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Tunable hydrogen coverage on electron-deficient platinum nanoparticles for efficient hydrogenation reactions

Nano Research 2023年第7期16卷 8751-8756页

作者： Lu-Han Sun Qi-Yuan Li Yu-Shuai Xu Si-Yuan Xia Dong Xu Xiu Lin Jingsan Xu Jie-Sheng Chen Guo-Dong Li Xin-Hao Li School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China School of Chemistry and Physics Faculty of ScienceCentre for Materials ScienceQueensland University of TechnologyBrisbaneQLD 4001Australia State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China

Dissociation of active H species over the catalytic sites with the carbon-supported Pt metals as the mainstream catalysts is crucial to facilitate hydrogen donation and accelerate the hydrogen addition process in catalytic hydrogenation systems to produce polymers,pharmaceuticals,agrochemicals,fragrances,and biofuels at million-ton *** attention has been paid to the design of the more active catalytic site to effectively adsorb and activate reactants and H_(2) *** the same time,there is still a huge room to develop powerful strategies to accelerate the donation of acted H species to the reactants from the Pt surface further to boost the final catalytic efficiencies of Pt catalysts and depress the total Pt ***,we present a new strategy for promoting the Pt-H bond dissociation by increasing surface hydrogen coverage on designed electron-deficient Pt *** electron deficiency of Pt nanoparticles has been successfully tuned by constructing a rectifying contact with an even“noble”boron-rich carbon support(Pt/BC).Theoretical and experimental results confirm the dominant role of the pronounced electron deficiencies of Pt nanoparticles in enhancing the H coverage for 2.3 times higher than that of neutral Pt nanoparticles,significantly boosting the Pt-H bond dissociation and thus the whole hydrogenation process as reflected by the extremely high turnover frequency(TOF)value of 388 h^(-1)at 30℃ and 10 bar H_(2) for phenol hydrogenation on the Pt/BC,outperforming the bench-marked catalysts by a factor of 9.

关键词： hydrogenation hydrogen coverage Schottky barrier heterogeneous catalysis

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