Enhanced water splitting activity through flame made heterojunctions of doped and functionalized mixed metal oxide nanoparticles predicted by combinatorial computational materials design

我们建议开发由无毒金属氧化物材料制成的光解电池，其带边经过优化，可以收集大部分太阳光谱，从而提高效率。我们通过将现代生产技术与组合计算材料设计相结合来实现这一目标：两种或多种金属氧化物纳米颗粒的异质结将使用我们新型的双火焰喷雾热解装置来生产，在该装置中，将合成具有特定性能（高稳定性和均匀性，低溶解度和优化带结构）的纯，掺杂和混合（即固溶体）金属氧化物纳米颗粒。在新概念中，基于第一性原理（密度泛函理论）计算，通过组合计算技术预测了性能最佳的（混合）金属氧化物材料的组成，该技术允许筛选大量候选系统。新粒子将使用实验-理论相结合的方法进行全面表征，包括XRD， （HR）TEM， XANES和EELS的测量和模拟。我们将继续进行电极沉积和实际生活测试，并计划在第二个资助期内采取措施减少过电位，并将继续制造设备。

We propose to develop photoelectrolysis cells made of non-toxic metal oxide materials with optimized band edges to allow harvesting a large fraction of the solar spectrum and hence a high efficiency. We pursue this goal by combining a modern production technique with combinatorial computational materials design: heterojunctions of two or more metal oxide nanoparticles will be produced using our novel double flame spray pyrolysis apparatus, where pure, doped and mixed (that is, solid solutions) metal oxide nanoparticles with tailored properties (high stability and homogeneity, low solubility and optimized band structure) will be synthesized. The compositions of the best-performing (mixed) metal oxide materials are predicted by combinatorial computational techniques on the basis of first principles (density-functional theory) calculations in a new concept that allows screening a large manifold of candidate systems. The new particles will be thoroughly characterized using a combined experimental-theoretical approach that involves measurement and simulation of XRD, (HR)TEM, XANES and EELS. Electrode deposition and real life tests will be pursued, and we plan for the 2nd funding period measures to reduce the overpotential and will proceed to build devices.