石油学报(石油加工) ›› 2021, Vol. 37 ›› Issue (1): 218-223.doi: 10.3969/j.issn.1001-8719.2021.01.023

• 研究报道 • 上一篇    下一篇

甲烷干重整反应中CO2解离路径的分子模拟

赵晓光, 曲亚坤, 张荣俊   

  1. 中国石化 石油化工科学研究院,北京100083
  • 收稿日期:2018-12-20 修回日期:2020-02-19 出版日期:2021-01-25 发布日期:2021-01-12
  • 通讯作者: 赵晓光,女,高级工程师,硕士,从事分子模拟 研究,E-mail:zhaoxg.ripp@sinopec.com E-mail:zhaoxg.ripp@sinopec.com
  • 作者简介:第一作者:赵晓光,女,高级工程师,硕士,从事分子模拟研究,E-mail:zhaoxg.ripp@sinopec.com
  • 基金资助:
    中国石油化工股份有限公司科技项目(XLY19008)资助

Molecular Simulation on CO2 Disaggregation of Methane Dry Reforming Reaction

ZHAO Xiaoguang, QU Yakun, ZHANG Rongjun   

  1. Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, China
  • Received:2018-12-20 Revised:2020-02-19 Online:2021-01-25 Published:2021-01-12

摘要: 采用量子化学计算方法考察Ni基催化剂上甲烷干重整反应中CO2解离路径的能量、结构和电荷分布。计算结果表明,CO2的直接解离和氢助解离路径总体都是吸热反应。其中活化能较低的路径为:CO2中碳原子先被氢进攻生成甲酸基(—COOH),随后甲酸基(—COOH)裂解生成CO(g)和—OH。CO2更容易沿此活化能较低的路径解离。随后分析了CO2分子内Mulliken电荷分布等性质,进一步解释了CO2氢助解离路径的电子转移过程,为设计具有更高活性和抗积炭性能催化剂提供理论基础。

关键词: 甲烷干重整;二氧化碳(CO2)解离;Ni, 量子化学计算

Abstract: Quantum theory was used to investigate the energy, structure and charge distribution of CO2 disaggregation reaction catalyzed by Ni in the reaction of methane dry reforming. Results show that CO2 dissociation is endothermic reaction. The pathway in which H radical attacks the C atom of CO2 is preferred in three proposed mechanisms. The Mulliken charge population analysis and other calculated results are in accordance with the activation energy calculation. The results provide theoretical foundation for the design of catalysts with higher activity and stronger resistance to carbon deposition.

Key words: methane dry reforming, carbon dioxide(CO2) dissociation, nickel; the quantum chemical calculation

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