Synthesis Pd/biomass-based carbon microsheet composite for efficient dehydrogenation from formic acid

Shi, Ying; Xiang, Zhongqing; Deng, Jiawei; Nan, Jixing; Zhang, Bing

doi:10.1016/j.matlet.2018.11.074

Cited by 13 publications

(2 citation statements)

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“…As various hydrogen production technologies have become more feasible, efficient, and sustainable, the reasonable utilization of hydrogen energy has grown into an essential solution to the current energy and environmental concerns. − However, the practical application of hydrogen on the commercial scale is yet severely limited for lack of safe, efficient, and controllable hydrogen storage systems. Among many hydrogen storage systems available, chemical hydrides with high hydrogen density is regarded as ideal carriers. − Among them, ammonia borane (NH 3 BH 3 , AB) has attracted extensive attention owing to its high hydrogen storage density (19.6 wt %), mild dehydrogenation conditions, and excellent physical and chemical stability. − There are three main pathways for generating hydrogen from AB: hydrolysis, pyrolysis, and alcoholysis, of which hydrolysis is considered to be the most convenient and effective method. The hydrolysis reaction of AB on catalysts usually formulated as follows: Generally, noble metal catalysts (e.g., Pt, Ru, and Rh) are extensively employed in the hydrolysis of AB due to their excellent catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

Ultrafine PtCo Alloy Nanoclusters Confined in N-Doped Mesoporous Carbon Spheres for Efficient Ammonia Borane Hydrolysis

Yin

Zhang

Dai

et al. 2021

ACS Sustainable Chem. Eng.

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Developing cost-effective and high-efficiency catalysts for efficient ammonia borane (AB) hydrolysis is highly desirable but remains a great challenge. Ultrafine catalysts are attractive candidates in catalysis owing to abundant surface atoms. Herein, a series of ultrafine Pt x Co1–x alloy nanoclusters with an average size of 1.6 nm are homogeneously anchored within the mesoporous channels of N-doped mesoporous carbon spheres (N-MCSs) through an enhanced strong electrostatic adsorption (SEA) strategy. The ultrafine PtCo nanoclusters confined in N-MCSs lead to superior catalytic performance toward the AB hydrolysis reaction. Particularly, the optimal Pt0.33Co0.67/N-MCSs catalyst exhibits excellent performance toward the AB hydrolysis reaction. The results reveal that the highest specific rate achieves 4902 molH2 molPt –1 min–1, which is approximately 18 times higher than that of the monometallic Pt/N-MCSs catalyst. Mechanistic studies adopting kinetic isotope effects demonstrate that the O–H cleavage of H2O molecules is the rate-determine step in the AB hydrolysis reaction. Inspired by the above results, a possible reaction mechanism is proposed, which will give a new viewpoint for the rational design of cost-effective catalysts for AB hydrolysis.

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Section: Introductionmentioning

confidence: 99%

Ultrafine PtCo Alloy Nanoclusters Confined in N-Doped Mesoporous Carbon Spheres for Efficient Ammonia Borane Hydrolysis

Yin

Zhang

Dai

et al. 2021

ACS Sustainable Chem. Eng.

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“…Extensive efforts have been made to improve the catalyst performance with different combinations of active metal [13,[74][75][76][77][78] and different support materials [79][80][81][82][83][84] . However, the side product CO can cause catalyst deactivation which would be an obstacle for using formic acid in the energy applications.…”

Section: Formic Acidmentioning

confidence: 99%

Three-phase catalytic reactions in aqueous solutions: enhancing mass transfer via dewetting

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The kinetics of nitrite hydrogenation over a Pd/γ-Al2O3 catalyst was studied in a semibatch slurry reactor at atmospheric pressure, in absence of any mass transfer effects.The hydrogen concentration and pH were kept constant during an experiment by continuously flowing a gas mixture containing hydrogen and 10 % v/v CO2. The kinetic experiments were performed in an unprecedented wide concentration window of nitrite and hydrogen, revealing extreme variation in the apparent orders in hydrogen and nitrite, including reaction orders in hydrogen between 2 and 0.3, whereas the order in nitrite varied between 0.4 and -0.9. The rate of reaction is almost exclusively determined by the rate of formation of N2 as the selectivity to ammonia is very low. A Langmuir-Hinshelwood mechanism with competitive adsorption is in operation.Several mechanistic pathways, as well as possible rate determining steps in those pathways, are discussed based on these observations in combination with prior knowledge on the mechanism in literature, resulting in a revised mechanistic scheme.It is concluded that formation of NH via dissociative hydrogenation of HNOH is the rate determining step, whereas molecular N2 forms via reaction of NH with either NO, NOH or HNOH. N-N bond formation via dimerization of adsorbed NO or adsorbed N can be excluded.Three-phase catalytic reactions in aqueous solutions--Enhancing mass transfer via dewetting 29 * + * ⇋ * + * ( equilibrium reaction 4, 4 )

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Sugar Acid–Assisted Thermolysis of All‐Solid‐State Ammonia Borane Hydrogen Fuel

2020

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An all‐solid‐state hydrogen fuel composite composed of ammonia borane (AB), a chemical hydride containing 19.6 wt% hydrogen, and mucic acid (MA) is used as a hydrogen fuel source in thermal dehydrogenation. AB thermolysis provides a hydrogen‐driven proton‐exchange membrane fuel cell with selective, on‐demand hydrogen generation by simply heating the pellet‐type composite. MA, a six‐carbon sugar acid containing two carboxylic acid groups at the C1 and C6 positions and four hydroxyl groups at the C2, C3, C4, and C5 positions, forms an optimized composite with AB (AB:MA = 8:2) to undergo a thermal dehydrogenation reaction to produce 10.77 wt% pure H2 at 80 °C in 1 min. Adipic acid (AA), a six‐carbon dioic acid without hydroxyl groups, is used as an analogue of MA and shows no catalytic effect in the AB+AA thermolysis process. It is believed that the AB+MA composite obeys the conventional alcoholysis mechanism in the thermolysis process.

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Synthesis Pd/biomass-based carbon microsheet composite for efficient dehydrogenation from formic acid

Cited by 13 publications

References 13 publications

Ultrafine PtCo Alloy Nanoclusters Confined in N-Doped Mesoporous Carbon Spheres for Efficient Ammonia Borane Hydrolysis

Ultrafine PtCo Alloy Nanoclusters Confined in N-Doped Mesoporous Carbon Spheres for Efficient Ammonia Borane Hydrolysis

Three-phase catalytic reactions in aqueous solutions: enhancing mass transfer via dewetting

Sugar Acid–Assisted Thermolysis of All‐Solid‐State Ammonia Borane Hydrogen Fuel

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