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1.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(36):10847-10850
Highly active and durable oxygen reduction catalysts are needed to reduce the costs and enhance the service life of polymer electrolyte fuel cells (PEFCs). This can be accomplished by alloying Pt with a transition metal (for example Ni) and by eliminating the corrodible, carbon‐based catalyst support. However, materials combining both approaches have seldom been implemented in PEFC cathodes. In this work, an unsupported Pt‐Ni alloy nanochain ensemble (aerogel) demonstrates high current PEFC performance commensurate with that of a carbon‐supported benchmark (Pt/C) following optimization of the aerogel's catalyst layer (CL) structure. The latter is accomplished using a soluble filler to shift the CL's pore size distribution towards larger pores which improves reactant and product transport. Chiefly, the optimized PEFC aerogel cathodes display a circa 2.5‐fold larger surface‐specific ORR activity than Pt/C and maintain 90 % of the initial activity after an accelerated stress test (vs. 40 % for Pt/C). 相似文献
2.
Metal‐Nitrogen‐doped Porous Carbons Derived from Metal‐Containing Ionic Liquids for Oxygen Reduction Reaction
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Cancan Wang Dr. Jiangna Guo Dr. Dan Xu Juewen Zhang Muzi Chen Prof. Feng Yan 《化学:亚洲杂志》2018,13(8):1029-1037
This study describes a self‐doping and additive‐free strategy for the synthesis of metal‐nitrogen‐doped porous carbon materials (CMs) via carbonizing well‐tailored precursors, metal‐containing ionic liquids (M‐ILs). The organic skeleton in M‐ILs serves as both carbon and nitrogen sources, while metal ions acts as porogen and metallic dopants. A high nitrogen content, appropriate content of metallic species and hierarchical porosity synergistically endow the resultant CMs (MIBA‐M‐T) as effective electrocatalysts for the oxygen reduction reaction (ORR). MIBA‐Fe‐900 with a high specific surface area of 1567 m2 g?1 exhibits an activity similar to that of Pt/C catalyst, a higher tolerance to methanol than Pt/C, and long‐term durability. This work supplies a simple and convenient route for the preparation of metal‐containing carbon electrocatalysts. 相似文献
3.
《化学:亚洲杂志》2018,13(18):2714-2722
Currently, the base‐free aerobic oxidation of biomass‐derived 5‐hydroxymethylfurfural (HMF) to produce 2,5‐furandicarboxylic acid (FDCA) is attracting intense interest due to its prospects for the green, sustainable, and promising production of biomass‐based aromatic polymers. Herein, we have developed a new Pt catalyst supported on nitrogen‐doped‐carbon‐decorated CeO2 (NC‐CeO2) for the aerobic oxidation of HMF in water without the addition of any homogeneous base. It was demonstrated that the small‐sized Pt particles could be well dispersed on the surface of the hybrid NC‐CeO2 support, and the activity of the supported Pt catalyst depended strongly on the surface structure and properties of the catalysts. The as‐fabricated Pt/NC‐CeO2 catalyst, with abundant surface defects, enhanced basicity, and favorable electron‐deficient metallic Pt species, enabled an almost 100 % yield of FDCA in water with molecular oxygen (0.4 MPa) at 110 °C for 8 h without the addition of any homogeneous base, which is indicative of exceptional catalytic performance. Furthermore, this Pt/NC‐CeO2 catalyst also showed good stability and reusability owing to strong metal–support interactions. An understanding of the role of surface structural defects and basicity of the hybrid NC‐CeO2 support provides a basis for the rational design of high‐performance and stable supported metal catalysts with practical applications in various transformations of biomass‐derived compounds. 相似文献
4.
Guoqiang He Zaoxue Yan Dr. Mei Cai Prof. Dr. Pei Kang Shen Dr. Min‐Rui Gao Dr. Hong‐Bin Yao Prof. Dr. Shu‐Hong Yu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(27):8490-8497
Carbide‐based electrocatalysts are superior to traditional carbon‐based electrocatalysts, such as the commercial Pt/C electrocatalysts, in terms of their mass activity and stability. Herein, we report a general approach for the preparation of a nanocomposite electrocatalyst of platinum and vanadium carbide nanoparticles that are loaded onto graphitized carbon. The nanocomposite, which was prepared in a localized and controlled fashion by using an ion‐exchange process, was an effective electrocatalyst for the oxygen‐reduction reaction (ORR). Both the stability and the durability of the Pt‐VC/GC nanocomposite catalyst could be enhanced compared with the state‐of‐the‐art Pt/C. This approach can be extended to the synthesis of other metal‐carbide‐based nanocatalysts. Moreover, this straightforward synthesis of high‐performance composite nanocatalysts can be scaled up to meet the requirements for mass production. 相似文献
5.
The capillary condensation is affected by micropore and nanopore of catalyst layer on fuel cell. Due to limitation of sluggish mass transport and electrocatalytic activity, to retain the pore skeleton of carbon and metal nanoparticles are very significant for enhanced utilizations of pore structure in electrochemical reaction. Besides, thickness of electrocatalyst layer is very crucial due to one of the factor affected by cell performance of direct methanol fuel cell. Highly loaded four Pt?Ru anode catalysts supported on resorcinol‐formaldehyde (RF) polymer based on meso‐porous carbons (80 wt.% Pt?Ru/carbon cryogel, 80 wt.% Pt?Ru/carbon xerogel and 80 wt.% Pt?Ru/carbon aerogel) and conventional carbon (80 wt.% Pt?Ru/Vulcan XC‐72) were prepared by colloidal method for direct methanol fuel cell. These catalysts were characterized by X‐Ray diffraction (XRD), High resolution transmission electron microscopy (HR‐TEM) and X‐ray photoemission (XPS). The results of CO stripping voltammetry, cyclic voltammetry (CV) and single cell test performed on DMFC show that Pt?Ru/carbon cryogel and Pt?Ru/carbon aerogel exhibits better performances in comparison to Pt?Ru/carbon xerogel and Pt?Ru/Vulcan XC‐72. It is thus considered that particle size, oxidation state of metal and electrochemical active surface area of these catalysts are important role in electrocatalytic activity in DMFC. 相似文献
6.
Yu Qiao Yangyang Ni Fantan Kong Ruijing Li Chaoqi Zhang Aiguo Kong Yongkui Shan 《化学:亚洲杂志》2019,14(15):2676-2684
Well‐dispersed carbon‐coated or nitrogen‐doped carbon‐coated copper‐iron alloy nanoparticles (FeCu@C or FeCu@C?N) in carbon‐based supports are obtained using a bimetallic metal‐organic framework (Cu/Fe‐MOF‐74) or a mixture of Cu/Fe‐MOF‐74 and melamine as sacrificial templates and an active‐component precursor by using a pyrolysis method. The investigation results attest formation of Cu?Fe alloy nanoparticles. The obtained FeCu@C catalyst exhibits a catalytic activity with a half‐wave potential of 0.83 V for oxygen reduction reaction (ORR) in alkaline medium, comparable to that on commercial Pt/C catalyst (0.84 V). The catalytic activity of FeCu@C?N for ORR (Ehalf‐wave=0.87 V) outshines all reported analogues. The excellent performance of FeCu@C?N should be attributed to a change in the energy of the d‐band center of Cu resulting from the formation of the copper–iron alloy, the interaction between alloy nanoparticles and supports and N‐doping in the carbon matrix. Moreover, FeCu@C and FeCu@C?N show better electrochemical stability and methanol tolerance than commercial Pt/C and are expected to be widely used in practical applications. 相似文献
7.
Highly Stable,Water‐Dispersible Metal‐Nanoparticle‐Decorated Polymer Nanocapsules and Their Catalytic Applications
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Gyeongwon Yun Dr. Zahid Hassan Jiyeong Lee Jeehong Kim Dr. Nam‐Suk Lee Dr. Nam Hoon Kim Dr. Kangkyun Baek Dr. Ilha Hwang Prof. Dr. Chan Gyung Park Prof. Dr. Kimoon Kim 《Angewandte Chemie (International ed. in English)》2014,53(25):6414-6418
A facile synthesis of highly stable, water‐dispersible metal‐nanoparticle‐decorated polymer nanocapsules (M@CB‐PNs: M=Pd, Au, and Pt) was achieved by a simple two‐step process employing a polymer nanocapsule (CB‐PN) made of cucurbit[6]uril (CB[6]) and metal salts. The CB‐PN serves as a versatile platform where various metal nanoparticles with a controlled size can be introduced on the surface and stabilized to prepare new water‐dispersible nanostructures useful for many applications. The Pd nanoparticles on CB‐PN exhibit high stability and dispersibility in water as well as excellent catalytic activity and recyclability in carbon–carbon and carbon–nitrogen bond‐forming reactions in aqueous medium suggesting potential applications as a green catalyst. 相似文献
8.
Gyeongwon Yun Zahid Hassan Jiyeong Lee Jeehong Kim Nam‐Suk Lee Nam Hoon Kim Kangkyun Baek Ilha Hwang Chan Gyung Park Kimoon Kim 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2014,126(25):6532-6536
A facile synthesis of highly stable, water‐dispersible metal‐nanoparticle‐decorated polymer nanocapsules (M@CB‐PNs: M=Pd, Au, and Pt) was achieved by a simple two‐step process employing a polymer nanocapsule (CB‐PN) made of cucurbit[6]uril (CB[6]) and metal salts. The CB‐PN serves as a versatile platform where various metal nanoparticles with a controlled size can be introduced on the surface and stabilized to prepare new water‐dispersible nanostructures useful for many applications. The Pd nanoparticles on CB‐PN exhibit high stability and dispersibility in water as well as excellent catalytic activity and recyclability in carbon–carbon and carbon–nitrogen bond‐forming reactions in aqueous medium suggesting potential applications as a green catalyst. 相似文献
9.
Aqueous Synthesis of Ultrathin Platinum/Non‐Noble Metal Alloy Nanowires for Enhanced Hydrogen Evolution Activity
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Zhaojun Liu Jing Qi Moxuan Liu Shumeng Zhang Qikui Fan Hongpo Liu Kai Liu Prof. Haoquan Zheng Prof. Yadong Yin Prof. Chuanbo Gao 《Angewandte Chemie (International ed. in English)》2018,57(36):11678-11682
Although aqueous synthesis of nanocrystals is advantageous in terms of the cost, convenience, environmental friendliness, and surface cleanness of the product, nanocrystals of Pt and non‐noble metal alloys are difficult to obtain with controlled morphology and composition from this synthesis owing to a huge gap between the reduction potentials of respective metal salts. This huge gap could now be remedied by introducing a sulfite into the aqueous synthesis, which is believed to resemble an electroless plating mechanism, giving rise to a colloid of Pt‐M (M=Ni, Co, Fe) alloy nanowires with an ultrasmall thickness (ca. 2.6 nm) in a high yield. The sulfite also leads to the formation of surface M?S bonds and thus atomic‐level Pt/M–S(OH) interfaces for greatly boosted hydrogen evolution kinetics under alkaline conditions. An activity of 75.3 mA cm?2 has been achieved with 3 μg of Pt in 1 m KOH at an overpotential of 70 mV, which is superior to previously reported catalysts. 相似文献
10.
Yubing Zhou Bharath Natarajan Yanchen Fan Hua Xie Chunpeng Yang Shaomao Xu Yonggang Yao Feng Jiang Qianfan Zhang Jeffrey W. Gilman Liangbing Hu 《Angewandte Chemie (International ed. in English)》2018,57(10):2625-2629
The interaction between metal nanoparticles (NPs) and their substrate plays a critical role in determining the particle morphology, distribution, and properties. The pronounced impact of a thin oxide coating on the dispersion of metal NPs on a carbon substrate is presented. Al2O3‐supported Pt NPs are compared to the direct synthesis of Pt NPs on bare carbon surfaces. Pt NPs with an average size of about 2 nm and a size distribution ranging between 0.5 nm and 4.0 nm are synthesized on the Al2O3 coated carbon nanofiber, a significant improvement compared to those directly synthesized on a bare carbon surface. First‐principles modeling verifies the stronger adsorption of Pt clusters on Al2O3 than on carbon, which attributes the formation of ultrafine Pt NPs. This strategy paves the way towards the rational design of NPs with enhanced dispersion and controlled particle size, which are promising in energy storage and electrocatalysis. 相似文献
11.
Shin Wook Kang Young Wook Lee Minjung Kim Jong Wook Hong Prof. Dr. Sang Woo Han 《化学:亚洲杂志》2011,6(3):909-913
One‐pot synthesis of carbon‐supported Pd‐Au alloy nanoparticles with well‐defined dendritic shape (Pd‐Auden/C) was achieved by co‐reduction of K2PdCl4/HAuCl4 mixtures in a molar ratio of 1:1 with hydrazine in the presence of Vulcan XC‐72R. The prepared Pd‐Auden/C exhibited significantly enhanced performance in the electrocatalytic oxidation of ethanol compared with dendritic Pd nanoparticles and a commercial Pd/C catalyst. Pd‐Auden/C even showed higher durability in electro‐oxidation of ethanol than the supported catalyst prepared by the deposition of presynthesized dendritic Pd‐Au nanoparticles on the carbon support. The experimental results clearly indicate that enhanced interaction between nanoparticle catalysts and carbon support through the one‐pot synthesis protocol can improve the durability of the electrocatalysts. 相似文献
12.
Effects of Adsorbate Coverage and Bond‐Length Disorder on the d‐Band Center of Carbon‐Supported Pt Catalysts
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Dr. Matthew W. Small Dr. Joshua J. Kas Dr. Kristina O. Kvashnina Prof. Dr. John J. Rehr Prof. Dr. Ralph G. Nuzzo Prof. Dr. Moniek Tromp Prof. Dr. Anatoly I. Frenkel 《Chemphyschem》2014,15(8):1569-1572
Determination of the factors that affect the d‐band center of catalysts is required to explain their catalytic properties. Resonant inelastic X‐ray scattering (RIXS) enables direct imaging of electronic transitions in the d‐band of Pt catalysts in real time and in realistic environmental conditions. Through a combination of in situ, temperature‐resolved RIXS measurements and theoretical simulations we isolated and quantified the effects of bond‐length disorder and adsorbate coverage (CO and H2) on the d‐band center of 1.25 nm size Pt catalysts supported on carbon. We found that the decrease in adsorbate coverage at elevated temperatures is responsible for the d band shifts towards higher energies relative to the Fermi level, whereas the effect of the increase in bond‐length disorder on the d‐band center is negligible. Although these results were obtained for a specific case of non‐interacting support and weak temperature dependence of the metal–metal bond length in a model catalyst, this work can be extended to a broad range of real catalysts. 相似文献
13.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(51):16589-16593
Nitrones are key intermediates in organic synthesis and the pharmaceutical industry. The heterogeneous synthesis of nitrones with multifunctional catalysts is extremely attractive but rarely explored. Herein, we report ultrasmall platinum nanoclusters (PtNCs) encapsulated in amine‐functionalized Zr metal–organic framework (MOF), UiO‐66‐NH2 (Pt@UiO‐66‐NH2) as a multifunctional catalyst in the one‐pot tandem synthesis of nitrones. By virtue of the cooperative interplay among the selective hydrogenation activity provided by the ultrasmall PtNCs and Lewis acidity/basicity/nanoconfinement endowed by UiO‐66‐NH2, Pt@UiO‐66‐NH2 exhibits remarkable activity and selectivity, in comparison to Pt/carbon, Pt@UiO‐66, and Pd@UiO‐66‐NH2. Pt@UiO‐66‐NH2 also outperforms Pt nanoparticles supported on the external surface of the same MOF (Pt/UiO‐66‐NH2). To our knowledge, this work demonstrates the first examples of one‐pot synthesis of nitrones using recyclable multifunctional heterogeneous catalysts. 相似文献
14.
Fundamental understanding about the thermal stability of nanoparticles and deliberate control of structural and morphological changes under reactive conditions is of general importance for a wide range of reaction processes in heterogeneous and electrochemical catalysis. Herein, we present a parametric study of the thermal stability of carbon‐supported Pt nanoparticles at 80 °C and 160 °C, with an initial particle size below 3 nm, using in situ high‐temperature X‐ray diffraction (HT‐XRD). The effects on the thermal stability of carbon‐supported Pt nanoparticles are investigated with control parameters such as Brunauer–Emmet–Teller (BET) surface area, metal loading, temperature, and gas environment. We demonstrate that the growth rate exhibits a complex, nonlinear behavior and is largely controlled by the temperature, the initial particle size, and the interparticle distance. In addition, an ex situ transmission electron microscopy study was performed to verify our results obtained from the in situ HT‐XRD study. 相似文献
15.
Dr. Jong Wook Hong Yena Kim Dae Han Wi Seunghoon Lee Su‐Un Lee Young Wook Lee Prof. Sang‐Il Choi Prof. Sang Woo Han 《Angewandte Chemie (International ed. in English)》2016,55(8):2753-2758
A synthesis strategy for the preparation of ultrathin free‐standing ternary‐alloy nanosheets is reported. Ultrathin Pd‐Pt‐Ag nanosheets with a thickness of approximately 3 nm were successfully prepared by co‐reduction of the metal precursors in an appropriate molar ratio in the presence of CO. Both the presence of CO and the interplay between the constituent metals provide fine control over the anisotropic two‐dimensional growth of the ternary‐alloy nanostructure. The prepared Pd‐Pt‐Ag nanosheets were superior catalysts of ethanol electrooxidation owing to their specific structural and compositional characteristics. This approach will pave the way for the design of multicomponent 2D nanomaterials with unprecedented functions. 相似文献
16.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(30):8954-8959
Core–shell architectures offer an effective way to tune and enhance the properties of noble‐metal catalysts. Herein, we demonstrate the synthesis of Pt shell on titanium tungsten nitride core nanoparticles (Pt/TiWN) by high temperature ammonia nitridation of a parent core–shell carbide material (Pt/TiWC). X‐ray photoelectron spectroscopy revealed significant core‐level shifts for Pt shells supported on TiWN cores, corresponding to increased stabilization of the Pt valence d‐states. The modulation of the electronic structure of the Pt shell by the nitride core translated into enhanced CO tolerance during hydrogen electrooxidation in the presence of CO. The ability to control shell coverage and vary the heterometallic composition of the shell and nitride core opens up attractive opportunities to synthesize a broad range of new materials with tunable catalytic properties. 相似文献
17.
Platinum‐Free Binary Co‐Ni Alloy Counter Electrodes for Efficient Dye‐Sensitized Solar Cells
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Xiaoxu Chen Prof. Qunwei Tang Dr. Benlin He Dr. Lin Lin Prof. Liangmin Yu 《Angewandte Chemie (International ed. in English)》2014,53(40):10799-10803
Dye‐sensitized solar cells (DSSCs) have attracted growing interest because of their application in renewable energy technologies in developing modern low‐carbon economies. However, the commercial application of DSSCs has been hindered by the high expenses of platinum (Pt) counter electrodes (CEs). Here we use Pt‐free binary Co‐Ni alloys synthesized by a mild hydrothermal strategy as CE materials in efficient DSSCs. As a result of the rapid charge transfer, good electrical conduction, and reasonable electrocatalysis, the power conversion efficiencies of Co‐Ni‐based DSSCs are higher than those of Pt‐only CEs, and the fabrication expense is markedly reduced. The DSSCs based on a CoNi0.25 alloy CE displays an impressive power conversion efficiency of 8.39 %, fast start‐up, multiple start/stop cycling, and good stability under extended irradiation. 相似文献
18.
The Direct Synthesis of Hydrogen Peroxide Using Platinum‐Promoted Gold–Palladium Catalysts
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Dr. Jennifer K. Edwards James Pritchard Li Lu Marco Piccinini Greg Shaw Dr. Albert F. Carley David J. Morgan Prof. Christopher J. Kiely Prof. Graham J. Hutchings 《Angewandte Chemie (International ed. in English)》2014,53(9):2381-2384
The direct synthesis of hydrogen peroxide offers a potentially green route to the production of this important commodity chemical. Early studies showed that Pd is a suitable catalyst, but recent work indicated that the addition of Au enhances the activity and selectivity significantly. The addition of a third metal using impregnation as a facile preparation method was thus investigated. The addition of a small amount of Pt to a CeO2‐supported AuPd (weight ratio of 1:1) catalyst significantly enhanced the activity in the direct synthesis of H2O2 and decreased the non‐desired over‐hydrogenation and decomposition reactions. The addition of Pt to the AuPd nanoparticles influenced the surface composition, thus leading to the marked effects that were observed on the catalytic formation of hydrogen peroxide. In addition, an experimental approach that can help to identify the optimal nominal ternary alloy compositions for this reaction is demonstrated. 相似文献
19.
Bentian Zhang Gengtao Fu Yutao Li Lecheng Liang Nicholas S. Grundish Yawen Tang John B. Goodenough Zhiming Cui 《Angewandte Chemie (International ed. in English)》2020,59(20):7857-7863
Controllable synthesis of atomically ordered intermetallic nanoparticles (NPs) is crucial to obtain superior electrocatalytic performance for fuel cell reactions, but still remains arduous. Herein, we demonstrate a novel and general hydrogel‐freeze drying strategy for the synthesis of reduced graphene oxide (rGO) supported Pt3M (M=Mn, Cr, Fe, Co, etc.) intermetallic NPs (Pt3M/rGO‐HF) with ultrasmall particle size (about 3 nm) and dramatic monodispersity. The formation of hydrogel prevents the aggregation of graphene oxide and significantly promotes their excellent dispersion, while a freeze‐drying can retain the hydrogel derived three‐dimensionally (3D) porous structure and immobilize the metal precursors with defined atomic ratio on GO support during solvent sublimation, which is not afforded by traditional oven drying. The subsequent annealing process produces rGO supported ultrasmall ordered Pt3M intermetallic NPs (≈3 nm) due to confinement effect of 3D porous structure. Such Pt3M intermetallic NPs exhibit the smallest particle size among the reported ordered Pt‐based intermetallic catalysts. A detailed study of the synthesis of ordered intermetallic Pt3Mn/rGO catalyst is provided as an example of a generally applicable method. This study provides an economical and scalable route for the controlled synthesis of Pt‐based intermetallic catalysts, which can pave a way for the commercialization of fuel cell technologies. 相似文献
20.
Podlike N‐Doped Carbon Nanotubes Encapsulating FeNi Alloy Nanoparticles: High‐Performance Counter Electrode Materials for Dye‐Sensitized Solar Cells
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Xiaojia Zheng Jiao Deng Nan Wang Prof. Dehui Deng Prof. Wen‐Hua Zhang Prof. Xinhe Bao Prof. Can Li 《Angewandte Chemie (International ed. in English)》2014,53(27):7023-7027
Podlike nitrogen‐doped carbon nanotubes encapsulating FeNi alloy nanoparticles (Pod(N)‐FeNi) were prepared by the direct pyrolysis of organometallic precursors. Cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and Tafel polarization measurements revealed their excellent electrocatalytic activities in the I?/I3? redox reaction of dye‐sensitized solar cells (DSSCs). This is suggested to arise from the modification of the surface electronic properties of the carbon by the encapsulated metal alloy nanoparticles (NPs). Sequential scanning with EIS and CV further showed the high electrochemical stability of the Pod(N)‐FeNi composite. DSSCs with Pod(N)‐FeNi as the counter electrode (CE) presented a power conversion efficiency of 8.82 %, which is superior to that of the control device with sputtered Pt as the CE. The Pod(N)‐FeNi composite thus shows promise as an environmentally friendly, low‐cost, and highly efficient CE material for DSSCs. 相似文献