Porous hollow Ni/CaO dual functional materials for integrated CO2 capture and methanation

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Abstract

Excessive CO2 emissions present significant environmental and energy challenges, driving the need for effective strategies to reduce CO2. Integrated CO2 capture and utilization (ICCU) processes have drawn considerable attention by combing carbon capture and catalytic conversion in a unified process. The rational design of efficient dual-functional materials (DFMs) is key to achieving high-efficiency ICCU processes. Here, we synthesized a series of CaO-based DFMs with varying Ni loadings, in which the porous hollow CaO prepared by a sacrificial template method was employed as the adsorbent. The porous hollow structure are effectively to improve the diffusion of CO2 species and provide sufficient space for volume expansion after CO2 capture. The optimized conditions for adsorption and catalytic sites were determined to be at 550 °C with 5wt% Ni loading. Under these conditions, the adsorption capacity of 5 %Ni/CaO-P reached 7.02 mmol·g−1 DFM, with a CH4 yield of 2.85 mmol·g−1 DFM and a CH4 selectivity of 94.09 %. After 19 cycles, the adsorption capacity of 5 %Ni/CaO-P is maintained at 4.50 mmol·g−1 DFM with a CH4 yield remaining stable at 0.50 mmol·g−1 DFM due to the slight sintering of Ni species. Integrated CO2 capture and methanation offer a pathway for carbon recycling, emissions reduction, and sustainable development.

用于集成二氧化碳捕获和甲烷化的多孔空心 Ni/CaO 双功能材料
过量的二氧化碳排放给环境和能源带来了巨大挑战,因此需要制定有效的二氧化碳减排战略。二氧化碳捕集与利用(ICCU)工艺将碳捕集和催化转化结合在一个统一的过程中,因而备受关注。合理设计高效的双功能材料(DFMs)是实现高效 ICCU 工艺的关键。在此,我们合成了一系列不同镍负载量的 CaO 基 DFMs,其中采用牺牲模板法制备的多孔空心 CaO 作为吸附剂。多孔中空结构有效地改善了二氧化碳的扩散,并为二氧化碳捕获后的体积膨胀提供了足够的空间。吸附和催化位点的优化条件被确定为 550 °C,镍的负载量为 5wt%。在这些条件下,5%Ni/CaO-P 的吸附容量达到 7.02 mmol-g-1 DFM,CH4 产率为 2.85 mmol-g-1 DFM,CH4 选择性为 94.09%。经过 19 次循环后,5%Ni/CaO-P 的吸附容量保持在 4.50 mmol-g-1 DFM,由于镍的轻微烧结,CH4 产率稳定在 0.50 mmol-g-1 DFM。综合二氧化碳捕集与甲烷化为碳回收、减排和可持续发展提供了一条途径。
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