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

Sep 29, 2026

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. The review synthesizes advances in porous-supported catalysts that enable tailored control of morphology, metal dispersion, and interfacial chemistry, spanning alumina, mesoporous silica, carbon frameworks, and Mg/Al layered oxides. It analyzes monometallic and bimetallic Pt-based systems, linking d-band, BEP, and SMSI concepts to hydrogen desorption, coke resistance, and structural stability. It further emphasizes support engineering to tune acidity, isolate sites, and promote selective C−H activation under mild conditions, forming a design framework for robust, regenerable dehydrogenation catalysts supporting LOHC deployment and green energy integration.

LanguageEnglish

CategoryResearch & Report

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Pages17

Reading Time43 min

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Abstract

Introduction

This article is licensed under CC-BY-NC-ND 4.0 [http://pubs.acs.org/journal/acsodf](http://pubs.acs.org/journal/acsodf) Review Engineering Porous-Supported Bimetallic Catalysts for Efficient LOHC Dehydrogenation: From Interfacial Modulation to Sustainable Hydrogen Release Ruolan Du* and Yuanzhe Li* Cite This: ACS Omega 2025, 10, 57995−58011 Read Online | | | | | | --- | --- | --- | --- | | ACCESS | Metrics & More | | Article Recommendations | ABSTRACT: 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. 1. INTRODUCTION The growing imperative for global energy decarbonization has intensified efforts to develop hydrogen storage technologies that are both efficient and scalable. Liquid organic hydrogen carriers (LOHCs) have emerged as a promising solution owing to their favorable hydrogen densities (both volumetric and gravimetric), compatibility with current fuel infrastructure, and inherent safety in handling, transportation, and storage. LOHCs are defined as organic compounds that remain in liquid or lowmelting-solid form under ambient conditions and operate via reversible hydrogenation−dehydrogenation cycles. In this system, hydrogen is chemically stored through exothermic catalytic hydrogenation of hydrogen-lean species and subsequently released via endothermic catalytic dehydrogenation of hydrogen-rich counterparts under controlled temperatures and pressure. LOHC technology dates to 1975, when Sultan and Shaw first developed the concept ofusing aromatic compounds: toluene (TOL)/methylcyclohexane (MCH) system as storage carriers for hydrogen.1 MCH has emerged as a leading candidate for consideration due to its noteworthy capacity to interact with established conventional transport, storage, and distribution systems in spite of its lower hydrogen storage capacity (6.2 wt % or 47.3 kg H2 m−3) compared to that of cyclohexane (CHE)(CH: 7.2 wt %) and decalin (DEC: 7.3 wt %).2 Diverse pairs of LOHC have been investigated in recent decades, such as (H18-DBT)/dibenzyltoluene (H0-DBT), decalin/naphthalene,3 or cyclohexane (CHE)/benzene, store hydrogen via catalytic reactions without forming new covalent backbones, thus offering a closed, cyclic hydrogen vector platform. Despite their notable advantages, the large-scale implementation ofLOHC systems is hindered by the limited efficiency and stability of existing dehydrogenation catalysts, especially under industrially relevant conditions. As an inherently endothermic and kinetically challenging process, dehydrogenation necessitates elevated temperatures and highly active catalytic surfaces to enable selective C−H bond activation while minimizing side reactions such as cracking, isomerization, and coke deposition. To enhance the reaction efficiency, advanced catalysts are engineered to lower activation barriers and modulate react

FAQs

Why are porous-supported catalysts important for LOHC dehydrogenation?

Porous supports enable precise control over catalyst morphology, metal dispersion, and interfacial chemistry, which directly improves hydrogen release efficiency and sustainability.

Which catalyst systems are covered in the review?

The review examines monometallic systems (Pt, Pd, Ir) and bimetallic systems such as Pt−Sn, Pt−Pd, and Pt−Ir, focusing on how their behavior relates to interfacial and electronic effects.

How do interfacial effects influence catalytic performance?

The review links hydrogen desorption, coke resistance, and structural stability to factors such as d-band theory, BEP relationships, and strong metal−support interactions (SMSI), along with engineered support acidity and site isolation.

Sep 29, 2026

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