Integrated carbon capture and utilization (ICCU) has emerged as a promising strategy toward carbon neutrality. However, most existing studies rely on simulated flue gas compositions, neglecting the impact of common impurities such as sulfur oxides (SOx) and nitrogen oxides (NOx), thereby limiting the practical industrial applicability of ICCU technologies. Herein, we systematically investigate the effects of SO2 and NO2 at various concentrations on the adsorption–catalysis performance based on a representative Ni–Ca dual functional material (DFM) in the ICCU–dry reforming of methane (ICCU-DRM) process. Exposure to 100 ppm SO2 showed a negligible influence on catalytic activity but markedly inhibited carbon deposition. Further increasing the SO2 concentration to 500 ppm led to complete deactivation of the DFM. NO2 exhibited a similar concentration-dependent trend to SO2, albeit with a comparatively lower impact. Mechanistic analysis revealed that both SO2 and NO2 promote the formation of a coating layer of calcium-containing compounds on the surface of Ni nanoparticles, accounting for the partial or total deactivation. These findings offer critical insights into the industrial applications of ICCU systems under realistic flue gas conditions.
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The presence of sulfur compounds, particularly SO2, is known to significantly degrade the performance of metal-based catalysts, posing a significant challenge in CO2 hydrogenation reactions. In this study, we systematically investigate the impact of SO2 on Cu–ZnO–Al2O3 catalysts for CO2 hydrogenation to elucidate the deactivation mechanisms. Our findings reveal that SO2 adsorption leads to the formation of surface sulfate and sulfite species, which effectively block active sites, impeding the adsorption and activation of reactants. Moreover, SO2 exposure inhibits CO desorption, further compromising catalytic efficiency. In parallel, progressive sulfidation of Cu and ZnO results in the formation of catalytically inactive CuS, Cu2S, and ZnS phases, ultimately leading to complete catalyst deactivation. These results highlight the dual role of sulfur species in both surface passivation via sulfates/sulfites deposition and irreversible structural transformation via sulfidation. Our study provides new insights into the SO2-induced catalyst deactivation in CO2 hydrogenation and offers a theoretical foundation for enhancing CO2 hydrogenation reactions, with implications for optimizing environmentally sustainable catalytic systems in industrial applications.
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In the quest for low-temperature polyolefins upcycling, overcoming the decomposition temperature limitations caused by chemically inert carbon-hydrogen (C(sp3)–H) bonds remains a challenge. Here we report a tandem endothermic-exothermic magnetocatalytic (EEM) strategy for upcycling of polypropylene (PP) and polyethylene (PE) below their decomposition temperature (typically 300 °C). A series of commodity polyolefins (PP, PE, and their mixtures (PP+PE)) can be deconstructed magnetocatalytically at 290 °C, for which a high H2 selectivity up to 86% can be achieved. Magneto-thermal coupling simulations revealed that the interfacial temperature gap was the key to upcycling of polyolefins at low temperature. Overall, EEM method potentially provides a sustainable approach for end-of-life plastics upcycling.
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