Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 54, Issue 46, Pages 13701-13705Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201506062
Keywords
carbon dioxide fixation; carbon nanotubes; carbon monoxide selectivity; electrochemistry; nitrogen defects
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Funding
- National Science Foundation [DMR-1006113]
- U.S. Air Force Office of Scientific Research 3D MURI [FA9550-12-1-0035]
- Office of Naval Research grant [N00014-15-1-2251]
- UGC India for Raman Fellowship under Indo-US 21st Century Knowledge Initiative
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1006113] Funding Source: National Science Foundation
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Nitrogen-doped carbon nanotubes (NCNTs) have been considered as a promising electrocatalyst for carbon-dioxide-reduction reactions, but two fundamental chemistry questions remain obscure: 1)What are the active centers with respect to various defect species and 2)what is the role of defect density on the selectivity of NCNTs? The aim of this work is to address these questions. The catalytic activity of NCNTs depends on the structural nature of nitrogen in CNTs and defect density. Comparing with pristine CNTs, the presence of graphitic and pyridinic nitrogen significantly decreases the overpotential (ca. -0.18V) and increases the selectivity (ca. 80%) towards the formation of CO. The experimental results are in congruent with DFT calculations, which show that pyridinic defects retain a lone pair of electrons that are capable of binding CO2. However, for graphitic-like nitrogen, electrons are located in the * antibonding orbital, making them less accessible for CO2 binding.
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