Atomic layer deposited Pt/TiO2-SiO2 and Pt/ZrO2-SiO2 for sequential adsorption and oxidation of VOCs
Atomic layer deposited Pt/TiO2-SiO2 and Pt/ZrO2-SiO2 for sequential adsorption and oxidation of VOCs
复制标题
原子层沉积 Pt/TiO2-SiO2 和 Pt/ZrO2-SiO2，用于连续吸附和氧化 VOC
DOI：
10.1016/j.cej.2022.136603
复制
发表时间：
2022
影响因子：
15.1
通讯作者：
Rezaei, Fateme
中科院分区：
文献类型：
--
作者：
Adebayo, Busuyi O.;Yu, Han;Rownaghi, Ali A.;Liang, Xinhua;Rezaei, Fateme
在这项工作中，Pt纳米粒子负载在SiO2，TiO 2-薄膜改性的SiO2（TiO 2-SiO2），或ZrO 2-薄膜改性的SiO2（ZrO 2-SiO2）颗粒和复合材料的顺序吸附和脱附/催化氧化苯进行了研究。采用溶胶-凝胶法制备SiO2，采用原子层沉积法在SiO2颗粒表面包覆TiO 2或ZrO 2薄膜，制备了TiO 2-SiO2和ZrO 2-SiO2。在顺序捕获反应试验中，材料首先暴露于ca。在25 °C和1个大气压下，500 ppmv苯气体，直到达到5%穿透，然后串联解吸和催化氧化，同时将床温升高至200 °C。苯蒸气的吸附等温线符合IV型等温线分类，揭示了单层，多层和毛细管凝聚吸附机制的顺序组合。与xPt/TiO 2-SiO2相比，xPt/ZrO 2-SiO2材料具有上级的捕获-转换能力。其中，经3次Pt ALD制备的3 Pt/ZrO 2-SiO2的最大原位转化率为100%，转化频率为17.1 mmolC 6 H6/molPt/s，动态吸附容量为0.45 mmol/g，表明Pt纳米颗粒和ZrO 2在ALD基双功能材料中具有协同效应。
In this work, Pt nanoparticles were loaded on SiO2, TiO2-thin-film-modified SiO2(TiO2-SiO2), or ZrO2-thin-film-modified SiO2(ZrO2-SiO2) particles and the composites were investigated for sequential adsorption and desorption/catalytic oxidation of benzene. The SiO2was prepared via sol–gel method, while TiO2-SiO2and ZrO2-SiO2were synthesized via atomic layer deposition (ALD) thin film coating of TiO2or ZrO2on SiO2particles substrate. In the sequential capture-reaction tests, the materials were first exposed to ca. 500 ppmvbenzene gas at 25 °C and 1 atm until 5% breakthrough was attained, followed by tandem desorption and catalytic oxidation while raising bed temperature to 200 °C. The benzene vapor adsorption isotherms followed type-IV isotherm classification, revealing a combination of monolayer, multilayer and capillary condensation adsorption mechanisms in sequence. ThexPt/ZrO2-SiO2materials exhibited superior capture-conversion capabilities relative to theirxPt/TiO2-SiO2. In particular, 3Pt/ZrO2-SiO2, prepared with 3 cycles of Pt ALD, exhibited the maximumin-situconversion at ∼ 100% and turnover frequency of 17.1 mmolC6H6/molPt/s with a dynamic adsorption capacity of 0.45 mmol/g, indicating synergistic effects of Pt nanoparticles and ZrO2in the ALD-based dual-function materials.