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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.

Project description:Ammonia borane (NH3-BH3) is of interest as a hydrogen storage material because of its ease of use and its ability to release three molar equivalents of H2(g) via catalytic hydrolysis. Most heterogeneous catalysts for ammonia borane hydrolysis are nanoparticles containing expensive noble metals. Here, we show that metal ruthenate perovskites function as active and durable catalysts for ammonia borane hydrolysis. As a bulk powder, CaRuO3 catalyzes the hydrolysis of ammonia borane at room temperature and is recyclable and reusable. CaRuO3 facilitates the release of H2(g) from aqueous ammonia borane solutions at comparable rates to some other heterogeneous catalyst systems while having a low noble metal content. Other ruthenium-based perovskites, including SrRuO3, Ca2LaRuO6, Sr2CoRuO6, and SrLaCoRuO6, are similarly active catalysts for room-temperature ammonia borane hydrolysis.

| S-EPMC6641281 | biostudies-literature

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

Project description:Development of non-noble metal catalysts with similar activity and stability to noble metals is of significant importance in the conversion and utilization of clean energy. The catalytic hydrolysis of ammonia borane (AB) to produce 3 equiv. of H2, as an example of where noble metal catalysts significantly outperform their non-noble peers, serves as an excellent test site for the design and optimization of non-noble metal catalysts. Our kinetic isotopic effect measurements reveal, for the first time, that the kinetic key step of the hydrolysis is the activation of H2O. Deducibly, a transition metal with an optimal electronic structure that bonds H2O and -OH in intermediate strengths would favor the hydrolysis of AB. By employing a covalent triazine framework (CTF), a newly developed porous material capable of donating electrons through the lone pairs on N, the electron densities of nano-sized Co and Ni supported on CTF are markedly increased, as well as their catalytic activities. Specifically, Co/CTF exhibits a total turnover frequency of 42.3 molH2 molCo-1 min-1 at room temperature, which is superior to all peer non-noble metal catalysts ever reported and even comparable to some noble metal catalysts.

| S-EPMC5299936 | biostudies-literature

Ammonia-triphenyl-borane.

Project description:The asymmetric unit of the title compound, C(18)H(18)BN or (C(6)H(5))(3)B·NH(3), comprises two crystallographically independent but virtually identical mol-ecules. Mol-ecules of one type are linked with each other by N-H?? inter-actions, generating an infinite column aligned along the b-axis direction. The columns of different types of mol-ecules are inter-connected by C-H?? inter-actions, producing a three-dimensional array.

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Hexagonal CuCo₂O₄ Nanoplatelets, a Highly Active Catalyst for the Hydrolysis of Ammonia Borane for Hydrogen Production.

Project description:Catalytic hydrolysis of ammonia borane (AB) has been considered as an effective and safe method to generate hydrogen. Development of highly active and low-cost catalysts is one of the key tasks for this technology. In this work, hexagonal CuCo₂O₄ nanoplatelets with a thickness of approximately 55 nm were prepared. In AB hydrolysis, those nanoplatelets exhibited ultrahigh catalytic activity with turnover frequency (TOF) of 73.4 molhydrogen min-1 molcat-1. As far as we know, this is one of the highest TOF values ever reported for non-noble metal catalysts. In addition, the effects of viscosity and different alkalis on the hydrolysis were also investigated. It is revealed that high viscosity of the reaction medium will retard the hydrolysis reaction. The presence of NaOH, KOH, and Na₂CO₃ in the reaction solution is favorable for hydrolytic process. In contrast, NH₃·H₂O will slow down the hydrolysis rate of ammonia borane. This work can provide some novel insight into the design of catalysts with both high performance and low cost. Besides, some findings in the present study can also offer us some information about how to improve the hydrolysis rates by optimizing the hydrolysis condition.

| S-EPMC6473973 | biostudies-literature

In Situ Formation of AgCo Stabilized on Graphitic Carbon Nitride and Concomitant Hydrolysis of Ammonia Borane to Hydrogen.

Project description:The development of highly-efficient heterogeneous supported catalysts for catalytic hydrolysis of ammonia borane to yield hydrogen is of significant importance considering the versatile usages of hydrogen. Herein, we reported the in situ synthesis of AgCo bimetallic nanoparticles supported on g-C₃N₄ and concomitant hydrolysis of ammonia borane for hydrogen evolution at room temperature. The as-synthesized Ag0.1Co0.9/g-C₃N₄ catalysts displayed the highest turnover frequency (TOF) value of 249.02 mol H₂·(molAg·min)−1 for hydrogen evolution from the hydrolysis of ammonia borane, which was higher than many other reported values. Furthermore, the Ag0.1Co0.9/g-C₃N₄ catalyst could be recycled during five consecutive runs. The study proves that Ag0.1Co0.9/g-C₃N₄ is a potential catalytic material toward the hydrolysis of ammonia borane for hydrogen production.

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Efficient Organocatalytic Dehydrogenation of Ammonia Borane.

Project description:Dehydrogenation of ammonia borane by sterically encumbered pyridones as organocatalysts is reported. With 6-tert-butyl-2-thiopyridone as the catalyst, a turnover frequency (TOF) of 88 h-1 was achieved. Experimental mechanistic investigations, substantiated by DLPNO-CCSD(T) computations, indicate a mechanistic scenario that commences with the protonation of a B-H bond by the mercaptopyridine form of the catalyst. The reactive intermediate formed by this initial protonation was observed by NMR spectroscopy and the molecular structure of a surrogate determined by SCXRD. An intramolecular proton transfer in this intermediate from the NH3 group to the pyridine ring with concomitant breaking of the S-B bond regenerates the thiopyridone and closes the catalytic cycle. This step can be described as an inorganic retro-ene reaction.

| S-EPMC7003781 | biostudies-literature

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

Project description:Self-assembly of short de novo designed peptides gives rise to catalytic amyloids capable of facilitating multiple chemical transformations. We show that catalytic amyloids can efficiently hydrolyze paraoxon, a widely used, highly toxic organophosphate pesticide. Moreover, these robust and inexpensive metal-containing materials can be easily deposited on various surfaces producing catalytic flow devices. Finally, functional promiscuity of catalytic amyloids promotes tandem hydrolysis/oxidation reactions. High efficiency discovered in a very small library of peptides suggests an enormous potential for further improvement of catalytic properties both in terms of catalytic efficiency and substrate scope.

| S-EPMC6181230 | biostudies-literature

Dihydrogen Phosphate Stabilized Ruthenium(0) Nanoparticles: Efficient Nanocatalyst for The Hydrolysis of Ammonia-Borane at Room Temperature.

Project description:Intensive efforts have been devoted to the development of new materials for safe and efficient hydrogen storage. Among them, ammonia-borane appears to be a promising candidate due to its high gravimetric hydrogen storage capacity. Ammonia-borane can release hydrogen on hydrolysis in aqueous solution under mild conditions in the presence of a suitable catalyst. Herein, we report the synthesis of ruthenium(0) nanoparticles stabilized by dihydrogenphosphate anions with an average particle size of 2.9 ± 0.9 nm acting as a water-dispersible nanocatalyst in the hydrolysis of ammonia-borane. They provide an initial turnover frequency (TOF) value of 80 min-1 in hydrogen generation from the hydrolysis of ammonia-borane at room temperature. Moreover, the high stability of these ruthenium(0) nanoparticles makes them long-lived and reusable nanocatalysts for the hydrolysis of ammonia-borane. They provide 56,800 total turnovers and retain ~80% of their initial activity even at the fifth catalytic run in the hydrolysis of ammonia-borane at room temperature.

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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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Bi(I)-Catalyzed Transfer-Hydrogenation with Ammonia-Borane.

Project description:A catalytic transfer-hydrogenation utilizing a well-defined Bi(I) complex as catalyst and ammonia-borane as transfer agent has been developed. This transformation represents a unique example of low-valent pnictogen catalysis cycling between oxidation states I and III, and proved useful for the hydrogenation of azoarenes and the partial reduction of nitroarenes. Interestingly, the bismuthinidene catalyst performs well in the presence of low-valent transition-metal sensitive functional groups and presents orthogonal reactivity compared to analogous phosphorus-based catalysis. Mechanistic investigations suggest the intermediacy of an elusive bismuthine species, which is proposed to be responsible for the hydrogenation and the formation of hydrogen.

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