Engineering Porous-Supported Bimetallic Catalysts for Efficient LOHC Dehydrogenation: From Interfacial Modulation to Sustainable Hydrogen Release

Porous materials play a pivotal role in engineering catalytic systems for efficient and sustainable hydrogen release from Liquid Organic Hydrogen Carriers (LOHCs), a critical vector in clean energy and decarbonization strategies. This review highlights advances in porous-supported catalysts (encompassing γ-/η-Al₂O₃, mesoporous silica, carbon frameworks, and Mg/Al layered oxides) that facilitate precise control over catalyst morphology, metal dispersion, and interfacial chemistry. We examine monometallic (Pt, Pd, Ir) and bimetallic (Pt-Sn, Pt-Pd, Pt-Ir) systems, elucidating how d-band theory, Brønsted-Evans-Polanyi (BEP) relationships, and strong metal-support interactions (SMSI) govern hydrogen desorption, coke resistance, and structural stability. Special focus is placed on engineering supports to modulate acidity, enhance site isolation, and promote selective C-H activation under mild operating conditions. By integrating atomic-scale insights with mesostructural engineering, this review proposes a rational framework for designing robust, regenerable dehydrogenation catalysts that advance LOHC technology for biomaterial-compatible hydrogen storage and green energy integration.