Efficient electroreduction of carbon dioxide to multicarbon products in aqueous solution is of great importance and challenging. Unfortunately, the low efficiency of the production of C2 products limits implementation at scale. Here, we report reduction of carbon dioxide to C2 products (acetic acid and ethanol) over a 3D dendritic copper-cuprous oxide composite fabricated by in situ reduction of an electrodeposited copper complex. In potassium chloride aqueous electrolyte, the applied potential was as low as −0.4 V vs reversible hydrogen electrode, the overpotential is only 0.53 V (for acetic acid) and 0.48 V (for ethanol) with high C2 Faradaic efficiency of 80% and a current density of 11.5 mA cm−2. The outstanding performance of the electrode for producing the C2 products results mainly from near zero contacting resistance between the electrocatalysts and copper substrate, abundant exposed active sites in the 3D dendritic structure and suitable copper(I)/copper(0) ratio of the electrocatalysts.
17 January 2014 in Instrumentation Science & Technology
This article presents the development and current state of a small-angle X-ray scattering station at beamline 1W2A of the Beijing Synchrotron Radiation Facility, China. The source of the beamline is introduced from a 14-pole wiggler. A triangular bending Si(111) crystal is used to horizontally focus the beam and provide a monochromatic X-ray beam (8.052 keV). A bending cylindrical mirror coated with rhodium downstream from the monochromator is used to vertically focus the beam. The X-ray beam is focused on the detector which is fixed at 30 m from the source. The focused beam size (full width at half maximum) is 1.4 × 0.2 mm2 (horizontal × vertical) with a flux of 5.5 × 1011 phs/s at 2.5 GeV and 250 mA. Besides the routine mode of small-angle X-ray scattering, the combination of small- and wide-angle X-ray scattering, grazing incidence small-angle X-ray scattering, and time-resolved small-angle X-ray scattering in sub-second level are also available for the users. Dependent on the measurement requirements, several detectors can be chosen for the collection of scattering signals. Furthermore, multiple sample environments, including temperature, stress-strain, and liquid sampling are available for in situ measurements. In a typical camera length of 1.5 m, the small-angle X-ray scattering resolution is about 115 nm. The steady operation of the small-angle X-ray scattering station at Beijing Synchrotron Radiation Facility not only provides the small-angle X-ray scattering beam time for users, but also promotes the development and application of these techniques in China.
Amorphous nano-metal catalysts often exhibit appealing catalytic properties, because the intrinsic linear scaling relationship can be broken. However, accurate control synthesis of amorphous nano-metal catalysts with desired size and morphology is a challenge. In this work, we discover that Cu(0) could be oxidized to amorphous CuxO species by supercritical CO2. The formation process of the amorphous CuxO is elucidated with the aid of machine learning. Based on this finding, a method to prepare Cu nanoparticles with an amorphous shell is proposed by supercritical CO2 treatment followed by electroreduction. The unique feature of this method is that the size of the particles with amorphous shell can be easily controlled because their size depends on that of the original crystal Cu nanoparticles. Moreover, the thickness of the amorphous shell can be easily controlled by CO2 pressure and/or treatment time. The obtained amorphous Cu shell exhibits high selectivity for C2+ products with the Faradaic efficiency of 84% and current density of 320 mA cm−2. Especially, the FE of C2+ oxygenates can reach up to 65.3 %, which is different obviously from the crystalline Cu catalysts.
15 September 2020 in Journal of the American Chemical Society