Au-decorated NdFeO3/g-C3N4 type II heterojunction photoanodes for enhanced hydrogen evolution: Integrated computational and experimental insights

The rational design of efficient visible-light-driven photocatalysts remains a challenge for sustainable hydrogen production. Herein, we present a combined computational and experimental study on NdFeO 3 /g-C 3 N 4 heterojunctions, determined through a systematic screening of perovskite/2D‐material combinations. From a pool of eleven theoretically promising heterojunctions, NdFeO 3 /g-C 3 N 4 type-II heterojunction was selected for in-depth analysis due to its favorable band alignment and anticipated charge separation properties. Both pristine and Au-decorated NdFeO 3 /g-C 3 N 4 composites were synthesized and thoroughly characterized using various analytical tools. Our results reveal that the heterojunction exhibits an internal electric field at the interface, which suppresses charge carrier recombination. The incorporation of Au nanoparticles introduces ohmic contacts that drastically reduce the interfacial electron transfer resistance, thereby enhancing charge extraction efficiency. Photoelectrocatalytic measurements under standard AM1.5G solar illumination reveal a remarkable enhancement in hydrogen evolution activity, an 18-fold increase of hydrogen production is recorded for the Au(NFO 0.9 /g-CN 0.1 ) composite relative to bare NdFeO 3 . These findings underscore the potential of integrating high-throughput computational screening with targeted synthesis to accelerate the rational design of next-generation type-II photocatalysts for solar-driven hydrogen generation. • Python workflow identified promising perovskite/2D type-II heterojunctions. • Synthesis confirmed type-II alignment in NdFeO 3 /g-C 3 N 4 composite. • NdFeO 3 /g-C 3 N 4 showed reduced recombination and higher photocurrent density. • Au–decorated composite reached ∼3.9 % efficiency and 18 × H 2 yield vs. bare NFO. • Combined computation and experiments accelerate visible-light photocatalyst design.