[1]王昕晔,李静漪,杜 荣,等.CO/CH4在Ni(111)表面协同催化裂解机制[J].南京师范大学学报(工程技术版),2019,(01):072.[doi:10.3969/j.issn.1672-1292.2019.01.010]
 Wang Xinye,Li Jingyi,Du Rong,et al.Mechanisms on Synergetic Catalysis Crackingof CO/CH4 on Ni(111)[J].Journal of Nanjing Normal University(Engineering and Technology),2019,(01):072.[doi:10.3969/j.issn.1672-1292.2019.01.010]
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CO/CH4在Ni(111)表面协同催化裂解机制
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南京师范大学学报(工程技术版)[ISSN:1006-6977/CN:61-1281/TN]

卷:
期数:
2019年01期
页码:
072
栏目:
化学工程
出版日期:
2019-03-30

文章信息/Info

Title:
Mechanisms on Synergetic Catalysis Crackingof CO/CH4 on Ni(111)
文章编号:
1672-1292(2019)01-0072-06
作者:
王昕晔12李静漪12杜 荣12张居兵12卜昌盛12陈丹丹12朴桂林12
(1.南京师范大学能源与机械工程学院,江苏 南京 210042)(2.南京师范大学江苏省物质循环与污染控制重点实验室,江苏 南京 210042)
Author(s):
Wang Xinye12Li Jingyi12Du Rong12Zhang Jubing12Bu Changsheng12Chen Dandan12Piao Guilin12
(1.School of Energy and Mechanical Engineering,Nanjing Normal University,Nanjing 210042,China)(2.Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control,Nanjing Normal University,Nanjing 210042,China)
关键词:
甲烷一氧化碳催化裂解协同
Keywords:
methanecarbon monoxidecatalytic decompositionnickelsynergetic
分类号:
TQ546
DOI:
10.3969/j.issn.1672-1292.2019.01.010
文献标志码:
A
摘要:
采用理论计算研究了CO与CH4在Ni催化裂解过程中存在显著协同作用的机制. 结果表明:CH4逐步裂解过程中的速控步为第一个和最后一个H解离,反应能垒分别为106 kJ/mol和131 kJ/mol; CO在Ni(111)表面直接裂解为C和O,反应能垒为362 kJ/mol; CO/CH4催化裂解过程中,CO裂解产物O可改变CH4最后一步裂解的路径,其步骤为CH+O→CHO→C+OH,该步骤反应能垒低于CH直接裂解反应能垒; CH4裂解产物H可改变CO裂解的路径,其步骤为CO+H→COH→C+OH,该步骤反应能垒低于CO直接裂解反应能垒; 中间产物OH可改变CH4裂解最后一步裂解的路径,其步骤为CH+OH→CHOH→C+H2O,该步骤反应能垒低于CH直接裂解反应能垒.
Abstract:
The previous studies have found that CO/CH4 two-component system has a significant synergistic effect during catalysis cracking. This paper analyzes the mechanisms of this synergistic effect by theoretical calculation. The rate-determining steps of CH4 cracking process are the dissociation of the first H atom and the last H atom with the reaction energy barriers of 106 kJ/mol and 131 kJ/mol,respectively. CO is cracked directly into C and O on the Ni(111)surface with the reaction energy barrier of 362 kJ/mol. During the catalytic cracking of CO/CH4,the O atom from CO cracking changes the path of the final step of CH4 cracking by the step of CH+O→CHO→C+OH,which has lower reaction energy barrier than CH direct cracking. The H atom from CH4 cracking changes the path of CO cracking by the step of CO+H→COH→C+OH,which has lower reaction energy barrier than CO direct cracking. The intermediate product OH changes the path of the final step of CH4 cracking by the step of CH+OH→CHOH→C+H2O,which has lower reaction energy barrier than CH direct cracking.

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备注/Memo

备注/Memo:
收稿日期:2018-08-13.
基金项目:中国博士后科学基金(2017M621778)、江苏省高校自然科学研究面上项目(17KJB470007)、江苏省博士后科研资助计划(1701160B).
通讯联系人:王昕晔,博士,讲师,研究方向:化石燃料清洁利用. E-mail:xinye.wang@njnu.edu.cn
更新日期/Last Update: 2019-03-30