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Catalytic Behavior of Iron-Containing Cubic Spinel in the Hydrolysis and Hydrothermolysis of Ammonia Borane.

ABSTRACT: The paper presents a comparative study of the activity of magnetite (Fe₃O₄) and copper and cobalt ferrites with the structure of a cubic spinel synthesized by combustion of glycine-nitrate precursors in the reactions of ammonia borane (NH₃BH₃) hydrolysis and hydrothermolysis. It was shown that the use of copper ferrite in the studied reactions of NH₃BH₃ dehydrogenation has the advantages of a high catalytic activity and the absence of an induction period in the H₂ generation curve due to the activating action of copper on the reduction of iron. Two methods have been proposed to improve catalytic activity of Fe₃O₄-based systems: (1) replacement of a portion of Fe²⁺ cations in the spinel by active cations including Cu²⁺ and (2) preparation of highly dispersed multiphase oxide systems, involving oxide of copper.

SUBMITTER: Komova OV

PROVIDER: S-EPMC8468860 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Metal Ruthenate Perovskites as Heterogeneous Catalysts for the Hydrolysis of Ammonia Borane.

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Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design.

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Copper-Containing Catalytic Amyloids Promote Phosphoester Hydrolysis and Tandem Reactions.

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Project description:The reduction of nitrogen (N2) to ammonia (NH3) is a requisite transformation for life. Although it is widely appreciated that the iron-rich cofactors of nitrogenase enzymes facilitate this transformation, how they do so remains poorly understood. A central element of debate has been the exact site or sites of N2 coordination and reduction. In synthetic inorganic chemistry, an early emphasis was placed on molybdenum because it was thought to be an essential element of nitrogenases and because it had been established that well-defined molybdenum model complexes could mediate the stoichiometric conversion of N2 to NH3 (ref. 9). This chemical transformation can be performed in a catalytic fashion by two well-defined molecular systems that feature molybdenum centres. However, it is now thought that iron is the only transition metal essential to all nitrogenases, and recent biochemical and spectroscopic data have implicated iron instead of molybdenum as the site of N2 binding in the FeMo-cofactor. Here we describe a tris(phosphine)borane-supported iron complex that catalyses the reduction of N2 to NH3 under mild conditions, and in which more than 40 per cent of the proton and reducing equivalents are delivered to N2. Our results indicate that a single iron site may be capable of stabilizing the various NxHy intermediates generated during catalytic NH3 formation. Geometric tunability at iron imparted by a flexible iron-boron interaction in our model system seems to be important for efficient catalysis. We propose that the interstitial carbon atom recently assigned in the nitrogenase cofactor may have a similar role, perhaps by enabling a single iron site to mediate the enzymatic catalysis through a flexible iron-carbon interaction.

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Project description:The catalytic hydrolysis of ammonia borane (AB) is a promising route to produce hydrogen for mobile hydrogen?oxygen fuel cells. In this study, we have successfully synthesized a variety of Ni0.5Cu0.5Co2O4 nanocomposites with different morphology, including nanoplatelets, nanoparticles, and urchin-like microspheres. The catalytic performance of those Ni0.5Cu0.5Co2O4 composites in AB hydrolysis is investigated. The Ni0.5Cu0.5Co2O4 nanoplatelets show the best catalytic performance despite having the smallest specific surface area, with a turnover frequency (TOF) of 80.2 molhydrogen·min-1·mol-1cat. The results reveal that, in contrast to the Ni0.5Cu0.5Co2O4 nanoparticles and microspheres, the Ni0.5Cu0.5Co2O4 nanoplatelets are more readily reduced, leading to the fast formation of active species for AB hydrolysis. These findings provide some insight into the design of high-performance oxide-based catalysts for AB hydrolysis. Considering their low cost and high catalytic activity, Ni0.5Cu0.5Co2O4 nanoplatelets are a strong candidate catalyst for the production of hydrogen through AB hydrolysis in practical applications.

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