CuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO<sub>2</sub> Reduction to Syngas: Tuning of H<sub>2</sub>/CO Ratio
Inspired by the knowledge of the thermocatalytic CO<sub>2</sub> reduction process, novel nanocrystalline CuZnAl-oxide based catalysts with pyramidal mesoporous structures are here proposed for the CO<sub>2</sub> electrochemical reduction under ambient conditions. The XPS anal...
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2021
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oai:doaj.org-article:5ccd035654084df5b217b8f40d85e9112021-11-25T18:32:02ZCuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO<sub>2</sub> Reduction to Syngas: Tuning of H<sub>2</sub>/CO Ratio10.3390/nano111130522079-4991https://doaj.org/article/5ccd035654084df5b217b8f40d85e9112021-11-01T00:00:00Zhttps://www.mdpi.com/2079-4991/11/11/3052https://doaj.org/toc/2079-4991Inspired by the knowledge of the thermocatalytic CO<sub>2</sub> reduction process, novel nanocrystalline CuZnAl-oxide based catalysts with pyramidal mesoporous structures are here proposed for the CO<sub>2</sub> electrochemical reduction under ambient conditions. The XPS analyses revealed that the co-presence of ZnO and Al<sub>2</sub>O<sub>3</sub> into the Cu-based catalyst stabilize the CuO crystalline structure and introduce basic sites on the ternary as-synthesized catalyst. In contrast, the as-prepared CuZn- and Cu-based materials contain a higher amount of superficial Cu<sup>0</sup> and Cu<sup>1+</sup> species. The CuZnAl-catalyst exhibited enhanced catalytic performance for the CO and H<sub>2</sub> production, reaching a Faradaic efficiency (FE) towards syngas of almost 95% at −0.89 V vs. RHE and a remarkable current density of up to 90 mA cm<sup>−2</sup> for the CO<sub>2</sub> reduction at −2.4 V vs. RHE. The physico-chemical characterizations confirmed that the pyramidal mesoporous structure of this material, which is constituted by a high pore volume and small CuO crystals, plays a fundamental role in its low diffusional mass-transfer resistance. The CO-productivity on the CuZnAl-catalyst increased at more negative applied potentials, leading to the production of syngas with a tunable H<sub>2</sub>/CO ratio (from 2 to 7), depending on the applied potential. These results pave the way to substitute state-of-the-art noble metals (e.g., Ag, Au) with this abundant and cost-effective catalyst to produce syngas. Moreover, the post-reaction analyses demonstrated the stabilization of Cu<sub>2</sub>O species, avoiding its complete reduction to Cu<sup>0</sup> under the CO<sub>2</sub> electroreduction conditions.Hilmar GuzmánDaniela RoldánAdriano SaccoMicaela CastellinoMarco FontanaNunzio RussoSimelys HernándezMDPI AGarticleCO<sub>2</sub> electrochemical reductionCO<sub>2</sub> utilizationmetal oxide electrocatalystselectrochemical impedance spectroscopyChemistryQD1-999ENNanomaterials, Vol 11, Iss 3052, p 3052 (2021) |
| institution |
DOAJ |
| collection |
DOAJ |
| language |
EN |
| topic |
CO<sub>2</sub> electrochemical reduction CO<sub>2</sub> utilization metal oxide electrocatalysts electrochemical impedance spectroscopy Chemistry QD1-999 |
| spellingShingle |
CO<sub>2</sub> electrochemical reduction CO<sub>2</sub> utilization metal oxide electrocatalysts electrochemical impedance spectroscopy Chemistry QD1-999 Hilmar Guzmán Daniela Roldán Adriano Sacco Micaela Castellino Marco Fontana Nunzio Russo Simelys Hernández CuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO<sub>2</sub> Reduction to Syngas: Tuning of H<sub>2</sub>/CO Ratio |
| description |
Inspired by the knowledge of the thermocatalytic CO<sub>2</sub> reduction process, novel nanocrystalline CuZnAl-oxide based catalysts with pyramidal mesoporous structures are here proposed for the CO<sub>2</sub> electrochemical reduction under ambient conditions. The XPS analyses revealed that the co-presence of ZnO and Al<sub>2</sub>O<sub>3</sub> into the Cu-based catalyst stabilize the CuO crystalline structure and introduce basic sites on the ternary as-synthesized catalyst. In contrast, the as-prepared CuZn- and Cu-based materials contain a higher amount of superficial Cu<sup>0</sup> and Cu<sup>1+</sup> species. The CuZnAl-catalyst exhibited enhanced catalytic performance for the CO and H<sub>2</sub> production, reaching a Faradaic efficiency (FE) towards syngas of almost 95% at −0.89 V vs. RHE and a remarkable current density of up to 90 mA cm<sup>−2</sup> for the CO<sub>2</sub> reduction at −2.4 V vs. RHE. The physico-chemical characterizations confirmed that the pyramidal mesoporous structure of this material, which is constituted by a high pore volume and small CuO crystals, plays a fundamental role in its low diffusional mass-transfer resistance. The CO-productivity on the CuZnAl-catalyst increased at more negative applied potentials, leading to the production of syngas with a tunable H<sub>2</sub>/CO ratio (from 2 to 7), depending on the applied potential. These results pave the way to substitute state-of-the-art noble metals (e.g., Ag, Au) with this abundant and cost-effective catalyst to produce syngas. Moreover, the post-reaction analyses demonstrated the stabilization of Cu<sub>2</sub>O species, avoiding its complete reduction to Cu<sup>0</sup> under the CO<sub>2</sub> electroreduction conditions. |
| format |
article |
| author |
Hilmar Guzmán Daniela Roldán Adriano Sacco Micaela Castellino Marco Fontana Nunzio Russo Simelys Hernández |
| author_facet |
Hilmar Guzmán Daniela Roldán Adriano Sacco Micaela Castellino Marco Fontana Nunzio Russo Simelys Hernández |
| author_sort |
Hilmar Guzmán |
| title |
CuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO<sub>2</sub> Reduction to Syngas: Tuning of H<sub>2</sub>/CO Ratio |
| title_short |
CuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO<sub>2</sub> Reduction to Syngas: Tuning of H<sub>2</sub>/CO Ratio |
| title_full |
CuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO<sub>2</sub> Reduction to Syngas: Tuning of H<sub>2</sub>/CO Ratio |
| title_fullStr |
CuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO<sub>2</sub> Reduction to Syngas: Tuning of H<sub>2</sub>/CO Ratio |
| title_full_unstemmed |
CuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO<sub>2</sub> Reduction to Syngas: Tuning of H<sub>2</sub>/CO Ratio |
| title_sort |
cuznal-oxide nanopyramidal mesoporous materials for the electrocatalytic co<sub>2</sub> reduction to syngas: tuning of h<sub>2</sub>/co ratio |
| publisher |
MDPI AG |
| publishDate |
2021 |
| url |
https://doaj.org/article/5ccd035654084df5b217b8f40d85e911 |
| work_keys_str_mv |
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