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Mechanistic insight into efficient H₂ generation upon HCOONa hydrolysis.

ABSTRACT: 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.

SUBMITTER: Xu F

PROVIDER: S-EPMC10119764 | biostudies-literature | 2023 Apr

REPOSITORIES: biostudies-literature

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Mechanistic insight into efficient H2 generation upon HCOONa hydrolysis.

Xu Fuhua F Yan Jiaying J Wang Yanlan Y Liu Xiang X

iScience 20230328 4

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 hydrolysi ...[more]

PMID: 37091254

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Project description:Solid-state synthesis has historically focused on reactants and end products; however, knowledge of reaction pathways, intermediate phases and their formation may provide mechanistic insight of solid-state reactions. With an increased understanding of reaction progressions, design principles can be deduced, affording more predictive power in materials synthesis. In pursuit of this goal, in situ powder X-ray diffraction is employed to observe crystalline phase evolution over the course of the reaction, thereby constructing a "panoramic" view of the reaction from beginning to end. We conducted in situ diffraction studies in the K-Bi-Q (Q = S, Se) system to understand the formation of phases occurring in this system in the course of their reactions. Powder mixtures of K2Q to Bi2Q3 in 1 : 1 and 1.5 : 1 ratios were heated to 800 °C or 650 °C, while simultaneously collecting diffraction data. Three new phases, K3BiS3, β-KBiS2, and β-KBiSe2, were discovered. Panoramic synthesis showed that K3BiQ3 serves an important mechanistic role as a structural intermediate in both chalcogen systems (Q = S, Se) in the path to form the KBiQ2 structure. Thermal analysis and calculations at the density functional theory (DFT) level show that the cation-ordered β-KBiQ2 polymorphs are the thermodynamically stable phase in this compositional space, while Pair Distribution Function (PDF) analysis shows that all α-KBiQ2 structures have local disorder due to stereochemically active lone pair expression of the bismuth atoms. The formation of the β-KBiQ2 structures, both of which crystallize in the α-NaFeO2 structure type, show a boundary where the structure can be disordered or ordered with regards to the alkali metal and bismuth. A cation radius tolerance for six-coordinate cation site sharing of ∼ 1.3 is proposed. The mechanistic insight the panoramic synthesis technique provides in the K-Bi-Q system is progress towards the overarching goal of synthesis-by-design.

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Mechanistic insight into efficient H₂ generation upon HCOONa hydrolysis.

Publications

Mechanistic insight into efficient H<sub>2</sub> generation upon HCOONa hydrolysis.

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