Wang, Xingbo; Hu, Deng; Wang, Ke; Xu, Wenqing; Wei, Wei; Sun, Nannan

SEPARATION AND PURIFICATION TECHNOLOGY

2025, ,

Wang, Xingbo; Hu, Deng; Wang, Ke; Xu, Wenqing; Wei, Wei; Sun, Nannan

Integrated carbon capture and conversion (ICCC) offers a promising strategy to reduce the operational costs associated with conventional carbon capture, utilization, and storage (CCUS) systems. The present study elucidates the impact of metal-support interactions (MSI) in Ni-MgO-ZrO2 dual-functional materials (DFMs) on their ICCCCH4 performance, with particular emphasis on continuous decarbonization mode, which is widely overlooked in previous literatures. Comprehensive structural characterization indicated that the NMZ-cop sample prepared by coprecipitation exhibits stronger MSI, and thus leading to higher porosity (87 m(2)g(-1)) and superior Ni dispersion (18.4 %), these are considerably higher than samples prepared from impregnation or mixing methods. As a result, NMZ-cop is characterized by stable Ni-MgO interface that suppresses Ni nanoparticle sintering while promoting the regeneration of the CO2 adsorption sites, which in turn led to exceptional performance in continuous ICCCCH4 operation (>97 % CO2 capture ratio, similar to 100 % conversion of the captured CO2, and 2.1 mmolg(DFM)(-1)h(-1) CH4 spatio-temporal yield). Mechanistic insights from CO2-temperature-programmed desorption (CO2-TPD), In-situ Fourier transform infrared spectroscopy (FT-IR), and dynamic cycling tests indicated that the strong MSI facilitated synergistic coupling between MgO-based CO2 adsorption sites and Ni-based catalytic centers. This interaction enables efficient formation of a CO2 pool and its subsequent hydrogenation to CH4 via the formate pathway. The findings provide fundamental design principles for advanced DFMs for ICCC and highlight MSI engineering as a critical parameter.