Combined Capture and Utilization of CO2 for Syngas Production over Dual-Function Materials
Combined Capture and Utilization of CO2 for Syngas Production over Dual-Function Materials
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DOI：
10.1021/acssuschemeng.8b03769
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发表时间：
2018-10-01
影响因子：
8.4
通讯作者：
Rezaei, Fateme
中科院分区：
文献类型：
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作者：
Al-Mamoori, Ahmed;Rownaghi, Ali A.;Rezaei, Fateme
二氧化碳捕获和转化的整合最近被证明是在生产增值化学品和燃料的同时解决二氧化碳排放的一种有希望的方法。在此，我们报道了在乙烷（DRE）干重整（DRE）合成气生产中，通过由γ - al2o3负载的ni -浸渍CaO-和mgo -基双盐组成的双功能材料（DFMs）原位捕获和利用CO2。采用N-2吸附、XRD、CO2-TPD、NH3-TPD、H-2-TPR和XPS等方法对所制得的DFMs进行表征。γ - al2o3负载型吸附催化剂材料在650℃下的CO2吸附-解吸性能表明，吸附的CO2 100%从DFMs表面解吸，随后与C2H6反应。反应温度为650℃，WHSV为2250 mL g(-1) h（-1）时，Ni-20@(K-Ca)(50)/(γ - al2o3)（50）和Ni-20@(Na-Ca)(50)/(γ - al2o3)（50）表现出最佳活性，C2H6转化率为100%，CO2转化率分别为65%和75%。对废DFMs的分析显示，低程度的焦炭形成（类似于9 wt %），这降低了DFMs的稳定性仅5%。本调查报告的结果强调了联合捕集-反应系统作为一种经济有效的技术的重要性，该技术利用排放的二氧化碳作为原料来制造有价值的化学品、材料和燃料。
The integration of CO2 capture and conversion has been recently demonstrated as a promising approach to address CO2 emissions while producing value-added chemicals and fuels. Herein, we report in situ capture and utilization of CO2 in syngas production from dry reforming of ethane (DRE) over dual-function materials (DFMs) consisting of Ni-impregnated CaO- and MgO-based double salts supported on gamma-Al2O3. The N-2 physisorption, XRD, CO2-TPD, NH3-TPD, H-2-TPR, and XPS analyses were performed to characterize the obtained DFMs. The CO2 adsorption-desorption performance of gamma-Al2O3-supported adsorbent catalyst materials at 650 degrees C indicated that 100% of the adsorbed CO2 was desorbed from the DFMs surface for subsequent reaction with C2H6. At a reaction temperature of 650 degrees C and WHSV of 2250 mL g(-1) h(-1), the Ni-20@(K-Ca)(50)/(gamma-Al2O3)(50) and Ni-20@(Na-Ca)(50)/(gamma-Al2O3)(50) showed the best activity with 100% C2H6 conversion and 65% and 75% CO2 conversion, respectively. Analysis of the spent DFMs revealed a low degree of coke formation (similar to 9 wt %) which reduced the stability of DFMs by only 5%. The results reported in this investigation highlight the importance of combined capture-reaction system as a cost-effective technology for utilizing the emitted CO2 as a feedstock to make valuable chemicals, materials, and fuels.