Sustainable fuel production through earth abundant catalysts

传统的碳基化石燃料燃烧目前提供了全球80%以上的能源需求。然而，这一过程产生了氧化副产品，如与全球变暖密切相关的温室气体。这一点，加上不断增长的全球人口，推动了无碳替代燃料生产的研究领域。替代燃料的一个例子是分子氢(H2)，它在燃烧时产生环境友好的水(H2O)作为唯一的产品，使H2成为未来有吸引力的替代燃料。目前最先进的氢气生产技术使用稀有的、因此昂贵的金属，如铂，这在经济上是不可取的。具有成本效益的氢气生产将是其广泛工业应用的关键。此外，将二氧化碳化学还原为可重复使用的燃料仍然是一个有吸引力的途径，可以结束化石燃料燃烧的人为循环。*本提案概述了我的研究计划的总体目标，该计划将支持12名本科生和2名理科硕士。在接下来的5年里，学生们将专注于开发廉价、水稳定的过渡金属催化剂来生产氢气。从水中制取氢气可以分为两个反应：水的氧化和质子(H+)的还原。这两个反应的中心是H+向金属活性中心和从金属活性中心的转移。因此，关键的催化剂设计包括将H+穿梭功能连接到目标配体支架上，与没有这些功能的催化剂相比，这有望表现出更快的反应速度。模块化配体合成允许对目标化合物进行微妙的结构和电子调节，以揭示在电催化和光催化条件下的最佳催化性能。这些项目中研究的催化剂也可以用于二氧化碳还原，它们的共价固定在固体电极上将产生多相催化剂。这些未来的方向将为我的研究计划带来令人兴奋的新维度，可能导致多相催化普遍存在的行业合作。*通过这些项目，学生将获得HQP培训，内容包括现代合成技术、分子过渡金属络合物及其共价固定化化合物的光谱表征和催化评估。我完全期待从我的实验室毕业的学生具备在学术界或工业界、在加拿大或世界各地成功从事科学事业所需的知识和技能。

Conventional carbon-based fossil fuel combustion currently supplies over 80% of the global energy demand. However, this process yields oxidized byproducts such as greenhouse gases that have been heavily linked to global warming. This, along with the ever-growing global population, has driven the research field of carbon-free alternative fuels production. One example of an alternative fuel is molecular hydrogen (H2), which produces environmentally benign water (H2O) as the sole product upon combustion, making H2 an attractive alternative fuel of the future. Current state-of-the-art technologies for H2 production uses scarce, and thus expensive, metals such as platinum, which is economically undesirable. The cost effective production of H2 will be key to its widespread use industrially. In addition, the chemical reduction of CO2 into reusable fuels remains an attractive route of closing the anthropogenic cycle from fossil fuel combustion.******This proposal outlines the overarching goals of my research program, which will support 12 undergraduate and 2 M.Sc. students over the next 5 years, focusing on the development of inexpensive, water stable transition metal catalysts for H2 production. The production of H2 from H2O can be split into two reaction: H2O oxidation and proton (H+) reduction. Central to both reactions is the transport of H+ to and from the metal active site. Thus, the key catalyst design involves attaching H+ shuttling functionalities onto target ligand scaffolds, which is envisaged to exhibit accelerated reaction rates in comparison to catalysts without these functionalities. Modular ligand syntheses allow for subtle structural and electronic tuning of target complexes to reveal optimal catalytic properties under both electrocatalytic and photocatalytic conditions. Catalysts investigated in these projects can also be put towards CO2 reduction, and their covalent immobilization onto solid electrodes will yield heterogeneous catalysts. These future directions will introduce exciting new dimensions into my research program, potentially leading to industrial collaborations where heterogeneous catalysis is commonplace. ******Through these projects, students will gain HQP training in modern synthetic techniques, spectroscopic characterization and catalytic evaluations of molecular transition metal complexes and their covalently immobilized counterparts. I fully expect students graduating from my laboratory to be well-equipped with knowledge and skills necessary for a successful scientific career in both academia or industry, in Canada or worldwide.