PMID- 25897553 OWN - NLM STAT- PubMed-not-MEDLINE DCOM- 20150824 LR - 20150526 IS - 1936-086X (Electronic) IS - 1936-0851 (Linking) VI - 9 IP - 5 DP - 2015 May 26 TI - Achieving Highly Efficient, Selective, and Stable CO2 Reduction on Nitrogen-Doped Carbon Nanotubes. PG - 5364-71 LID - 10.1021/acsnano.5b01079 [doi] AB - 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. FAU - Wu, Jingjie AU - Wu J AD - daggerDepartment of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States. FAU - Yadav, Ram Manohar AU - Yadav RM AD - daggerDepartment of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States. FAU - Liu, Mingjie AU - Liu M AD - daggerDepartment of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States. FAU - Sharma, Pranav P AU - Sharma PP AD - double daggerDepartment of Chemical Engineering, University of South Carolina, Columbia, South Carolina 29201, United States. FAU - Tiwary, Chandra Sekhar AU - Tiwary CS AD - section signDepartment of Materials Engineering, Indian Institute of Science, Bangalore 560012, India. FAU - Ma, Lulu AU - Ma L AD - daggerDepartment of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States. FAU - Zou, Xiaolong AU - Zou X AD - daggerDepartment of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States. FAU - Zhou, Xiao-Dong AU - Zhou XD AD - double daggerDepartment of Chemical Engineering, University of South Carolina, Columbia, South Carolina 29201, United States. FAU - Yakobson, Boris I AU - Yakobson BI AD - daggerDepartment of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States. FAU - Lou, Jun AU - Lou J AD - daggerDepartment of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States. FAU - Ajayan, Pulickel M AU - Ajayan PM AD - daggerDepartment of Material Science and NanoEngineering, Rice University, Houston, Texas 77005, United States. LA - eng PT - Journal Article PT - Research Support, Non-U.S. Gov't PT - Research Support, U.S. Gov't, Non-P.H.S. DEP - 20150423 PL - United States TA - ACS Nano JT - ACS nano JID - 101313589 OTO - NOTNLM OT - CO2 reduction OT - carbon nanotubes OT - high durability OT - high selectivity OT - low overpotential OT - pyridinic nitrogen EDAT- 2015/04/22 06:00 MHDA- 2015/04/22 06:01 CRDT- 2015/04/22 06:00 PHST- 2015/04/22 06:00 [entrez] PHST- 2015/04/22 06:00 [pubmed] PHST- 2015/04/22 06:01 [medline] AID - 10.1021/acsnano.5b01079 [doi] PST - ppublish SO - ACS Nano. 2015 May 26;9(5):5364-71. doi: 10.1021/acsnano.5b01079. Epub 2015 Apr 23.