Prototyping of catalyst pore-systems by a combined synthetic, analytical and computational approach: Application to mesoporous TiO2
Prototyping of catalyst pore-systems by a combined synthetic, analytical and computational approach: Application to mesoporous TiO2
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DOI：
10.1016/j.cej.2014.02.004
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发表时间：
2014-07
影响因子：
15.1
通讯作者：
V. Novák;E. Ortel;B. Winter;B. Butz;B. Paul;P. Kočí;M. Marek;E. Spiecker;R. Kraehnert
中科院分区：
文献类型：
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作者：
V. Novák;E. Ortel;B. Winter;B. Butz;B. Paul;P. Kočí;M. Marek;E. Spiecker;R. Kraehnert
在过去的十年中，表面反应的量子化学计算已经成为催化位点设计的基础。然而，允许优化催化剂载体的适当孔结构的相应方法迄今尚未达到相同的复杂程度。这尤其适用于现实的孔隙系统，可以实际合成一个合理的effort.We提出了一个战略，使虚拟原型和计算优化的固体催化剂的孔隙系统。该方法结合了具有可调孔隙空间形态的多孔金属氧化物的模板辅助合成、通过HAADF STEM模式下的现有技术电子断层扫描对催化剂纳米结构的3D成像以及提供孔径分布的计算评估的多尺度数学建模，在重构系统中的有效扩散率和弯曲度以及催化层在反应物转化方面的宏观性能。这种一般的方法是证明介孔TiO2层。
During the last decade, quantum-chemical calculations of surface reactions have become well established for the design of catalytic sites. However, the corresponding methods allowing optimization of adequate pore structures for catalyst supports have so far not reached the same level of sophistication. This holds in particular for realistic pore systems that can be practically synthesized with a reasonable effort.We propose a strategy that enables virtual prototyping and computational optimization of the pore system of a solid catalyst. The method combines template-assisted synthesis of porous metal oxides with tunable pore-space morphology, 3D imaging of the catalysts nanostructure by the state-of-the-art electron tomography in HAADF STEM mode, and multi-scale mathematical modeling that provides computational evaluation of the pore size distribution, effective diffusivity and tortuosity in the reconstructed system as well as macroscopic performance of the catalytic layer in terms of reactant conversion. This general approach is demonstrated on mesoporous TiO2layers.