Interfacial Dynamics of Novel Nanostructured Perovskite Electrodes

替代能源的生产和储存是可持续清洁能源技术发展的主要挑战之一。结合太阳能和燃料电池技术的电化学能量转换为发电/储存问题提供了一个解决方案。在这种方法中，太阳的能量可以用来驱动丰富的化学反应物（水、二氧化碳）转化为能量密集的燃料（氢、碳氢化合物），这些燃料随后可以被消耗来发电。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）电催化剂表面与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需要的副产物，从而大大降低效率和选择性。迄今为止，选择性促进关键（光）电催化反应的大多数活性材料都需要使用昂贵的贵金属及其合金或氧化物。实际上，这严重限制了大规模采用，并突出了迫切需要基于地球丰度元素创造新的高活性和选择性电催化剂。特别是钙钛矿结构，它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，并激发了我们的长期研究目标：s

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 s