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

ABSTRACT: 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.

SUBMITTER: Liao J

PROVIDER: S-EPMC6473973 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Cu@Pd/C with Controllable Pd Dispersion as a Highly Efficient Catalyst for Hydrogen Evolution from Ammonia Borane.

Project description:A series of Cu@Pd/C with different Pd contents was prepared using the galvanic reduction method to disperse Pd on the surface of Cu nanoparticles on Cu/C. The dispersion of Pd was regulated by the Cu(I) on the surface, which was introduced by pulse oxidation. The Cu2O did not react during the galvanic reduction process and restricted the Pd atoms to a specific area. The pulse oxidation method was demonstrated to be an effective process to control the oxidization degree of Cu on Cu/C and then to govern the dispersion of Pd. The catalysts were characterized by transmission electron microscopy (TEM), high-resolution transmission electron microscope (HRTEM), high angular annular dark field scanning TEM (HAADF-STEM), energy-dispersive spectroscopy (EDS) mapping, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), auger electron spectroscopy (AES), and inductively coupled plasma optical emission spectrometer (ICP-OES), which were used to catalyze the hydrogen evolution from ammonia borane. The Cu@Pd/C had much higher activity than the PdCu/C, which was prepared by the impregnation method. The TOF increased as the Cu2O in Cu/C used for the preparation of Cu@Pd/C increased, and the maximum TOF was 465 molH2 min-1 molPd-1 at 298 K on Cu@Pd0.5/C-640 (0.5 wt % of Pd, 640 mL of air was pulsed during the preparation of Cu/C-640). The activity could be maintained in five continuous processes, showing the strong stability of the catalysts.

| S-EPMC7558311 | biostudies-literature

Bracelet-Like Ni0.4Cu0.6O Microstructure Composed of Well-Aligned Nanoplatelets as a Superior Catalyst to the Hydrolysis of Ammonia Borane.

Project description:The development of novel catalysts with both high catalytic activity and low cost toward the hydrolysis of ammonia borane is an important subject in the field of hydrogen energy. In this communications, NixCu1-xO microstructures with different morphology have been synthesized and their catalytic activities in AB hydrolysis is studied. It's found that bracelet-like nanoplatelets were obtained at x = 0.4 and exhibit highest catalytic performance with turnover frequency of 33.43 molhydrogen min-1 mol cat - 1 , which much higher than those of most of CuNi-based catalysts in the literature. Pronounced synergistic effects between CuO and NiO in AB hydrolysis also have been observed. Due to the superior catalytic performance and cheapness, the prepared bracelet-like nanoplatelets Ni0.4Cu0.6O catalysts can be a strong catalyst candidate in AB hydrolysis.

| S-EPMC6868442 | biostudies-literature

Ruthenium nanoparticles confined in SBA-15 as highly efficient catalyst for hydrolytic dehydrogenation of ammonia borane and hydrazine borane.

Project description:Ultrafine ruthenium nanoparticles (NPs) within the mesopores of the SBA-15 have been successfully prepared by using a "double solvents" method, in which n-hexane is used as a hydrophobic solvent and RuCl3 aqueous solution is used as a hydrophilic solvent. After the impregnation and reduction processes, the samples were characterized by XRD, TEM, EDX, XPS, N2 adsorption-desorption, and ICP techniques. The TEM images show that small sized Ru NPs with an average size of 3.0 ± 0.8 nm are uniformly dispersed in the mesopores of SBA-15. The as-synthesized Ru@SBA-15 nanocomposites (NCs) display exceptional catalytic activity for hydrogen generation by the hydrolysis of ammonia borane (NH3BH3, AB) and hydrazine borane (N2H4BH3, HB) at room temperature with the turnover frequency (TOF) value of 316 and 706 mol H2 (mol Ru min)(-1), respectively, relatively high values reported so far for the same reaction. The activation energies (Ea) for the hydrolysis of AB and HB catalyzed by Ru@SBA-15 NCs are measured to be 34.8 ± 2 and 41.3 ± 2 kJ mol(-1), respectively. Moreover, Ru@SBA-15 NCs also show satisfied durable stability for the hydrolytic dehydrogenation of AB and HB, respectively.

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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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A Highly Active Bidentate Magnesium Catalyst for Amine-Borane Dehydrocoupling: Kinetic and Mechanistic Studies.

Project description:A magnesium complex (1) featuring a bidentate aminopyridinato ligand is a remarkably selective catalyst for the dehydrocoupling of amine-boranes. This reaction proceeds to completion with low catalyst loadings (1 mol %) under mild conditions (60 °C), exceeding previously reported s-block systems in terms of selectivity, rate, and turnover number (TON). Mechanistic studies by in situ NMR analysis reveals the reaction to be first order in both catalyst and substrate. A reaction mechanism is proposed to account for these findings, with the high TON of the catalyst attributed to the bidentate nature of the ligand, which allows for reversible deprotonation of the substrate and regeneration of 1 as a stable resting state.

| S-EPMC6563444 | biostudies-literature

Synergistic Pt-WO3 Dual Active Sites to Boost Hydrogen Production from Ammonia Borane.

Project description:Development of synergistic heterogeneous catalysts with active sites working cooperatively has been a pursuit of chemists. Herein, we report for the first time the fabrication and manipulation of Pt-WO3 dual-active-sites to boost hydrogen generation from ammonia borane. A combination of DFT calculations, structural characterization, and kinetic (isotopic) analysis reveals that Pt and WO3 act as the active sites for ammonia borane and H2O activation, respectively. A trade-off between the promoting effect of WO3 and the negative effect of decreased Pt binding energy contributes to a volcano-shaped activity, and Pt/CNT-5W delivers a 4-fold increased activity of 710.1 molH2·molPt-1·min-1. Moreover, WO3 is suggested to simultaneously act as the sacrificial site that can divert B-containing by-products away from Pt sites against deactivation, yielding an increase from 24% to 68% of the initial activity after five cycles. The strategy demonstrated here could shed a new light on the design and manipulation of dual-active-site catalysts.

| S-EPMC7052519 | biostudies-literature

MoO₃-Doped MnCo₂O₄ Microspheres Consisting of Nanosheets: An Inexpensive Nanostructured Catalyst to Hydrolyze Ammonia Borane for Hydrogen Generation.

Project description:Production of hydrogen by catalytically hydrolyzing ammonia borane (AB) has attracted extensive attention in the field of catalysis and energy. However, it is still a challenge to develop a both inexpensive and active catalyst for AB hydrolysis. In this work, we designed a series of MoO₃-doped MnCo₂O₄ (x) catalysts, which were fabricated by a hydrothermal process. The morphology, crystalline structure, and chemical components of the catalysts were systematically analyzed. The catalytic behavior of the catalyst in AB hydrolysis was investigated. Among these catalysts, MoO₃-doped MnCo₂O₄ (0.10) microspheres composed of nanosheets exhibited the highest catalytic activity. The apparent activation energy is 34.24 kJ mol-1 and the corresponding turnover frequency is 26.4 molhydrogen min-1 molcat-1. Taking into consideration the low cost and high performance, the MoO₃-doped MnCo₂O₄ (0.10) microspheres composed of nanosheets represent a promising catalyst to hydrolyze AB for hydrogen production.

| S-EPMC6359025 | biostudies-literature

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

Dehydrogenation of ammonia borane through the third equivalent of hydrogen.

Project description:Ammonia borane (AB) has high hydrogen density (19.6 wt%), and can, in principle, release up to 3 equivalents of H2 under mild catalytic conditions. A limited number of catalysts are capable of non-hydrolytic dehydrogenation of AB beyond 2 equivalents of H2 under mild conditions, but none of these is shown directly to derivatise borazine, the product formed after 2 equivalents of H2 are released. We present here a high productivity ruthenium-based catalyst for non-hydrolytic AB dehydrogenation that is capable of borazine dehydrogenation, and thus exhibits among the highest H2 productivity reported to date for anhydrous AB dehydrogenation. At 1 mol% loading, (phen)Ru(OAc)2(CO)2 () effects AB dehydrogenation through 2.7 equivalents of H2 at 70 °C, is robust through multiple charges of AB, and is water and air stable. We further demonstrate that catalyst has the ability both to dehydrogenate borazine in isolation and dehydrogenate AB itself. This is important, both because borazine derivatisation is productivity-limiting in AB dehydrogenation and because borazine is a fuel cell poison that is commonly released in H2 production from this medium.

| S-EPMC4856539 | biostudies-literature

A Three-Stage Mechanistic Model for Ammonia Borane Dehydrogenation by Shvo's Catalyst.

Project description:We propose a mechanistic model for three-stage dehydrogenation of ammonia borane (AB) catalyzed by Shvo's cyclopentadienone-ligated ruthenium complex. We provide evidence for a plausible mechanism for catalyst deactivation, the transition from fast catalysis to slow catalysis, and relate those findings to the invention of a second-generation catalyst that does not suffer from the same deactivation chemistry.The primary mechanism of catalyst deactivation is borazine-mediated hydroboration of the ruthenium species that is the active oxidant in the fast catalysis case. This transition is characterized by a change in the rate law for the reaction and changes in the apparent resting state of the catalyst. Also, in this slow catalysis situation, we see an additional intermediate in the sequence of boron, nitrogen species, aminodiborane. This occurs with concurrent generation of NH(3), which itself does not strongly affect the rate of AB dehydrogenation.

| S-EPMC3546831 | biostudies-literature

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