Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction

Kim, Hyo Won; Park, Hun; Roh, Ji Soo; Shin, Jae Eun; Lee, Tae Hoon; Zhang, Liang; Cho, Young Hoon; Yoon, Hee Wook; Bukas, Vanessa J.; Guo, Jinghua; Park, Ho Bum; Han, Tae Hee; McCloskey, Bryan D.

doi:10.1021/acs.chemmater.9b00210

Title: Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction

Journal Article · Wed May 29 00:00:00 EDT 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b00210· OSTI ID:1547070

^[1]; Park, Hun ^[2]; Roh, Ji Soo ^[2]; Shin, Jae Eun ^[2]; Lee, Tae Hoon ^[2];

^[3];

^[4]; Yoon, Hee Wook ^[5];

^[6];

^[7];

^[2];

^[8]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Hanyang Univ., Seoul (Korea, Republic of)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Korea Research Inst. of Chemical Technology, Daejeon (Korea, Republic of)
Univ. of Texas, Austin, TX (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Santa Cruz, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

© 2019 American Chemical Society. Numerous modified-carbon catalysts have been developed for the direct synthesis of hydrogen peroxide through electrochemical oxygen reduction. However, given the complex structure of most porous carbons and the poor oxygen reduction reaction (ORR) selectivity typically observed when they are used as catalysts, it is still unclear which carbon defects are responsible for the high two-electron ORR activity typically observed in these materials. Here, we study electrocatalytic peroxide formation activity of nitrogen-doped reduced graphene oxide (N-rGO) materials to relate carbon defects to electrocatalytic activity. To do so, we selected two N-rGO electrodes that selectively produce peroxide at all potentials studied (0.70-0.10 V vs RHE) under alkaline conditions. Oxygen reduction studies, combined with material characterization, especially solid-state 13carbon nuclear magnetic resonance coupled with magic angle spinning and cross-polarization, demonstrate that epoxy or ether groups in the N-rGO catalyst are likely associated with the active sites that form peroxide at the lowest overpotential in alkaline media.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-76SF00515; 2017R1A2B4010771; 2016R1A6A3A03012382; 2014M1A8A1049307; CBET-1604927; AC02-05CH11231

OSTI ID:: 1547070

Alternate ID(s):: OSTI ID: 1656517

Journal Information:: Chemistry of Materials, Vol. 31, Issue 11; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 62 works

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