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Enhanced ethanol oxidation over pd nanoparticles supported porous graphene-doped MXene using polystyrene particles as sacrificial templates

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Rare Metals 2022年第9期41卷 3170-3179页

作者： Yi-Zhe Chen Ming Zhou Yu-Fu Huang Yan-Yun Ma Luo-Yi Yan Xin-Wen Zhou Xin-Zhou Ma Xue-Ling Zhao Cheng Chen Juan Bai Dong-Hai Lin Shanghai Engineering Research Center of Advanced Thermal Functional Materials Shanghai Key Laboratory of Engineering Materials Application and EvaluationSchool of Energy and MaterialsShanghai Polytechnic UniversityShanghai201209China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China College of Biological and Pharmaceutical Sciences China Three Gorges UniversityYichang443002China School of Materials Science and Hydrogen Energy Foshan UniversityFoshan528000China School of Chemistry and Physics Queensland University of TechnologyBrisbaneQLD4000Australia

Fabrication of superior catalytic performance palladium-based catalysts with affordable cost is the key to develop direct ethanol fuel cell.Herein,pd-decorated three-dimensional(3D)porous constructed from graphene oxide(GO)and MXene combining with polystyrene(PS)particles as sacrificial templates(pd/GO-MXene-PS)to elevate the catalytic performance for ethanol oxidation was proposed.The 3D porous interconnected structure of pd/GO-MXene-PS was characterized by scanning electron microscope(SEM),transmission electron microscope(TEM)and Brunner−Emmet−Teller(BET).By optimizing the doping ratio of MXene to GO,the mass activity of pd/GO_(5)-MXene_(5)-PS(2944.0 mA·mg^(−1))was 3.0 times higher than that of commercial pd/C(950.4 mA·mg^(−1))toward ethanol oxidation in base solution.Meanwhile,the rotating disk electrode(RDE)results demonstrated that pd/GO5-MXene5-PS had a faster kinetics of ethanol oxidation.The enhanced ethanol oxidation over pd/GO5-MXene5-PS could attribute to the excellent 3D interconnected porous structure,large surface area,good conductivity and homogeneous pd distribution.This work provided a new idea for creating 3D porous MXene composite materials in electrocatalysis.

关键词： pd nanoparticles Ethanol oxidation Graphene MXene Polystyrene(PS)template Rotating disk electrode(RDE)

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Highly dispersed pd clusters/nanoparticles encapsulated in MOFs via in situ auto-reduction method for aqueous phenol hydrogenation

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Journal of Materials Science & Technology 2022年第14期109卷 167-175页

作者： Xiubing Huang Xiaoyu Li Wei Xia Bin Hu Martin Muhler Baoxiang Peng Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 10083China Laboratory of Industrial Chemistry Faculty of Chemistry and BiochemistryRuhr University BochumBochum 44780Germany Max Planck Institute for Chemical Energy Conversion Mülheim a.d.Ruhr 45470Germany

In this work,a novel in situ auto-reduction strategy was developed to encapsulate uniformly dispersed pd clusters/nanoparticles in MIL-125-NH_(2).It is demonstrated that the amino groups in MIL-125-NH_(2)can react with formaldehyde to form novel reducing groups(-NH-CH_(2)OH),which can in situ auto-reduce the encapsulated pd^(2+)ions to metallic pd clusters/nanoparticles.As no additional reductants are required,the strategy limits the aggregation and migration of pd clusters and the formation of large pd nanoparticles via controlling the amount of pd^(2+)precursor.When applied as catalysts in the hydrogenation of phenol in the aqueous phase,the obtained pd(1.5)/MIL-125-NH-CH_(2)OH catalyst with highly dispersed pd clusters/nanoparticles with the size of around 2 nm exhibited 100%of phenol conversion and 100%of cyclohexanone selectivity at 70℃ after 5 h,as well as remarkable reusability for at least five cycles due to the large MOF surface area,the highly dispersed pd clusters/nanoparticles and their excellent stability within the MIL-125-NH-CH_(2)OH framework.

关键词： pd clusters pd nanoparticles MIL-125-NH_(2) In situ auto-reduction Double solvent method Hydrogenation of phenol

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Efficient adjustment of product selectivity using controllable pd nanoparticles in nitroarene hydrogenation

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Particuology 2020年第1期18卷 13-18页

作者： Jian Zhang Liang Wang Fang Chen Feng-Shou Xiao Key Laboratory of Applied Chemistry of Zhejiang Province and Department of Chemistry Zhejiang UniversityHangzhou 310028China

Product selectivity adjustment is a much-studied topic in mesoscience that is critical for industrial processes and strongly related to reaction intermediates formed by interactions between catalytic active sites and reactants.Herein,we report efficient adjustment of the product selectivity in the hydrogenation of substituted nitroarenes via rational reaction intermediates achieved using controllable pd nanoparticles.pd nanoparticles fixed within zeolite Beta crystals(pd@Beta)afforded rational pd-NO2 interactions,in which the pd nanoparticle-adsorbed substituted nitroarenes,such as nitrobenzaldehyde,were reasonably hydrogenated into the corresponding aminobenzaldehyde.However,for pd nanoparticles supported on the external surfaces of zeolite beta crystals,various side products were obtained owing to the coexistence of pd-NO2 and pd-C=O interactions.When pd nanoparticles were artificially controlled in various positions in a fixed-bed reactor,the product selectivity was significantly affected.These results demonstrate the importance of molecular adsorption and diffusion processes in adjusting product selectivity in catalytic reactions.

关键词： Product selectivity Nitroarene hydrogenation pd nanoparticles Zeolite crystals

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Highly dispersed pd nanoparticles on chemically modified graphene with aminophenyl groups for formic acid oxidation

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Chinese Physics B 2011年第11期20卷 190-196页

作者：杨苏东申承民佟浩何卫张校刚高鸿钧 College of Material Science and Engineering Nanjing University of Aeronautics and Astronautics Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of Sciences

A novel electrode material based on chemically modified graphene （CMG） with aminophenyl groups is covalently functionalized by a nucleophilic ring-opening reaction between the epoxy groups of graphene oxide and the aminophenyl groups of p-phenylenediamine. Palladium nanoparticles with an average diameter of 4.2 nm are deposited on the CMG by a liquid-phase borohydride reduction. The electrocatalytic activity and stability of the pd/CMG composite towards formic acid oxidation are found to be higher than those of reduced graphene oxide and commercial carbon materials such as Vulcan XC-72 supported pd electrocatalysts.

关键词： chemically modified graphene fuel cell electrocatalysis pd nanoparticles

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Recovery of In Situ-generated pd nanoparticles with Linear Polystyrene

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Green and Sustainable Chemistry 2011年第2期1卷 19-25页

作者： Atsushi Ohtaka Ryozo Kuroki Takuto Teratani Tsutomu Shinagawa Go Hamasaka Yasuhiro Uozumi Osamu Shimomura Ryoki Nomura Department of Applied Chemistry Faculty of EngineeringOsaka Institute of TechnologyOsakaJapan Electronic Materials Research Division Osaka Municipal Technical Research InstituteOsakaJapan Institute for Molecular Science(IMS) OkazakiJapan Nanomaterials and Microdevices Research Center Osaka Institute of TechnologyOsakaJapan

Palladium nanoparticles generated in situ for Suzuki coupling reactions and aerobic alcohol oxidation in water were recovered completely using linear polystyrene. The resultant polystyrene-stabilized palladium nanopar... 详细信息

关键词： Polystyrene pd nanoparticles Water Suzuki Coupling Alcohol Oxidation

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Graphene-nickel nitride hybrids supporting palladium nanoparticles for enhanced ethanol electrooxidation

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Journal of Energy Chemistry 2021年第4期30卷 48-54页

作者： Tong Wu Xiao Wang Ahmet Emrehan Emre Jinchen Fan Yulin Min Qunjie Xu Shigang Sun Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power Shanghai Engineering Research Center of Energy-Saving in Heat Exchange SystemsShanghai University of Electric PowerShanghai 200090China Department of Chemical Engineering and Biointerfaces Institute University of MichiganAnn Arbor 48109MIUnited States Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Electrocatalysts for ethanol oxidation reaction(EOR)are generally limited by their poor durability because of the catalyst poisoning induced by the reaction intermediate carbon monoxide(CO).Therefore,the rapid oxidation removal of CO intermediates is crucial to the durability of EOR-based catalysts.Herein,in order to effectively avoiding the catalyst CO poisoning and improve the durability,the graphene-nickel nitride hybrids(AG-Ni_(3)N)were designed for supporting palladium nanoparticles(pd/AG-Ni_(3)N)and then used for ethanol electrooxidation.The density functional theory(DFT)calculations demonstrated the introduction of AG-Ni_(3)N depresses the CO absorption and simultaneously promotes the adsorption of OH species for CO oxidation removal.The fabricated pd/AG-Ni_(3)N catalyst distinctively exhibits excellent electroactivity with the mass catalytic activity of 3499.5 m A mg^(-1) on EOR in alkaline media,which is around 5.24 times higher than pd/C(commercial catalyst).Notably,the pd/AG-Ni_(3)N hybrids display excellent stability and durability after chronoamperometric measurements with a total operation time of 150,000 s.

关键词： Graphene pd nanoparticles Nickel nitride Ethanol electrooxidation

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“On-off”switch for H_(2)and O_(2)generation from HCOOH resp.H_(2)O_(2)

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Carbon Energy 2023年第3期5卷 75-86页

作者： Wenkai Huang Fuhua Xu Dong‐Sheng Li Didier Astruc Xiang Liu Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials College of Materials and Chemical EngineeringChina Three Gorges UniversityYichangHubeiChina ISM UMR CNRS N°5255Universitéde BordeauxTalence CedexFrance

In spite of the numerous advances in the development of H_(2)and O_(2)evolutions upon water splitting,the separation of H_(2)from O_(2)still remains a severe challenge.Herein,the novel dual-functional nanocatalysts pd/carbon nanosphere(CNS),obtained via immobilization of ultrafine pd nanoparticles onto CNS,are developed and employed for both selective H_(2)generation from HCOOH dehydrogenation and O_(2)evolution from H_(2)O_(2)decomposition.In these reactions,the highest activities for pd/CNS-800(i.e.,calcinated at 800℃)are 2478 h−1 and 993 min^(−1)for H_(2)and O_(2)evolution,respectively.The highly efficient and selective“on-off”switch for selective H_(2)generation from HCOOH is successfully realized by pH adjustment.This novel and highly efficient nanocatalyst pd/CNS-800 not only provides new approaches for the promising application of HCOOH and H_(2)O_(2)as economic and safe H_(2)and O_(2)carriers,respectively,for fuel cells,but also promotes the development of“on-off”switch for on-demand H_(2)evolution.

关键词： carbon nanospheres H_(2)generation O_(2)evolution “on-off”switch pd nanoparticles

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Au,pd and maghemite nanofunctionalized hydroxyapatite scaffolds for bone regeneration

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Regenerative Biomaterials 2020年第5期7卷 461-469页

作者： Giovanna Calabrese Salvatore Petralia Claudia Fabbi Stefano Forte Domenico Franco Salvatore Guglielmino Emanuela Esposito Salvatore Cuzzocrea Francesco Traina Sabrina Conoci Department of Chemistry Biology Pharmacy and Environmental Science University of MessinaPiazza Pugliatti198122 MessinaSiciliaItaly Research and Development Applied Chemical WorksPaternoCataniaItaly Department of Chemical Science Fin-Ceramica FaenzaVia Granarolo 177/3Faenza 48018Italy Istituto Oncologico del Mediterraneo Ricerca ViagrandeCatania 95029Italy Dipartimento Biomorf Universita degli Studi di MessinaMessinaItaly Rizzoli Orthopedic Institute IRCSSBolognaItaly Distretto Tecnologico Micro e Nano Sistemi Sicilia CataniaItaly

Nanotechnology plays a key role in the development of innovative scaffolds for bone tissue engineering(BTE)allowing the incorporation of nanomaterials able to improve cell proliferation and differentiation.In this study,Mg-HA-Coll type I scaffolds(Mg-HA-based scaffolds)were nanofunctionalized with gold nanorods(Au NRs),palladium nanoparticles(pd NPs)and maghemite nanoparticles(MAG NPs).Nanofunctionalized Mg-HA-based scaffolds(NF-HA-Ss)were tested for their ability to promote both the proliferation and the differentiation of adipose-derived mesenchymal stem cells(hADSCs).Results clearly highlight that MAG nanofunctionalization substantially improves cell proliferation up to 70% compared with the control(Mg-HA-based scaffold),whereas both Au NRs and pd NPs nanofunctionalization induce a cell growth inhibition of 94% and 89%,respectively.Similar evidences were found for the osteoinductive properties showing relevant calcium deposits(25% higher than the control)for MAG nanofunctionalization,while a decreasing of cell differentiation(20% lower than the control)for both Au NRs and pd NPs derivatization.These results are in agreement with previous studies that found cytotoxic effects for both pd NPs and Au NRs.The excellent improvement of both osteoconductivity and osteoinductivity of the MAG NF-HA-S could be attributed to the high intrinsic magnetic field of superparamagnetic MAG NPs.These findings may pave the way for the development of innovative nanostructured scaffolds for BTE.

关键词： bone regeneration hydroxyapatite scaffold tissue engineering gold nanoroads pd nanoparticles maghemite nanoparticles

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Investigation of Co_3O_4 nanorods supported pd anode catalyst for methanol oxidation in alkaline solution

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Journal of Energy Chemistry 2014年第6期23卷 801-808页

作者： Yanbiao Ren Shichao Zhang Hua Fang Xin Wei Puheng Yang School of Materials Science and Engineering Beijing University of Aeronautics and Astronautics

A CO3O4 nanorod supported pd electro-catalyst for the methanol electro-oxidation （MEO） has been fabricated by the combination of hydrother- mal synthesis and microwave-assisted polyol reduction processes. The crystallographic property and microstructure have been characterized using XRD, SEM and TEM. The results demonstrate that pd nanoparticles （pdNPs） with a narrow particle size distribution （3-5 nm） are uni- formly deposited onto the surface of Co304 nanorods. Electrochemical measurements show that this catalyst having a larger electrochemically active surface area and a more negative onset-potential exhibits enhanced catalytic activity of 504 mA/mg pd for MEO comparing with the pd/C catalyst （448 mA/mg pd）. The dependency of log/against logv reveals that MEO on pd-CO304 electrode is under a diffusion control. Electrochemical impedance spectroscopy （EIS） measurement agrees well with the CV results. The minimum charge transfer resistance of MEO on pd-CO304 is observed at -0.05 V, which coincides with the potential of MEO peak.

关键词： pd nanoparticles C0304 nanorods methanol electrooxidation catalytic activity charge transfer resistance

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Facile construction of highly efficient MOF-based pd@UiO-66-NH_(2)@ZnIn_(2)S_(4)flower-like nanocomposites for visible-light-driven photocatalytic hydrogen production

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Journal of Materials Science & Technology 2021年第17期76卷 189-199页

作者： Mengting Cao Fengli Yang Quan Zhang Juhua Zhang Lu Zhang Lingfeng Li Xiaohao Wang Wei-Lin Dai Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan UniversityShanghai 200438China

Construction of metal-organic-frame works-based composite photocatalysts has attracted much attention for the reasonable band gap and high surface areas to improve the photocatalytic activity.In this study,the ternary heterojunction pd@UiO-66-NH_(2)@ZnIn_(2)S_(4)nanocomposites were facilely prepared for the first time by a two-step method.The visible-light-promoted hydrogen production rate of 0.3%pd@UiO-66-NH_(2)@ZnIn_(2)S_(4)reaches up to 5.26 mmol g^(-1)h^(-1),which is evidently much higher than pure UiO-66-NH_(2),ZnIn_(2)S_(4)and binary UiO-66-NH_(2)/ZnIn_(2)S_(4)composites.Such a huge improvement in the photocatalytic performance is mainly attributed to the matched band gap of ZnIn_(2)S_(4)and UiO-66-NH_(2),and the introduction of pd NPs into photocatalysts that broaden spectral response range and promote the photon induced charge carrier separation.This work may provide a feasible approach for the design and construction of metal-organic-frameworks-based photocatalytic materials.

关键词： Metal-organic frameworks(MOFs) UiO-66-NH_(2) ZnIn_(2)S_4 pd nanoparticles Photocatalytic hydrogen production

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