Reactive Intermediates or Inert Graphene? Temperature- and Pressure-Determined Evolution of Carbon in the CH4–Ni(111) System

Yuan, Kaidi; Zhong, Jian-Qiang; Sun, Shuo; Ren, Yinjuan; Zhang, Jia Lin; Chen, Wei

doi:10.1021/acscatal.7b01880

Title: Reactive Intermediates or Inert Graphene? Temperature- and Pressure-Determined Evolution of Carbon in the CH₄–Ni(111) System

Journal Article · Tue Aug 15 00:00:00 EDT 2017 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.7b01880· OSTI ID:1407473

^[1];

^[2]; Sun, Shuo ^[3]; Ren, Yinjuan ^[3]; Zhang, Jia Lin ^[3]; Chen, Wei ^[1]

National Univ. of Singapore (Suzhou) Research Inst., Suzhou (China); National Univ. of Singapore (Singapore)
Brookhaven National Lab. (BNL), Upton, NY (United States)
National Univ. of Singapore (Singapore)

Atomic-level identification of carbon intermediates under reaction conditions is essential for carbon-related heterogeneous catalysis. Using the in operando technique of near-ambient-pressure X-ray photoelectron spectroscopy, we have identified in this paper various carbon intermediates during the thermal decomposition of CH₄ on Ni(111), including *CH, *C₁/Ni₃C, *C_n (n ≥ 2), and clock-reconstructed Ni₂C at different temperature regions (300–900 K). These “reactive” carbon precursors can either react with probing molecules such as O₂ at room temperature or be etched away by CH₄. They can also develop into graphene flakes under controlled conditions: a temperature between 800 and 900 K and a suitable CH₄ pressure (10^–3–10^–1 mbar, depending on temperature). The growth rate of graphene is significantly restrained at higher CH₄ pressures, due to the accelerated etching of its carbon precursors. The identification of in operando carbon intermediates and the control of their evolution have great potential in designing heterogeneous catalysts for the direct conversion of methane. Finally, the observed carbon aggregation/etching equilibrium reveals an underlying mechanism in coking prevention and in the fabrication of large-area single-crystal graphene, where the suppression of seeding density and etching up of small grains are required.

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Research Organization:: National Univ. of Singapore (Singapore); National Univ. of Singapore (Suzhou) Research Inst., Suzhou (China); Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: SC0012704; 91645102

OSTI ID:: 1407473

Report Number(s):: BNL-114500-2017-JA; R&D Project: 16068; KC0403020

Journal Information:: ACS Catalysis, Vol. 7, Issue 9; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 12 works

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Journal Article · Wed Dec 01 00:00:00 EST 2004 · Journal of Applied Physics · OSTI ID:1407473

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Isolation and structural characterization of the copper-barium-alkoxide cluster Ba sub 2 Cu sub 2 (OR) sub 4 (acac) sub 4 ter dot 2HOR (R = CH sub 2 CH sub 2 OCH sub 3 ) from precursor solutions to YBa sub 2 Cu sub 3 O sub 7 thin films

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
carbon
catalyst
graphene
intermediate
methane
NAP-XPS
nickel

Title: Reactive Intermediates or Inert Graphene? Temperature- and Pressure-Determined Evolution of Carbon in the CH4–Ni(111) System

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Title: Reactive Intermediates or Inert Graphene? Temperature- and Pressure-Determined Evolution of Carbon in the CH₄–Ni(111) System