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The remarkable activity and stability of a highly dispersive beta-brass Cu-Zn catalyst for the production of ethylene glycol.

ABSTRACT: Incorporation of Zn atoms into a nanosize Cu lattice is known to alter the electronic properties of Cu, improving catalytic performance in a number of industrially important reactions. However the structural influence of Zn on the Cu phase is not well studied. Here, we show that Cu nano-clusters modified with increasing concentration of Zn, derived from ZnO support doped with Ga(3+), can dramatically enhance their stability against metal sintering. As a result, the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol, an important reaction well known for deactivation from copper nanoparticle sintering, can show greatly enhanced activity and stability with the CuZn alloy catalysts due to no noticeable sintering. HRTEM, nano-diffraction and EXAFS characterization reveal the presence of a small beta-brass CuZn alloy phase (body-centred cubic, bcc) which appears to greatly stabilise Cu atoms from aggregation in accelerated deactivation tests. DFT calculations also indicate that the small bcc CuZn phase is more stable against Cu adatom migration than the fcc CuZn phase with the ability to maintain a higher Cu dispersion on its surface.

SUBMITTER: Li MM

PROVIDER: S-EPMC4746617 | biostudies-literature | 2016 Feb

REPOSITORIES: biostudies-literature

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The remarkable activity and stability of a highly dispersive beta-brass Cu-Zn catalyst for the production of ethylene glycol.

Li Molly Meng-Jung MM Zheng Jianwei J Qu Jin J Liao Fenglin F Raine Elizabeth E Kuo Winson C H WC Su Shei Sia SS Po Pang P Yuan Youzhu Y Tsang Shik Chi Edman SC

Scientific reports 20160209

Incorporation of Zn atoms into a nanosize Cu lattice is known to alter the electronic properties of Cu, improving catalytic performance in a number of industrially important reactions. However the structural influence of Zn on the Cu phase is not well studied. Here, we show that Cu nano-clusters modified with increasing concentration of Zn, derived from ZnO support doped with Ga(3+), can dramatically enhance their stability against metal sintering. As a result, the hydrogenation of dimethyl oxal ...[more]

PMID: 26856760

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Project description:Developing stable nanofluids and improving their thermo-physical properties are highly important in heat transfer applications. In the present work, the stability, thermal conductivity, and rheological properties of tungsten disulphide (WS2) nanoparticles (NPs) with ethylene glycol (EG) were profoundly examined using a particle size analyzer, zeta-sizer, thermal property analyzer, rheometer, and pH measuring system. WS2 NPs were characterized by various techniques, such as XRD (X-Ray Diffraction), FTIR (Fourier Transform Infrared Spectroscopy), FESEM (Field emission scanning electron microscopy), and high-resolution transmission electron microscopy (HRTEM). The nanofluids were obtained with the two-step method by employing three volume concentrations (0.005%, 0.01%, and 0.02%) of WS2. The influence of different surfactants (Sodium dodecyl sulphate (SDS), Sodium dodecylbenzenesulfonate (SDBS), Cetyltrimethylammonium bromide (CTAB)) with various volume concentrations (0.05-2%) on the measured properties has also been evaluated. Pristine WS2/EG nanofluids exhibit low zeta potential values, i.e., -7.9 mV, -9.3 mV, and -5 mV, corresponding to 0.005%, 0.01%, and 0.02% nanofluid, respectively. However, the zeta potential surpassed the threshold (±30 mV) and the maximum values reached of -52 mV, -45 mV, and 42 mV for SDS, SDBS, and CTAB-containing nanofluids. This showed the successful adsorption of surfactants onto WS2, which was also observed through the increased agglomerate size of up to 1720 nm. Concurrently, particularly for 0.05% SDS with 0.005% WS2, thermal conductivity was enhanced by up to 4.5%, with a corresponding decrease in viscosity of up to 10.5% in a temperature range of (25-70 °C), as compared to EG. Conversely, the viscoelastic analysis has indicated considerable yield stress due to the presence of surfactants, while the pristine nanofluids exhibited enhanced fluidity over the entire tested deformation range. The shear flow behavior showed a transition from a non-Newtonian to a Newtonian fluid at a low shear rate of 10 s-1. Besides this, the temperature sweep analysis has shown a viscosity reduction in a range of temperatures (25-70 °C), with an indication of a critical temperature limit. However, owing to an anomalous reduction in the dynamic viscosity of up to 10.5% and an enhancement in the thermal conductivity of up to 6.9%, WS2/EG nanofluids could be considered as a potential candidate for heat transfer applications.

Dataset Information

The remarkable activity and stability of a highly dispersive beta-brass Cu-Zn catalyst for the production of ethylene glycol.

Publications

The remarkable activity and stability of a highly dispersive beta-brass Cu-Zn catalyst for the production of ethylene glycol.

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