Transformation of CO2 into precursors for chemicals and fuels by self-contained reducing gas contaminants (for example, CH4) is attractive from a carbon economy perspective. Reducing as much CO2 as possible using a limited amount of reducing gas would be ideal, but general dry reforming (DRM) schemes consume stoichiometric amounts of methane for CO2 reduction. Here we develop a process with high reducibility of methane relative to conventional DRM, using up to 2.9 mol of CO2 per mol of CH4. 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 CO2. This process achieves an energy cost for reducing CO2 of 113.6 kJ per mol CO2, which is 31.9% lower than the conventional DRM process with stoichiometric transformation of CO2 and methane. In addition, the rigid zeolite framework could minimize coke formation and prevent Ni sintering.
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This work was supported by the National Key Research and Development Program of China (2021YFA1500404), and the National Natural Science Foundation of China (U21B20101 and 21932006).
The authors declare no competing interests.
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Zhu, Q., Zhou, H., Wang, L. et al. Enhanced CO2 utilization in dry reforming of methane achieved through nickel-mediated hydrogen spillover in zeolite crystals. Nat Catal (2022). https://doi.org/10.1038/s41929-022-00870-8