Achieving Highly Efficient, Selective, and Stable CO2 Reduction on Nitrogen-Doped Carbon Nanotubes

Wu, Jingjie; Yadav, Ram Manohar; Liu, Mingjie; Sharma, Pranav P.; Tiwary, Chandra Sekhar; Ma, Lulu; Zou, Xiaolong; Zhou, Xiao-Dong; Yakobson, Boris I.; Lou, Jun; Ajayan, Pulickel M.

doi:10.1021/acsnano.5b01079

Cited by 652CO2 Reduction Techniques and CatalystsElectrocatalysts for Energy ConversionCatalysts for Methane Reforming

Achieving Highly Efficient, Selective, and Stable CO2 Reduction on Nitrogen-Doped Carbon Nanotubes

Wu, Jingjie, Yadav, Ram Manohar, Liu, Mingjie, Sharma, Pranav P., Tiwary, Chandra Sekhar, Ma, Lulu, Zou, Xiaolong, Zhou, Xiao-Dong +3 more·2015·ACS Nano

DOI 10.1021/acsnano.5b01079

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Abstract

The challenge in the electrosynthesis of fuels from CO2 is to achieve durable and active performance with cost-effective catalysts. Here, we report that carbon nanotubes (CNTs), doped with nitrogen to form resident electron-rich defects, can act as highly efficient and, more importantly, stable catalysts for the conversion of CO2 to CO. The unprecedented overpotential (-0.18 V) and selectivity (80%) observed on nitrogen-doped CNTs (NCNTs) are attributed to their unique features to facilitate the reaction, including (i) high electrical conductivity, (ii) preferable catalytic sites (pyridinic N defects), and (iii) low free energy for CO2 activation and high barrier for hydrogen evolution. Indeed, DFT calculations show a low free energy barrier for the potential-limiting step to form key intermediate COOH as well as strong binding energy of adsorbed COOH and weak binding energy for the adsorbed CO. The highest selective site toward CO production is pyridinic N, and the NCNT-based electrodes exhibit no degradation over 10 h of continuous operation, suggesting the structural stability of the electrode.

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Various studies have utilized bulk sensitive in situ XANES spectroscopy to show that Cu+ is stable during the course of CO2RR, a finding recently supported by another study using in situ soft XAS measurements.
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From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [101]
These findings enable high selectivity towards C2 products to be attributed to the residual Cu+.
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From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [101]

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Authors: Wu, J., Yadav, R. M., Liu, M., Sharma, P. P., Tiwary, C. S., Ma, L., Zou, X., Zhou, X.-D., Yakobson, B. I., Lou, J., & Ajayan, P. M.
Affiliations: Rice University (US)
University of South Carolina (US)
Indian Institute of Science Bangalore (IN)
Corresponding author: Zhou, Xiao-Dong
Lou, Jun
Ajayan, Pulickel M.
ORCID: Wu, Jingjie
Yadav, Ram Manohar
Liu, Mingjie
Tiwary, Chandra Sekhar
Ma, Lulu
Zou, Xiaolong
Zhou, Xiao-Dong
Yakobson, Boris I.
Lou, Jun
Ajayan, Pulickel M.
Venue: ACS Nano
Publisher: American Chemical Society (ACS)
Published: 2015-04-23
Volume: 9
Issue: 5
Pages: 5364-5371
ISSN: 1936-0851 (ISSN-L)
1936-086X
DOI: 10.1021/acsnano.5b01079
OpenAlex: W1966763428
Cited by: 652
References: 31
Citations by year: 2026: 21 · 2025: 42 · 2024: 49 · 2023: 43 · 2022: 52 · 2021: 78 · 2020: 86 · 2019: 97 · 2018: 86 · 2017: 53 · 2016: 34 · 2015: 11
FWCI: 18.13
Type: journal article
Language: en
Open access: closed
Locations: ACS Nano (publishedVersion)
PubMed (publishedVersion)
NOT FOUND REPOSITORY (Indian Institute of Science Bangalore) (acceptedVersion)
Funders: University Grants Commission
Air Force Office of Scientific Research (FA9550-12-1-0035, FA9550-14-1-0268)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
Keywords: CO2 reduction, nitrogen-doped carbon nanotubes, electrocatalysis, co-production, COOH intermediate, hydrogen evolution suppression, catalyst stability, overpotential, adsorption energy, DFT calculations

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Achieving Highly Efficient, Selective, and Stable CO2 Reduction on Nitrogen-Doped Carbon Nanotubes

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