Unveiling the Roles of Precursor Structure and Controlled Sintering on Ni-Phyllosilicate-Derived Catalysts for Low-Temperature Methane Decomposition

Catalytic methane decomposition (CMD) is a promising technology for large-scale production of COx-free H2 from natural gas that can also produce valuable carbon byproducts. Although equilibrium conversions and reaction rates of CMD generally increase with temperature, operation in a low-temperature regime with simultaneous H2 recovery could potentially lead to operating cost and energy savings. Here, we report that well-dispersed Ni–SiO2, derived from high-temperature reduction of nickel phyllosilicates, is active for CMD at temperatures below 500 °C, with initial H2 production rates of up to 5.3 mol H2/gcat·h at 25% CH4 conversion. This ability to achieve rates comparable to other well-established catalysts is contrary to expectations that small (