Enhanced CO 2 utilization in dry reforming of methane achieved through nickel-mediated hydrogen spillover in zeolite crystals

Transformation of CO 2 into precursors for chemicals and fuels by self-contained reducing gas contaminants (for example, CH 4 ) is attractive from a carbon economy perspective. Reducing as much CO 2 as possible using a limited amount of reducing gas would be ideal, but general dry reforming (DRM) schemes consume stoichiometric amounts of methane for CO 2 reduction. Here we develop a process with high reducibility of methane relative to conventional DRM, using up to 2.9 mol of CO 2 per mol of CH 4 . Key to this success are Ni nanoparticles, fixed within the matrix of an aluminosilicate zeolite catalyst (Ni@HZSM-5), that enhance hydrogen spillover to favour the reduction of CO 2 . This process achieves an energy cost for reducing CO 2 of 113.6 kJ per mol CO 2 , which is 31.9% lower than the conventional DRM process with stoichiometric transformation of CO 2 and methane. In addition, the rigid zeolite framework could minimize coke formation and prevent Ni sintering.