Catalytic decomposition of methane into hydrogen and high-value carbons: combined experimental and DFT computational study

Wang, I-Wen; Dagle, Robert A.; Khan, Tuhin S.; Lopez-Ruiz, Juan A.; Kovarik, Libor; Jiang, Yuan; Xu, Mengze; Wang, Yi; Jiang, Changle; Davidson, Stephen D.; Tavadze, Pedram; Li, Lili; Hu, Jianli (John)

doi:10.1039/D1CY00287B

Catalytic decomposition of methane into hydrogen and high-value carbons: combined experimental and DFT computational study

Journal Article · 21 July 2021 · Catalysis Science & Technology

DOI:https://doi.org/10.1039/D1CY00287B· OSTI ID:1810708

Wang, I-Wen ^[1]; ^[2]; Khan, Tuhin S. ^[3]; ^[2]; Kovarik, Libor ^[2]; Jiang, Yuan ^[2]; Xu, Mengze ^[2]; Wang, Yi ^[1]; Jiang, Changle ^[1]; ^[2]; Tavadze, Pedram ^[1]; Li, Lili ^[4]; Hu, Jianli (John) ^[1]

West Virginia University
BATTELLE (PACIFIC NW LAB)
works with academic partner (doing computational catalysis)
Zhoukou Normal University

Thermocatalytic decomposition (TCD) of methane can produce hydrogen and valuable nanocarbon co-products with low to near-zero CO2 emission. In this study, a series of Pd promoted Ni catalysts, prepared with various Ni/Pd ratios on a CNT support, were evaluated for methane TCD performance. Characterization and calculations using density functional theory (DFT) were carried out to elucidate the activity–structure relationship and growth mechanism of carbon nanomaterials. It was found that the methane conversion and stability of the catalysts were highly dependent on the Ni/Pd ratio and reaction temperature. DFT calculations revealed that the diffusion of carbon in the metal sublayer required for CNT growth was more favorable in the Ni–Pd alloy lattice suggesting that the buildup of carbon in the metal alloy sublayer facilitated the formation of CNTs and CNFs. A cyclic reaction–regeneration process for self-sustained TCD was experimentally demonstrated. In each cycle, a portion of the separated CNT product was used to re-synthesize the Ni–Pd/CNT catalyst for use in the next reaction cycle. After five cycles of operation, the CH4 conversion, morphology and crystallinity of the carbon product remained unchanged.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1810708

Report Number(s):: PNNL-SA-163856

Journal Information:: Catalysis Science & Technology, Journal Name: Catalysis Science & Technology Journal Issue: 14 Vol. 11

Country of Publication:: United States

Language:: English

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