Carbon dioxide electroreduction (CO2R) is being actively studied as a promising route to convert carbon emissions to valuable chemicals and fuels. However, the fraction of input CO2 that is productively reduced has typically been very low, <2% for multicarbon products; the balance reacts with hydroxide to form carbonate in both alkaline and neutral reactors. Acidic electrolytes would overcome this limitation, but hydrogen evolution has hitherto dominated under those conditions. We report that concentrating potassium cations in the vicinity of electrochemically active sites accelerates CO2 activation to enable efficient CO2R in acid. We achieve CO2R on copper at pH <1 with a single-pass CO2 utilization of 77%, including a conversion efficiency of 50% toward multicarbon products (ethylene, ethanol, and 1-propanol) at a current density of 1.2 amperes per square centimeter and a full-cell voltage of 4.2 volts.
A versatile synthetic method based on solvothermal technique has been developed for the fabrication of TiO(2) nanocrystals with different shapes such as rhombic, truncated rhombic, spherical, dog-bone, truncated and elongated rhombic, and bar. The central features of our approach are the use of water vapor as hydrolysis agent to accelerate the reaction and the use of both oleic acid and oleylamine as two distinct capping surfactants which have different binding strengths to control the growth of the TiO(2) nanoparticles. We also show that the presence of an appropriate amount of water vapor along with the desired oleic acid/oleylamine molar ratio plays a crucial role in controlling size and shape of TiO(2) nanocrystals.
The carbon dioxide reduction reaction (CO 2 RR) presents the opportunity to consume CO 2 and produce desirable products. However, the alkaline conditions required for productive CO 2 RR result in the bulk of input CO 2 being lost to bicarbonate and carbonate. This loss imposes a 25% limit on the conversion of CO 2 to multicarbon (C 2+ ) products for systems that use anions as the charge carrierand overcoming this limit is a challenge of singular importance to the field. Here, we find that cation exchange membranes (CEMs) do not provide the required locally alkaline conditions, and bipolar membranes (BPMs) are unstable, delaminating at the membrane−membrane interface. We develop a permeable CO 2 regeneration layer (PCRL) that provides an alkaline environment at the CO 2 RR catalyst surface and enables local CO 2 regeneration. With the PCRL strategy, CO 2 crossover is limited to 15% of the amount of CO 2 converted into products, in all cases. Low crossover and low flow rate combine to enable a single pass CO 2 conversion of 85% (at 100 mA/cm 2 ), with a C 2+ faradaic efficiency and full cell voltage comparable to the anion-conducting membrane electrode assembly.
In alkaline and neutral MEA CO2 electrolyzers, CO2 rapidly converts to (bi)carbonate, imposing a significant energy penalty arising from separating CO2 from the anode gas outlets. Here we report a CO2 electrolyzer uses a bipolar membrane (BPM) to convert (bi)carbonate back to CO2, preventing crossover; and that surpasses the single-pass utilization (SPU) limit (25% for multi-carbon products, C2+) suffered by previous neutral-media electrolyzers. We employ a stationary unbuffered catholyte layer between BPM and cathode to promote C2+ products while ensuring that (bi)carbonate is converted back, in situ, to CO2 near the cathode. We develop a model that enables the design of the catholyte layer, finding that limiting the diffusion path length of reverted CO2 to ~10 μm balances the CO2 diffusion flux with the regeneration rate. We report a single-pass CO2 utilization of 78%, which lowers the energy associated with downstream separation of CO2 by 10× compared with past systems.
Silver orthophosphate nanocrystals with controlled particle size have been synthesized using a simple, reproducible and easily scaled up route based on the reaction between silver ions, oleylamine and phosphoric acid. The obtained nanocrystals are highly uniform in size and exhibit high visible light activity for the photodecomposition of organic compounds.
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