具备介孔结构的交互式纳米复合材料提高医药废弃物治理效果  

Efficacy improvement of pharmaceutical waste remediation using interactive nanocomposites with tunable mesopores and structure

作　　者：李翠霞[1,2,3] 张玉杭 胡瑞兵 BASHIR Sajid 刘静波 LI Cuixia;ZHANG Yuhang;HU Ruibing;BASHIR Sajid;LIU Jingbo Louise(School of Materials Science and Engineering,Lanzhou University of Technology,Lanzhou 730073,China;State Key Laboratory of Advanced Processing and Recycling of Non-Ferrous Metals,Lanzhou University of Technology,Lanzhou 730070,China;Department of Chemistry,Texas A&M University-Kingsville,Kingsville 78363,United States;Texas A&M Energy Institute,College Station 77843,United States)

机构地区：[1]兰州理工大学材料科学与工程学院,兰州730073 [2]兰州理工大学有色金属先进加工与回收国家重点实验室,兰州730070 [3]德克萨斯农机大学金斯维尔分校化学系,美国金斯维尔78363 [4]德克萨斯A&M能源研究所,美国学院站77843

出　　处：《黑龙江大学自然科学学报》2021年第5期549-573,共25页Journal of Natural Science of Heilongjiang University

基　　金：Supported by the National Nature Science Foundation of China(51764039);the Chinese Scholarship Council(201608625038);the Petroleum Research Fund of the American Chemical Society(53827-UR10);the Robert Welch Foundation(Departmental Grant,AC-0006)。

摘　　要：两种不同类型的纳米材料,TiO_(2)和还原氧化石墨烯(Reduced graphene oxide,RGO)复合制备出性能优异的复合纳米光催化材料(RGO-TiO_(2))。具备商业化前景的湿化学法制备的交互式光催化剂不仅可以对环境刺激做出反应,而且能够自我调节其结构和生物化学性质。采用溶胶-凝胶结合原位模板法制备了纳米复合粒子RGO-TiO_(2),其粒径约为10.5 nm,引入水溶性聚合物聚乙烯吡咯烷酮(PVP)对RGO-TiO_(2)多孔纳米材料进行改性,以控制其内部通道和孔隙率,介孔孔径从3.41 nm增大到4.81 nm,大幅提高了对四环素(TCH,C_(22)H_(24)N_(2)O_(8))的光催化降解效率。高降解效率主要源于催化剂表面H_(2)O和·OH吸附和扩散速率的提高以及异质结对光催化剂固有性能的改善。当其用于降解四环素医药废物时,其反应活性提高了30%。利用电子显微镜研究推断出了可能的“电子拓扑”,Ti中从p轨道移动到d轨道时采用的是电子态的形状传播。电子局域化抑制了激发态电子和空穴的复合,延长带电载流子(电子、空穴和激子)寿命,从而提高了对TCH的降解效率。Combination of two different types of nanomaterials,titania(TiO_(2))and reduced graphene oxide(RGO)yielded a unique photo-catalytical nanocomposite(RGO-TiO_(2)).A wet-chemistry with commercial potential derived interactive photocatalysts could respond to the environmental stimuli and self-regulate their structures and biochemical properties.The RGO-TiO_(2) porous nanomaterials were modified using a mesoporous water-soluble polymer,polyvinylpyrrolidone(PVP)to control the internal channel and porosity.The pore size of these catalysts was increased from 3.41 to 4.81 nm,which maximized the photo-catalytical efficacy of tetracycline(TCH,C_(22)H_(24)N_(2)O_(8)).This in-situ templating was carried out using a feasible sol-gel synthesis to produce different mesoporous RGO-TiO_(2) nanocomposites sized at 10.5 nm.High degradation rate for TCH was achieved due to rapid H_(2)O and·OH species adsorption and diffusion.It was also found that immobilization of electrons at the heterojunction improved intrinsic property of photocatalysts.Its reactivity was found to be improved by >30% when applied for degradation of the above pharmaceutical wastes.The electron microscopic study inferred“electron topology”allowed for the shape propagation of electron states adopted as they moved from p to d orbitals in Ti.The individual localization of the electrons successfully prevented the recombination of excited electrons and holes.The life spans of these charge carries(electrons,holes,and excitons)were extended to secure the high efficacy of the TCH degradation under moderate conditions.

关 键 词：纳米复合材料 还原氧化石墨烯负载二氧化钛 介孔模板 湿化学合成 光催化 四环素降解 

分 类 号：TB321[一般工业技术—材料科学与工程]