CO
2 emissions in the atmosphere have been increasing rapidly in recent years, causing global warming. CO
2 methanation reaction is deemed to be a way to combat these emissions by converting CO
2 into synthetic natural gas, i.e., CH
4. NiRu/CeAl
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CO
2 emissions in the atmosphere have been increasing rapidly in recent years, causing global warming. CO
2 methanation reaction is deemed to be a way to combat these emissions by converting CO
2 into synthetic natural gas, i.e., CH
4. NiRu/CeAl and NiRu/CeZr both demonstrated favourable activity for CO
2 methanation, with NiRu/CeAl approaching equilibrium conversion at 350 °C with 100% CH
4 selectivity. Its stability under high space velocity (400 L·g
−1·h
−1) was also commendable. By adding an adsorbent, potassium, the CO
2 adsorption capability of NiRu/CeAl was boosted, allowing it to function as a dual-function material (DFM) for integrated CO
2 capture and utilisation, producing 0.264 mol of CH
4/kg of sample from captured CO
2. Furthermore, time-resolved operando DRIFTS-MS measurements were performed to gain insights into the process mechanism. The obtained results demonstrate that CO
2 was captured on basic sites and was also dissociated on metallic sites in such a way that during the reduction step, methane was produced by two different pathways. This study reveals that by adding an adsorbent to the formulation of an effective NiRu methanation catalyst, advanced dual-function materials can be designed.
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