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Catalytic performance of Ni/CaO-Ca12Al14O33 catalyst in the green synthesis gas production via CO2 reforming of CH4
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2021-01-22 , DOI: 10.1016/j.jcou.2021.101447
Silvera Scaccia , Livia Della Seta , Daniele Mirabile Gattia , Giuseppina Vanga

Dry Reforming of Methane over 15wt.% Ni/CaO-Ca12Al14O33 catalyst was performed in a microreactor in the temperature range 600−800°C under atmospheric pressure, at WHSV of 120 Lg−1h−1 and by time on stream of 12 h for producing synthesis gas. The novel catalyst was prepared by Ni wet impregnation of a mixed calcium-aluminum-oxide (CAO) ceramic support. Similarly, a Ni/γ-Al2O3 reference catalyst was prepared. Characterizations were conducted by TGA-FTIR, XRD, SEM-EDS, N2 physisorption, H2-TPR, CO2-TPD, and CO2-TPRn techniques. After calcination(500°C)/reduction(700°C) steps in situ formed CaO promoter was highly dispersed on Ca12Al14O33 carrier, which induced strong basicity. A good anchorage of NiO on CAO support was evidenced by reduction peaks at 490°C and 650°C on the H2-TPR profile. The reduced mesoporous catalyst presented high SBET, large pores volume, and unimodal pore size distribution. High reactants conversions, good H2 and CO selectivity, and H2/CO molar ratio close to unity at 800°C were achieved. Although the catalytic activity of Ni/γ-Al2O3 reference catalyst was slightly better than that of Ni/CaO-Ca12Al14O33 catalyst the stability was worse owing to the excessive carbon build-ups, whereas the novel catalyst displayed a very low carbon deposit on spent catalyst at 600 and 700°C, and negligible coke deposit at 800°C. It was established that the basicity of CaO-Ca12Al14O33 support can play a key role in preventing coke deposition during DRM. The Ni CaO-Ca12Al14O33 can serve as sorbent for CO2 capture and simultaneously for its catalytic conversion in a valuable fuel.



中文翻译:

Ni / CaO-Ca 12 Al 14 O 33催化剂在CH 4的CO 2重整生成绿色合成气中的催化性能

在微型反应器中,在大气压力下,于600-800°C的温度范围内,在WHSV为120 Lg -1 h -1的条件下按时间对15%。Ni / CaO-Ca 12 Al 14 O 33催化剂进行甲烷干重整。在12小时内用于生产合成气。通过镍湿法浸渍混合的钙铝氧化物(CAO)陶瓷载体制备了新型催化剂。类似地,由Ni /γ-Al系2 ö 3制备参考催化剂。通过TGA-FTIR,XRD,SEM-EDS,N 2物理吸附,H 2 -TPR,CO 2 -TPD和CO 2进行表征-TPRn技术。在煅烧(500℃)/还原(700℃)步骤后,原位形成的CaO促进剂高度分散在Ca 12 Al 14 O 33载体上,引起强碱性。通过在H 2 -TPR曲线上的490°C和650°C的还原峰可以证明NiO在CAO载体上具有良好的锚固性。还原的中孔催化剂表现出高的S BET,大的孔体积和单峰孔径分布。获得了高的反应物转化率,良好的H 2和CO选择性以及在800℃下接近于1的H 2 / CO摩尔比。虽然镍的催化活性/γ-Al系2 ö 3参比催化剂比Ni / CaO-Ca 12 Al 14 O 33催化剂稍好,但由于积碳过多,稳定性较差,而新型催化剂在600和700°C时在废催化剂上的积碳非常低C,在800°C下可忽略不计的焦炭沉积。已经确定,CaO-Ca 12 Al 14 O 33载体的碱性可以在防止DRM期间积炭的过程中发挥关键作用。Ni CaO-Ca 12 Al 14 O 33可用作吸附剂,用于捕获CO 2并同时用于其在有价值的燃料中的催化转化。

更新日期:2021-01-22
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