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1.
Xu Zhao Sarah E. Cleary Ceren Zor Nicole Grobert Holly A. Reeve Kylie A. Vincent 《Chemical science》2021,12(23):8105
Heterogeneous biocatalytic hydrogenation is an attractive strategy for clean, enantioselective C X reduction. This approach relies on enzymes powered by H2-driven NADH recycling. Commercially available carbon-supported metal (metal/C) catalysts are investigated here for direct H2-driven NAD+ reduction. Selected metal/C catalysts are then used for H2 oxidation with electrons transferred via the conductive carbon support material to an adsorbed enzyme for NAD+ reduction. These chemo-bio catalysts show improved activity and selectivity for generating bioactive NADH under ambient reaction conditions compared to metal/C catalysts. The metal/C catalysts and carbon support materials (all activated carbon or carbon black) are characterised to probe which properties potentially influence catalyst activity. The optimised chemo-bio catalysts are then used to supply NADH to an alcohol dehydrogenase for enantioselective (>99% ee) ketone reductions, leading to high cofactor turnover numbers and Pd and NAD+ reductase activities of 441 h−1 and 2347 h−1, respectively. This method demonstrates a new way of combining chemo- and biocatalysis on carbon supports, highlighted here for selective hydrogenation reactions.Heterogeneous chemo-bio catalytic hydrogenation is an attractive strategy for clean, enantioselective C X reduction. 相似文献
2.
Terrones M Banhart F Grobert N Charlier JC Terrones H Ajayan PM 《Physical review letters》2002,89(7):075505
Crossing single-walled carbon nanotubes can be joined by electron beam welding to form molecular junctions. Stable junctions of various geometries are created in situ in a transmission electron microscope. Electron beam exposure at high temperatures induces structural defects which promote the joining of tubes via cross-linking of dangling bonds. The observations are supported by molecular dynamics simulations which show that the creation of vacancies and interstitials induces the formation of junctions involving seven- or eight-membered carbon rings at the surface between the tubes. 相似文献
3.
D. Golberg P.S. Dorozhkin Y. Bando Z.-C. Dong C.C. Tang Y. Uemura N. Grobert M. Reyes-Reyes H. Terrones M. Terrones 《Applied Physics A: Materials Science & Processing》2003,76(4):499-507
Transport and field-emission properties of as-synthesized CNx and BNCx (x<0.1) multi-walled nanotubes were compared in detail. Individual ropes made of these nanotubes and macrofilms of those
were tested. Before measurements, the nanotubes were thoroughly characterized using high-resolution and energy-filtered electron
microscopy, electron diffraction and electron-energy-loss spectroscopy. Individual ropes composed of dozens of CNx nanotubes displayed well-defined metallic behavior and low resistivities of ∼10–100 kΩ or less at room temperature, whereas
those made of BNCx nanotubes exhibited semiconducting properties and high resistivities of ∼50–300 MΩ. Both types of ropes revealed good field-emission
properties with emitting currents per rope reaching ∼4 μA(CNx) and ∼2 μA (BNCx), albeit the latter ropes se- verely deteriorated during the field emission. Macrofilms made of randomly oriented CNx or BNCx nanotubes displayed low and similar turn-on fields of ∼2–3 V/μm. 3 mA/cm2 (BNCx) and 5.5 mA/cm2 (CNx) current densities were reached at 5.5 V/μm macroscopic fields. At a current density of 0.2–0.4 mA/cm2 both types of compound nanotubes exhibited equally good emission stability over tens of minutes; by contrast, on increasing
the current density to 0.2–0.4 A/cm2, only CNx films continued to emit steadily, while the field emission from BNCx nanotube films was prone to fast degradation within several tens of seconds, likely due to arcing and/or resistive heating.
Received: 29 October 2002 / Accepted: 1 November 2002 / Published online: 10 March 2003
RID="*"
ID="*"Corresponding author. Fax: +81-298/51-6280, E-mail: golberg.dmitri@nims.go.jp 相似文献
4.
J. Piccard R. Kayser C. H. Wolff R. Vlbricht E. List E. Biltz Louvet B. Haas Leo Liebermann A. Dupré A. Pizzi C. Jegel H. Macagno Pellet und de Grobert 《Fresenius' Journal of Analytical Chemistry》1882,21(1):424-432
Ohne Zusammenfassung 相似文献
5.
M. Terrones P.M. Ajayan F. Banhart X. Blase D.L. Carroll J.C. Charlier R. Czerw B. Foley N. Grobert R. Kamalakaran P. Kohler-Redlich M. Rühle T. Seeger H. Terrones 《Applied Physics A: Materials Science & Processing》2002,74(3):355-361
Self-assembly pyrolytic routes to large arrays (<2.5 cm2) of aligned CNx nanotubes (15–80 nm OD and <100 μm in length) are presented. The method involves the thermolysis of ferrocene/melamine mixtures
(5:95) at 900–1000 °C in the presence of Ar. Electron energy loss spectroscopy (EELS) reveals that the N content varies from
2–10%, and can be bonded to C in two different fashions (double-bonded and triple-bonded nitrogen). The electronic densities
of states (DOS) of these CNx nanotubes, using scanning tunneling spectroscopy (STS), are presented. The doped nanotubes exhibit strong features in the
conduction band close to the Fermi level (0.18 eV). Using tight-binding and ab initio calculations, we confirm that pyridine-like
(double-bonded) N is responsible for introducing donor states close to the Fermi Level. These electron-rich structures are
the first example of n-type nanotubes. Finally, it will be shown that moderate electron irradiation at 700–800 °C is capable
of coalescing single-walled nanotubes (SWNTs). The process has also been studied using tight-binding molecular dynamics (TBMD).
Vacancies induce the coalescence via a zipper-like mechanism, which has also been observed experimentally. These vacancies
trigger the organization of atoms on the tube lattices within adjacent tubes. These results pave the way to the fabrication
of nanotube heterojunctions, robust composites, contacts, nanocircuits and strong 3D composites using N-doped tubes as well
as SWNTs.
Received: 10 October 2001 / Accepted: 3 December 2001 / Published online: 4 March 2002 相似文献
6.
Mandel K Dillon F Koos AA Aslam Z Jurkschat K Cullen F Crossley A Bishop H Moh K Cavelius C Arzt E Grobert N 《Chemical communications (Cambridge, England)》2011,47(14):4108-4110
Monodisperse, size-controlled Ni-P nanoparticles were synthesised in a single step process using triphenyl-phosphane (TPP), oleylamine (OA), and Ni(II)acetyl-acetonate. The nanoparticles were amorphous, contained ~30 at% P and their size was controlled between 7-21 nm simply by varying the amount of TPP. They are catalytically active for tailored carbon nanotube growth. 相似文献
7.
Solid-phase production of carbon nanotubes 总被引:4,自引:0,他引:4
W.K. Hsu Y.Q. Zhu S. Trasobares H. Terrones M. Terrones N. Grobert H. Takikawa J.P. Hare H.W. Kroto D.R.M. Walton 《Applied Physics A: Materials Science & Processing》1999,68(4):493-495
4 C3) are heated to 1000–1100 °C for 2–4 hr in an argon flow. Carbon nanotubes are formed when metal powders, e.g. Fe, Co, Y and
Ni, are also present.
Received: 2 February 1999 / Accepted: 3 February 1999 相似文献
8.
Yoon M Han S Kim G Lee SB Berber S Osawa E Ihm J Terrones M Banhart F Charlier JC Grobert N Terrones H Ajayan PM Tománek D 《Physical review letters》2004,92(7):075504
We propose a new microscopic mechanism to explain the unusually fast fusion process of carbon nanotubes. We identify the detailed pathway for two adjacent (5,5) nanotubes to gradually merge into a (10,10) tube, and characterize the transition states. The propagation of the fused region is energetically favorable and proceeds in a morphology reminiscent of a Y junction via a zipper mechanism, involving only Stone-Wales bond rearrangements with low activation barriers. The zipper mechanism of fusion is supported by a time series of high-resolution transmission electron microscopy observations. 相似文献
9.
Terrones H Terrones M Hernandez E Grobert N Charlier JC Ajayan PM 《Physical review letters》2000,84(8):1716-1719
We propose a new family of layered sp(2)-like carbon crystals, incorporating five-, six-, and seven-membered rings in 2D Bravais lattices. These periodic sheets can be rolled so as to generate nanotubes of different diameter and chirality. We demonstrate that these sheets and tubes are metastable and more favorable than C60, and it is also shown that their mechanical properties are similar to those of graphene. Density of states calculations of all structures revealed an intrinsic metallic behavior, independent of orientation, tube diameter, and chirality. 相似文献
10.
P. Waentig W. Gierisch C. Mannich Käthe Lenz F. Kaulfersch H. T. Brown A. R. Ling Th Rendle T. Cl Taylor H. A. Iddles J. C. Small H. I. Waterman H. de Wijs M. Wagenaar W. D. Horne J. F. Brewster V. Skola de Grobert R. Gillet K. Andrlik C. Müller E. Saillard H. Pellet C. S. Hudson T. S. Harding P. Beyersdorfer und F. W. Reynolds 《Fresenius' Journal of Analytical Chemistry》1928,74(12):460-470
Ohne Zusammenfassung 相似文献