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Construction of trace silver modified core@shell structured Pt-Ni nanoframe@CeO2 for semihydrogenation of phenylacetylene

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Nano Research 2019年第4期12卷 869-875页

作者： Yan Long Jian Li Lanlan Wu Qishun Wang Yu Liu Xiao Wang Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022 China University of Chinese Academy of Sciences Beijing 100049 China University of Science and Technology of China Hefei 230026 China

The Pt-Ni nanoframe catalysts have attracted great interest owing to their unique electronic structure and excellent catalytic performance. However, the stability of the tenu ous edges of nano frame-structures is dissatisfactory and their un iversal applicati ons in catalytic market beyond electrocatalytic reactions are yet to be tapped and explored. Herein, we developed a new core@ shell structured Pt-Ni nanoframe@CeO2 (Pt-Ni NF@CeO2) composite via etching the Ni from inhomogeneous Pt-Ni rhombic dodecahedra (Pt-Ni RD) by cerium(lll) acetate hydrate (Ce(OAc)3). In this path, Pt-Ni RD was used as self-sacrificial 怕mplate, while the Ce(OAc)3 serves as the provider of the Ce3* source and OH' for the formation of CeO2 shell, etchant of Pt-Ni RD, and the surface modification agent. By this way, the etching of Pt-Ni RD and the formation of the CeO2 shell are simultaneously proceeded to form the final Pt-Ni NF@CeO2 in one step. The obtained Pt-Ni NF@CeO2 exhibits strong in terfacial charge tran sfer interactio n betwee n Pt-Ni NF core and CeO2 shell eve n without reductio n treatment, leading to enhan ced catalytic activity in the hydrogenation of phenylacetylene. After introduction of trace silver, the Pt-Ni-Ag4.9 NF@CeO2 achieves remarkable catalytic performa nee for the selective con versi on of phe ny lacetyle ne to styrene: high con version (100%), styre ne selectivity (86.5%), and good stability. It reveals that enc apsulatio n n oble metal nano frames into metal oxide to form core @ shell structured hybrids will in deed enhance their stability and catalytic properties. Particularly, this work expends the application of noble metal nanoframes materials to hydrogenation reacti ons.

关键词： CeO2 Pt-Ni nanoframes core@shell sturcuture silver modification hydrogenation of phenylacetylene

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Electrocatalysts based on metal@carbon core@shell nanocomposites:An overview

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Green Energy & Environment 2018年第4期3卷 335-351页

作者： Yi Peng Shaowei Chen Department of Chemistry and Biochemistry University of California

Developing low-cost, high-performance catalysts is of fundamental significance for electrochemical energy conversion and storage. In recent years, metal@carbon core@shell nanocomposites have emerged as a unique class of functional nanomaterials that show apparent electrocatalytic activity towards a range of reactions, such as hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, and CO2 reduction reaction, that are important in water splitting, fuel cells and metal-air batteries. The activity is primarily attributed to interfacial charge transfer from the metal core to the carbon shell that manipulate the electronic interactions between the catalyst surface and reaction intermediates, and varies with the structures and morphologies of the metal core(elemental composition, core size, etc.) and carbon shell(doping,layer thickness, etc.). Further manipulation can be achieved by the incorporation of a third structural component. A perspective is also included highlighting the current gap between theoretical modeling and experimental results, and technical challenges for future research.

关键词： Metal@carbon core@shell nanocomposite Electrocatalysis Hydrogen evolution reaction Oxygen evolution reaction Oxygen reduction reaction

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S1-supported Pd@CeO_(2) quasi-core@shell materials as advanced catalysts for selective hydrogenation of furfural

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Chinese Chemical Letters 2024年第3期35卷 493-496页

作者： Xiang Chu Lingling Zhang Ke Wang Rui Zhang Xiao Wang Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Bare Pd metal nanoparticles invariably suffer from poor selectivity in furfural hydrogenation by forming flat configurations,with the aromatic ring of the substrate molecules parallel to the metal ***,we put forward a promising solution by using CeO_(2)as promoters to modify Pd nanoparticles for modulating the adsorption behaviors of furfural *** achieve the highly-desired ultra-small Pd@CeO_(2)core@shell nanostructure,a“constrained auto-redox”synthesis is developed,in which silicalite-1 supports play the key role of providing their surface as the landing place of PdO_(x)precursors for inhibiting the overgrowth and the *** the best of our knowledge,this is one of the smallest core@shell materials obtained from aqueous *** evaluated as catalysts,Pd@CeO_(2)/S-1 gives 98.9%conversion of furfural with 94.3%selectivity for furfural alcohol in 15 h,which is much better than that of Pd/S-1(88.6%conversion with 44.3%selectively).The DFT simulation reveals a strong interaction between the defects of CeO_(2)and the oxygen atom of the–CHO group in furfural molecules,which benefits the selective hydrogenation occurred in the–CHO group rather than the furan ring.

关键词： core@shell Palladium Ceria Auto-redox synthesis Hydrogenation

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Mass production of Co3O4@CeO2 core@shell nanowires for catalytic CO oxidation

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Nano Research 2015年第6期8卷 1944-1955页

作者： Jiangman Zhen Xiao Wang Dapeng Liu Zhuo Wang Junqi Li Fan Wang Yinghui Wang Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022 Jilin China University of the Chinese Academy of Sciences Beijing 100039 China

In this study, Co3O4@CeO2 core@shell nanowires were successfully prepared via thermal decomposition of Co（CO3）0.5（OH）.0.11H2O@CeO2 core@shell nanowire precursors. As a CO oxidation catalyst, Co3O4@CeO2 shows remarkably enhanced catalytic performance compared to Co3O4 nanowires and CeO2 nanoparticles （NPs）, indicating obvious synergistic effects between the two components. It also suggests that the CeO2 shell coating can effectively prevent Co3O4 nanowires from agglomerating, hence effecting a substantial improvement in the structural stability of the Co3O4 catalyst. Furthermore, the fabrication of the welbdisperse4 core@shell structure results in a maximized interface area between Co3O4 and CeO2, as well as a reduced Co3O4 size, which may be responsible for the enhanced catalytic activity of Co3O4@CeO2. Further examination revealed that CO oxidation may occur at the interface of Co3O4 and CeO2. The influence of calcination temperatures and the component ratio between Co3O4 and CeO2 were then investigated in detail to determine the catalytic performance of Co3O4@CeO2 core@shell nanowires, the best of which was obtained by calcination at 250 ℃ for 3 h with a Ce molar concentration of about 38.5%. This sample achieved 100% CO conversion at a reduced temperature of 160 ℃. More importantly, more than 2.5 g of the Co3O4@CeO2 core@shell nanowires were produced in one pot by this simple process, which may be beneficial for practical applications as automobile-exhaust gas-treatment catalysts.

关键词： Co3O4@CeO2 core@shell nanowires CO oxidation synergistic effects

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core@shell structured Au@Sn O2 nanoparticles with improved N2 adsorption/activation and electrical conductivity for efficient N2 fixation

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Science Bulletin 2020年第5期65卷 350-358页

作者： Pengtang Wang Yujin Ji Qi Shao Youyong Li Xiaoqing Huang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123China

The design of electrocatalysts with enhanced adsorption and activation of nitrogen(N2)is critical for boosting the electrochemical N2reduction(ENR).Herein,we developed an efficient strategy to facilitate N2 adsorption and activation for N2 electroreduction into ammonia(NH3)by vacancy engineering of core@shell structured Au@Sn O2 nanoparticles(NPs).We found that the ultrathin amorphous SnO2 shell with enriched oxygen vacancies was conducive to adsorb N2as well as promoted the N2 activation,meanwhile the metallic Au core ensured the good electrical conductivity for accelerating electrons transport during the electrochemical N2 reduction reaction,synergistically boosting the N2 electroreduction *** confirmed by the15N-labeling and controlled experiments,the core@shell Au@amorphous SnO2 NPs with abundant oxygen vacancies show the best performance for N2 electroreduction with the NH3 yield rate of 21.9 lg h-1mg-1catand faradaic efficiency of 15.2%at-10.2 VRHE,which surpass the Au@crystalline SnO2 NPs,individual Au NPs and all reported Au-based catalysts for ENR.

关键词： core@shell Electroreduction Nitrogen fixation Vacancy engineering Amorphous

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The Synthesis of Hierachical structured core@shell LTL Zeolites with Microporous, Mesoporurs and Macroporous by post-treatment Technique

The Synthesis of Hierachical structured core@shell LTL Zeoli...

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第18届全国分子筛学术大会

作者： Ling Ni Runwei Wang Ying Wang Chuanyin Sun Shang Jiang xinzheng Yue Shangjing Zeng Shilun Qiu Zongtao Zhang College of Chemistry and Synthesis State Key Laboratory of Inorganic and Preparative Chemistry Jilin University

The traditional zeolite LTL is hard to possess fine properties both the adsorption and the activity of catalysis for big organic compounds. Here, we report that hierarchical structured LTL zeolites were prepared using a post-treatment technique with microporous, mesoporous and macroporous. The as-prepared samples were characterized by X-ray diffraction（XRD）, scanning electron microscopy（SEM）, Transmission electron microscopy（TEM）, nitrogen adsorption,Temperature-programmed-desorption of ammonia（TPD-NH3） and Fourier Transform Infrared Spectroscopy（FTIR）. Meanwhile, the hierarchical structured LTL zeolites were used to carry out catalytic cracking reaction of 1, 3, 5- isopropyl benzene and n-hexadecane. Data showed that this modified LTL displayed improved catalytic activity and selectivity than that of traditional LTL,ZSM-5, Beta, Al-MCM-41, etc.

关键词： core@shell post-treatment technique hierarchical structure zeolite LTL

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Spatially asymmetric cascade nanocatalysts for enhanced chemodynamic therapy

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Nano Research 2023年第7期16卷 9642-9650页

作者： Minchao Liu Hongyue Yu Liang Chen Tiancong Zhao Meng Fang Mengli Liu Qiaoyu Zhou Fatemah Farraj AlHarbi Ahmed Mohamed El-Toni Fan Zhang Dongyuan Zhao Xiaomin Li Department of Chemistry State Key Laboratory of Molecular Engineering of PolymersiChemShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200433China Department of Musculoskeletal Cancer Surgery Fudan University Shanghai Cancer CenterShanghai 200032China Department of Physics College of SciencePrincess Nourah bint Abdulrahman UniversityP.O.Box 84428Riyadh 11671Saudi Arabia King Abdullah Institute for Nanotechnology King Saud UniversityRiyadh 11451Saudi Arabia

Chemodynamic therapy(CDT)based on cascade catalytic nanomedicine has emerged as a promising cancer treatment ***,most of the reported cascade catalytic systems are designed based on symmetric-or co-assembly of multiple catalytic active sites,in which their functions are difficult to perform independently and may interfere with each *** in cascade catalytic system that involves fragile natural-enzymes,the strong oxidation of free-radicals toward natural-enzymes should be carefully considered,and the spatial distribution of the multiple catalytic active sites should be carefully organized to avoid the degradation of the enzyme catalytic ***,a spatially-asymmetric cascade nanocatalyst is developed for enhanced CDT,which is composed by a Fe_(3)O_(4)head and a closely connected mesoporous silica nanorod immobilized with glucose oxidase(mSiO_(2)-GOx).The mSiO_(2)-GOx subunit could effectively deplete glucose in tumor cells,and meanwhile produce a considerable amount of H_(2)O_(2)for subsequent Fenton reaction under the catalysis of Fe_(3)O_(4)subunit in the tumor *** the advantage of the spatial isolation of mSiO_(2)-GOx and Fe_(3)O_(4)subunits,the catalysis of GOx and freeradicals generation occur at different domains of the asymmetric nanocomposite,minimizing the strong oxidation of free-radicals toward the activity of GOx at the other *** addition,direct exposure of Fe_(3)O_(4)subunit without any shelter could further enhance the strong oxidation of free-radicals toward ***,compared with traditional core@shell structure,the long-term stability and efficiency of the asymmetric cascade catalytic for CDT is greatly increased by 138%,thus realizing improved cancer cell killing and tumor restrain efficiency.

关键词： mesoporous nanocatalytic medicine chemodynamic therapy asymmetric nanostructure core@shell

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Antiangiogenesis-Combined Photothermal Therapy in the Second Near-Infrared Window at Laser Powers Below the Skin Tolerance Threshold

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Nano-Micro Letters 2019年第4期11卷 630-649页

作者： Jian-Li Chen Han Zhang Xue-Qin Huang Hong-Ye Wan Jie Li Xing-Xing Fan Kathy Qian Luo Jinhua Wang Xiao-Ming Zhu Jianfang Wang State Key Laboratory of Quality Research in Chinese Medicine Macao Institute for Applied Research in Medicine and HealthMacao University of Science and TechnologyTaipaMacao SARPeople’s Republic of China Department of Physics The Chinese University of Hong KongShatinHong Kong SARPeople’s Republic of China Faculty of Health Sciences University of MacaoTaipaMacao SARPeople’s Republic of China Beijing Key Laboratory of Drug Targets Research and New Drug Screening Institute of Materia MedicaChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100050People’s Republic of China

Photothermal agents with strong light absorption in the second near-infrared(NIR-II)region(1000-1350 nm)are strongly desired for successful photothermal therapy(PTT).In this work,titania-coated Au nanobipyramids(NBP@TiO2)with a strong plasmon resonance in the NIR-II window were *** NBP@TiO2 nanostructures have a high photothermal conversion efficiency of(93.3±5.2)%under 1064-nm laser *** are also capable for loading an anticancer drug combretastatin A-4 phosphate(CA4P).In vitro PTT studies reveal that 1064-nm laser irradiation can efficiently ablate human lung cancer A549 cells and enhance the anticancer effect of ***,the CA4P-loaded NBP@TiO2 nanostructures combined with PTT induce a synergistic antiangiogenesis *** vivo studies show that such CA4Ploaded NBP@TiO2 nanostructures under mild 1064-nm laser irradiation at an optical power density of 0.4 W cm?2,which is lower than the skin tolerance threshold value,exhibit a superior antitumor *** work presents not only the development of the NBP@TiO2 nanostructures as a novel photothermal agent responsive in the NIR-II window but also a unique combined chemo-photothermal therapy strategy for cancer therapy.

关键词： Antiangiogenesis therapy core@shell nanostructures Gold nanobipyramids Photothermal therapy Plasmon resonance

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Oxygen-sulfur Co-substitutional Fe@C nanocapsules for improving microwave absorption properties

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Science Bulletin 2020年第8期65卷 623-630,M0003页

作者： Yixing Li Xinyu Chen Qian Wei Weiwei Liu Yanhui Zhang Gaowu Qin Zhen Shi Xuefeng Zhang School of Materials Science and Engineering Key Laboratory for Anisotropy and Texture of Materials(MOE)Northeastern UniversityShenyang 110819China Institute of Advanced Magnetic Materials College of Materials and Environmental EngineeringHangzhou Dianzi UniversityHangzhou 310012China

Heteroatom substitution has been investigated to be a feasible way to optimize microwave absorption properties of core-shell structural nanocapsules at *** dielectric capacity has been increased at specific frequency with substituted absorbents,its broadband absorption performance is still relatively poor ascribed to the low dipole oscillation amplitude of single substituted *** this study we demonstrate that sulfur and oxygen co-substituted heterostructure leads to high microwave absorption property of core-shell structural Fe@C nanocapsules at broadened frequency range,comparable to the single sulfur substitutional Fe@C *** characterizations coupled with first-principles calculations reveal that the microwave absorption enhancement is triggered by the sulfur-oxygen co-substitution,which results in the serious symmetry breaking and thus leads to the charge separation at the co-substituted *** particular,the nanocapsules exhibt the minimum reflection loss capcacity R(d B)of-52 d B at 6.8 GHz and the bandwith for R(d B)<-20 dB is in the frequency range of 3.1-12.7 *** present study not only offers a deep insight into the relationship between heteroatom and microwave absorption property,but also puts forward a mentality for further designing microwave absorbents.

关键词： Microwave absorption Electric-dipole Substitution core@shell Sulfur-oxygen doped

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Synthesis and Surface Modification of Spindle-Type Magnetic Nanoparticles: Gold Coating and PEG Functionalization

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Journal of Biomaterials and Nanobiotechnology 2013年第3期4卷 222-228页

作者： Juan Mendez-Garza Biran Wang Alexandra Madeira Christophe Di Giorgio Georges Bossis Institut de Chimie de Nice UMR 7272 Université de Nice-Sophia Antipolis CNRS Parc Valrose Nice France Laboratoire de Physique de la Matière Condensée UMR 7336 Université de Nice-Sophia Antipolis CNRS Parc Valrose Nice France

In this paper, we describe the synthesis of gold coated spindle-type iron nanoparticles and its surface modification by a thiolated fluorescently-labelled polyethylene glycol (PEG) polymer. A forced hydrolysis of ferric salts in the presence of phosphate ions was used to produce α-Fe2O3 spindle-type particles. The oxide powders were first reduced to α-iron under high temperature and controlled dihydrogen atmosphere. Then, the resulting magnetic spindle-type particles were covered by a shell of gold. The formation of the core@shell structure was driven by a redox-transmetalation reaction between iron(0) at the surface of particles and a gold(III) salt. Protected against oxidation, the Fe@Au core@shell nanoparticles were then grafted with a water soluble fluorescent-PEG-thiol. TEM, XRD, EDX and measurements of magnetic properties of particles confirm 1) the conversion of hematite into iron and 2) their subsequent surface protection with a gold shell. Furthermore, the functionalization of the gold nanoparticle surface with a PEG carrying a fluorescent dye was unambiguously attested by confocal laser scanning microscopy.

关键词： core@shell Spindle-Type Hematite Magnetic Particles Gold Coating Fluorescent-PEG

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