Mechanistic insight into efficient H(2) generation upon HCOONa hydrolysis

HCOONa水解高效生成H₂的机理研究

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Abstract

Sodium formate (SF) is regarded as a technological additive to improve H(2) generation upon HCOOH dehydrogenation. The development of SF as a hydrogen storage material is still a challenge. Herein, we report the design and synthesis of carbon nanosphere-stabilized Pd nanoparticles (Pd/CNS) for the direct H(2) generation upon SF hydrolysis in the presence of Fe(3+). The tandem reaction, isotopic mass spectrometry, and gas chromatograms result confirmed that SF hydrolysis generates H(2) with one H atom provided by SF and other H by H(2)O. The kinetic study and detailed mechanistic investigations have demonstrated that the concerted process between the cleavage of O-H bond in H(2)O and -O(2)C-H bond oxidative addition is the rate-controlling step in SF hydrolysis. This work offers a new chemical hydrogen storage material (HCOONa) for the high-efficiency generation, transport, and storage of H(2).

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