Lewis-base ligand-reshaped interfacial hydrogen-bond network boosts CO2 electrolysis

Electrocatalytic semi‐hydrogenation of alkynols holds tremendous advantages over conventional thermocatalysis process. However, the selectivity‐activity seesaw effect is a principal obstacle to its further development. Inspired by interfacial self‐assembled monolayers, alkanethiols with different alkyl chain lengths are employed to modify the Cu surface for controllably modulating the activity and selectivity in the semi‐hydrogenation of alkynols. 1‐dodecanethiol‐modified Cu nanowires (Cu NWs) exhibit the optimal electrosynthesis of 2‐methyl‐3‐buten‐2‐ol with excellent specific selectivity (above 93%) in the semi‐hydrogenation of 2‐methyl‐3‐butyn‐2‐ol. Mechanistic studies reveal that the proportion of liquid‐like water increases while the proportion of isolated water reduces at the hydrophobic interface. Moreover, we assemble a larger 3 × 100 cm2 electrolyzer stack, which can deliver a single‐pass alkynol conversion rate of 95% and an excellent alkenol selectivity of 94% at a 15 A stack current. Eventually, the Cu NWs catalyst with thiol treatment is also applicable to the semi‐hydrogenation of various unsaturated alkynols.

Thiol treatment tunes interfacial wettability for electrochemical alkynol semi‐hydrogenation

Zha,

Zhao,

Jiang

et al. 2024

Tailoring the interfacial microenvironment by electrolyte engineering boosts bicarbonate electrolysis

Lin,

Sheng,

et al. 2024

Bicarbonate electrolysis, as a carbon utilization technology with high efficiency and potential for industrial applications, provides a promising pathway for CO2 emission reduction. However, how to inhibit serious hydrogen evolution reaction (HER) and increase the relatively low CO2 concentration at the electrode‐electrolyte interfacial is challenging. Here, we introduce three typical aminopolycarboxylic acids (APCAs) with different amounts of carboxylic acid roots into 3 M KHCO3 to enhance the Faradaic efficiency of CO (FECO) from 51.2% to 68.0% at 100 mA cm−2. Spectroscopic characterization confirms that the role of APCAs in confining the activity of water dissociation and improving the availability of CO2. The strategy adopted in this work that introducing APCAs into the electrolyte to balance the content of CO2 and H2O for improving the electrocatalytic performance, can serve as a reference for other electrocatalytic systems.

Stabilization of cu^σ+ via strong Cu‐O‐Si interface for efficient electrocatalytic acetylene semi‐hydrogenation

Jiang,

Ge,

Fan

et al. 2024

The development of a high‐performance electrocatalytic acetylene semi‐hydrogenation catalyst is the key to the selective removal of acetylene from industrial ethylene gas and non‐oil route to ethylene production. However, it is still hampered by the deactivation of the catalyst and hydrogen evolution interference. Here, we proposed an interface engineering strategy involving the Cu and cupric oxide nanoparticles dispersed on amorphous SiO2 (Cu/CuOx/SiO2) by a simple stöber method. x‐ray photoelectron spectroscopy demonstrated the strong interfacial interaction between cupric oxide nanoparticles and SiO2. The formed Cu‐O‐Si interface stabilized the Cuσ+ at high reduction potentials, thus improving the activity and stability of the acetylene reduction reaction, as confirmed by in situ Raman spectroscopy. Consequently, the electrochemical test results showed that at 0.5 M KHCO3, the maximum Faraday efficiency (FE) of ethylene on the optimized Cu/CuOx/SiO2 reached 96%. And ethylene FE remains above 85% at −100 mA cm−2 for 40 h.