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

Wu, Jingjie and Yadav, Ram Manohar and Liu, Mingjie and Sharma, Pranav P and Tiwary, Chandra Sekhar and Ma, Lulu and Zou, Xiaolong and Zhou, Xiao-Dong and Yakobson, Boris I and Lou, Jun and Ajayan, Pulickel M (2015) Achieving Highly Efficient, Selective, and Stable CO2 Reduction on Nitrogen-Doped Carbon Nanotubes. In: ACS NANO, 9 (5). pp. 5364-5371.

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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 CON 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.

Item Type:	Journal Article
Publication:	ACS NANO
Publisher:	AMER CHEMICAL SOC
Additional Information:	Copy right for this article belongs to the AMER CHEMICAL SOC, 1155 16TH ST, NW, WASHINGTON, DC 20036 USA
Keywords:	carbon nanotubes; pyridinic nitrogen; CO2 reduction; low overpotential; high selectivity; high durability
Department/Centre:	Division of Mechanical Sciences > Materials Engineering (formerly Metallurgy)
Date Deposited:	19 Jul 2015 09:21
Last Modified:	19 Jul 2015 09:21
URI:	http://eprints.iisc.ac.in/id/eprint/51826

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