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Experimental and theoretical investigation of high-entropy-alloy/support as a catalyst for reduction reactions

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Journal of Energy Chemistry 2023年第6期81卷 132-142,I0005页

作者： Wail Al Zoubi Bassem Assfour Abdul Wahab Allaf Stefano Leoni Jee-Hyun Kang Young Gun Ko Materials Electrochemistry Laboratory School of Materials Science and EngineeringYeungnam UniversityGyeongsan 38541Republic of Korea Atomic Energy Commission Department of ChemistryP.O.Box 6091DamascusSyria Arab International University Department of Pharmaceutical Chemistry and Quality ControlFaculty of PharmacyGhabaghibDarraSyria Cardiff University School of ChemistryPark PlaceCF103AT CardiffUnited Kingdom School of Materials Science and Engineering Institute of Materials TechnologyYeungnam UniversityGyeongsan 38541Republic of Korea

Control of chemical composition and incorporation of multiple metallic elements into a single metal nanoparticle(NP)in an alloyed or a phase-segregated state hold potential scientific merit;however,developing libraries of such structures using effective strategies is challenging owing to the thermodynamic immiscibility of repelling constituent metallic elements.Herein,we present a one-pot interfacial plasma-discharge-driven(IP-D)synthesis strategy for fabricating stable high-entropy-alloy(HEA)NPs exhibiting ultrasmall size on a porous support surface.Accordingly,an electric field was applied for 120 s to enhance the incorporation of multiple metallic elements(i.e.,CuAgFe,CuAgNi,and CuAgNiFe)into ally HEA-NPs.Further,NPs were attached to a porous magnesium oxide surface via rapid cooling.With solar light as the sole energy input,the CuAgNiFe catalyst was investigated as a reusable and sustainable material exhibiting excellent catalytic performance(100%conversion and 99% selectivity within1 min for a hydrogenation reaction)and consistent activity even after 20 cycles for a reduction reaction,considerably outperforming the majority of the conventional photocatalysts.Thus,the proposed strategy establishes a novel method for designing and synthesizing highly efficient and stable catalysts for the convertion of nitroarenes to anilines via chemical reduction.

关键词： Plasma Miscible Multicomponent metal nanoparticle Nanocatalysts

Robust hydrogen production from HCOOH over amino-modified KIT-6-confined Pd Ir alloy nanoparticles

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Chinese Chemical Letters 2022年第3期33卷 1403-1406页

作者： Wenfang Peng Shiwen Liu Xiugang Li Gang Feng Jianhui Xia Zhang-Hui Lu Key Laboratory of Functional Small Molecules for Ministry of Education College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022China Jiangxi Provincial Center for Disease Control and Prevention Nanchang 330029China College of Chemistry Nanchang UniversityNanchang 330031China

Formic acid (FA), which can be produced via CO_(2) reduction and biomass conversion, has received extensive interest as a convenient and safe hydrogen carrier due to its wide range of sources, renewable, high hydrogen content (4.4 wt%), and convenient storage/transportation. Designing highly efficient catalysts is the main challenge to realize the hydrogen production from FA. In this work, well-dispersed and electron-rich PdIr alloy nanoparticles with a size of 1.8 nm are confined in amino-modified 3D mesoporous silica KIT-6 and applied as a highly efficient catalyst for robust hydrogen production from FA at ambient temperature. Small PdIr alloy nanoparticles confined by amino-modified KIT-6 (PdIr/KIT-6-NH_(2)) lead to better catalytic activity compared to that of Pd/KIT-6-NH_(2) and PdIr confined by bare KIT-6, achieving a high turnover frequency (TOF) value of 3533 h-1 at ambient temperature (303 K), 100% H_(2) selectivity and conversion toward the dehydrogenation of FA, which is comparable to the best heterogeneous catalysts ever reported. The high catalytic activity of PdIr/KIT-6-NH_(2) can be attributed to the synergistic effect between Pd and Ir, strong interaction between PdIr and KIT-6-NH_(2), as well as the amino-groups of KIT-6-NH_(2) which can act as a proton scavenger to promote the breaking of O-H bond of formic acid.

关键词： Formic acid Hydrogen production Palladium metal nanoparticle 3D mesoporous silica

Laser-induced Synthesis of Ultrafine Gold nanoparticles in Covalent Organic Frameworks

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Chemical Research in Chinese Universities 2022年第2期38卷 468-471页

作者： ZHANG Yin MA Shengqian Department of Chemistry University of North TexasDentonTX 76201USA

metal nanoparticles in porous supports are of great importance for catalysis, separation and sensing, but their controllable preparation is still largely unmet. Herein, we describe a simple laser-induced synthesis of ultrafine gold nanoparticles in the covalent organic framework. Gold nanoparticles are well embedded, and they are about (1±0.1) nm in size. This work is universal for the preparation of well-dispersed and ultrafine metal nanoparticles in porous supports.

关键词： metal nanoparticle Covalent organic framework(COF) Ultrafine Photoreduction

Thermodynamic analysis and modification of Gibbs–Thomson equation for melting point depression of metal nanoparticles

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Chinese Journal of Chemical Engineering 2021年第3期34卷 198-205页

作者： Nanhua Wu Xiaohua Lu Rong An Xiaoyan Ji Division of Energy Science/Energy Engineering LuleåUniversity of Technology97187 LuleåSweden State Key Laboratory of Materials-Oriented and Chemical Engineering Nanjing Tech UniversityNanjing 211816China Key Laboratory of Advanced Catalytic Materials and Technology School of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China Herbert Gleiter Institute of Nanoscience Nanjing University of Science&TechnologyNanjing 210094China

Abnormal melting point depression of metal nanoparticles often occurs in heterogeneous catalytic reactions,which leads to a reduction in the stability of reactive nanoclusters.To study this abnormal phenomenon,the original and surface-energy modified Gibbs-Thomson equations were analyzed in this work and further modified by considering the effect of the substrate.The results revealed that the original Gibbs-Thomson equation was not suitable for the particles with radii smaller than 10 nm.Moreover,the performance of the surface-energy modified Gibbs-Thomson equation was improved,and the deviation was reduced to(-350-100)K,although further modification of the equation by considering the interfacial effect was necessary for the small particles(rmetal and substrate.Additionally,the micro-wetting parameterα_W can be used to qualitatively study the overall impact of the substrate on the melting point depression.

关键词： Melting point depression metal nanoparticle Gibbs–Thomson equation Substrate Interfacial effect

Inorganic shell nanostructures to enhance performance and stability of metal nanoparticles in catalytic applications

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Rare metals 2020年第7期39卷 767-783页

作者： Inhee Choi Hyeon Kyeong Lee Gyoung Woo Lee Jiyull Kim Ji Bong Joo Department of Life Science University of SeoulSeoul 02504Republic of Korea Division of Chemical Engineering Konkuk UniversitySeoul 05029Republic of Korea

In this article,we review the recent progress and our research activity on the synthesis of inorganic shell nanostructures to enhance the catalytic performance and stability of metal nanoparticles in catalytic applications.First,we introduce general synthetic strategies for the fabrication of inorganic nanoscale shell layers,including template-assisted sol-gel coating,hydrothermal(or solvothermal)synthesis and the self-templating process.We also discuss recent examples of metal nanoparticles(NPs)with nanoscale shell layers,namely core-shell,yolk-shell and multiple NPs-embedded nanoscale shell.We then discuss the performance and stability of metal particles in practical catalytic applications.Finally,we conclude with a summary and perspective on the further progress of inorganic nanostructure with nanoscale shell layers for catalytic applications.

关键词： Nanostructures Inorganic shell metal nanoparticle Stabilization Performance enhancement Catalyst

Fabrication of metal nanoparticles on highly dispersed pristine carbon nanotubes

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International Journal of Smart and Nano Materials 2011年第2期2卷 92-100页

作者： Jianhua Zou Binh Tran Lei Zhai NanoScience Technology Center and Department of Chemistry University of Central FloridaOrlandoFL 32826USA

A convenient approach to fabricate metal(i.***.gold,platinum,and palladium)nanoparticles on highly dispersed pristine carbon nanotubes(CNTs)was developed using a conjugated block copolymer of poly(3-hexylthiophene)-b-poly(vinylpyrrolidone)(P3HT-b-PVP).P3HT-b-PVP not only provides a stable dispersion of pristine CNTs through theπ–πinteractions between P3HT block and CNTs,but also introduces PVP groups on CNT surfaces to induce the heterogeneous nucleation of metal nanoparticles and protect them from aggregating.The density of metal nanoparticles on CNT surfaces was controlled by the metal salt/CNT feed ratio.The simple processing procedure,versatility in synthesizing various metal nanoparticles,high metal nanoparticle loading capacity,and excellent dispersibility and processability of the product make this approach a promising method to fabricate metal nanoparticles on CNTs.

关键词： metal nanoparticle carbon nanotube composite

Conversion of Methane to Ethylene with BaCe_(0.9)Y_(0.1)Co_(x)O_(3-δ)Hydrogen Permeation Membrane

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Chinese Journal of Structural Chemistry 2021年第7期40卷 901-907,839页

作者：刘允袁盛泽谢奎 College of Chemistry Fuzhou UniversityFuzhou 350116China Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China

Dehydrogenation coupling of methane(DCM),which can be effectively used to produce low carbon alkenes,has the advantages of rich raw materials,simple reaction device,low energy consumption,etc.Herein,we report a series of Co doped perovskite porous-dense BaCe_(0.9)Y_(0.1)Co_(x)O_(3-δ)(BCYCx)membrane for DCM.After treatment in a reduced atmosphere,a large number of Co nanoparticles will exsolute on the surface of BCY.The metal-oxide interface is helpful to activate the C–H bonds,inhibit the carbon deposition,and so on.The XRD,SEM and XPS prove that Co nanoparticles homogeneously distributed on the BCYCx porous layers,which will create a large quantity of catalytic active sites.At 1100℃,the highest concentration of C_(2)product was 5.66%(5.25%ethane+0.41%ethylene)in output gas when methane conversion reaches a maximum value of 24.8%,and the C_(2)selectivity gets to 45.6%.We further demonstrate the catalytic performance of high-temperature DCM without obvious decrease after running for 30 hours.

关键词： mixed-conducting dehydrogenation methane metal nanoparticle membrane

Pillarene-Involved metallic Supramolecular Nanostructures

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中国化学:英文版 2015年第3期33卷 319-328页

作者： Chang-Wei Zhang Li-Jun Chen Hai-Bo Yang Shanghai Key Laboratory of Green Chemistry and Chemical Processes Department of ChemistryEast China Normal UniversityShanghai 200062China

Pillarenes(or pillararenes),as a new and rapidly developing class of covalent macrocycles,have stimulated a tremendous upsurge of interest in supramolecular chemistry because of their unique features and potentials in fabri-cating functional materials.In addition,metallo-supramolecular chemistry has grown steadily over the last few decades.The presence of metal in supramolecular architectures enables the systematic tuning of their properties and endows them with optical,magnetic,and electric etcetera unusual properties.The marriage of these two fields offers new possibilities for the fabrication of novel functional materials and devices.This review article provides an over-view of recent advancements on pillararene-based metallic supramolecular assemblies.The fabrication and func-tionalities of pillararene-decorated metallic macrocycles,metal-organic frameworks(MOFs),and metal nanoparti-cles are comprehensively summarized and discussed.

关键词： self-assembly pillararene metallacycle metal−organic frameworks metal nanoparticle

Conversion of Methane to Ethylene with BaCe;Y;Co;O;Hydrogen Permeation Membrane

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Chinese Journal of Structural Chemistry 2021年

作者：刘允袁盛泽谢奎 CollegeofChemistry，FuzhouUniversity KeyLaboratoryofDesignandAssemblyofFunctionalNanostructures，FujianInstituteofResearchontheStructureofMatter，ChineseAcademyofSciences CollegeofChemistryandMaterialsScience，FujianNormalUniversity

Dehydrogenation coupling of methane （DCM）， which can be effectively used to produce low carbon alkenes， has the advantages of rich raw materials， simple reaction device， low energy consumption， etc. Herein， we report a series of Co doped perovskite porous-dense BaCe;Y;Co;O;（BCYCx） membrane for DCM. After treatment in a reduced atmosphere， a large number of Co nanoparticles will exsolute on the surface of BCY. The metal-oxide interface is helpful to activate the C–H bonds， inhibit the carbon deposition， and so on. The XRD， SEM and XPS prove that Co nanoparticles homogeneously distributed on the BCYCx porous layers， which will create a large quantity of catalytic active sites. At 1100 ℃， the highest concentration of C;product was 5.66% （5.25% ethane + 0.41% ethylene） in output gas when methane conversion reaches a maximum value of 24.8%， and the C;selectivity gets to 45.6%. We further demonstrate the catalytic performance of high-temperature DCM without obvious decrease after running for 30 hours.

关键词： mixed-conducting dehydrogenation methane metal nanoparticle membrane