Promotional role of NiCu alloy in catalytic performance and carbon properties for CO2-free H2 production from thermocatalytic decomposition of methane

• Published in: Catalysis science & technology 2023-03, Vol.13 (11), p.3231-3244
• Main Authors: Xu, Mengze, Lopez-Ruiz, Juan A, Riedel, Nickolas W, Weber, Robert S, Bowden, Mark E, Kovarik, Libor, Jiang, Changle, Hu, Jianli, Dagle, Robert A
• Format: Article
• Language: English
• Subjects: Carbon dioxide; Catalysts; Copper; Decomposition; Hydrogen production; Metal particles; Methane; Morphology; Multi wall carbon nanotubes; Nickel; Operating temperature; Stability
• ISSN: 2044-4753; 2044-4761
• DOI: 10.1039/d2cy01782b

Thermocatalytic decomposition (TCD) of methane produces CO2-free hydrogen and valuable co-product, solid carbon. In this study, a series of NiCu/CNT catalysts, prepared with varying Ni/Cu metal ratios and synthesis methods, were evaluated for methane TCD performance at various temperatures. Catalysts before and after reaction, and properties of the carbon product, were characterized to identify activity–structure relationships. At 550 °C, a 10 wt% Ni/CNT catalyst was active; however, it deactivated within 1 h of reaction at >600 °C. The addition of Cu increased its stability. At temperatures above 650 °C, only the catalyst with Cu loadings above 10 wt% remained active and stable. Catalyst characterization revealed that changes in i) Ni/Cu ratio, ii) metal particle size, and iii) operating temperature are key factors for TCD activity, stability, and carbon coproduct morphology. The carbon co-product is mainly composed of multiwalled carbon nanotubes (MWCNTs) whose morphology changes with Ni/Cu ratio and reaction temperature.