Regulating the selectivity toward a target hydrocarbon product is still the focus of CO2electroreduction. Here, we discover that the original surface Cu species in Cu gas‐diffusion electrodes plays a more important role than the surface roughness, local pH, and facet in governing the selectivity toward C1or C2hydrocarbons. The selectivity toward C2H4progressively increases, while CH4decreases steadily upon lowering the Cu oxidation species fraction. At a relatively low electrodeposition voltage of 1.5 V, the Cu gas‐diffusion electrode with the highest Cuδ+/Cu0ratio favors the pathways of hydrogenation to form CH4with maximum Faradaic efficiency of 65.4% and partial current density of 228 mA cm−2at −0.83 V vs RHE. At 2.0 V, the Cu gas‐diffusion electrode with the lowest Cuδ+/Cu0ratio prefers C–C coupling to form C2+products with Faradaic efficiency topping 80.1% at −0.75 V vs RHE, where the Faradaic efficiency of C2H4accounts for 46.4% and the partial current density of C2H4achieves 279 mA cm−2. This work demonstrates that the selectivity from CH4to C2H4is switchable by tuning surface Cu species composition of Cu gas‐diffusion electrodes.
more »
« less
This content will become publicly available on February 26, 2026
Rate-Based Model Simulation with Experimental Mixture Properties for R-410A Separation Using 1-Ethyl-3-methylimidazolium Bis(trifluoromethylsulfonyl)imide [C 2 C 1 im][Tf 2 N]
- Award ID(s):
- 2213965
- PAR ID:
- 10634631
- Publisher / Repository:
- ACS
- Date Published:
- Journal Name:
- Industrial & Engineering Chemistry Research
- Volume:
- 64
- Issue:
- 8
- ISSN:
- 0888-5885
- Page Range / eLocation ID:
- 4604 to 4615
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract We present laboratory rotational spectroscopy of five isomers of cyanoindene (2-, 4-, 5-, 6-, and 7-cyanoindene) using a cavity Fourier transform microwave spectrometer operating between 6 and 40 GHz. Based on these measurements, we report the detection of 2-cyanoindene (1H-indene-2-carbonitrile; 2- C 9 H 7 CN ) in GOTHAM line survey observations of the dark molecular cloud TMC-1 using the Green Bank Telescope at centimeter wavelengths. Using a combination of Markov Chain Monte Carlo, spectral stacking, and matched filtering techniques, we find evidence for the presence of this molecule at the 6.3 σ level. This provides the first direct observation of the ratio of a cyano-substituted polycyclic aromatic hydrocarbon to its pure hydrocarbon counterpart, in this case indene, in the same source. We discuss the possible formation chemistry of this species, including why we have only detected one of the isomers in TMC-1. We then examine the overall hydrocarbon:CN-substituted ratio across this and other simpler species, as well as compare to those ratios predicted by astrochemical models. We conclude that while astrochemical models are not yet sufficiently accurate to reproduce absolute abundances of these species, they do a good job at predicting the ratios of hydrocarbon:CN-substituted species, further solidifying -CN tagged species as excellent proxies for their fully symmetric counterparts.more » « less
-
We unravel, for the very first time, the formation pathways of hydroxyacetone (CH 3 COCH 2 OH), methyl acetate (CH 3 COOCH 3 ), and 3-hydroxypropanal (HCOCH 2 CH 2 OH), as well as their enol tautomers within mixed ices of methanol (CH 3 OH) and acetaldehyde (CH 3 CHO) analogous to interstellar ices in the ISM exposed to ionizing radiation at ultralow temperatures of 5 K. Exploiting photoionization reflectron time-of-flight mass spectrometry (PI-ReToF-MS) and isotopically labeled ices, the reaction products were selectively photoionized allowing for isomer discrimination during the temperature-programmed desorption phase. Based on the distinct mass-to-charge ratios and ionization energies of the identified species, we reveal the formation pathways of hydroxyacetone (CH 3 COCH 2 OH), methyl acetate (CH 3 COOCH 3 ), and 3-hydroxypropanal (HCOCH 2 CH 2 OH) via radical–radical recombination reactions and of their enol tautomers (prop-1-ene-1,2-diol (CH 3 C(OH)CHOH), prop-2-ene-1,2-diol (CH 2 C(OH)CH 2 OH), 1-methoxyethen-1-ol (CH 3 OC(OH)CH 2 ) and prop-1-ene-1,3-diol (HOCH 2 CHCHOH)) via keto-enol tautomerization. To the best of our knowledge, 1-methoxyethen-1-ol (CH 3 OC(OH)CH 2 ) and prop-1-ene-1,3-diol (HOCH 2 CHCHOH) are experimentally identified for the first time. Our findings help to constrain the formation mechanism of hydroxyacetone and methyl acetate detected within star-forming regions and suggest that the hitherto astronomically unobserved isomer 3-hydroxypropanal and its enol tautomers represent promising candidates for future astronomical searches. These enol tautomers may contribute to the molecular synthesis of biologically relevant molecules in deep space due to their nucleophilic character and high reactivity.more » « less
An official website of the United States government
