孔隙填充、配体吸附和氢键作用,催化降解过程·OH和^(1)O_(2)为主要活性物种,且^(1)O_(2)占主导地位,Fe^(2+)/Fe^(3+)和Cu^(+)/Cu^(2+)的氧化还原循环加速了类Fenton体系中活性物种的生成。 Iron-copper modified coal gangue(Fe_(2)O_(3)-CuO/rCG)was prepared using coal gangue(CG)as raw material through calcination,acid leaching and metal modification.The morphology and structure of Fe_(2)O_(3)-CuO/rCG were characterized and analyzed,and the degradation efficiency and mechanism of Fe_(2)O_(3)-CuO/rCG system on benzotri⁃azole(BTA)were studied.The results showed that the specific surface area and total pore volume of Fe_(2)O_(3)-CuO/rCG significantly increased after modification.Fe_(2)O_(3)and CuO were successfully filled inside the pores of materials.The optimal preparation conditions for Fe_(2)O_(3)-CuO/rCG were calcination temperature of 650℃,calcination time of 3 hours,and metal ion loading concentration of 0.07 mol/L.The optimal conditions for BTA degradation in Fe_(2)O_(3)-CuO/rCG/H_(2)O_(2)system were BTA concentration of 30 mg/L,Fe_(2)O_(3)-CuO/rCG dosage of 2 g/L,H_(2)O_(2)concentration of 7 mmol/L,temperature of 25℃,and rotational speed of 240 r/min.After 2 hours of reaction,the highest degradation rate of BTA in system could reach 94.86%,and the removal rates of TOC and TN could reach 87.69%and 84.27%,respectively.The Fe_(2)O_(3)-CuO/rCG coupled Fenton system had two main mechanisms for removing BTA:adsorption and catalytic degradation.Adsorption mainly involved gap filling,ligand adsorption,and hydrogen bonding.During the catalytic degradation process,·OH and^(1)O_(2)were the main active species,with dominated by^(1)O_(2).Moreover,the redox cycle of Fe^(2+)/Fe^(3+)and Cu^(+)/Cu^(2+)accelerated the generation of active species in Fenton-like system.
作者 郭紫瑞 李红艳 张峰 崔佳丽 杨群 李赟 GUO Zirui;LI Hongyan;ZHANG Feng;CUI Jiali;YANG Qun;LI Yun(School of Environmental Science and Engineering,Taiyuan University of Technology,Jinzhong 030600,China;Shanxi Municipal Engineering Graduate Education Innovation Center,Jinzhong 030600,China;Linxian Fenglin Modern Agricultural Development Co.,Ltd.,Lüliang 033200,China)
出处 《工业水处理》 CAS CSCD 北大核心 2024年第9期118-126,共9页 Industrial Water Treatment
基金 山西省自然科学基金面上项目(202203021221060) 吕梁市引进高层次科技人才重点研发项目(2021RC-1-22)。
关键词 煤矸石 催化剂 吸附 催化降解 苯并三氮唑 coal gangue catalyst adsorption catalytic degradation benzotriazole
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