In Situ Formation of Ni‐P‐O‐C Interfaces in DLP‐Printed Carbon Microlattices for Efficient Alkaline Hydrogen Evolution

ABSTRACT Architected electrodes that improve catalytic activity, mass transport, and scalability in one system are critical in the progression of alkaline water electrolysis. However, most 3D printed systems require multistep post‐fabrication modifications and consequently, the catalyst is only integrated into surface layers, leading to poor stability. Here, we demonstrate a print‐to‐catalyst approach integrated with nickel and phosphorus precursors directly into digital light processing (DLP) resin that can be used to fabricate programmable Ni–P‐doping porous carbon microlattices for scalable fabrication with in situ processes for the activation of active phases in carbonization. This type of approach incorporates structural and chemical design, where lattice topology is optimized giving minimal transport losses and identifying an X‐Cell geometry with favorable limitations for electrolyte penetration and gas bubble removal, with Ni loading and phosphorus incorporation modulating the electronic structure of Ni to create efficient Ni–P–O–C active interfaces. Comprehensive characterization confirms homogeneous dispersion of Ni, NiO x and Ni–P species embedded in carbon structure to produce catalytically active interfaces. The overpotential of the optimized electrode is 106 mV at 10 mA cm −2 in 1 M KOH, and the electrode's low charge transfer resistance and stable operation for 100 h are also observed.