Electron-Rich Nickel Enabled by Charge Transfer in Multimetal Nanostructures for Efficient Ammonia-to-Hydrogen Conversion.

Authors

Donghyeok Kim, Su-Jin Kim, Gayeong Kim, Hyoseok Kim, Jongkyoung Kim, Myeung-Jin Lee, Bora Jeong, Minkyu Kim, Hong-Dae Kim, Seungho Cho

Published in

Advanced science (Weinheim, Baden-Wurttemberg, Germany). Pages e78184. Oct 06, 2026. Epub Oct 06, 2026.

Abstract

Achieving noble-metal-like reactivity in earth-abundant catalysts requires materials platforms that can simultaneously stabilize active sites and program their electronic states. Ammonia-to-hydrogen conversion is a demanding example, because Ru-free catalysts must overcome the intrinsically sluggish kinetics of ammonia decomposition. Here, we report a catalyst design that couples precursor-level cation mixing and active-site dispersion with charge-transfer engineering of Ni to address this challenge. Density functional theory calculations identify Cr as the most effective electron-donating promoter for Ni among metal cations incorporable into the precursor framework. Guided by this prediction, we construct a NiCrAl reduced mixed-metal oxide catalyst in which atomically mixed precursors stabilize highly dispersed Ni species, while Cr-to-Ni charge transfer generates electron-rich Ni active sites. Multiscale spectroscopic analyses verify this electronic modulation, and combined theoretical and in situ mechanistic analyses indicate that electron-rich Ni favors NH₃ adsorption in a reaction-relevant Lewis-acid configuration, favorably modifies the dehydrogenation energetics, and weakens N₂ binding to facilitate product desorption. NiCrAl-RMMO reaches 95.5% NH₃ conversion at 550°C and 22.83 mmol H₂ g_cat ^-1 min^-1 at 500°C, with stable operation over 100 h. More broadly, this work establishes charge-transfer engineering in LDH-derived mixed-metal nanostructures as a general strategy for designing high-performance, Ru-free catalysts for ammonia-to-hydrogen conversion.

PMID:
42839588
Bibliographic data and abstract were imported from PubMed on 07 Oct 2026.

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