Tailoring microenvironment for enhanced electrochemical CO2 reduction on ultrathin tin oxide derived nanosheets

Hai Liu; Yaqiong Su; Zhihui Liu; Hongyuan Chuai; Sheng Zhang; Xinbin Ma

doi:10.1016/j.nanoen.2022.108031

Tailoring microenvironment for enhanced electrochemical CO₂ reduction on ultrathin tin oxide derived nanosheets

Hai Liu, Yaqiong Su, Zhihui Liu, Hongyuan Chuai, Sheng Zhang, Xinbin Ma (Corresponding author)

Inorganic Materials & Catalysis

Onderzoeksoutput: Bijdrage aan tijdschrift › Tijdschriftartikel › Academic › peer review

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Samenvatting

Electrocatalytic CO₂ reduction powered by renewable electricity has been considered as a promising approach for sustainable energy storage and chemicals production. Herein, ultrathin few-layer SnO₂ nanosheets exposed with (001) facets were synthesized and exhibited a rather broad potential window (0.8 V) for selective CO₂ conversion to formate. Both DFT calculations and operando spectroscopic characterizations were carried out to identify key intermediate *OCHO. Systematically tailoring microenvironment in the catalyst layer of gas diffusion electrode (GDE) indicate that both flexible Nafion and solid polytetraﬂuoroethylene (PTFE) nanoparticles are essential to create abundant and robust triple-phase boundaries (TPB) with more active sites, where CO₂ and H₂O meet at nanosheet surface to output a high formate partial current density of 380 mA·cm^-2 with the selectivity of 88.4%. Moreover, such novel Nafion/PTFE/SnO₂ TPB porous structures above largely enhance the single-pass carbon efficiency up to 29.3% in 1 M KOH. This study implies that engineering TPB active sites is an effective approach to the design of advanced CO₂ electrolyzers.

Originele taal-2	Engels
Artikelnummer	108031
Aantal pagina's	8
Tijdschrift	Nano Energy
Volume	105
DOI's	https://doi.org/10.1016/j.nanoen.2022.108031
Status	Gepubliceerd - jan. 2023

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© 2022 Elsevier Ltd

Financiering

The authors are grateful to the financial support from the National Nature Science Foundation of China (Grant No. 22078232 and 21938008), and the Science and Technology Major Project of Tianjin (Grant No. 20JCYBJC00870 and 19ZXNCGX00030). Y. Su acknowledge the “Young Talent Support Plan” of Xi'an Jiaotong University. Supercomputing facilities were provided by Hefei Advanced Computing Center. The authors are grateful to the financial support from the National Nature Science Foundation of China (Grant No. 22078232 and 21938008 ), and the Science and Technology Major Project of Tianjin (Grant No. 20JCYBJC00870 and 19ZXNCGX00030 ). Y. Su acknowledge the “Young Talent Support Plan” of Xi'an Jiaotong University. Supercomputing facilities were provided by Hefei Advanced Computing Center .

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title = "Tailoring microenvironment for enhanced electrochemical CO2 reduction on ultrathin tin oxide derived nanosheets",

abstract = "Electrocatalytic CO2 reduction powered by renewable electricity has been considered as a promising approach for sustainable energy storage and chemicals production. Herein, ultrathin few-layer SnO2 nanosheets exposed with (001) facets were synthesized and exhibited a rather broad potential window (0.8 V) for selective CO2 conversion to formate. Both DFT calculations and operando spectroscopic characterizations were carried out to identify key intermediate *OCHO. Systematically tailoring microenvironment in the catalyst layer of gas diffusion electrode (GDE) indicate that both flexible Nafion and solid polytetraﬂuoroethylene (PTFE) nanoparticles are essential to create abundant and robust triple-phase boundaries (TPB) with more active sites, where CO2 and H2O meet at nanosheet surface to output a high formate partial current density of 380 mA·cm-2 with the selectivity of 88.4%. Moreover, such novel Nafion/PTFE/SnO2 TPB porous structures above largely enhance the single-pass carbon efficiency up to 29.3% in 1 M KOH. This study implies that engineering TPB active sites is an effective approach to the design of advanced CO2 electrolyzers.",

keywords = "CO reduction, Gas diffusion electrode, Microenvironment, SnO nanosheets, Triple phase boundaries",

author = "Hai Liu and Yaqiong Su and Zhihui Liu and Hongyuan Chuai and Sheng Zhang and Xinbin Ma",

note = "Funding Information: The authors are grateful to the financial support from the National Nature Science Foundation of China (Grant No. 22078232 and 21938008), and the Science and Technology Major Project of Tianjin (Grant No. 20JCYBJC00870 and 19ZXNCGX00030). Y. Su acknowledge the “Young Talent Support Plan” of Xi'an Jiaotong University. Supercomputing facilities were provided by Hefei Advanced Computing Center. ",

year = "2023",

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AU - Liu, Hai

AU - Su, Yaqiong

AU - Liu, Zhihui

AU - Chuai, Hongyuan

AU - Zhang, Sheng

AU - Ma, Xinbin

N1 - Funding Information: The authors are grateful to the financial support from the National Nature Science Foundation of China (Grant No. 22078232 and 21938008), and the Science and Technology Major Project of Tianjin (Grant No. 20JCYBJC00870 and 19ZXNCGX00030). Y. Su acknowledge the “Young Talent Support Plan” of Xi'an Jiaotong University. Supercomputing facilities were provided by Hefei Advanced Computing Center.

PY - 2023/1

Y1 - 2023/1

N2 - Electrocatalytic CO2 reduction powered by renewable electricity has been considered as a promising approach for sustainable energy storage and chemicals production. Herein, ultrathin few-layer SnO2 nanosheets exposed with (001) facets were synthesized and exhibited a rather broad potential window (0.8 V) for selective CO2 conversion to formate. Both DFT calculations and operando spectroscopic characterizations were carried out to identify key intermediate *OCHO. Systematically tailoring microenvironment in the catalyst layer of gas diffusion electrode (GDE) indicate that both flexible Nafion and solid polytetraﬂuoroethylene (PTFE) nanoparticles are essential to create abundant and robust triple-phase boundaries (TPB) with more active sites, where CO2 and H2O meet at nanosheet surface to output a high formate partial current density of 380 mA·cm-2 with the selectivity of 88.4%. Moreover, such novel Nafion/PTFE/SnO2 TPB porous structures above largely enhance the single-pass carbon efficiency up to 29.3% in 1 M KOH. This study implies that engineering TPB active sites is an effective approach to the design of advanced CO2 electrolyzers.

AB - Electrocatalytic CO2 reduction powered by renewable electricity has been considered as a promising approach for sustainable energy storage and chemicals production. Herein, ultrathin few-layer SnO2 nanosheets exposed with (001) facets were synthesized and exhibited a rather broad potential window (0.8 V) for selective CO2 conversion to formate. Both DFT calculations and operando spectroscopic characterizations were carried out to identify key intermediate *OCHO. Systematically tailoring microenvironment in the catalyst layer of gas diffusion electrode (GDE) indicate that both flexible Nafion and solid polytetraﬂuoroethylene (PTFE) nanoparticles are essential to create abundant and robust triple-phase boundaries (TPB) with more active sites, where CO2 and H2O meet at nanosheet surface to output a high formate partial current density of 380 mA·cm-2 with the selectivity of 88.4%. Moreover, such novel Nafion/PTFE/SnO2 TPB porous structures above largely enhance the single-pass carbon efficiency up to 29.3% in 1 M KOH. This study implies that engineering TPB active sites is an effective approach to the design of advanced CO2 electrolyzers.

KW - CO reduction

KW - Gas diffusion electrode

KW - Microenvironment

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