Sulfur-Accelerated Ceria Catalyst for Efficient CH4/CO2 Reforming: Unraveling the Special Role of Redox Functions and Its Reaction Mechanism

Sulfur-Accelerated Ceria Catalyst for Efficient CH4/CO2 Reforming: Unraveling the Special Role of Redox Functions and Its Reaction Mechanism
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DOI:
10.1021/acscatal.3c00752
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发表时间:
2023-08
期刊:
影响因子:
12.9
通讯作者:
Dedong He;Ju Yan;Kezhen Chen;Lei Zhang;Jichang Lu;Jiangping Liu;Yongming Luo
Dedong He;Ju Yan;Kezhen Chen;Lei Zhang;Jichang Lu;Jiangping Liu;Yongming Luo
中科院分区:
化学1区
文献类型:
--
作者:
Dedong He;Ju Yan;Kezhen Chen;Lei Zhang;Jichang Lu;Jiangping Liu;Yongming Luo

文献摘要

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甲烷干重整工业应用中存在严重的硫中毒问题,开发高活性、高耐久性的催化剂具有重要的环境意义。同时,设计一种以CeO 2代替传统金属Ni的刘易斯酸催化剂,用于具有挑战性的甲烷活化反应也是一个值得关注的课题。在此,有价值的见解的作用,H2S在促进二氧化铈催化剂的甲烷干重整的催化活性。通过准原位XPS、原位CH_4/CO_2-TPSR、原位DRIFTS和DFT计算,揭示了氧化还原功能在硫促进CeO_2催化剂上的特殊作用及其反应机理。本工作给出了一个独特的例子,硫加速氧化铈催化剂的有效CH 4/CO2重整。
Sulfur poisoning remains a severe problem in industrial applications for CH4dry reforming, and developing a highly active and durable catalyst is of great environmental importance. Meanwhile, designing a Lewis acid catalyst of CeO2to replace traditional metal Ni for the challenging activation of CH4is interesting. Herein, valuable insights into the role of H2S in promoting the catalytic activity of ceria catalysts for the dry reforming of methane are presented. Moreover, the special role of redox functions over the sulfur-accelerated CeO2catalyst and its reaction mechanism are unraveled by using quasi in situ XPS, in situ CH4/CO2-TPSR, and in situ DRIFTS and DFT calculations. This work gives a distinctive example of a sulfur-accelerated ceria catalyst for efficient CH4/CO2reforming.