Combination of nanoparticles with single-metal sites synergistically boosts co-catalyzed formic acid dehydrogenation

Yanzhe Shi, Bingcheng Luo, Rui Sang, Dandan Cui, Ye Sun (), Runqi Liu, Zili Zhang, Yifei Sun (), Henrik Junge, Matthias Beller () and Xiang Li ()
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Yanzhe Shi: Beihang University
Bingcheng Luo: China Agricultural University
Rui Sang: Leibniz-Institut für Katalyse
Dandan Cui: Beihang University
Ye Sun: Beihang University
Runqi Liu: Beihang University
Zili Zhang: China University of Geosciences
Yifei Sun: Beihang University
Henrik Junge: Leibniz-Institut für Katalyse
Matthias Beller: Leibniz-Institut für Katalyse
Xiang Li: Beihang University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract The development of hydrogen technologies is at the heart of a green economy. As prerequisite for implementation of hydrogen storage, active and stable catalysts for (de)hydrogenation reactions are needed. So far, the use of precious metals associated with expensive costs dominates in this area. Herein, we present a new class of lower-cost Co-based catalysts (Co-SAs/NPs@NC) in which highly distributed single-metal sites are synergistically combined with small defined nanoparticles allowing efficient formic acid dehydrogenation. The optimal material with atomically dispersed CoN2C2 units and encapsulated 7-8 nm nanoparticles achieves an excellent gas yield of 1403.8 mL·g−1·h−1 using propylene carbonate as solvent, with no activity loss after 5 cycles, which is 15 times higher than that of the commercial Pd/C. In situ analytic experiments show that Co-SAs/NPs@NC enhances the adsorption and activation of the key intermediate monodentate HCOO*, thereby facilitating the following C-H bond breaking, compared to related single metal atom and nanoparticle catalysts. Theoretical calculations show that the integration of cobalt nanoparticles elevates the d-band center of the Co single atoms as the active center, which consequently enhances the coupling of the carbonyl O of the HCOO* intermediate to the Co centers, thereby lowering the energy barrier.

Date: 2024
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DOI: 10.1038/s41467-024-52517-w

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