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Partial oxidation of methane over monometallic and bimetallic Ni-, Rh-, Re-based catalysts: Effects of Re addition, co-fed reactants and catalyst support
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2018-06-25 , DOI: 10.1016/j.apcata.2018.06.032
Chanittar Cheephat , Pornlada Daorattanachai , Sakamon Devahastin , Navadol Laosiripojana

Partial oxidation reactions of CH4 over monometallic Ni, Rh, Re and bimetallic Re-Ni catalysts supported by Al2O3 were studied at 400–700 °C. Among monometallic catalysts, Rh/Al2O3 exhibited the highest catalytic activity. Lower CH4 conversion and H2 yield were observed over Ni/Al2O3 catalyst, while Re/Al2O3 catalyst did not promote the reaction under the studied condition. Addition of Re over Ni to form a bimetallic catalyst considerably promoted the activity of Ni/Al2O3 catalyst, particularly at a higher temperature (600 °C). Re-Ni proportion was then optimized; Re-Ni/Al2O3 at Re:Ni ratio of 3:7 resulted in a significantly higher CH4 conversion as well as H2 and CO yields when compared to noble-metal Rh/Al2O3 catalyst. Stability testing of Re-Ni/Al2O3, Ni/Al2O3 and Rh/Al2O3 catalysts was also conducted. After 18-h operation, Re-Ni/Al2O3 catalyst still exhibited high stability with slight deactivation in terms of H2 yield, whereas Ni/Al2O3 and Rh/Al2O3 catalysts showed higher deactivation rates. Post-reaction temperature programmed oxidation confirmed the better resistance toward carbon deposition of Re-Ni/Al2O3 catalyst. The effect of steam and CO2 addition on the Re-Ni/Al2O3 catalyst performance was also investigated. The presence of a suitable H2O content could increase H2 and CO yields and reduce the amount of carbon deposition, whereas the presence of CO2 showed undesirable influence on the reaction by reducing CH4 conversion and H2/CO ratio. Lastly, Re-Ni/Gd-CeO2 catalyst was prepared and tested to study the effect of catalyst support. The catalyst stability and resistance toward carbon deposition were significantly improved, which could be due to the high oxygen storage capacity of Gd-CeO2.



中文翻译:

单金属和双金属镍,铑,Re基催化剂上甲烷的部分氧化:of添加,共进料反应物和催化剂载体的影响

研究了在400–700°C下,由Al 2 O 3负载的单金属Ni,Rh,Re和双金属Re-Ni催化剂上CH 4的部分氧化反应。在单金属催化剂中,Rh / Al 2 O 3表现出最高的催化活性。在研究条件下,Ni / Al 2 O 3催化剂的CH 4转化率和H 2产率较低,而Re / Al 2 O 3催化剂没有促进反应。在Ni上添加Re形成双金属催化剂大大提高了Ni / Al 2 O 3的活性催化剂,尤其是在较高温度(600°C)下。然后优化了Re-Ni的比例。与贵金属Rh / Al 2 O 3催化剂相比,Re:Ni比为3:7的Re-Ni / Al 2 O 3导致CH 4转化率以及H 2和CO产率显着提高。还进行了Re-Ni / Al 2 O 3,Ni / Al 2 O 3和Rh / Al 2 O 3催化剂的稳定性测试。在运行18小时后,Re-Ni / Al 2 O 3催化剂仍表现出高稳定性,并且在H 2方面略有失活Ni / Al 2 O 3和Rh / Al 2 O 3催化剂显示出更高的失活速率。反应后温度程序控制的氧化证实了Re-Ni / Al 2 O 3催化剂对碳沉积具有更好的抵抗力。还研究了蒸汽和CO 2添加对Re-Ni / Al 2 O 3催化剂性能的影响。合适的H 2 O含量的存在可以提高H 2和CO的收率并减少碳沉积的量,而CO 2的存在通过减少CH 4表现出对反应的不良影响转化率和H 2 / CO比。最后,制备了Re-Ni / Gd-CeO 2催化剂并进行了测试,以研究催化剂载体的作用。由于Gd-CeO 2的高储氧能力,催化剂的稳定性和抗碳沉积性得到了显着提高。

更新日期:2018-06-25
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