Breaking trade-off between catalytic activity and carbon deposit by tailoring d-band center of NiFe alloy for dry reforming of carbonate

The dry reforming of carbonate with methane (CaDRM) can be one of the breakthrough technologies to address the challenge of mitigating inevitable CO 2 emissions into value-added chemicals but remains great challenges for efficient catalysts design. In this study, we break the trade-off between the catalytic activity and the carbon deposit by tailoring the d-band center of Ni through Fe doping, which matches the energy level of CH 4 * dehydrogenation but is far away from that of the over cleavage of CH* . In this light, the porous spherical Fe x Ni/Al 2 O 3 catalysts with Ni 3 Fe alloy nanoaggregates are obtained through a one-step spray drying method. The optimized Fe 0.6 Ni/Al 2 O 3 catalyst shows an excellent catalytic activity with a superior CO selectivity of 91.75 % at a complete CaCO 3 conversion at 700°C, and successfully prevents the carbon deposit to maintain its excellent stability. Moreover, the extremely low activation energy of 45.2 kJ/mol and the good porosity of Fe x Ni/Al 2 O 3 ensure its fast dynamics. Therefore, this tailoring d-band center approach through the formation of alloy catalysts supplied a novel strategy for effectively cracking hydrogen species while avoiding over cleavage of CH x * in the thermal catalysis, which promoted the CaDRM technology to be a promising solution for carbon neutrality in industrial sectors in near future.