Merkouri Loukia-Pantzechroula, Martín-Espejo Juan Luis, Bobadilla Luis Francisco, Odriozola José Antonio, Duyar Melis Seher, Reina Tomas Ramirez
School of Chemistry and Chemical Engineering, University of Surrey, Guildford GU2 7XH, UK.
Department of Inorganic Chemistry and Materials Sciences Institute, University of Seville-CSIC, 41092 Seville, Spain.
Nanomaterials (Basel). 2023 Jan 27;13(3):506. doi: 10.3390/nano13030506.
CO emissions in the atmosphere have been increasing rapidly in recent years, causing global warming. CO methanation reaction is deemed to be a way to combat these emissions by converting CO into synthetic natural gas, i.e., CH. NiRu/CeAl and NiRu/CeZr both demonstrated favourable activity for CO methanation, with NiRu/CeAl approaching equilibrium conversion at 350 °C with 100% CH selectivity. Its stability under high space velocity (400 L·g·h) was also commendable. By adding an adsorbent, potassium, the CO adsorption capability of NiRu/CeAl was boosted, allowing it to function as a dual-function material (DFM) for integrated CO capture and utilisation, producing 0.264 mol of CH/kg of sample from captured CO. Furthermore, time-resolved operando DRIFTS-MS measurements were performed to gain insights into the process mechanism. The obtained results demonstrate that CO 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.
近年来,大气中的一氧化碳(CO)排放量迅速增加,导致全球变暖。CO甲烷化反应被认为是一种通过将CO转化为合成天然气(即CH₄)来应对这些排放的方法。NiRu/CeAl和NiRu/CeZr对CO甲烷化均表现出良好的活性,NiRu/CeAl在350℃时接近平衡转化率,CH₄选择性为100%。其在高空速(400 L·g⁻¹·h⁻¹)下的稳定性也值得称赞。通过添加吸附剂钾,提高了NiRu/CeAl对CO的吸附能力,使其能够作为一种用于集成CO捕集和利用的双功能材料(DFM),从捕获的CO中产生0.264 mol CH₄/kg样品。此外,还进行了时间分辨的原位漫反射红外傅里叶变换光谱-质谱(DRIFTS-MS)测量,以深入了解该过程的机理。所得结果表明,CO在碱性位点上被捕获,并且在金属位点上也发生解离,使得在还原步骤中,甲烷通过两种不同的途径生成。这项研究表明,通过在有效的NiRu甲烷化催化剂配方中添加吸附剂,可以设计出先进的双功能材料。