Scalable synthesis of wrinkled mesoporous titania microspheres with uniform large micron sizes for efficient removal of Cr(VI)
Scalable synthesis of wrinkled mesoporous titania microspheres with uniform large micron sizes for efficient removal of Cr(VI)
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可大规模合成具有均匀大微米尺寸的皱纹介孔二氧化钛微球，用于有效去除 Cr(VI)
DOI：
10.1039/c8ta00488a
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发表时间：
2018-02
影响因子：
11.9
通讯作者：
Zhao Dongyuan
中科院分区：
文献类型：
--
作者：
Yu Zhikai;Gao Xingmin;Yao Yan;Zhang Xiangcheng;Bian Guo-Qing;Wu Winston Duo;Chen Xiao Dong;Li Wei;Selomulya Cordelia;Wu Zhangxiong;Zhao Dongyuan
气溶胶辅助法具有较强的合成二氧化钛微球的能力。对于动态分离应用，需要具有均匀大微米尺寸、高外表面积与体积比、高表面积、均匀介孔和丰富羟基的粗糙TiO2微球。在此，我们展示了蒸发诱导自组装（EISA）与微流体喷射喷雾干燥工艺相结合，在静态和动态条件下可扩展合成具有上述Cr（VI）去除性能的新型介孔TiO2材料。TiO2材料呈球形，具有均匀的大微米尺寸（~ 45 μm）。它们具有褶皱的表面，因此具有很高的颗粒外表面面积与体积比。它们具有高表面积（22-138 m2 g−1）、大孔体积（0.15-0.27 cm3 g−1）和均匀的介孔（5.2-20.7 nm）。由于氧空位和Ti3+价态的存在，它们表面携带大量的Ti-OH基团。几个实验参数，如干燥和煅烧温度的变化，导致TiO2样品具有可调的表面积和介孔大小。它们具有吸附速率快、吸附容量大、吸附ph依赖性强等特点，可作为间歇吸附剂用于水中Cr（VI）的去除。部分吸附的Cr（VI）在酸性溶液中可还原为Cr（III）。研究了吸附剂性能对吸附性能的影响。均匀的大微米尺寸使其成为动态流动中高效分离Cr（VI）的优良填料，其性能与静态条件相似，且易于再生，循环稳定性高。其在流动条件下的吸附性能远优于传统EISA法制备的TiO2纳米颗粒和介孔TiO2材料，因此在实际的动态分离应用中具有很大的吸引力。
Aerosol-assisted methods possess a strong capability for synthesis of titania (TiO2) microspheres. For dynamic separation applications, rough TiO2 microspheres with uniform large micron sizes, high external-surface-area-to-volume ratios, high surface areas, uniform mesopores and abundant hydroxyl groups are desirable. Herein, we demonstrate the combination of evaporation induced self-assembly (EISA) with a microfluidic-jet spray drying process for scalable synthesis of novel mesoporous TiO2 materials with the above-mentioned properties for Cr(VI) removal under both static and dynamic conditions. The TiO2 materials are spherical with uniform large micron sizes (∼45 μm). They possess wrinkled surfaces and thus have high particle external-surface-area-to-volume ratios. They show high surface areas (22–138 m2 g−1), large pore volumes (0.15–0.27 cm3 g−1) and uniform mesopores (5.2–20.7 nm). They carry abundant surface Ti–OH groups due to the presence of oxygen vacancies and the Ti3+ valence state. Several experimental parameters, such as drying and calcination temperatures, are varied, leading to TiO2 samples with tunable surface areas and mesopore sizes. They can be adopted as batch sorbents for removal of Cr(VI) in water with fast adsorption rates, large capacities and pH-dependent adsorption behavior. Part of the adsorbed Cr(VI) can be reduced to Cr(III) in acidic solutions. The influences of adsorbent properties on adsorption performance are elucidated. Moreover, their uniform large micron sizes make them excellent fillers for efficient separation of Cr(VI) in dynamic flows with similar performance to that under static conditions, as well as easy regeneration and high cycling stability. Their adsorption performance under flowing conditions is much better than those of commercial TiO2 nanoparticles and mesoporous TiO2 materials prepared by a conventional EISA method, which make them very attractive for practical dynamic separation applications.
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DOI：
--
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