[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),2019,19(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),2019,19(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:
19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1; 2; 李静漪1; 2; 杜 荣1; 2; 张居兵1; 2; 卜昌盛1; 2; 陈丹丹1; 2; 朴桂林1; 2
(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 Xinye1; 2; Li Jingyi1; 2; Du Rong1; 2; Zhang Jubing1; 2; Bu Changsheng1; 2; Chen Dandan1; 2; Piao Guilin1; 2
(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; 镍; 协同
Keywords:
methane; carbon monoxide; catalytic decomposition; nickel; synergetic
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.

参考文献/References:

[1] 英国石油公司. BP世界统计年鉴[M]. 北京:中国统计出版社,2018.
BP P.L.C. BP world energy statistical yearbook[M]. Beijing:China Statistics Press,2018.(in Chinese)
[2]李佳懋. 掺铜镍基催化剂甲烷催化裂解反应机理研究[D]. 绵阳:中国工程物理研究院,2016.
LI J M. Study on mechanism of methane catalytic cracking reaction of copper-doped catalysts[D]. Mianyang:China Academy of Engineering Physics,2016.(in Chinese)
[3]张志,唐涛,陆光达. 甲烷催化裂解制氢技术研究进展[J]. 化学研究与应用,2007(1):1-9.
ZHANG Z,TANG T,LU G D. Catalytic decomposition of methane for preparation of hydrogen[J]. Chemical research and application,2007(1):1-9.(in Chinese)
[4]CHEN P,ZHANG H B,LIN G D,et al. Growth of carbon nanotubes by catalytic decomposition of CH4 or CO on a Ni-MgO catalyst[J]. Carbon,1997,35(10):1495-1501.
[5]张百强. 流化床条件下多组分碳源气催化制备碳纳米管的研究[D]. 南京:南京师范大学,2016.
ZHANG B Q. Study on catalytic preparation of carbon nanotubes by multi-component carbon source gas under fluidized bed conditions[D]. Nanjing:Nanjing Normal University,2016.(in Chinese)
[6]LIU Z,NUTT M A,IGLESIA E. The effects of CO2,CO and H2 Co-reactants on methane reactions catalyzed by Mo/H-ZSM-5[J]. Catalysis letters,2002,81(3/4):271-279.
[7]LI J,CROISET E,RICARDEZ-SANDOVAL L. Methane dissociation on Ni(1 0 0),Ni(1 1 1),and Ni(5 5 3):a comparative density functional theory study[J]. Journal of molecular catalysis A chemical,2012,365(4):103-114.
[8]KOZLOV S M,NEYMAN K M. Insights from methane decomposition on nanostructured palladium[J]. J Catal,2016,337:111-121.
[9]徐文媛,胡林,龙威,等. 镍基上羟基活化催化CH4—CO2重整的理论计算[J]. 浙江大学学报(理学版),2013,40(2):177-181.
XU W Y,HU L,LONG W,et al. A study of the methane’s hydrozyl-activate-reforming with carbon dioxide over nicke[J]. Journal of Zhejiang university(science edition),2013,40(2):177-181.(in Chinese)
[10]LIU H,YAN R,ZHANG R,et al. A DFT theoretical study of CH4 dissociation on gold-alloyed Ni(111)surface[J]. Journal of energy chemistry,2011,20(6):611-617.

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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