In Situ Generation of Active Pd Nanoparticles within a Macroreticular Acidic Resin: Efficient Catalyst for the Direct Synthesis of Hydrogen Peroxide

Mori, Kohsuke; Hanafusa, Akihiro; Che, Michel; Yamashita, Hiromi

doi:10.1021/jz100509x

Cited by 29 publications

(14 citation statements)

References 27 publications

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“…9i In the present catalytic system, it is reasonable to conclude that the existence of suitable amine functionality in the vicinity of active PdCu centers exerts a cooperative action without the additional dosage of amine reagents. Consequently, catalytically active species generated within a functional resin matrix essentially differ from conventional solid supported metal catalysts 14…”

Section: Resultsmentioning

confidence: 99%

“…Consequently,c atalytically active speciesg enerated within af unctional resin matrix essentially differ from conventional solid supported metal catalysts. [14] Recently,P dAg and PdAu bimetallic catalysts including alloy, core-shell structure, and monodispersed NPs were extensively studied for the decomposition of formic acid. In general, such bimetallic catalysts were reported to possess improved HCOOHd ehydrogenation activity and stabilityr elative to monometallic Pd catalysts.…”

Section: Mechanistic Investigationsmentioning

confidence: 99%

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Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid

Mori

Tanaka

Dojo

et al. 2015

Chemistry A European J

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106

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Highly dispersed PdCu alloy nanoparticles have been successfully prepared within a macroreticular basic resin bearing N(CH3 )2 functional groups. This previously unappreciated combination of alloy is first proven to be responsible for the efficient production of high-purity H2 from formic acid (HCOOH) dehydrogenation for chemical hydrogen storage. By the addition of Cu, the electronically promoted Pd sites show significantly higher catalytic activity as well as a better tolerance towards CO poisoning as compared to their monometallic Pd counterparts. Experimental and DFT calculation studies revealed not only the synergic alloying effect but also cooperative action by the N(CH3 )2 groups within the resin play crucial roles in achieving exceptional catalytic performances. In addition to the advantages such as, facile preparation method, free of additives, recyclable without leaching of active component, and suppression of unfavorable CO formation less than 3 ppm, the present catalytic system is cost-effective because of the superior catalytic activity compared with that of well-established precious PdAg or PdAu catalysts. The present catalytic system is particularly desirable for an ideal hydrogen vector in terms of potential industrial application for fuel cells.

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Section: Resultsmentioning

confidence: 99%

Section: Mechanistic Investigationsmentioning

confidence: 99%

Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid

Mori

Tanaka

Dojo

et al. 2015

Chemistry A European J

Self Cite

106

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“…Functional resins have also been reported as suitable supports for H 2 O 2 synthesis. 104 Blanco-Brieva et al 48 reported that the anchorage of Pd II ions into mesoporous ion-exchange resins functionalized with sulfonic groups produced highly efficient catalysts, resulting in hydrogen peroxide production rates close to 1100 mol H 2 O 2 kg Pd −1 h −1 when using methanol as a solvent at 40 °C and 10.0 MPa. This high performance was attributed to the ability of the sulfonic acid groups of the resin to interact with and stabilize the Pd II ions without further reduction to Pd 0 .…”

Section: Membrane Reactorsmentioning

confidence: 99%

Engineering in direct synthesis of hydrogen peroxide: targets, reactors and guidelines for operational conditions

et al. 2014

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The demand for hydrogen peroxide is booming since it is considered as one of the most environmentally friendly and versatile chemical oxidants available and has a wide range of applications. The annual market, close to 3000 kt per year being produced via the auto-oxidation process (with 2-ethyl anthraquinone (traditional) or amyl anthraquinone for mega-plants), is mostly supplied by the company Solvay (30%), followed by Evonik (20%) and Arkema (13%). Nevertheless, the dream of a direct synthesis process is close to a century old and it has gained momentum in research efforts during the last decade with more than 15 groups active in the world. In this review, we focus the discussion on the targets, e.g. plant tonnage, the reactors and the most feasible industrial operational conditions, based on our experience and point of view using the chemical engineering tools available. Thus, direct synthesis can be competitive when on-site production is required and capacities less than 10 kt per year are He has led and participated in 3 EU, 6 national/regional projects and 10+ SME contracts and has published 30+ research papers. Teresa MorenoTeresa Moreno obtained her degree in Chemical Engineering from Complutense University (Madrid, Spain) and later completed her PhD in Chemical Engineering at the University of Valladolid (Spain, 2011) studying the catalytic direct synthesis of hydrogen peroxide in supercritical CO 2 and the online determination of the product using Raman spectroscopy. She is currently a Research Scientist in the Industrial Bioactive Technologies Group at Callaghan Innovation (New Zealand) working on the development of processes for adding value to natural materials toward high value products and applications, including the development of sustainable technologies using supercritical fluids. View Article OnlineView Journal | View Issue and semi-continuous modes of operation. However, at the moment, demonstrations of continuous operations as well as carefully determined kinetics are needed in order to scale up the process. Finally, operational conditions, including the catalyst composition (active metal, oxidation state and support), promoters (halides and acids-pH-isoelectric point), solvents, pressure and temperature need to be carefully analysed. In our opinion, as we try to show here, H 2 O 2 direct synthesis is a competitive process and is ready for larger scale demonstration. Also, more than a hundred patents within the area support this claim, although the barriers of technology demonstration and further licensing are still pending.

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“…We found that an acidic resin bearing SO 3 H functional groups within its reticular structure acts as an efficient support for the in situ formation of highly active Pd NPs responsible for the direct synthesis of H 2 O 2 from H 2 and O 2 . 116 The PdCl 2 precursor species was easily deposited on an acidic resin bearing SO 3 H functional groups by a simple ion exchange method (Pd/resin A). As a comparison, a resin having NMe 3 Cl groups was also employed as a basic support (Pd/resin B).…”

Section: In Situ Generation Of Active Nps Within a Macroreticular Resinmentioning

confidence: 99%

Progress in design and architecture of metal nanoparticles for catalytic applications

Mori

Yamashita

2010

Phys. Chem. Chem. Phys.

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Over the past few years, nanometer-sized transition metal particles have been intensively pursued as potentially advanced catalysts because their special properties lie between those of single metal atoms and bulk metal. Achieving the accurate control of particle size and overall particle size distribution is one of the most crucial challenges to provide unique chemical and physical properties. We highlight herein our recent progress in the exploitation of promising nanoparticle (NP)-based catalysts designed by precise architecture that enable efficient and selective chemical transformations and can be completely separated and are recyclable. This perspective article consists of the following two specific topics: (i) multifunctional catalysts based on magnetic NPs and (ii) new routes for the preparation of supported metal NPs catalysts. The synthetic strategies described here are simple and general for practical catalyst design, thus allowing a strong protocol for creating various nanostructured catalysts.

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In Situ Generation of Active Pd Nanoparticles within a Macroreticular Acidic Resin: Efficient Catalyst for the Direct Synthesis of Hydrogen Peroxide

Cited by 29 publications

References 27 publications

Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid

Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid

Engineering in direct synthesis of hydrogen peroxide: targets, reactors and guidelines for operational conditions

Progress in design and architecture of metal nanoparticles for catalytic applications

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