Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Waste-biomass-derived activated carbon supported Co–Cu–P nanocatalysts for hydrolytic dehydrogenation of ammonia borane† † Electronic supplementary information (ESI) available: ICP results of the prepared catalysts, and XPS spectrum of B 1s of the reused catalyst. See DOI: https://doi.org/10.1039/d3ra00247k

ABSTRACT: Hydrolytic dehydrogenation of ammonia borane is a significant and promising approach for on-site hydrogen production at ambient conditions, and developing highly efficient and low-cost catalysts has attracted considerable attention. Herein, waste-biomass-derived activated carbon (AC) was prepared by hydrothermal carbonization and alkali-assisted activation, and non-precious bimetal phosphides (Co–Cu–P) nanocatalysts with a series of different Co/Cu ratios were synthesized on the AC surface through in situ phosphidation method. Owing to the synergetic effects, the optimal Co0.8Cu0.2P/AC presents an outstanding turnover frequency of 26.5 min−1 (25 °C), which is much higher than that of many reported catalysts. The reaction activation energy was measured to be 34.6 kJ mol−1. Benefiting from the ferromagnetic nature of the phosphides, the Co0.8Cu0.2P/AC can be magnetically separated and reused again. After recycling six times, the catalyst still retains 72% of the initial activity, thus indicating great potential for practical applications. Biomass activated carbon was prepared using waste ginkgo leaves and then used as a support material for a Co0.8Cu0.2P nanocatalyst, and the obtained catalyst presents excellent performance for ammonia borane hydrolysis to generate hydrogen.

SUBMITTER: Wei L

PROVIDER: S-EPMC9993064 | biostudies-literature | 2023 Mar

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Porous Materials for Hydrolytic Dehydrogenation of Ammonia Borane.

Project description:Hydrogen storage is still one of the most significant issues hindering the development of a "hydrogen energy economy". Ammonia borane is notable for its high hydrogen densities. For the material, one of the main challenges is to release efficiently the maximum amount of the stored hydrogen. Hydrolysis reaction is a promising process by which hydrogen can be easily generated from this compound. High purity hydrogen from this compound can be evolved in the presence of solid acid or metal based catalyst. The reaction performance depends on the morphology and/or structure of these materials. In this review, we survey the research on nanostructured materials, especially porous materials for hydrogen generation from hydrolysis of ammonia borane.

| S-EPMC5455654 | biostudies-other

One-pot synthesis of core-shell Cu@SiO2 nanospheres and their catalysis for hydrolytic dehydrogenation of ammonia borane and hydrazine borane.

Project description:Ultrafine copper nanoparticles (Cu NPs) within porous silica nanospheres (Cu@SiO2) were prepared via a simple one-pot synthetic route in a reverse micelle system and characterized by SEM, TEM, EDX, XRD, N2 adsorption-desorption, CO-TPD, XPS, and ICP methods. The characterized results show that ultrafine Cu NPs with diameter of around 2 nm are effectively embedded in the center of well-proportioned spherical SiO2 NPs of about 25 nm in diameter. Compared to commercial SiO2 supported Cu NPs, SiO2 nanospheres supported Cu NPs, and free Cu NPs, the synthesized core-shell nanospheres Cu@SiO2 exhibit a superior catalytic activity for the hydrolytic dehydrogenation of ammonia borane (AB, NH3BH3) and hydrazine borane (HB, N2H4BH3) under ambient atmosphere at room temperature. The turnover frequencies (TOF) for the hydrolysis of AB and HB in the presence of Cu@SiO2 nanospheres were measured to be 3.24 and 7.58 mol H2 (mol Cu min)(-1), respectively, relatively high values for Cu nanocatalysts in the same reaction. In addition, the recycle tests show that the Cu@SiO2 nanospheres are still highly active in the hydrolysis of AB and HB, preserving 90 and 85% of their initial catalytic activity even after ten recycles, respectively.

| S-EPMC4274509 | 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.

| S-EPMC4607937 | biostudies-literature

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

Synthesis of rGO supported Cu@FeCo catalyst and catalytic hydrolysis of ammonia borane.

Project description:Highly dispersed Cu@FeCo/rGO catalysts have been prepared by two-step reduction method and used for hydrogen production from ammonia borane (NH3BH3, AB) hydrolysis at 298 K. The activity and reusability of synthesized composite catalyst were much more higher than Cu@FeCo for AB hydrolysis dehydrogenation at 298 K. Kinetic study manifested that AB hydrolysis dehydrogenation with Cu@FeCo/rGO catalysts was approaching to the first order at different catalyst concentrations. The hydrolysis reaction completed within four minutes, and its maximum hydrogen production rate reached to 7863.0 ml min-1 g-1 at 298 K.

| S-EPMC9782385 | biostudies-literature

Ultrafine Pd Nanoparticles Supported on Soft Nitriding Porous Carbon for Hydrogen Production from Hydrolytic Dehydrogenation of Dimethyl Amine-Borane.

Project description:Simple and efficient synthesis of a nano-catalyst with an excellent catalytic property for hydrogen generation from hydrolysis of dimethyl amine-borane (DMAB) is a missing piece. Herein, effective and recycled palladium (Pd) nanoparticles (NPs) supported on soft nitriding porous carbon (NPC) are fabricated and applied for DMAB hydrolysis. It is discovered that the soft nitriding via a low-temperature urea-pretreatment induces abundant nitrogen-containing species on the NPC support, thus promoting the affinity of the Pd precursor and hindering the agglomeration of formed Pd NPs onto the NPC surface during the preparation process. Surface-clean Pd NPs with a diameter of sub-2.0 nm deposited on the NPC support (Pd/NPC) exhibit an outstanding catalytic performance with a turnover frequency (TOF) of 2758 h-1 toward DMAB hydrolysis, better than many previous reported Pd-based catalysts. It should be emphasized that the Pd/NPC also possesses a good stability without an obvious decrease in catalytic activity for DMAB hydrolysis in five successive recycling runs. This study provides a facile but efficient way for preparing high-performance Pd catalysts for catalytic hydrogen productions.

| S-EPMC7466676 | biostudies-literature

Molybdenum catalyzed ammonia borane dehydrogenation: oxidation state specific mechanisms.

Project description:Though numerous catalysts for the dehydrogenation of ammonia borane (AB) are known, those that release >2 equiv of H2 are uncommon. Herein, we report the synthesis of Mo complexes supported by a para-terphenyl diphosphine ligand, 1, displaying metal-arene interactions. Both a Mo(0) N2 complex, 5, and a Mo(II) bis(acetonitrile) complex, 4, exhibit high levels of AB dehydrogenation, releasing over 2.0 equiv of H2. The reaction rate, extent of dehydrogenation, and reaction mechanism vary as a function of the precatalyst oxidation state. Several Mo hydrides (Mo(II)(H)2, [Mo(II)(H)](+), and [Mo(IV)(H)3](+)) relevant to AB chemistry were characterized.

| S-EPMC4140452 | biostudies-literature

Amine-functionalized MIL-53(Al) with embedded ruthenium nanoparticles as a highly efficient catalyst for the hydrolytic dehydrogenation of ammonia borane.

Project description:Well-dispersed ruthenium nanoparticles (Ru NPs) are immobilized within the pores of amine-functionalized MIL-53 via an in situ impregnation-reduction method. The resulting Ru/MIL-53(Al)-NH2 catalyst exhibits superior catalytic performance for the dehydrogenation of ammonia borane (AB) at ambient temperature relative to the Ru/MIL-53(Al) catalyst; it has a turnover frequency (TOF) of 287 mol H2 min-1 (mol Ru)-1 and an activation energy (E a) of 30.5 kJ mol-1. The amine groups present in the MIL-53(Al)-NH2 framework facilitate the formation and stabilization of ultra-small Ru NPs by preventing their aggregation. Additionally, the Ru/MIL-53(Al)-NH2 catalyst exhibits satisfactory durability and reusability: 72.4% and 86.3% of the initial catalytic activity was maintained after the fifth successive cycle of the hydrolytic dehydrogenation of AB in the two respective tests.

| S-EPMC9079245 | 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

Correction to Molybdenum catalyzed ammonia borane dehydrogenation: oxidation state specific mechanisms.

Project description: Not available

| S-EPMC4634713 | biostudies-literature