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电解电池，其具有优化的带边，以允许收集大部分太阳光谱，从而获得高效率。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：将使用我们的新型双火焰喷雾热解装置生产两种或更多种金属氧化物纳米颗粒的异质结，其中将合成具有定制特性（高稳定性和均匀性，低溶解度和优化能带结构）的纯，掺杂和混合（即固溶体）金属氧化物纳米颗粒。最佳性能的（混合）金属氧化物材料的组合物预测的第一原理（密度泛函理论）计算的基础上，在一个新的概念，允许筛选一个大的多方面的候选系统的组合计算技术。新颗粒将使用实验-理论相结合的方法进行彻底表征，该方法涉及XRD，（HR）TEM，XANES和EELS的测量和模拟。将进行电极沉积和真实的寿命测试，我们计划在第二个资助期采取措施来降低过电位，并将继续建造设备。

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.