PMID- 23036092 OWN - NLM STAT- MEDLINE DCOM- 20130516 LR - 20131121 IS - 1936-086X (Electronic) IS - 1936-0851 (Linking) VI - 6 IP - 11 DP - 2012 Nov 27 TI - Nitrogen-doped graphene-rich catalysts derived from heteroatom polymers for oxygen reduction in nonaqueous lithium-O2 battery cathodes. PG - 9764-76 LID - 10.1021/nn303275d [doi] AB - In this work, we present a synthesis approach for nitrogen-doped graphene-sheet-like nanostructures via the graphitization of a heteroatom polymer, in particular, polyaniline, under the catalysis of a cobalt species using multiwalled carbon nanotubes (MWNTs) as a supporting template. The graphene-rich composite catalysts (Co-N-MWNTs) exhibit substantially improved activity for oxygen reduction in nonaqueous lithium-ion electrolyte as compared to those of currently used carbon blacks and Pt/carbon catalysts, evidenced by both rotating disk electrode and Li-O(2) battery experiments. The synthesis-structure-activity correlations for the graphene nanostructures were explored by tuning their synthetic chemistry (support, nitrogen precursor, heating temperature, and transition metal type and content) to investigate how the resulting morphology and nitrogen-doping functionalities (e.g., pyridinic, pyrrolic, and quaternary) influence the catalyst activity. In particular, an optimal temperature for heat treatment during synthesis is critical to creating a high-surface-area catalyst with favorable nitrogen doping. The sole Co phase, Co(9)S(8), was present in the catalyst but plays a negligible role in ORR. Nevertheless, the addition of Co species in the synthesis is indispensable for achieving high activity, due to its effects on the final catalyst morphology and structure, including surface area, nitrogen doping, and graphene formation. This new route for the preparation of a nitrogen-doped graphene nanocomposite with carbon nanotube offers synthetic control of morphology and nitrogen functionality and shows promise for applications in nonaqueous oxygen reduction electrocatalysis for Li-O(2) battery cathodes. FAU - Wu, Gang AU - Wu G AD - Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States. wugang@lanl.gov FAU - Mack, Nathan H AU - Mack NH FAU - Gao, Wei AU - Gao W FAU - Ma, Shuguo AU - Ma S FAU - Zhong, Ruiqin AU - Zhong R FAU - Han, Jiantao AU - Han J FAU - Baldwin, Jon K AU - Baldwin JK FAU - Zelenay, Piotr AU - Zelenay P LA - eng PT - Journal Article PT - Research Support, U.S. Gov't, Non-P.H.S. DEP - 20121010 PL - United States TA - ACS Nano JT - ACS nano JID - 101313589 RN - 0 (Polymers) RN - 059QF0KO0R (Water) RN - 7782-42-5 (Graphite) RN - 9FN79X2M3F (Lithium) RN - N762921K75 (Nitrogen) RN - S88TT14065 (Oxygen) SB - IM MH - Catalysis MH - *Electric Power Supplies MH - *Electrodes MH - Equipment Design MH - Equipment Failure Analysis MH - Graphite/*chemistry MH - Lithium/*chemistry MH - Nitrogen/*chemistry MH - Oxidation-Reduction MH - Oxygen/*chemistry MH - Polymers/*chemistry MH - Water/chemistry EDAT- 2012/10/06 06:00 MHDA- 2013/05/17 06:00 CRDT- 2012/10/06 06:00 PHST- 2012/10/06 06:00 [entrez] PHST- 2012/10/06 06:00 [pubmed] PHST- 2013/05/17 06:00 [medline] AID - 10.1021/nn303275d [doi] PST - ppublish SO - ACS Nano. 2012 Nov 27;6(11):9764-76. doi: 10.1021/nn303275d. Epub 2012 Oct 10.