An effective amino acid-assisted growth of ultrafine palladium nanocatalysts toward superior synergistic catalysis for hydrogen generation from formic acid

Hong, Cheng‐Bin; Zhu, Dejie; Ma, Dongdong; Wu, Xintao; Zhu, Qi‐Long

doi:10.1039/c9qi00037b

Cited by 15 publications

(14 citation statements)

References 46 publications

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“…Generally, Pd nanoparticle (NP) catalysts have shown an activity for CO 2 -neutral hydrogen storage/release systems. − Their activity can be enhanced by choosing a suitable support that increases the nanoparticle dispersion and alters the electronic structures of the active metals via the metal–support interactions, which determines the size and electronic effects of metal NPs. − Recent studies have shown that nitrogen-doped carbon nanomaterials are efficient, low-cost alternatives for numerous energy applications, such as batteries, supercapacitors, fuel cells, and catalyst supports due to their excellent physical, chemical, and mechanical properties. , To date, both computational and experimental studies have shown that co-doping N-doped carbon materials with a second heteroatom, such as B, S, or P, can modulate the electronic properties and surface polarities to further increase the catalytic activity. Additionally, co-doping with two elements with different electronegativities (χ), such as N (χ = 3.04) and P (χ = 2.19), can create a unique electronic structure that produces a synergistic coupling effect between heteroatoms.…”

Section: Introductionmentioning

confidence: 99%

Pd Nanoparticles Supported on N- and P-Co-doped Carbon as Catalysts for Reversible Formate-Based Chemical Hydrogen Storage

Shao

Miao

Zhang

et al. 2020

ACS Appl. Nano Mater.

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Efficient and reversible hydrogen-storage systems derived from liquid organic compounds are promising alternatives for sustainable energy supplies. Here, we report a Pd nanoparticle catalyst supported on porous carbon co-doped with nitrogen and phosphorous for reversible formate-based chemical hydrogen storage. The materials showed good catalytic performance for both formate dehydrogenation and bicarbonate hydrogenation. The N,P-dual-doped carbon was fabricated by directly pyrolyzing a mixture of 1,10-phenanthroline and triphenylphosphine. Initial density functional theory (DFT) studies suggested that N and P codopants played synergistic roles in modulating the electronic properties of the carbon support. X-ray photoelectron spectroscopy and CO pulse adsorption experiments revealed that the resulting metal−support interactions enriched the electron density at the Pd active site. This promoted the activity of Pd nanoparticles for formate dehydrogenation with a turnover frequency of 3254 h −1 , and a high formate yield exceeding that of individual N-doped or P-doped catalysts was also obtained for the hydrogenation of bicarbonate.

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Section: Introductionmentioning

confidence: 99%

Pd Nanoparticles Supported on N- and P-Co-doped Carbon as Catalysts for Reversible Formate-Based Chemical Hydrogen Storage

Shao

Miao

Zhang

et al. 2020

ACS Appl. Nano Mater.

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“…The increase in ΔG ‡ with increase in temperature shown in Table 4 suggested greater favorability of the Cr(VI) conversion process at lower temperature. Given that, as detailed in previous studies of the dehydrogenation of HCOOH on Pd-based catalysts 63 , 64 , the rate of hydrogen gas generation by adsorbed hydrogen atom recombination following the decarboxylation of HCOOH (Fig. 2 ) also increases with increase in temperature, favorability of the Cr(VI) conversion process at lower temperature could be attributed to diminution of the hydrogen recombination stage of HCOOH dehydrogenation.…”

Section: Resultsmentioning

confidence: 53%

Application of polymer-coated Macadamia integrifolia nutshell biomass impregnated with palladium for chromium(VI) remediation

Moyo

Modise

Pakade

2021

Sci Rep

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Freely suspended and porous basket restrained granules of palladium nanoparticles supported on polymer-grafted Macadamia nutshell biomass (Pd@Polym-MNS) composite were used for the treatment chromium(VI)-containing water. In the presence of formic acid, the Pd@Polym-MNS demonstrated its activity in the adsorption-reduction-based conversion of noxious chromium(VI) to less toxic chromium(III) with a low activation energy of 13.4 kJ mol–1, ΔH0 (+ 10.8 kJ mol–1), ΔS0 (−270.0 J mol–1 K–1), and ΔG0 (+ 91.3 to + 98.0 kJ mol–1) indicated the exothermic, endergonic and non-spontaneous nature of the catalytic redox reaction. In addition to facilitating easy recovery, rinsing, and reuse, restraining the Pd@Polym-MNS in the basket reactor helped maintain the integrity of the catalysts by preventing violent collisions of suspended granules with the mixing apparatus and the walls of the reaction vessel. Whereas the pseudo-first-order rate constant was recorded as 0.157 min–1 upon initial use, values of the mean and relative standard deviation for the second, third and fourth consecutive uses were found to be 0.219 min–1 and 1.3%, respectively. According to a response surface methodological approach to batch experimentation, the initial concentration of chromium(VI) and catalyst dosage had the greatest impact on the redox reaction rate, accounting for 85.7% and 11.6% of the variability in the value of the pseudo-first-order rate constant, respectively. Mutually beneficial effects of the combinations of high formic acid and low chromium(VI) concentration, high temperature and catalyst dosage as well as high formic acid and catalyst dosage were recorded.

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“…To evaluate the performance of Pd NPs @SBA-15/DTC (2.89 wt% Pd, determined by ICP analysis), for catalytic H 2 production, we utilize FA/SF (1: 1) as the reaction substrate. Very recently, a variety of noble metal NPs [54][55][56] has been used to catalyze the selective dehydrogenation of FA under mild conditions. Remarkably, Pd NPs @SBA-15/DTC had catalytic activity comparable to immobilized Pd complex (Pd (II) @SBA-15/ DTC), Pd (II) @SBA-15, SBA-15/DTC, and SBA-15 without the use of any additive in presence ultrasonic wave.…”

Section: Resultsmentioning

confidence: 99%

Anchoring Pd-nanoparticles on dithiocarbamate- functionalized SBA-15 for hydrogen generation from formic acid

Farajzadeh

Alamgholiloo

Nasibipour

et al. 2020

Sci Rep

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Hydrogen (H2) generation from natural biological metabolic products has remained a huge challenge for the energy arena. However, designing a catalytic system with complementary properties including high surface area, high loading, and easy separation offers a promising route for efficient utilization of nanoreactors for prospective H2 suppliers to a fuel cell. Herein, selective dehydrogenation of formic acid (FA) as a natural biological metabolic product to H2 and CO2 gas mixtures has been studied by supporting ultrafine palladium nanoparticles on organosulfur-functionalized SBA-15 nanoreactor under ultrasonic irradiation. The effects of the porous structure as a nanoreactor, and organosulfur groups, which presented around the Pd due to their prominent roles in anchoring and stabilizing of Pd NPs, studied as a superior catalyst for selective dehydrogenation of FA. Whole catalytic systems were utilized in ultrasonic irradiation in the absence of additives to provide excellent TOF/TON values. It was found that propose catalyst is a greener, recyclable, and more suitable option for the large-scale application and provide some new insights into stabilization of ultra-fine metal nanoparticle for a variety of applications.

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An effective amino acid-assisted growth of ultrafine palladium nanocatalysts toward superior synergistic catalysis for hydrogen generation from formic acid

Abstract: An amino acid-assisted approach is developed to immobilize ultrafine Pd NPs onto mesoporous carbon, which exhibits remarkable catalytic activity for hydrogen generation.

Cited by 15 publications

References 46 publications

Pd Nanoparticles Supported on N- and P-Co-doped Carbon as Catalysts for Reversible Formate-Based Chemical Hydrogen Storage

Pd Nanoparticles Supported on N- and P-Co-doped Carbon as Catalysts for Reversible Formate-Based Chemical Hydrogen Storage

Application of polymer-coated Macadamia integrifolia nutshell biomass impregnated with palladium for chromium(VI) remediation

Anchoring Pd-nanoparticles on dithiocarbamate- functionalized SBA-15 for hydrogen generation from formic acid

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