· 논문명 : Engineering Pt3Ni and Pt3Co Catalysts for High-Performance Methylcyclohexane Dehydrogenation 

               in Liquid Organic Hydrogen Carrier Systems

· 저   자 : Monica Malik, Jin Suk Chung*, Sung Gu Kang*

· 게재지 : Materials Chemistry and Physics (2026, 352, 132013)

· 초록

Liquid organic hydrogen carriers (LOHCs) serve as a powerful solution for efficient hydrogen storage, tackling essential challenges

in advancing the hydrogen economy. Among LOHC systems, the methylcyclohexane/toluene pair has demonstrated industrial 

viability, yet the dehydrogenation process persists as energy-intensive and is significantly dependent on costly platinum-group 

metals. Density functional theory(DFT) computations were done to examine ordered intermetallic Pt3Ni(111), and Pt3Co(111) 

catalysts as alternatives to pure Pt(111), with dual aims of reducing the precious metal loading and enhancing catalytic efficacy. 

Through methodical mapping of the complete six-step MCH dehydrogenation network, we demonstrate that ordered Pt3Ni (111)

consistently diminishes every C–H cleavage barrier relative to Pt(111) while reducing Pt content by 25 %. Furthermore, strategic

surface modification with lithium promoter compresses the kinetic span to 0.37–0.83eV on Pt3Ni(111), significantly expediting

the rate-determining steps. In contrast, the potassium promotion elevates the early-stage barriers (1.1eV) while rendering the

final dehydrogenation step exergonic, illustrating orthogonal control over kinetics and thermodynamics. Biaxial strain engineering

(±3 %) was investigated but demonstrated negligible synergistic effects. Crystal orbital Hamilton population (COHP) analysis

elucidates that the superior performance of Pt3Ni (111) arises from optimal Pt–C and Pt–H bonding interactions, with lithium 

further modulating the electronic structure through charge redistribution. This research highlights essential design guidelines for

future LOHC catalysts that balance performance, selectivity, and the utilization of precious metals, thus promoting the practical 

rollout of hydrogen transport technologies.