Selectivity Control of Cu Nanocrystals in a Gas-Fed Flow Cell through CO2 Pulsed Electroreduction
| العنوان: | Selectivity Control of Cu Nanocrystals in a Gas-Fed Flow Cell through CO2 Pulsed Electroreduction |
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| المؤلفون: | Beatriz Roldan Cuenya, Aram Yoon, Janis Timoshenko, Hyo Sang Jeon, Sebastian Z. Oener, Clara Rettenmaier, Uta Hejral, Felix T. Haase, Antonia Herzog, See Wee Chee |
| المصدر: | Journal of the American Chemical Society Journal of the American Chemical Society 143(19), 7578-7587 (2021). doi:10.1021/jacs.1c03443 |
| بيانات النشر: | American Chemical Society (ACS), 2021. |
| سنة النشر: | 2021 |
| مصطلحات موضوعية: | X-ray absorption spectroscopy, Electrolysis, Chemistry, Inorganic chemistry, General Chemistry, 010402 general chemistry, 01 natural sciences, Biochemistry, Article, Catalysis, Product distribution, 0104 chemical sciences, law.invention, Colloid and Surface Chemistry, Operando spectroscopy, Nanocrystal, 13. Climate action, law, ddc:540, Grain boundary, Selectivity |
| الوصف: | In this study, we have taken advantage of a pulsed CO$_2$ electroreduction reaction (CO$_2$RR) approach to tune the product distribution at industrially relevant current densities in a gas-fed flow cell. We compared the CO$_2$RR selectivity of Cu catalysts subjected to either potentiostatic conditions (fixed applied potential of −0.7 V$_{RHE}$) or pulsed electrolysis conditions (1 s pulses at oxidative potentials ranging from $E_{an}$ = 0.6 to 1.5 V$_{RHE}$, followed by 1 s pulses at −0.7 VRHE) and identified the main parameters responsible for the enhanced product selectivity observed in the latter case. Herein, two distinct regimes were observed: (i) for $E_{an}$ = 0.9 V$_{RHE}$ we obtained 10% enhanced C$_2$ product selectivity (FE$_{C_2H_4}$ = 43.6% and FE$_{C_2H_5OH}$ = 19.8%) in comparison to the potentiostatic CO$_2$RR at −0.7 V$_{RHE}$ (FE$_{C_2H_4}$ = 40.9% and FE$_{C_2H_5OH}$ = 11%), (ii) while for $E_{an}$ = 1.2 V$_{RHE}$, high CH$_4$ selectivity (FE$_{CH_4}$ = 48.3% vs 0.1% at constant −0.7 V$_{RHE}$) was observed. Operando spectroscopy (XAS, SERS) and ex situ microscopy (SEM and TEM) measurements revealed that these differences in catalyst selectivity can be ascribed to structural modifications and local pH effects. The morphological reconstruction of the catalyst observed after pulsed electrolysis with $E_{an}$ = 0.9 V$_{RHE}$, including the presence of highly defective interfaces and grain boundaries, was found to play a key role in the enhancement of the C$_2$ product formation. In turn, pulsed electrolysis with $E_{an}$ = 1.2 V$_{RHE}$ caused the consumption of OH$^–$ species near the catalyst surface, leading to an OH-poor environment favorable for CH$_4$ production. |
| وصف الملف: | application/pdf |
| تدمد: | 1520-5126 0002-7863 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::73407a1bbde8311a78b1674c9cb153c2 https://doi.org/10.1021/jacs.1c03443 |
| حقوق: | OPEN |
| رقم الأكسشن: | edsair.doi.dedup.....73407a1bbde8311a78b1674c9cb153c2 |
| قاعدة البيانات: | OpenAIRE |
Find this issue from the American Chemical Society | تدمد: | 15205126 00027863 |
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