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Bin Fang Jin Luo Peter N. Njoki Rameshwori Loukrakpam Derrick Mott Bridgid Wanjala Xiang Hu Chuan-Jian Zhong 《Electrochemistry communications》2009,11(6):1139-1141
This paper reports new findings of an investigation of the electrocatalytic performance of nanostructured PtVFe catalysts in proton exchange membrane fuel cells (PEMFC). The membrane electrode assembly was prepared using nano-engineered PtVFe nanoparticles with controlled composition and size supported on carbon as the cathode electrocatalysts. The results reveal that the PtVFe/C catalysts exhibited excellent fuel cell performance, better than that using the commercial Pt/C catalyst. This finding provides the first example demonstrating the viability of the PEMFC application of the nanostructured trimetallic catalysts. 相似文献
2.
L Yang S Shan R Loukrakpam V Petkov Y Ren BN Wanjala MH Engelhard J Luo J Yin Y Chen CJ Zhong 《Journal of the American Chemical Society》2012,134(36):15048-15060
The understanding of the atomic-scale structural and chemical ordering in supported nanosized alloy particles is fundamental for achieving active catalysts by design. This report shows how such knowledge can be obtained by a combination of techniques including X-ray photoelectron spectroscopy and synchrotron radiation based X-ray fine structure absorption spectroscopy and high-energy X-ray diffraction coupled to atomic pair distribution function analysis, and how the support-nanoalloy interaction influences the catalytic activity of ternary nanoalloy (platinum-nickel-cobalt) particles on three different supports: carbon, silica, and titania. The reaction of carbon monoxide with oxygen is employed as a probe to the catalytic activity. The thermochemical processing of this ternary composition, in combination with the different support materials, is demonstrated to be capable of fine-tuning the catalytic activity and stability. The support-nanoalloy interaction is shown to influence structural and chemical ordering in the nanoparticles, leading to support-tunable active sites on the nanoalloys for oxygen activation in the catalytic oxidation of carbon monoxide. A nickel/cobalt-tuned catalytic site on the surface of nanoalloy is revealed for oxygen activation, which differs from the traditional oxygen-activation sites known for oxide-supported noble metal catalysts. The discovery of such support-nanoalloy interaction-enabled oxygen-activation sites introduces a very promising strategy for designing active catalysts in heterogeneous catalysis. 相似文献
3.
Wanjala BN Fang B Luo J Chen Y Yin J Engelhard MH Loukrakpam R Zhong CJ 《Journal of the American Chemical Society》2011,133(32):12714-12727
This Article describes findings of the correlation between the atomic scale structure and the electrocatalytic performance of nanoengineered PtNiFe/C catalysts treated at different temperatures for oxygen reduction reaction, aiming at providing a new fundamental insight into the role of the detailed atomic alloying and interaction structures of the catalysts in fuel cell reactions. Both mass and specific activities of the catalysts were determined using rotating disk electrode and proton exchange membrane fuel cell. The mass activities extracted from the kinetic regions in both measurements revealed a consistent trend of decreasing activity with increasing temperature. However, the specific activity data from RDE revealed an opposite trend, that is, increasing activity with increasing temperature. In addition to TEM, XRD, and XPS characterizations, a detailed XAFS analysis of the atomic scale coordination structures was carried out, revealing increased heteroatomic coordination with improved alloying structures for the catalyst treated at the elevated temperatures. XPS analysis has further revealed a reduced surface concentration of Pt for the catalyst for the high temperature treated catalyst. The higher mass activity for the lower temperature treated catalyst is due to Pt surface enrichment on the surface sites, whereas the higher specific activity for the higher temperature treated catalyst reflects an enhanced Pt-alloying surface sites. These findings have thus provided a new insight for assessing the structural correlation of the electrocatalytic activity with the fcc-type lattice change and the atomic scale alloying characteristics. Implications of these findings to the design of highly active alloy electrocatalysts are discussed, along with their enhanced electrocatalytic performance in the fuel cell. 相似文献
4.
Yan H Luo J Xie HM Xie DX Su Q Yin J Wanjala BN Diao H An DL Zhong CJ 《Physical chemistry chemical physics : PCCP》2011,13(13):5824-5830
A nanoparticle-based strategy has been demonstrated using structurally-tailored tert-butylcalixarenes immobilized on gold nanoparticles to tune the guest access to the calixarene cone cavity for cationic recognition. This strategy exploits the interparticle charge-induced aggregation upon selective capture of metal cations into the nanoparticle-immobilized tert-butylcalixarenes, which produces calorimetric changes for the detection. A possible pathway for the binding of M(n+) into the t-BCA structure and the interparticle interaction is proposed for the formation of an electric double layer inducing the interparticle association responsible for the red-shifted surface plasmon resonance band of the nanoparticles. The value of this class of calorimetric nanoprobes will be in the area of designing advanced host-guest probes using a variety of calixarene ligands for ionic recognition in a simplistic detection format. 相似文献
5.
Background
Elevated numbers of regulatory T cells (Tregs) have been implicated in certain cancers. Depletion of Tregs has been shown to increase anti-tumor immunity. Tregs also play a critical role in the suppression of autoimmune responses. The study of Tregs has been hampered by a lack of adequate surface markers. Leucine Rich Repeat Containing 32 (LRRC32), also known as Glycoprotein A Repetitions Predominant (GARP), has been postulated as a novel surface marker of activated Tregs. However, there is limited information regarding the processing of LRRC32 or the regulatory phenotype and functional activity of Tregs expressing LRRC32.Results
Using naturally-occurring freshly isolated Tregs, we demonstrate that low levels of LRRC32 are present intracellularly prior to activation and that freshly isolated LRRC32+ Tregs are distinct from LRRC32- Tregs with respect to the expression of surface CD62L. Using LRRC32 transfectants of HEK cells, we demonstrate that the N-terminus of LRRC32 is cleaved prior to expression of the protein at the cell surface. Furthermore, we demonstrate using a construct containing a deleted putative signal peptide region that the presence of a signal peptide region is critical to cell surface expression of LRRC32. Finally, mixed lymphocyte assays demonstrate that LRRC32+ Tregs are more potent suppressors than LRRC32- Tregs.Conclusions
A cleaved signal peptide site in LRRC32 is necessary for surface localization of native LRRC32 following activation of naturally-occurring freshly-isolated regulatory T cells. LRRC32 expression appears to alter the surface expression of activation markers of T cells such as CD62L. LRRC32 surface expression may be useful as a marker that selects for more potent Treg populations. In summary, understanding the processing and expression of LRRC32 may provide insight into the mechanism of action of Tregs and the refinement of immunotherapeutic strategies aimed at targeting these cells. 相似文献6.
Yin J Hu P Wanjala B Malis O Zhong CJ 《Chemical communications (Cambridge, England)》2011,47(35):9885-9887
This report demonstrates a molecule-solid duality concept for nanoscale control of size, shape and alloying by showing novel evolution of binary copper and gold nanoclusters or nanoparticles towards alloy nanocubes, as evidenced by in situ real time synchrotron X-ray diffraction characterization. 相似文献
7.
We have investigated the superconducting properties of the Bi1.7 Pb0.3Sr2Ca2−xCe
x
Cu3O10+δ system with x=0.00, 0.02, 0.04, 0.08 and 0.1 by X-ray diffraction and magnetic susceptibility. The substitution of Ce for Ca has been found
to drastically change the superconducting properties of the system. X-ray diffraction studies on these compounds indicate
decrease in the c-parameter with increased substitution of Ce at Ca site and volume fraction of high T
c (2 : 2 : 2 : 3) phase decreases and low T
c phase increases. The magnetic susceptibility of this compound shows that the diamagnetic on set superconducting transition
temperature (onset) varies from 109 K to 51 K for x=0.00, 0.02, 0.04, 0.08 and 0.1. These results suggest the possible existence of Ce in a tetravalent state rather than a trivalent
state in this system; that is, Ca2+ → Ce4+ replacement changes the hole carrier concentration. Hole filling is the cause of lowering T
c of the system. 相似文献
8.
We have deposited relatively thick (∼60 nm) Ge layers on Br-passivated Si(111) substrates by thermal evaporation under high
vacuum conditions at room temperature. Ge has grown in a layer-plus-island mode although it is different from the Stranski-Krastanov
growth mode observed in epitaxial growth. Both the islands and the layer are nanocrystalline. This appears to be a consequence
of reduction of surface free energy of the Si(111) substrate by Br-passivation. The size distribution of the Ge nanoislands
has been determined. The Br-Si(111) substrates were prepared by a liquid treatment, which may not produce exactly reproducible
surfaces. Nevertheless, some basic features of the nanostructural island growth are reasonably reproducible, while there are
variations in the details of the island size distribution. 相似文献
9.
The molecular structures of 3 isoflavone glycosides isolated from the root wood of Erythrina latissima were established as 4'-hydroxyisoflavone-7-O-beta-D-glucopyranoside (compound 1); 4'-hydroxyisoflavone-7-O-alpha-L-rhamnosyl (1-->6)-beta-D-glucopyranoside (compound 2); and a new compound 4', 8-dimethoxy isoflavone-7-O-alpha-L-rhamnosyl (1-->6) glucopyranoside (8-O-methylretusin-7-O-alpha-L-rhamnosyl (1-6)-beta-D-glucopyranoside) (compound 3). 相似文献
10.
Wang L Wang X Luo J Wanjala BN Wang C Chernova NA Engelhard MH Liu Y Bae IT Zhong CJ 《Journal of the American Chemical Society》2010,132(50):17686-17689
We report a novel core-shell-structured ternary nanocube of MnZn ferrite synthesized by controlling the reaction temperature and composition in the absence of conventionally used reducing agents. The highly monodispersed core-shell structure consists of an Fe(3)O(4) core and an MnZn Ferrite shell. The observation of a Moire? pattern indicates that the core and the shell are two highly crystalline materials with slightly different lattice constants that are rotated relative to each other by a small angle. The ternary core-shell nanocubes display magnetic properties regulated by a combination of the core-shell composition and exhibit an increased coercivity and field-cooled/zero-field-cooled characteristics drastically different from those of regular MnZn ferrite nanoparticles. The ability to engineer the spatial nanostructures of ternary magnetic nanoparticles in terms of shape and composition offers atomic-level versatility in fine-tuning the nanoscale magnetic properties. 相似文献
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