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Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides

Author

Listed:
  • Mingwu Tan

    (Xiamen University)

  • Yanling Yang

    (Xiamen University)

  • Ying Yang

    (Xiamen University)

  • Jiali Chen

    (Xiamen University)

  • Zhaoxia Zhang

    (Xiamen University)

  • Gang Fu

    (Xiamen University)

  • Jingdong Lin

    (Xiamen University)

  • Shaolong Wan

    (Xiamen University)

  • Shuai Wang

    (Xiamen University)

  • Yong Wang

    (Washington State University)

Abstract

Spontaneous migration of atomic hydrogen species from metal particles to the surface of their support, known as hydrogen spillover, has been claimed to play a major role in catalytic processes involving hydrogen. While this phenomenon is well established on reducible oxide supports, its realization on much more commonly used non-reducible oxides is still challenged. Here we present a general strategy to enable effective hydrogen spillover over non-reducible SiO2 with aid of gaseous organic molecules containing a carbonyl group. By using hierarchically-porous-SiO2-supported bimetallic Pt-Fe catalysts with Pt nanoparticles exclusively deposited into the micropores, we demonstrate that activated hydrogen species generated on the Pt sites within the micropores can be readily transported by these oxygenate molecules to Fe sites located in macropores, leading to significantly accelerated hydrodeoxygenation rates on the latter sites. This finding provides a molecule-assisted approach to the rational design and optimization of multifunctional heterogeneous catalysts, reminiscent of the role of molecular coenzymes in bio-catalysis.

Suggested Citation

  • Mingwu Tan & Yanling Yang & Ying Yang & Jiali Chen & Zhaoxia Zhang & Gang Fu & Jingdong Lin & Shaolong Wan & Shuai Wang & Yong Wang, 2022. "Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-29045-6
    DOI: 10.1038/s41467-022-29045-6
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    References listed on IDEAS

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    1. Waiz Karim & Clelia Spreafico & Armin Kleibert & Jens Gobrecht & Joost VandeVondele & Yasin Ekinci & Jeroen A. van Bokhoven, 2017. "Catalyst support effects on hydrogen spillover," Nature, Nature, vol. 541(7635), pages 68-71, January.
    2. Jiankang Zhang & Zhe Gao & Sen Wang & Guofu Wang & Xiaofeng Gao & Baiyan Zhang & Shuangfeng Xing & Shichao Zhao & Yong Qin, 2019. "Origin of synergistic effects in bicomponent cobalt oxide-platinum catalysts for selective hydrogenation reaction," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    3. Juhwan Im & Hyeyoung Shin & Haeyoun Jang & Hyungjun Kim & Minkee Choi, 2014. "Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures," Nature Communications, Nature, vol. 5(1), pages 1-8, May.
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    Cited by:

    1. Yijing Liu & Rankun Zhang & Le Lin & Yichao Wang & Changping Liu & Rentao Mu & Qiang Fu, 2023. "Direct observation of accelerating hydrogen spillover via surface-lattice-confinement effect," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    2. Xiao-Jue Bai & Caoyu Yang & Zhiyong Tang, 2024. "Enabling long-distance hydrogen spillover in nonreducible metal-organic frameworks for catalytic reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Zhida Gu & Mengke Li & Cheng Chen & Xinglong Zhang & Chengyang Luo & Yutao Yin & Ruifa Su & Suoying Zhang & Yu Shen & Yu Fu & Weina Zhang & Fengwei Huo, 2023. "Water-assisted hydrogen spillover in Pt nanoparticle-based metal–organic framework composites," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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