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Christian Engelbrekt Dmitrii Glukhov Yueqi Li Renat R. Nazmutdinov Jing Tang Jens Ulstrup Zixiao Wang Xinxin Xiao Jiawei Yan Xiaomei Yan Tamara Zinkicheva 《Current Opinion in Electrochemistry》2021
Structural mapping of intermediate size and large molecules and biomolecules at ultra-high resolution using single-crystal electrodes and in situ scanning tunnelling microscopy continues to disclose surprising findings. In situ scanning tunnelling spectroscopy has also recently disclosed new electrochemical conductivity features at the level of the single molecule. We overview briefly elements of this development over the last few years, with focus on three recent discoveries: (1) a new packing mode of a core monolayer target thiol, the amino acid cysteine (Cys) on Au(100)-electrodes, quite different from Cys packing on Au(111)- and Au(110)-electrodes; (2) transition of a core ferrocene in situ scanning tunnelling spectroscopy probe from stochastic single-molecule to macroscopic behaviour, a concept at the heart of nanoscience; and (3) unexpected behaviour of the large molybdenum enzyme sulfite oxidase, when going from macroscopic to single-molecule electrochemistry. We compare these studies with other recent discoveries of single-molecule protein conductivity and molecular scale inorganic nanostructures. 相似文献
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Construction of Insulin 18‐mer Nanoassemblies Driven by Coordination to Iron(II) and Zinc(II) Ions at Distinct Sites
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Dr. Henrik K. Munch Jesper Nygaard Dr. Niels Johan Christensen Dr. Christian Engelbrekt Mads Østergaard Dr. Trine Porsgaard Dr. Thomas Hoeg‐Jensen Prof. Dr. Jingdong Zhang Prof. Dr. Lise Arleth Prof. Dr. Peter W. Thulstrup Prof. Dr. Knud J. Jensen 《Angewandte Chemie (International ed. in English)》2016,55(7):2378-2381
Controlled self‐assembly (SA) of proteins offers the possibility to tune their properties or to create new materials. Herein, we present the synthesis of a modified human insulin (HI) with two distinct metal‐ion binding sites, one native, the other abiotic, enabling hierarchical SA through coordination with two different metal ions. Selective attachment of an abiotic 2,2′‐bipyridine (bipy) ligand to HI, yielding HI–bipy, enabled ZnII‐binding hexamers to SA into trimers of hexamers, [[HI–bipy]6]3, driven by octahedral coordination to a FeII ion. The structures were studied in solution by small‐angle X‐ray scattering and on surfaces with AFM. The abiotic metal ligand had a higher affinity for FeII than ZnII ions, enabling control of the hexamer formation with ZnII and the formation of trimers of hexamers with FeII ions. This precise control of protein SA to give oligomers of oligomers provides nanoscale structures with potential applications in nanomedicine. 相似文献
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Engelbrekt Christian Malcho Phillip Andersen Jonas Zhang Lijuan Ståhl Kenny Li Bin Hu Jun Zhang Jingdong 《Journal of nanoparticle research》2014,16(8):1-12
To investigate the shell deposited kinetics, CdSe quantum dots (QDs) and nanorods (NRs) with a maximum length of 17 nm were fabricated via organic synthesis routes. CdSe with a hexagonal crystal structure (wurtzite) favors epitaxial growth on the {002} surfaces when well-controlled conditions were used. The morphologies and sizes of CdSe samples depended strongly on chemicals and temperature. In the case of 320 °C, CdSe NRs with adjusted length of 7–17 nm were obtained from trioctylphosphine oxide (TOPO) and tetradecylphosphonic acid (TDPA). In contrast, short CdSe NRs (less than 10 nm) were created from octadecylphosphonic acid (ODPA) and trioctylamine (TOA). Spherical CdSe QDs were further fabricated using stearic acid (SA) and TOPO at 300 °C. CdSe cores were coated with Cd0.5Zn0.5S and CdTe shells. Anisotropic growth occurred during shell deposition because CdS shells grown preferentially on the {001} facet of the CdSe core. In the case of CdSe core prepared from TOPO and TDPA, CdSe/Cd0.5Zn0.5S core/shell samples prepared from long CdSe NRs (more than 10 nm) revealed a peanut morphology while the core/shell samples created from short ones (less than 10 nm) exhibited a spherical morphology. All of the CdSe/Cd0.5Zn0.5S core/shell samples revealed a similar length to that of the CdSe cores. This phenomenon was also observed for the core/shell samples fabricated using CdSe NRs prepared by ODPA and TOA. This is ascribed to the well-developed crystal structure of CdSe NRs fabricated using an organic synthesis at high temperature. In contrast, this anisotropic growth did not occur when spherical CdSe QDs prepared from SA and TOPO and the shell (Cd0.5Zn0.5S) coating carried out using SA and TOA. To indicate the shell depositing process, CdSe NRs fabricated using TDPA and TOPO were coated with a CdTe shell. CdTe monomers were deposited on the middle and tip parts of the CdSe NRs to form a tetrapod-like morphology at 220 °C. This is ascribed to the large difference of structure of CdSe (hexagonal) and CdTe (zinc blende). 相似文献
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The oxidative dehydrogenation of alcohols to aldehydes catalyzed by Ag nanoparticles supported on Al2O3 was studied.The catalyst promoted the direct formation of imines by tandem oxidative dehydrogenation and condensation of alcohols and amines.The reactions were performed under mild conditions and afforded the imines in high yield(up to 99%) without any byproducts other than H2O.The highest activity was obtained over 5 wt%Ag/Al2O3 in toluene with air as oxidant.The reactions were also performed under oxidant-free conditions where the reaction was driven to the product side by the production of H2 in the gas phase.The use of an efficient and selective Ag catalyst for the oxidative dehydrogenation of alcohol in the presence of amines gives a new green reaction protocol for imine synthesis. 相似文献
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