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Binary nanoparticle superlattices (BNSLs) comprised of polymer-grafted shaped nanoparticles enable the construction of new isotropic mesomaterial. 

Correction for ‘Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen’ by Yihuang Xionget al.,Energy Environ. Sci., 2021,14, 2335–2348; DOI: 10.1039/D0EE02984J. 

Abstract Catalytic interface of semiconductor photoelectrodes is critical for high-performance photoelectrochemical solar water splitting because of its multiple roles in light absorption, electrocatalysis, and corrosion protection. Nevertheless, simultaneously optimizing each of these processes represents a materials conundrum owing to conflicting requirements of materials attributes at the electrode surface. Here we show an approach that can circumvent these challenges by collaboratively exploiting corrosion-resistant surface stoichiometry and structurally-tailored reactive interface. Nanoporous, density-graded surface of ‘black’ gallium indium phosphide (GaInP₂), when combined with ammonium-sulfide-based surface passivation, effectively reduces reflection and surface recombination of photogenerated carriers for high efficiency photocatalysis in the hydrogen evolution half-reaction, but also augments electrochemical durability with lifetime over 124 h via strongly suppressed kinetics of corrosion. Such synergistic control of stoichiometry and structure at the reactive interface provides a practical pathway to concurrently enhance efficiency and durability of semiconductor photoelectrodes without solely relying on the development of new protective materials. 

The production of hydrogen fuels, via water splitting, is of practical relevance for meeting global energy needs and mitigating the environmental consequences of fossil-fuel-based transportation. Water photoelectrolysis has been proposed as a viable approach for generating hydrogen, provided that stable and inexpensive photocatalysts with conversion efficiencies over 10% can be discovered, synthesized at scale, and successfully deployed (Pinaud et al. , Energy Environ. Sci. , 2013, 6 , 1983). While a number of first-principles studies have focused on the data-driven discovery of photocatalysts, in the absence of systematic experimental validation, the success rate of these predictions may be limited. We address this problem by developing a screening procedure with co-validation between experiment and theory to expedite the synthesis, characterization, and testing of the computationally predicted, most desirable materials. Starting with 70 150 compounds in the Materials Project database, the proposed protocol yielded 71 candidate photocatalysts, 11 of which were synthesized as single-phase materials. Experiments confirmed hydrogen generation and favorable band alignment for 6 of the 11 compounds, with the most promising ones belonging to the families of alkali and alkaline-earth indates and orthoplumbates. This study shows the accuracy of a nonempirical, Hubbard-corrected density-functional theory method to predict band gaps and band offsets at a fraction of the computational cost of hybrid functionals, and outlines an effective strategy to identify photocatalysts for solar hydrogen generation.