Multicomponent Nitride/High-Entropy Alloy Heterostructures as Highly Active and Stable Electrocatalysts for Ampere-Level Water Oxidation
Corresponding Author: Qing Jiang
Nano-Micro Letters,
Vol. 19 (2027), Article Number: 46
Abstract
Developing highly active and stable oxygen evolution reaction catalysts is paramount for cost-effective large-scale green hydrogen production via water electrolysis. Here we report nonprecious metal-based multicomponent nitride/high-entropy alloy heterostructures as cost-effective electrocatalysts to efficiently mediate alkaline water oxidation by in-situ configurating cooperative Brønsted basic oxyanion-solid interfaces during phase transformation of multicomponent nitride into amorphous N-doped NiFeCoMoCrOOH along with partial dissolution of high-value metals of Mo and Cr to form molecular MoO42− and CrO42− species. The protonation of Brønsted basic oxyanions facilitates the critical *OOH intermediate formation on N-doped NiFeCoMoCrOOH with near-optimal adsorption energy, substantially accelerating the oxygen evolution reaction kinetics. Consequently, the heterostructure electrode exhibits superior oxygen evolution reaction electrocatalysis in 1 M KOH solution, delivering ultrahigh current density of ~ 2.5 A cm−2 at low overpotential of 300 mV. Its alkaline water electrolyzer operates stably at ampere-level current density for > 1700 h. Our findings reveal an unconventional molecule-assisted multi-site mechanism of multicomponent catalysts to accelerate multiple-intermediate reaction.
Highlights:
1 Nonprecious metal-based multicomponent nitride anchored on nanoporous high-entropy alloy skeleton is constructed for ampere-level water oxidation via in-situ configurating cooperative Brønsted basic oxyanion-solid multiple active interfaces.
2 The self-supported nanoporous (NiFeCo)3(MoCr)3N/HEA electrodes exhibit exceptional catalytic activity and durability by virtue of MoO42− and CrO42− ions acting as molecular co-catalysts to mediate proton spillover to facilitate the formation of *OOH.
3 The alkaline water electrolyzer assembled with nanoporous (NiFeCo)3(MoCr)3N/HEA anode and (MoCr)(NiFeCo)4/HEA cathode can operate stably at ampere-level current density for over 1700 h.
Keywords
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