Dataset Information

Boosting electrocatalytic CO₂-to-ethanol production via asymmetric C-C coupling.

ABSTRACT: Electroreduction of carbon dioxide (CO₂) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver-modified copper-oxide catalyst (dCu₂O/Ag_2.3%) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO₂-to-ethanol conversion under high current operation with partial current density of 326.4 mA cm^-2 at -0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu-based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the ^*CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C-C coupling for stablization of EtOH intermediates.

SUBMITTER: Wang P

PROVIDER: S-EPMC9243136 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Similar Datasets

Project description:Recently, photo-electrooxidation of fuel using a noble metal-semiconductor junction has been one of the most promising approaches in fuel cell systems. Herein, we report the development of a Pd-supported Bi2MoO6-Bi2O2CO3-CuO novel ternary heterojunction for ethanol oxidation in alkali in the presence and absence of visible light. Various spectroscopic and microscopic characterization techniques confirm strong coupling between palladium nanoparticles and Bi2MoO6-Bi2O2CO3-CuO ternary heterojunction supports. The photo-electrocatalytic efficacy of the synthesized catalysts was inspected by cyclic voltammetry (CV), chronoamperometry (CA), and electrochemical impedance spectroscopy (EIS). The CV study reveals that the forward peak current density (in mA mg-1 of Pd) of the synthesized quaternary heterojunction was about 1482.5, which is 2.4, 4, and 4.6 times higher than that of Pd/CuO (608.3), Pd/Bi2MoO6-Bi2O2CO3 (368.3), and similarly synthesized Pd catalyst (321.5) under visible light radiation. The best heterojunction catalyst shows 2.21-fold higher peak current density in visible light compared to that in dark. CA study reveals that after operation for 6000 s, the current density of the quaternary electrode is 1.5 and 3.4 times greater than that of Pd/CuO and Pd/C catalysts, respectively. The greater photocurrent response, lower photoluminescence (PL) emission intensity, and smaller semicircle arc in the Nyquist plot of the quaternary catalyst demonstrate the efficient segregation and higher charge transfer conductance of photogenerated charges to facilitate the photo-electrooxidation process of ethanol. The stability test shows that the quaternary catalyst loses only 9.8 and 7.7% of its maximum current density after 500 cycles of CV operation in the dark and light, respectively, indicating that light energy is more beneficial in establishing high stability. The dramatic enhancement of the photo-electrocatalytic activity of the quaternary electrode is owing to the lower band gap, high ECSA, enhanced charge separation of photogenerated carriers (e--h+), and all cocatalytic support of Bi2MoO6, Bi2O2CO3, and CuO in Pd/ Bi2MoO6-Bi2O2CO3-CuO under visible light radiation. The morphology and structure of the used quaternary catalyst are tested using FESEM and PXRD. Finally, ex situ FTIR spectroscopy and HPLC techniques help understand the ethanol electrooxidation reaction mechanism.

Dataset Information

Boosting electrocatalytic CO₂-to-ethanol production via asymmetric C-C coupling.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Dataset Information

Boosting electrocatalytic CO2-to-ethanol production via asymmetric C-C coupling.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Boosting electrocatalytic CO₂-to-ethanol production via asymmetric C-C coupling.