Inverse Design of Nanoclusters for Light-Controlled CO2-HCOOHInterconversion

:with global push of hydrogen economy, efficient scenarios for hydrogenstorage, transportation, and generation are indispensable. Here we devise a strategy forcontrollable hydrogen fuel storage and retrieval via light-switched CO2-to-HCOOHinterconversion. To realize it, palladium sulfide nanocluster catalysts with multiple specificfunctionalities are directly searched by our home-developed inverse design approach based ongenetic algorithm (IDOGA) andab initiocalculations. Over 500 low-energy PdxSy(x+y <= 30) clusters are sieved through a multiobjective function combining stability, activity, opticalabsorption, and reduction capability of photocarriers. The structure-property relationshipsand key factors governing the trade-offamong these stringent criteria are disclosed. Finally, 14candidate PdxSyclusters with proper sulfidation degree and high stability in an aqueousenvironment have been screened. Our IDOGA program provides a general approach forinverse search of nanoclusters with any designated elemental compositions and functionalitiesfor any device applications.

Automated summary

This study proposes a strategy for controllable hydrogen fuel storage and retrieval via light-switched CO2-to-HCOOH interconversion. Palladium sulfide nanocluster catalysts with multiple specific functionalities are found through an inverse design approach. The study provides insights into the structure-property relationships and key factors governing the trade-off among various criteria.