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Direct and highly selective conversion of captured CO2 into methane through integrated carbon capture and utilization over dual functional materials
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2020-02-14 , DOI: 10.1016/j.jcou.2020.02.001
Hongman Sun , Yu Zhang , Shaoliang Guan , Jun Huang , Chunfei Wu

Excessive atmospheric CO2 emission is regarded as one of the main factors causing global climate change. Thus, there is an urgent need to explore the possibility of CO2 capture and converting the captured CO2 to fuels or value-added products. Recently, an integrated carbon capture and utilization (ICCU) process performed in a single reactor under isothermal conditions draws intensive attentions due to the reduction of energy requirement for sorbent regeneration. However, from literature, normally a low loading of sorbent in dual functional materials (DFMs) was applied resulting in a very low CO2 capture capacity and consequent low CH4 yield in the ICCU process. Herein, we demonstrate the intermediate-temperature DFMs using inexpensive high-capacity MgO sorbent. The synthesized DFMs are a physical mixture of sorbent and Ru/CeO2 catalyst by the mass ratio of 2:1 allowing simultaneous regeneration of sorbent and conversion of CO2 in a single reactor at 300 °C. During the 1st cycle of ICCU process, 10Ru/CeO2-MgO exhibits the best ICCU performance with the highest CH4 yield of 7.07 mmol g−1 and CO2 conversion of 89 %. However, after 10 cycles of ICCU process, 5Ru/CeO2-MgO exhibits the highest CH4 yield (3.36 mmol g−1) and CO2 conversion (79 %), which are much higher than that of 2.5Ru/CeO2-MgO (1.13 mmol g−1 and 39 %) and 10Ru/CeO2-MgO (2.31 mmol g−1 and 69 %). It is mainly attributed to that more oxygen vacancies are remained in 5Ru/CeO2-MgO resulted from the metal-support interaction.



中文翻译:

通过集成的碳捕获和利用双功能材料的综合利用,将捕获的CO 2直接和高度选择性地转化为甲烷

大气中过量的CO 2排放被认为是导致全球气候变化的主要因素之一。因此,迫切需要探索CO的可能性2捕获变换所捕获的CO和2至燃料或增值产品。近来,由于减少了吸附剂再生的能量需求,在单个反应器中在等温条件下进行的集成碳捕获和利用(ICCU)工艺引起了广泛的关注。但是,根据文献,通常在双功能材料(DFM)中使用的吸附剂含量低,导致非常低的CO 2捕集能力并因此导致较低的CH 4ICCU过程中的产量。在这里,我们演示了使用廉价的高容量MgO吸附剂的中温DFM。合成的DFM是吸附剂和Ru / CeO 2催化剂的物理混合物,其质量比为2:1,可在300°C的单个反应器中同时再生吸附剂和转化CO 2。在ICCU工艺的第一个循环中,10Ru / CeO 2 -MgO表现出最佳的ICCU性能,最高的CH 4产率为7.07 mmol g -1,CO 2转化率为89%。然而,经过10个ICCU工艺循环,5Ru / CeO 2 -MgO表现出最高的CH 4产率(3.36 mmol g -1)和CO 2。转化率(79%),远高于2.5Ru / CeO 2 -MgO(1.13 mmol g -1和39%)和10Ru / CeO 2 -MgO(2.31 mmol g -1和69%)。这主要归因于金属-载体相互作用导致在5Ru / CeO 2 -MgO中保留了更多的氧空位。

更新日期:2020-03-05
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