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.
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.
Tin
oxide (SnO2) has recently emerged as a promising
electron transport layer for perovskite solar cells (PSCs) in light
of the material’s optical and electronic properties and its
low-temperature processing. However, SnO2 films are prone
to surface defect formation, which results in energy loss in PSCs.
We report that surface treatment using ammonium fluoride (NH4F) leads to reduced surface defects and that it also induces chemical
doping of the SnO2 substrate simultaneously. The effects
of NH4F treatment on SnO2 properties are revealed
by surface chemical analysis, computational studies, and energy level
investigations, and PSCs with the treatment achieve photovoltaic performance
of 23.2% in light of higher voltage than in relevant controls.
The all‐inorganic nature of CsPbI3 perovskites allows to enhance stability in perovskite devices. Research efforts have led to improved stability of the black phase in CsPbI3 films; however, these strategies—including strain and doping—are based on organic‐ligand‐capped perovskites, which prevent perovskites from forming the close‐packed quantum dot (QD) solids necessary to achieve high charge and thermal transport. We developed an inorganic ligand exchange that leads to CsPbI3 QD films with superior phase stability and increased thermal transport. The atomic‐ligand‐exchanged QD films, once mechanically coupled, exhibit improved phase stability, and we link this to distributing strain across the film. Operando measurements of the temperature of the LEDs indicate that KI‐exchanged QD films exhibit increased thermal transport compared to controls that rely on organic ligands. The LEDs exhibit a maximum EQE of 23 % with an electroluminescence emission centered at 640 nm (FWHM: ≈31 nm). These red LEDs provide an operating half‐lifetime of 10 h (luminance of 200 cd m−2) and an operating stability that is 6× higher than that of control devices.
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