Interfacial Dynamics of Novel Nanostructured Perovskite Electrodes

替代能源的产生和储存是发展可持续清洁能源技术的主要挑战之一。采用太阳能和燃料电池技术相结合的电化学能量转换技术为发电/储存问题提供了解决方案。在这种方法中，太阳的能量可以被用来驱动丰富的化学反应物(水、二氧化碳)转化为能量密集型燃料(氢、碳氢化合物)，这些燃料随后可以被用来发电。化学燃料的高效电催化生成和转化需要多个质子和电子的协同转移，并且强烈依赖于(光)电催化剂表面和靶分子之间的相互作用。由于这种表面敏感性，可能会无意中产生不想要的副产物，从而大大降低效率和选择性。到目前为止，选择性促进关键(光)电催化反应的最活跃的材料需要使用昂贵的贵金属及其合金或氧化物。实际上，这严重限制了广泛的采用，并突出了基于地球丰富的元素创造新的高活性和选择性的电催化剂的迫切需要。特别是，钙钛矿型结构可以容纳元素周期表中的大多数元素，为材料设计和合成提供了巨大的机会，并推动了我们的长期研究目标：合成和发现高活性和选择性的钙钛矿型(光)电催化剂纳米材料。 实现我们长期目标的核心是了解纳米级结构(晶相/取向、组成、形态)如何影响反应性。直到最近才有可能探索单个纳米材料的电化学来进行结构-活性相关性研究，这为材料设计和功能提供了巨大的洞察力。我们研究计划的学生将接受有关纳米级电化学最新创新的培训，以高通量方法在定义良好的微电极和纳米级电极上进行详细的结构-活性研究，以定量确定关键的动力学参数和反应路径，与互补的高分辨率结构表征技术相结合，将使我们能够揭示纳米级结构对活性和选择性的潜在作用。通过我们的基础研究，我们将寻求发现新材料，作为全球创新能源发电技术的一部分，这些技术可以为加拿大提供环境和经济利益。

The generation and storage of alternative energy sources is one of the major challenges in the development of sustainable clean energy technologies. Electrochemical energy conversion using a combination of solar and fuel cell technology offers a solution to the generation/storage problem. In this approach the sun’s energy can be used to drive the conversion of abundant chemical reactants (water, carbon dioxide) into energy dense fuels (hydrogen, hydrocarbons) that can subsequently be consumed to generate electricity. The efficient electrocatalytic generation and conversion of chemical fuels requires the concerted transfer of multiple protons and electrons, and depends strongly on the interaction between the (photo)electrocatalyst surface and target molecules. As a result of this surface sensitivity, unwanted by-products may be unintentionally generated that greatly reduce efficiency and selectivity. To date the most active materials that selectivity promote key (photo)electrocatalytic reactions require the use of expensive precious metals and their alloys or oxides. Practically, this severely limits wide scale adoption, and highlights an imperative need to create new highly active and selective electrocatalysts based on earth abundant elements. In particular, the perovskite structure, which can accommodate the majority of the elements in the periodic table, offers tremendous opportunity for materials design and synthesis, and motivates our long-term research objective: the synthesis and discovery of highly active and selective perovskite (photo)electrocatalyst nanomaterials. Central to the realization of our long term goal is an understanding of how nanoscale structure (crystal phase/orientation, composition, morphology) impacts reactivity. It has only recently become possible to explore the electrochemistry of individual nanomaterials for structure-activity correlation studies, which offer tremendous insight into materials design and function. Students in our research program will receive training in the most recent innovations in nanoscale electrochemistry to carry out detailed structure-activity investigations, in a high-throughput approach to screen a number of materials parameters, at well-defined micro- and nanoscale electrodes for the quantitative determination of key kinetic parameters and reaction pathways, which, when combined with complementary high-resolution structural characterization techniques will allow us to reveal the underlying role that nanoscale structure has on activity and selectivity. Through our fundamental studies we will seek to discover new materials as part of a larger global effort towards innovative energy generation technologies that can provide environmental and economic benefit to Canada.