Alkane upgrading by metal metal-modified zeolites

开发能够直接有效地将丰富的烃资源转化为更高价值产品的催化材料仍然是学术和工业研究的主要目标。特别地，开发利用甲烷作为碳源来升级其它烃流的路线是一个机会，以使这种极其便宜和丰富的原料价值化，避免通过合成气的能量密集型生产利用甲烷。沸石由于其具有成本效益的性质、鲁棒性和它们表现出的通常高的反应选择性而被广泛用作炼油厂和石油化工加工中的催化剂。（顶部。目录号：2009，52，1131）最近的研究表明，金属改性的沸石能够在温和条件下活化甲烷，并且所得物质可以与其他小分子进行后续反应以形成增值产品。(ACS目录号：2016年6月2965日）该项目的目的是开发催化工艺，用于将甲烷和其他碳氢化合物同时转化为高级化学产品。将探索支持在工业相关沸石框架上的目标主族和过渡金属，以及金属掺入的不同方法，以改善催化功能并开发结构功能模型。活性部位分布将通过合成方法，如选择性离子交换和有机金属接枝量身定制。将通过光谱技术（例如固态NMR和DRIFTS）筛选材料的烷烃活化，然后与乙烯、丙烯和甲苯等小分子进行反应。催化试验将在运行DRIFTS设施和安装在组内的流动反应器（例如FlowCat）上进行。反应机制将通过使用同位素标记研究来确定。

The development of catalytic materials that can directly and efficiently convert abundant hydrocarbon resources to higher value products remains a major goal of academic and industrial research. In particular, developing routes that utilise methane as a source of carbon to upgrade other hydrocarbon streams is an opportunity to valorise this extremely cheap and abundant feedstock avoiding methane utilisation via the energy intensive production of synthesis gas.Zeolites are widely used as catalysts in refinery and petrochemical processing due to their cost effective nature, robustness and the generally high reaction selectivities they exhibit. (Top. Catal., 2009, 52, 1131) Recent research has shown that metal-modified zeolites are able to activate methane under moderate conditions and that the resulting species can undergo subsequent reactions with other small molecules to form value added products.(ACS Catal., 2016, 6, 2965) The aim of this project is to develop catalytic processes for the simultaneous conversion of methane and other hydrocarbons to higher chemical products. Targeted main group and transition metals, supported on industrially relevant zeolite frameworks will be explored, as will different methods of metal incorporation in order to improve the catalytic functionality and develop structure function models. Active site distributions will be tailored through synthetic methodologies such as selective ion exchange and organometallic grafting. Materials will be screened for alkane activation through spectroscopic techniques (e.g. solid state NMR and DRIFTS), followed by reactivity with small molecules such as ethylene, propylene, and toluene. Catalytic testing will be conducted on an operando DRIFTS facility and on flow reactors (e.g. FlowCat) housed within the group. The mechanisms of reaction will be determined through the use of isotope labelling studies.