摘要
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•Cyclic reaction system integrates methane reforming with CO2 refluxed.•Direct carbon emissions reduced to 22% compared to conventional SRM process.•Pd enhances turnover frequency (1.33 s−1) and H2 yield (196.03 mmol gcat-1h−1)•CO removal improves catalyst stability and long-term operational performance.
The steam reforming of methane (SRM) is a primary method for large-scale hydrogen production but is associated with significant CO2 emissions, both directly from the reaction and indirectly due to energy consumption. To address these environmental concerns, this study explores the development of a NiPd@Al2O3 bimetallic nanoparticle cluster catalyst and introduces a cyclic reaction system to reduce CO2 emissions in SRM-based hydrogen production. The incorporation of Pd into the catalyst significantly enhances its catalytic performance, as evidenced by an increase in the turnover frequency (TOFCH4; 1.33 s−1) and hydrogen yield (YH2; 196.03 mmol gcat-1h−1) at 500 °C. This improvement is attributed to ability of Pd to lower activation energy of the rate-determining step, facilitating efficient methane reforming and hydrogen production. The cyclic reaction system enhances hydrogen production by 18 % and reduces direct carbon emissions to 22 % compared to the conventional SRM process. These findings demonstrate the potential of incorporating Pd into Ni-based catalysts within a cyclic reaction process for sustainable, low-carbon hydrogen production, showcasing the feasibility of continuous large-scale hydrogen production with reduced energy and carbon emissions.