混晶TiO2光催化剂的制备和降解水体二甲双胍性能
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1.西北大学 化工学院;2.太原理工大学 省部共建煤基能源清洁高效利用国家重点实验室

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TQ034

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陕西省创新能力支撑计划(2024RS-CXTD-53);陕西省重点研发计划项目(2024SF-YBXM-575);省部共建煤基能源清洁高效利用国家重点实验室开放基金资助项目(MJNYSKL202305)。


Photocatalytic degradation of polluted water containing metformin by mixed crystalline TiO2
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1.College of Chemical Engineering,Northwest University;2.State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology;3.College of Chemical Engineering,Northwest University,Xi''an

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    摘要:

    以冰乙酸和钛酸四丁酯为主要原料,采用溶胶-凝胶法制备了一种混晶TiO2光催化剂,将其用于紫外光下降解水体污染物二甲双胍(MET)催化剂,通过SEM、XRD、TEM、FTIR、EPR、PL、HRMS等对TiO2光催化剂的结构组成和光学参数进行表征,基于MET降解实验,考察n(去离子水)∶n(冰乙酸)∶n(钛酸四丁酯)、煅烧温度、水体溶液pH值等对TiO2光催化剂降解MET的影响,通过降解动力学计算、自由基捕获实验以及对降解产物的分析,推测MET的降解机理。结果表明,n(去离子水)∶n(冰乙酸)∶n(钛酸四丁酯)=6∶1.5∶1制备的凝胶成胶时间60 min,经550 ℃煅烧制备的混合晶型TiO2-550具有最佳的光催化性能,在pH=11,光照60 min后,MET的降解率高达78.03%,显著高于单一锐钛矿和金红石晶型TiO2;TiO2-550含有质量分数77%锐钛矿和23%的金红石,为聚集的球形颗粒,粒径约为20 nm;TiO2-550具有氧空位/Ti3+及较窄的禁带宽度(2.81 eV)。TiO2-550光催化降解MET过程符合拟一级动力学模型,降解速率常数为0.016 min-1;MET的降解遵循空穴和超氧基自由基、羟基自由基氧化机理,降解后分别生成1-甲基双胍(MBG)和4-氨基-2-亚胺-1-甲基-1,2-二氢-1,3,5-三嗪、METOOH和MBGOOH;TiO2-550持续循环使用5次后,对MET降解率从78.03%降至76.01%,利用率降低2.59%。

    Abstract:

    A mixed-crystal TiO2 was prepared by the sol-gel method for the degradation of the water pollutant metformin (MET) under ultraviolet light. The structure and photocatalytic activity of mixed-crystal TiO2 were explored by various characterization methods. The degradation mechanism of MET is revealed by degradation kinetics calculations, radical trapping experiments, and analysis of degradation products. SEM, TEM, XRD and FTIR showed that the TiO2 prepared at the optimal calcination temperature of 550 °C was a mixed crystalline structure, containing 77% anatase and 23% rutile, and the morphology was 20 nm spherical aggregation structure. The degradation experiments of MET showed that the effect of mixed crystal was better than that of single crystal, which was due to the oxygen vacancy/Ti3+ and narrow band gap of mixed TiO2. The MET degradation process conformed to the first-order kinetic model, and the degradation rate constant was 0.016 min-1. At the pH of 11, the degradation rate of MET reaches up to 78.03%, which is 2.2 times than anatase-type TiO2. Radical trapping experiments demonstrate that the degradation of MET follows a mechanism involving hole and ?OH、?O2? oxidation. Through the in-depth analysis of the degradation products, four degradation reaction paths were proposed. Furthermore, after five consecutive cycles, the catalyst exhibits only a 2.59% decrease in the degradation rate of MET, indicating its high photocatalytic activity and stability.

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仲梦如,田斌,司琦,王兴宝,李晶莹,徐龙.混晶TiO2光催化剂的制备和降解水体二甲双胍性能[J].精细化工,2026,43(1):

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  • 收稿日期:2024-11-14
  • 最后修改日期:2025-01-27
  • 录用日期:2024-12-25
  • 在线发布日期: 2026-01-16
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