Download file (5.2 MB)
Download as zip (4.88 MB)

Collection

Citation

Description:

Although sodium borohydride (NaBH4, SBH) has been investigated extensively as a high-capacity hydrogen-storage material that can be used to move towards a hydrogen-powered society, the development of efficient and cost-effective catalysts for the generation of hydrogen from SBH remains challenging. Here, we report that a mixed-valent [FeII−FeIII] iron hydroxide, which we term green rust (GR), treated with a CuCl2 solution, shows a good solar-light-assisted catalytic activity toward SBH hydrolysis at room temperature that is higher than existing catalysts based on precious and noble metals, including Pt nanoparticle-modified titanium dioxide (TiO2). Even without solar light, the GR-based catalyst exhibits turnover frequency (TOF) of up to 5000 min–1 for the hydrolysis of SBH at a higher temperature that is comparable to or one or two orders of magnitude higher than existing catalysts under similar conditions. Comprehensive spectral and microscopic analyses revealed that our catalyst was composed of GR plate-like particles with edges that are decorated with aggregated Cu2O clusters with particle sizes down to 5 nm. Molecular dynamics simulations, combined with experimental results, demonstrate that the Cu2O modifier not only provides adsorption sites for SBH molecules but also acts as a cocatalyst for the transfer of photoexcited electrons in the GR component to the adsorbed SBH, both of which enable the effective activation of the reactant (BH4−).

Rights:

• Creative Commons BY Attribution 4.0 International
  

Keyword: Mixed-valent ironcompound, Layered double hydroxide, Green rust, Copper, Hydrogen storage, Sodium borohydride, Hydrolysis

Date published: 2025-07-18

Publisher: American Chemical Society (ACS)

Journal:

• ACS Catalysis (ISSN: 21555435) vol. 15 issue. 14 p. 12269-12280

Funding:

• Ministry of Education, Culture, Sports, Science and Technology JPMXP1223NM51
• Ministry of Education, Culture, Sports, Science and Technology The World Premier International Research Center In

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.6069

First published URL: https://doi.org/10.1021/acscatal.5c01894

Related item:

Other identifier(s):

Contact agent:

Updated at: 2025-12-25 10:18:16 +0900

Published on MDR: 2025-12-25 12:19:50 +0900