Designed Synthesis of Zeolites for Environmental and Biorenewables Catalysis

在英国工业中，多相催化在商品和精细化学品的合成、燃料和环境保护方面发挥着重要作用，铝硅酸盐沸石是炼油和石化以及汽车排放控制中许多重要反应的首选催化剂。在工业固体催化剂中独一无二的是，它们的性能直接与它们的体晶体结构有关，通过它们的孔结构和活性位点的化学结构的重要细节，但是新材料的合成基本上依赖于反复试验的方法。我们的研究假设是，现在已经对沸石的合成及其作为催化剂的作用有了足够的了解，可以为选择的扩展催化技术计划和执行新型活性非均相催化剂的制备。这个雄心勃勃的研究项目涵盖了沸石催化剂的结构设计、水热合成和催化性能测试。晶体学、原子模型和原位光谱方法将有助于预测和阐明目标沸石的结晶和催化机制的细节。该计划将建立在我们最近在假设沸石结构的设计和新型沸石的目标制备方面的进展，以及沸石制备及其催化反应的固态核磁共振，拉曼和x射线光谱的原位监测。这些反应对于含氧化合物生成碳氢化合物和用氨选择性催化还原不需要的氮氧化物（SCR）是重要的。设计的新沸石合成将针对假设的框架，在计算筛选下，显示出SCR或氧合物转化为碳氢化合物的希望。最初的研究将开发“逆向合成”、以建模为主导的方法来模板化这些结构，而扩展的研究将旨在扩展这些结构，以设计可升级的、商业上可行的方法。这项工作将与英国领先的商业催化剂公司密切合作，不仅将制备具有性能和可专利性潜在优势的新型催化剂，而且还将开发一种完全连接的方法，用于合成嵌入计算和原位实验框架的新催化剂，用于研究结构和催化功能之间的关系。

Heterogeneous catalysis plays a major role in the synthesis of commodity and fine chemicals, fuels and environmental protection for UK industry and aluminosilicate zeolites are the catalysts of choice for many important reactions in oil refining and petrochemical and automobile emission control. Uniquely among industrial solid catalysts, their performance is directly related to their bulk crystal structure, via important details of their pore structure and the chemical structure of their active sites, but synthesis of new materials has by and large relied on trial-and-error approaches. Our research hypothesis is that enough is now known about the synthesis of zeolites and their action as catalysts to plan and execute the preparation of novel active heterogeneous catalysts for selected expanding catalytic technologies.This ambitious research program spans structural design, hydrothermal synthesis and catalytic performance testing of zeolite catalysts. It will be facilitated by crystallography, atomistic modelling and in situ spectroscopic methods to predict and elucidate details of the mechanisms of crystallisation and of catalysis over targeted zeolites. The program will build on our recent advances in the design of hypothetical zeolite structures and the targeted preparation of novel zeolites, and in the in situ monitoring by solid state NMR, Raman and X-ray spectroscopies of zeolite preparation and of their catalytic reactions. These reactions are important for hydrocarbon generation from oxygenates and for the selective catalytic reduction (SCR) of unwanted nitrogen oxides with ammonia. The designed synthesis of new zeolites will target hypothetical frameworks that, under computational screening, show promise for SCR or for oxygenates-to-hydrocarbons. Initial studies will develop 'retrosynthetic', modelling-led, approaches to templating these structures, while extended studies will aim to extend these to devise upscalable, commercially viable approaches.The work will be performed in close collaboration with the UK's leading commercial catalyst company and will not only prepare novel catalysts with potential advantages of performance and patentability over current materials, but will also develop a fully-connected methodology for the synthesis of new catalysts embedded in a computational and in situ experimental framework for the study of the relationship between structure and catalytic function.