Dimitra Papamichail, Filippo Franceschini, Imran Abbas, Deema Balalta, Trang Thi Hong Nguyen, Deepak Pant, Sara Bals, Irene Taurino, Ewald Janssens, Didier Grandjean and Peter Lievens
{"title":"纳米结构铜薄膜电极的CO2电还原制C2+产品","authors":"Dimitra Papamichail, Filippo Franceschini, Imran Abbas, Deema Balalta, Trang Thi Hong Nguyen, Deepak Pant, Sara Bals, Irene Taurino, Ewald Janssens, Didier Grandjean and Peter Lievens","doi":"10.1039/D5NR01514F","DOIUrl":null,"url":null,"abstract":"<p >The electrochemical CO<small><sub>2</sub></small> reduction reaction (CO<small><sub>2</sub></small>RR) is a promising approach for achieving carbon-neutral processes in the chemical industry. In this context, various nanostructures have been reported to enhance the C<small><sub>2+</sub></small> selectivity of Cu-based catalysts. Here, we prepared Cu nanoneedles (NN) from 300 nm sputtered Cu thin films through anodization under various conditions and investigated their performance in terms of C<small><sub>2+</sub></small> product selectivity. Various combinations of anodization potentials (+0.75 V<small><sub>RHE</sub></small>, +0.85 V<small><sub>RHE</sub></small>, and +0.95 V<small><sub>RHE</sub></small>) and KOH electrolyte concentrations (0.1 M, 0.5 M and 1.0 M) allow the tailoring of the NN length and density that are linked to their CO<small><sub>2</sub></small>RR product selectivity at −1.0 V<small><sub>RHE</sub></small>. The best performance using the C<small><sub>2+</sub></small> : C<small><sub>1</sub></small> ratio was achieved with a high NN surface density. A detailed analysis using high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy of the best performing sample shows that the anodization of a Cu thin film produces NNs composed of a uniform 3D network of 2 nm hydroxide nanoparticles (NPs) and reconstructs into a rougher metallic Cu NP network after the CO<small><sub>2</sub></small>RR. A high density of NNs with this inner structure may lead to an increase in the local CO concentration and thus to C<small><sub>2+</sub></small> products. This systematic work demonstrates that nanostructuring the surface of copper thin film electrodes can enhance the CO<small><sub>2</sub></small>RR selectivity to C<small><sub>2+</sub></small> products while the correlation between the NN morphology and their inner structure strengthens further their applications as CO<small><sub>2</sub></small> electrocatalysts.</p>","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":" 30","pages":" 17745-17757"},"PeriodicalIF":5.1000,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/nr/d5nr01514f?page=search","citationCount":"0","resultStr":"{\"title\":\"Nanostructuring copper thin film electrodes for CO2 electroreduction to C2+ products†\",\"authors\":\"Dimitra Papamichail, Filippo Franceschini, Imran Abbas, Deema Balalta, Trang Thi Hong Nguyen, Deepak Pant, Sara Bals, Irene Taurino, Ewald Janssens, Didier Grandjean and Peter Lievens\",\"doi\":\"10.1039/D5NR01514F\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The electrochemical CO<small><sub>2</sub></small> reduction reaction (CO<small><sub>2</sub></small>RR) is a promising approach for achieving carbon-neutral processes in the chemical industry. In this context, various nanostructures have been reported to enhance the C<small><sub>2+</sub></small> selectivity of Cu-based catalysts. Here, we prepared Cu nanoneedles (NN) from 300 nm sputtered Cu thin films through anodization under various conditions and investigated their performance in terms of C<small><sub>2+</sub></small> product selectivity. Various combinations of anodization potentials (+0.75 V<small><sub>RHE</sub></small>, +0.85 V<small><sub>RHE</sub></small>, and +0.95 V<small><sub>RHE</sub></small>) and KOH electrolyte concentrations (0.1 M, 0.5 M and 1.0 M) allow the tailoring of the NN length and density that are linked to their CO<small><sub>2</sub></small>RR product selectivity at −1.0 V<small><sub>RHE</sub></small>. The best performance using the C<small><sub>2+</sub></small> : C<small><sub>1</sub></small> ratio was achieved with a high NN surface density. A detailed analysis using high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy of the best performing sample shows that the anodization of a Cu thin film produces NNs composed of a uniform 3D network of 2 nm hydroxide nanoparticles (NPs) and reconstructs into a rougher metallic Cu NP network after the CO<small><sub>2</sub></small>RR. A high density of NNs with this inner structure may lead to an increase in the local CO concentration and thus to C<small><sub>2+</sub></small> products. 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Nanostructuring copper thin film electrodes for CO2 electroreduction to C2+ products†
The electrochemical CO2 reduction reaction (CO2RR) is a promising approach for achieving carbon-neutral processes in the chemical industry. In this context, various nanostructures have been reported to enhance the C2+ selectivity of Cu-based catalysts. Here, we prepared Cu nanoneedles (NN) from 300 nm sputtered Cu thin films through anodization under various conditions and investigated their performance in terms of C2+ product selectivity. Various combinations of anodization potentials (+0.75 VRHE, +0.85 VRHE, and +0.95 VRHE) and KOH electrolyte concentrations (0.1 M, 0.5 M and 1.0 M) allow the tailoring of the NN length and density that are linked to their CO2RR product selectivity at −1.0 VRHE. The best performance using the C2+ : C1 ratio was achieved with a high NN surface density. A detailed analysis using high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy of the best performing sample shows that the anodization of a Cu thin film produces NNs composed of a uniform 3D network of 2 nm hydroxide nanoparticles (NPs) and reconstructs into a rougher metallic Cu NP network after the CO2RR. A high density of NNs with this inner structure may lead to an increase in the local CO concentration and thus to C2+ products. This systematic work demonstrates that nanostructuring the surface of copper thin film electrodes can enhance the CO2RR selectivity to C2+ products while the correlation between the NN morphology and their inner structure strengthens further their applications as CO2 electrocatalysts.
期刊介绍:
Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.