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Breaking the Energy Linear Relationships between C≡C and C═C Bonds over Porous Intermetallic Pd2Ga Metallene Boosting
Kai Deng1, Jiabao Yu1, Qiqi Mao1
1State Key Laboratory of Green Chemical Synthesis and Conversion, Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, P. R. China.
Abstract:
The electrochemical semihydrogenation (ECSH) of 2-methyl-3-butyn-2-ol (MBY) to 2-methyl-3-buten-2-ol (MBE), using water as a hydrogen source, offers a sustainable pathway for chemical synthesis. However, conventional Pd-based catalysts are limited by the linear scaling relationships (LSRs) between the adsorption energies of C≡C and C═C bonds, often leading to overhydrogenation into 2-methyl-3-butan-2-ol (MBA) and, thus, reduced selectivity toward MBE. In this work, we report a solvothermal approach for synthesizing porous intermetallic Pd2Ga (PI-Pd2Ga) metallene as a high-performance catalyst for the ECSH of MBY to MBE. The PI-Pd2Ga metallene exhibits an optimized electronic structure and an expanded Pd interatomic distance (dPd-Pd), which facilitates MBY adsorption, H2O dissociation, and MBE* desorption. These distinctive structural properties effectively break the LSRs between C≡C and C═C bonds, resulting in a high MBE selectivity of 96.99%, an MBE Faradaic efficiency (FEMBE) of 92.85%, excellent stability, and broad substrate applicability. This work provides a strategy for the rational design and development of efficient catalysts for selective semihydrogenation reactions.
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