MIL-125(Ti)衍生介孔圆盘状N-TiO2高效光催化降解气态苯

doi:10.1016/S1872-2067(19)63516-3

催化学报 ›› 2020, Vol. 41 ›› Issue (8): 1186-1197.DOI: 10.1016/S1872-2067(19)63516-3

MIL-125(Ti)衍生介孔圆盘状N-TiO₂高效光催化降解气态苯

赵晨^a,b, 王志华^a, 陈肸^b, 楚弘宇^b, 付会芬^b, 王崇臣^b

a 北京化工大学化工资源有效利用国家重点实验室, 北京 100029;
b 北京建筑大学建筑结构与环境修复功能材料北京重点实验室, 北京 100044

收稿日期:2019-11-26 修回日期:2019-12-23 出版日期:2020-08-18 发布日期:2020-08-08
通讯作者: 王志华, 王崇臣
基金资助:
国家自然科学基金（21876008，51578034，51878023）；北京市属高等学校长城学者培养计划（CIT&TCD20180323）；北京市属高等学校创新团队建设与教师职业发展计划（IDHT20170508）；北京建筑大学市属高校基本科研业务费专项资金资助（X18075，X18076，X18124，X18125，X18276）；北京建筑大学科研基金（KYJJ2017033、KYJJ2017008）.

Robust photocatalytic benzene degradation using mesoporous disk-like N-TiO₂ derived from MIL-125(Ti)

Chen Zhao^a,b, Zhihua Wang^a, Xi Chen^b, Hongyu Chu^b, Huifen Fu^b, Chong-Chen Wang^b

a State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
b Beijing Key Laboratory of Functional Materials for Building Structure and Environment Remediation, Beijing University of Civil Engineering and Architecture, Beijing 100044, China

Received:2019-11-26 Revised:2019-12-23 Online:2020-08-18 Published:2020-08-08
Supported by:
This work was supported by the National Natural Science Foundation of China (21876008, 51578034 and 51878023), Great Wall Scholars Training Program Project of Beijing Municipality Universities (CIT&TCD20180323), Project of Construction of Innovation Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality (IDHT20170508), Beijing Talent Project (2018A35), Fundamental Research Funds for Beijing Universities (X18075/X18076/X18124/X18125/X18276), and Scientific Research Foundation of Beijing University of Civil Engineering and Architecture (KYJJ2017033/KYJJ2017008).

摘要/Abstract

摘要： 挥发性有机污染物（VOCs）对人或动物的危害较大，具有致癌、致畸和致突变性.气固相光催化法已经成为一种具有广阔应用前景的VOCs治理技术.传统半导体光催化剂TiO₂带隙较宽（E_g=3.2eV），太阳光利用效率低.特别是对光催化降解VOCs而言，反应过程中产生的含碳类中间产物易在TiO₂表面积累，致使其失活.因此，如何拓宽TiO₂的光谱响应范围，提高光量子效率及其在VOCs氧化过程中的循环利用性一直是研究重点.
由于O和N具有类似的化学结构和电子特征，对TiO₂进行N掺杂（N-TiO₂）是实现TiO₂可见光催化的有效途径.TiO₂前驱体和氮源的种类对N-TiO₂的带隙、N掺杂位点、N掺杂量、形貌和孔径影响较大.金属-有机骨架（MOFs）具有结构多样且可调、多孔性、比表面积大等优点，是制备特定形貌和结构的光催化材料的理想自牺牲模板.同时，有机配体易于在高温煅烧过程中从MOFs骨架中释放，其衍生物往往会继承MOFs的多孔性特征，有利于光催化反应中间体的传输与释放.
本文采用MIL-125（Ti）作为前驱体，三聚氰胺作为氮源，通过在空气氛围下高温煅烧（温度分别为500，600和700℃）的方法制备了一系列具有可见光光催化活性的圆盘状介孔锐钛矿-金红石混合晶型的N-TiO₂（分别标记为MM-500，MM-600和MM-700）.采用粉末X射线衍射（PXRD）、傅里叶变换红外光谱（FTIR）、扫描电子显微镜（SEM）、透射电子显微镜（TEM）、选区电子衍射（SAED）、X射线光电子能谱（XPS）、紫外-可见漫反射光谱（UV-vis DRS）和BET比表面积分析等对MM-500，MM-600和MM-700的形貌、组成及结构进行了表征.选取气态苯作为目标VOCs污染物探究了MM-500的光催化性能.
结果表明，随着煅烧温度的提高，N掺杂含量减少，所制备的光催化剂可见光吸收减弱，锐钛矿相所占比例降低，N-TiO₂晶粒尺寸增大，样品比表面积随之减少.由于MM-500优异的可见光吸收能力和传质能力，其对气态苯表现出优异的光催化降解性能.可见光照射480min后，MM-500对气态苯的去除效率高达99.1%，矿化率达到72.0%，均优于商业化二氧化钛（P-25）.循环实验表明MM-500具有较好的稳定性和重复利用性，10次光催化实验后，其对苯的去除效率仍达到84.8%.同时，电子顺磁共振（ESR）证明超氧自由基（^·O₂^-）与羟基自由基（^·OH）是苯光催化氧化过程中的主要活性氧物种.综上，本文以MIL-125（Ti）为前驱体所制备的N-TiO₂能高效光催化去除气态苯污染物.

关键词: 金属-有机骨架, N-二氧化钛, 可见光, 光催化氧化, 气态苯

Abstract: N-doped anatase-rutile titanium dioxide (N-TiO₂) is a classical semiconductor widely used in environmental remediation. Its photocatalytic performance is typically affected by its morphology, porous structure, and phase composition. Herein, disk-like mesoporous N-TiO₂ was prepared by calcining MIL-125(Ti) and melamine matrix at different temperatures in air. The photocatalytic efficiency of the prepared mesoporous N-TiO₂ for the photo-oxidation of gaseous benzene under visible-light irradiation was studied. With respect to light absorption and mass transfer, as-prepared N-TiO₂ annealed at 500℃ (MM-500) showed the best photocatalytic activity with corresponding photodegradation and mineralization efficiencies of 99.1% and 72.0%, respectively. In addition, MM-500 exhibited excellent reusability and stability in cyclic experiments, in which 84.8% of gaseous benzene could still be photodegraded after 10 experimental cycles. Furthermore, electron spin resonance analysis indicated that ^·OH and ^·O₂^- radicals were the dominating reactive oxygen species during the photo-oxidation process. Their excellent performance suggests that the as-prepared N-TiO₂ photocatalysts can be used to eliminate volatile organic compounds.

Key words: Metal-organic framework, N-TiO₂, Visible light, Photocatalytic oxidation, Gaseous benzene

赵晨, 王志华, 陈肸, 楚弘宇, 付会芬, 王崇臣. MIL-125(Ti)衍生介孔圆盘状N-TiO₂高效光催化降解气态苯[J]. 催化学报, 2020, 41(8): 1186-1197.

Chen Zhao, Zhihua Wang, Xi Chen, Hongyu Chu, Huifen Fu, Chong-Chen Wang. Robust photocatalytic benzene degradation using mesoporous disk-like N-TiO₂ derived from MIL-125(Ti)[J]. Chinese Journal of Catalysis, 2020, 41(8): 1186-1197.

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MIL-125(Ti)衍生介孔圆盘状N-TiO₂高效光催化降解气态苯

Robust photocatalytic benzene degradation using mesoporous disk-like N-TiO₂ derived from MIL-125(Ti)

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