Abstract

Methane cracking has emerged as a promising route for sustainable hydrogen production because it avoids direct carbon dioxide emissions while simultaneously enabling carbon sequestration in the form of solid carbon. In this work, a comprehensive and systematic experimental investigation of catalytic methane cracking was performed by directly comparing a commercial nickel catalyst (KATALCO™ 25-4MQ), an in-house catalyst prepared by wet impregnation using Fe(NO3)3·9H2O as the iron precursor and Puralox SCFa-160 Ce20 as the support, and non-catalytic thermal conditions under identical operating parameters. Experiments were carried out in a laboratory-scale fixed-bed reactor at atmospheric pressure by varying methane partial pressure (0.1–0.2 atm) and operating temperature (600–800 °C), while maintaining a constant methane-specific WHSV of 0.3 h−1. Continuous online gas analysis was employed to monitor reactor performance, and a dedicated post-processing methodology, including nitrogen-tracer-based carbon balance calculations, was developed to validate the experimental results. The results demonstrated the strong beneficial effects of both temperature and catalytic materials on methane decomposition. The Fe-based catalysts exhibited the highest performance, achieving average methane conversions and hydrogen yields approaching 50%, with peak values exceeding 90% under the most favorable conditions. Commercial Ni catalysts also showed promising activity, although a more pronounced deactivation tendency was observed during prolonged operation. Conversely, non-catalytic tests resulted in substantially lower performance. Overall, this work provides an experimentally assessed and integrated methodology together with benchmark performance indicators that may serve as useful guidance for researchers, process designers, and practitioners involved in the development, optimization, and future scale-up of methane cracking technologies for turquoise hydrogen production.

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