Highly selective synthesis of methanol from methane over carbon materials supported Pd-Au nanoparticles under mild conditions

He, Yingluo; Liang, J. Nellie; Imai, Yusuke; Ueda, Koki; Li, Hangjie; Guo, Xiaoyu; Yang, Guohui; Yoneyama, Yoshiharu; Tsubaki, Noritatsu

doi:10.1016/j.cattod.2019.10.017

Cited by 26 publications

(24 citation statements)

References 45 publications

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“…As the Pd content decreases, the binding energies of Pd 3d in alloyed Pd x Au y NWs show a gradual negative shift, which is attributed to a charge transfer between Pd and Au atom in the Pd x Au y interaction . Moreover, the Pd 3d of alloyed Pd 12 Au 1 NWs still exhibits a higher binding energy, compared with that of metallic Pd, which could become the active sites for the direct methane conversion . When an approximate 50 at% Pd alloy composition, an obvious shift is observed for the alloyed Pd 1 Au 1 NWs, due to the redistribution of occupied valence.…”

Section: Results and Discussionmentioning

confidence: 98%

“…29 Moreover, the Pd 3d of alloyed Pd 12 Au 1 NWs still exhibits a higher binding energy, compared with that of metallic Pd, which could become the active sites for the direct methane conversion. 33 When an approximate 50 at% Pd alloy composition, an obvious shift is observed for the alloyed Pd 1 Au 1 NWs, due to the redistribution of occupied valence.…”

Section: Characterizations Of Alloyed Pdmentioning

confidence: 99%

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Engineering PdAu Nanowires for Highly Efficient Direct Methane Conversion to Methanol under Mild Conditions

Zhong

et al. 2021

J. Phys. Chem. C

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The direct conversion of methane to high-value chemical feedstock is immensely meaningful but challenging. This work reports the preparation of alloyed Pd x Au y nanowires (NWs) with different Pd/Au atom ratios by using a simple and facile method. The influence of alloyed Pd x Au y NWs structure and reaction conditions have been methodically studied for the direct methane conversion process. It is proposed that the proper adsorption capacity of methane and the electronic synergy effect for alloyed Pd x Au y NWs are the key factors to improve methane conversion and methanol selectivity. In addition, alloyed Pd x Au y NWs show an excellent selectivity over 90% for methanol product due to the special one-dimensional structure, and the Pd12Au1 NWs catalyst exhibits the highest yield of methanol product of 522.5 μmol g–1 h–1 at 70 °C with adding 500 μmol H2O2. This work demonstrates the use of alloyed Pd x Au y NWs catalysts for the direct conversion of methane to methanol with high-efficiency and selectivity and offers intriguing pathways to further boost their performance in catalysis reactions.

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Section: Results and Discussionmentioning

confidence: 98%

Section: Characterizations Of Alloyed Pdmentioning

confidence: 99%

Engineering PdAu Nanowires for Highly Efficient Direct Methane Conversion to Methanol under Mild Conditions

Zhong

et al. 2021

J. Phys. Chem. C

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“…Because the zeolite has open micropores, the molecules, particularly those with small sizes, could easily escape from the zeolite crystals. For example, in the oxidation of methane with hydrogen and oxygen (CH 4 + H 2 + O 2 → CH 3 OH + H 2 O) over supported metal nanoparticles, the H 2 O 2 (or other peroxide intermediate species) generated from hydrogen and oxygen favors dissolution in the reaction liquor to form a dilute solution with poor activity. , By using the zeolite fixed metal catalysts, the H 2 O 2 species could be efficiently enriched. Considering the hydrophilicity of H 2 O 2 , we constructed a hydrophobic sheath around the zeolite crystals to hinder the H 2 O 2 diffusion (Figure a) .…”

Section: Catalytic Performances Adjusted By Zeolite Wettabilitymentioning

confidence: 99%

Zeolite Fixed Metal Nanoparticles: New Perspective in Catalysis

Wang

et al. 2021

Acc. Chem. Res.

159

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Conspectus Loading metal nanoparticles on the surface of solid supports has emerged as an efficient route for the preparation of heterogeneous catalysts. Notably, most of these supported metal nanoparticles still have shortcomings such as dissatisfactory activity and low product selectivity in catalysis. In addition, these metal nanoparticles also suffer from deactivation because of nanoparticle sintering, leaching, and coke formation under harsh conditions. The fixation of metal nanoparticles within zeolite crystals should have advantages of high activities for metal nanoparticles and excellent shape selectivity for zeolite micropores as well as extraordinary stability of metal nanoparticles immobilized with a stable zeolite framework, which is a good solution for the shortcomings of supported metal nanoparticles. Materials with metal nanostructures within the zeolite crystals are normally denoted as metal@zeolite, where the metal nanoparticles with diameters similar to those of industrial catalysts are usually larger than the micropore size. These metal nanoparticles are enveloped with the zeolite rigid framework to prevent migration under harsh reaction conditions, which is described as a fixed structure. The zeolite micropores allow the diffusion of reactants to the metal nanoparticles. As a result, metal@zeolite catalysts combine the features of both metal nanoparticles (high activity) and zeolites (shape selectivity and thermal stability), compared with the supported metal nanoparticles. In this Account, we describe how the zeolite micropore and metal nanoparticle synergistically work to improve the catalytic performance by the preparation of a variety of metal@zeolite catalysts. Multiple functions of zeolites with respect to the metal nanoparticles are highlighted, including control of the reactant/product diffusion in the micropores, the adjustment of reactant adsorption on the metal nanoparticles, and sieving the reactants and products with zeolite micropores. Furthermore, by optimizing the wettability of the zeolite external surface, the zeolite crystals could form a nanoreactor to efficiently enrich the crucial intermediates, thus boosting the performance in low-temperature methane oxidation. Also, the microporous confinement weakens the adsorption of C1 intermediates on the metal sites, accelerating the C–C coupling to improve C2 oxygenate productivity in syngas conversion. In particular, the zeolite framework efficiently stabilizes the metal nanoparticles against sintering and leaching to give durable catalysts. Clearly, this strategy not only guides the rational design of efficient heterogeneous catalysts for potential applications in a variety of industrial chemical reactions but also accelerates the fundamental understanding of the catalytic mechanisms by providing new model catalysts.

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“…The direct methane activation with in situ generation of H2O2 promoted methanol formation [32,66]. The high affinity for oxygen of gold facilitates the breakdown of H2O2 in OH•, which would be the activator of the C-H breakage [73,115,116].…”

Section: Materials For Methane Partial Oxidation Reactionmentioning

confidence: 99%

Partial Methane Oxidation in Fuel Cell-Type Reactors for Co-Generation of Energy and Chemicals

Souza¹,

Florio²,

Antolini³

et al. 2022

Preprint

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The conversion of methane into chemicals is of interest to achieve a decarbonized future. Fuel cells are electrochemical devices commonly used to obtain electrical energy, but can be utilized either for chemicals production or both energy and chemicals cogeneration. In this work, the partial oxidation of methane in fuel cells for electricity generation and valuable chemicals production at the same time is reviewed. For this purpose, different types of methane-fed fuel cells, both low temperature fuel cells, such as PEMFCs and AAEMFCs, and high temperature fuel cells, such as SOFCs, have been used. Also if few works have been devoted to this topic, the promising results drive the development of fuel cells using methane as the source for the cogeneration of power and valuable chemicals.

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Highly selective synthesis of methanol from methane over carbon materials supported Pd-Au nanoparticles under mild conditions

Cited by 26 publications

References 45 publications

Engineering PdAu Nanowires for Highly Efficient Direct Methane Conversion to Methanol under Mild Conditions

Engineering PdAu Nanowires for Highly Efficient Direct Methane Conversion to Methanol under Mild Conditions

Zeolite Fixed Metal Nanoparticles: New Perspective in Catalysis

Partial Methane Oxidation in Fuel Cell-Type Reactors for Co-Generation of Energy and Chemicals

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