摘要
A CO2-negative emission, fossil fuel-based hydrogen production is demonstrated via chemical looping of methane decomposition (CH4 -> C + 2H2) with CO2-utilized catalyst regeneration (i.e., the reverse Boudouard reaction, C + CO2 -> 2CO). Ni-FeOx-based hybrid nanoparticle clusters, prepared via gas-phase evaporation selfassembly, were employed as dual functional catalyst in the chemical looping. Using the optimal sample, 10Ni1Fe/5Al, the results show moderately-high methane (3.33 mmol/gcat & sdot;min) and CO2 (1.66 mmol/gcat & sdot;min) conversion rates and hydrogen production rate (6.66 mmol/gcat & sdot;min) achieved at a relatively low temperature (600 degrees C). As a result, exceptional total carbon removal efficiency (99.97 %) and negative CO2 emission rate (-0.0014 g/min) were achievable. Density functional theoretical studies confirmed the synergistic effect between Ni and FeOx, where Ni facilitated methane dissociation (Ea = 1.0 eV) and FeOx-1 enhanced CO2 reaction with the deposited carbon (Ea = 1.3 eV) at the Ni-FeOx interfaces. This work demonstrates sustainable advancements in the mass production of hydrogen, offering a promising and eco-friendly solution for H2-based industrial and energy applications.