PDA及其衍生NGC膜包覆A-TiO_(2)可见光催化氧化乙醛  

PDA and its derived NGC membrane coated A-TiO_(2)for visible-light-driven photocatalytic oxidation of acetaldehyde

作　　者：黄一维 朱梅萍 HUANG Yiwei;ZHU Meiping(School of Resources,Environment and Materials,Guangxi University,Nanning 530004,China;Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology,Nanning 530004,China)

机构地区：[1]广西大学资源环境与材料学院,广西南宁530004 [2]广西石化资源加工及过程强化技术重点实验室,广西南宁530004

出　　处：《广西大学学报（自然科学版）》2024年第4期867-881,共15页Journal of Guangxi University（Natural Science Edition）

基　　金：广西自然科学基金项目(2021GXNSFBA220074);广西石化资源加工及过程强化技术重点实验室开放基金项目(2021K010)。

摘　　要：针对TiO_(2)在可见光波段对连续流动态乙醛的催化降解性能弱等问题,采用贻贝仿生化学策略及高温炭化工艺构建了广谱性聚多巴胺(PDA)及其衍生N掺杂炭(NGC)膜包覆的核壳型锐钛矿TiO_(2)(AT)(AT@P和AT@C)。利用扫描电镜(SEM)、X射线衍射(XRD)、X射线光电子能谱(XPS)、紫外-可见光漫反射光谱(UV-vis DRS)、瞬时光电流密度-时间曲线(I-t)和交流阻抗(EIS)等手段对材料的物化性质及光电学性质进行表征,研究复合AT中不同PDA包覆量及最佳包覆量时炭化前、后微观成分和结构变化对乙醛的可见光催化性能的影响。结果表明:PDA的包覆显著增强了AT的可见光吸收能力和光生载流子分离能力,极大地提高了其在可见光照下光催化降解乙醛的活性。当多巴胺添加量为50 mg时获得的AT@P-50相比AT@P-10和AT@P-100展现出较高的降解效率(71%),是AT的2.09倍。π共轭结构高活性N(石墨化N)的转化可进一步提高材料的载流子分离效率和界面迁移率,促进AT的光催化活性及稳定性的提升。最佳PDA包覆量时炭化衍生NGC包覆的AT@C-50的乙醛可见光降解效率高达77%,分别是AT和AT@P-50的2.26、1.08倍。在相同的连续流动体系和乙醛浓度条件下,合成的AT@P-x(x=10、50和100)、AT@C-50相比其他精心设计的TiO_(2)复合材料对乙醛具有更为优异的可见光催化降解性能。此外,采用原位红外漫反射技术(in-situ DRIFTS)探究AT@C-50在乙醛催化过程中间产物的演变行为,并揭示了可能的催化路径和反应机制。In order to improve the catalytic degradation performance of TiO_(2)for continuous flowing acetaldehyde under visible light irradiation,core-shell type anatase TiO_(2)(AT)(AT@P and AT@C)wrapped by a broad-spectrum polydopamine(PDA)and its derived N-doped carbon(NGC)membrane were constructed using mussel bionic chemistry strategy and high-temperature carbonization process.Scanning electron microscopy(SEM),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),UV-visible diffuse reflection spectroscopy(UV-vis DRS),instantaneous photocurrent density-time curve(I-t)and A.C.impedance(EIS)were used to characterize the physicochemical and photoelectric properties of the materials.The effects of different coating amounts of PDA and the microscopic compositional and structural changes before and after carbonization at optimal coating amount on the visible light-driven catalytic performance of acetaldehyde were studied.The results showed that PDA coating significantly enhanced the visible light absorption and photo-induced carrier separation ability of AT,leading to a significant improvement of photocatalytic degradation activity of acetaldehyde under visible light irradiation.When the addition of DA was 50 mg,the degradation efficiency of acetaldehyde over AT@P 50(71%)was higher than that of AT@P 10 and AT@P 100,which was 2.09 times of that of AT.The conversion of highly active N(graphitized N)withπ-conjugate structures can further improved carrier separation efficiency and interfacial mobility of materials,thus promoting the photocatalytic activity and stability of AT.The degradation rate of AT@C 50 coated with NGC derived from the PDA with optimum amount is up to 77%,which is 2.26 and 1.08 times of AT and AT@P 50,respectively.Under the same continuous flowing system and acetaldehyde concentration conditions,the synthesized AT@P x(x=10,50 and 100)and AT@C 50 exhibited superior visible photocatalytic degradation of acetaldehyde compared to other well-designed TiO_(2)composites.In addition,In-situ infrared diffuse r

关 键 词：醛类挥发性有机物 光催化 锐钛矿TiO_(2) 聚多巴胺 反应机制 

分 类 号：TQ034[化学工程] X131.1[环境科学与工程—环境科学]