RESUMO
Charge transport in nanoparticle-based materials underlies many emerging energy-conversion technologies, yet assessing the impact of nanometre-scale structure on charge transport across micrometre-scale distances remains a challenge. Here we develop an approach for correlating the spatial distribution of crystalline and current-carrying domains in entire nanoparticle aggregates. We apply this approach to nanoparticle-based α-Fe2O3 electrodes that are of interest in solar-to-hydrogen energy conversion. In correlating structure and charge transport with nanometre resolution across micrometre-scale distances, we have identified the existence of champion nanoparticle aggregates that are most responsible for the high photoelectrochemical activity of the present electrodes. Indeed, when electrodes are fabricated with a high proportion of these champion nanostructures, the electrodes achieve the highest photocurrent of any metal oxide photoanode for photoelectrochemical water-splitting under 100 mW cm(-2) air mass 1.5 global sunlight.
Assuntos
Modelos Teóricos , Nanoestruturas/química , Eletrodos , Microscopia de Força Atômica , Microscopia Eletrônica de Varredura , Processos Fotoquímicos , Energia Solar , Propriedades de Superfície , Água/químicaRESUMO
LaTiO(2)N photoanodes for solar water splitting were prepared by electrophoretic deposition and demonstrated the best photocurrents ever reported for this material. Further important enhancement of the performance was obtained by the use of a sputtered In(2)O(3) overlayer.