Heterolytic Dissociation of H2 in Heterogeneous Catalysis
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Abstract
H2 dissociation plays crucial roles in catalytic hydrogenation reactions and hydrogen storage. Metal-nanoparticle-based heterogeneous catalysts often dissociate H2 via a homolytic pathway. The heterolytic H2 dissociation pathway was identified in several heterogeneous catalytic systems, including single-atom catalysts, metal–support interfaces, and bulk metal oxides/sulfides/nitrides/phosphides. The active site structures of these heterogeneous catalysts resemble homogeneous catalysts where the metal centers (Lewis acids) are coordinated with O/S/N/P atoms (Lewis bases). These Lewis acid–base pairs dissociate H2 molecules heterolytically into proton–hydride pairs, which favor the hydrogenation of polar functional groups in unsaturated hydrocarbons. In this review, we summarize the common structural features of heterogeneous, homogeneous, and enzyme catalysts in the heterolytic dissociation of H2. The active sites, Lewis acid–base pairs, are discussed throughout this review. The energy barriers and kinetic contributions of heterolytic and homolytic H2 dissociation pathways in heterogeneous catalytic systems are discussed. The spectroscopic evidence of the heterolytic H2 dissociation pathways is critically reviewed.
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