Atomically Dispersed Co and Cu on N-Doped Carbon for Reactions Involving C–H Activation

Xie, Jiahan; Kammert, James D.; Kaylor, Nicholas; Zheng, Jonathan W.; Choi, Eunjin; Pham, Hien N.; Sang, Xiahan; Stavitski, Eli; Attenkofer, Klaus; Unocic, Raymond R.; Datye, Abhaya K.; Davis, Robert J.

doi:10.1021/acscatal.8b00141

Title: Atomically Dispersed Co and Cu on N-Doped Carbon for Reactions Involving C–H Activation

Journal Article · Thu Mar 22 00:00:00 EDT 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b00141· OSTI ID:1464104

^[1]; Kammert, James D. ^[1]; Kaylor, Nicholas ^[1]; Zheng, Jonathan W. ^[1]; Choi, Eunjin ^[2]; Pham, Hien N. ^[3];

^[4]; Stavitski, Eli ^[5]; Attenkofer, Klaus ^[5];

^[4]; Datye, Abhaya K. ^[3];

^[1]

Univ. of Virginia, Charlottesville, VA (United States). Dept. of Chemical Engineering
Univ. of Virginia, Charlottesville, VA (United States). Dept. of Chemical Engineering; Daegu Gyeongbuk Inst. of Science and Technology, Daegu (Korea, Republic of). Dept. of Emerging Materials Science
Univ. of New Mexico, Albuquerque, NM (United States). Center for Micro-Engineered Materials (CMEM) and Dept. of Chemical and Biological Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Atomically dispersed Co(II) cations coordinated to nitrogen in a carbon matrix (Co-N-C) catalyze oxidative dehydrogenation of benzyl alcohol in water with a specific activity approaching that of supported Pt nanoparticles. Whereas Cu(II) cations in N-doped carbon also catalyze the reaction, they are about an order of magnitude less active compared with Co(II) cations. Results from X-ray absorption spectroscopy suggest that oxygen is also bound to N-coordinated Co(II) sites but that it can be partially removed by H2 treatments at 523–750 K. The N-coordinated Co(II) sites remained cationic in H2 up to 750 K, and these stable sites were demonstrated to be active for propane dehydrogenation. In situ characterization of Cu(II) in N-doped carbon revealed that reduction of the metal in H2 started at about 473 K, indicating a much lower thermal stability of Cu(II) in H2 relative to Co(II). The demonstrated high catalytic activity and thermal stability of Co-N-C in reducing environments suggests that this material may have broad utility in a variety of catalytic transformations.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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

Grant/Contract Number:: SC0012704; EEC-0813570; CBET-1157829; AC05-00OR22725

OSTI ID:: 1464104

Alternate ID(s):: OSTI ID: 1607270

Report Number(s):: BNL-207954-2018-JAAM

Journal Information:: ACS Catalysis, Vol. 8, Issue 5; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 50 works

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Title: Atomically Dispersed Co and Cu on N-Doped Carbon for Reactions Involving C–H Activation

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