Mechanistic insight into efficient H2 generation upon HCOONa hydrolysis

Abstract

Summary: Sodium formate (SF) is regarded as a technological additive to improve H2 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 H2 generation upon SF hydrolysis in the presence of Fe3+. The tandem reaction, isotopic mass spectrometry, and gas chromatograms result confirmed that SF hydrolysis generates H2 with one H atom provided by SF and other H by H2O. The kinetic study and detailed mechanistic investigations have demonstrated that the concerted process between the cleavage of O-H bond in H2O and -O2C-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 H2.

Keywords

• Chemical reaction
• Electrochemistry