Citation: XIA Wen-Sheng, CHANG Gang, HOU Yu-Hui, WENG Wei-Zheng, WAN Hui-Lin. Influence of Ni Chemical States on the Partial Oxidation Mechanism of Methane: An Energetics Analysis[J]. Acta Physico-Chimica Sinica, ;2011, 27(07): 1567-1573. doi: 10.3866/PKU.WHXB20110627 shu

Influence of Ni Chemical States on the Partial Oxidation Mechanism of Methane: An Energetics Analysis

1.
State Key Laboratory of Physical Chemistry for Solid State Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, Fujian Province Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China

Received Date: 1 April 2011
Available Online: 6 May 2011
Fund Project: 国家自然科学基金(21033006, 20923004) (21033006, 20923004) 福建省自然科学基金(2007J0168) (2007J0168)国家重点基础研究发展规划项目(973) (2010CB732303)资助 (973) (2010CB732303)

An energetics analysis of the possible elementary steps involved in the partial oxidation of methane (POM) over different chemical states of Ni was carried out using the unity bond index-quadratic exponential potential (UBI-QEP) method. The results show that the rate determining step for the partial oxidation mechanism of methane is related to the chemical state of the Ni. Over reduced Ni the rate determining step for CO formation is the association of surface CH₃ species with surface O species. Over a partial positive charged Ni surface the rate determining step is that methane dissociates into the CH_xO species with the assistance of oxygen. Over the reduced and partial positive charged Ni sites in coexistence, however, the rate determining step depends on the competition between the formation of surface CH₃ species and the recombination of surface CH₃ species with surface O species. This competition is related to the chemical states of the Ni sites. If the partial positive charged Ni sites are predominant on the surface, the recombination of surface C species with surface O species and the recombination of surface H atom species favor CO and H₂ formation because of decreasing barriers. The surface CHx species does not dissociate easily and surface carbon deposition is significantly inhibited.
- Partial oxidation of methane,
- Nickel,
- Chemical state,
- Rate determining step,
- Mechanism,
- Energetics
1. [1]
  
  (1) Trimm, D. L.; Onsan, Z. I. Catal. Rev. Sci. Eng. 2001, 43, 31.
2. [2]
  (2) Specchia, S.; Negro, G.; Saracco, G.; Specchia, V. Appl. Catal. B 2007, 70, 525.
3. [3]
  (3) Burke, N. R.; Trimm, D. L. Catal. Today 2006, 117, 248.
4. [4]
  (4) Enger, B. C.; Lodeng, R.; Holmen, A. Appl. Catal. A 2008, 346, 1.
5. [5]
  (5) York, A. P. E.; Xiao, T.; Green, M. L. H. Top. Catal. 2003, 22, 345.
6. [6]
  (6) Choudhary, T. V.; Choudhary, V. R. Angew. Chem. Int. Edit. 2008, 47, 1828.
7. [7]
  (7) Hu, Y. H.; Ruckenstein, E. Adv. Catal. 2004, 48, 297.
8. [8]
  (8) Lu, Y.; Xue, J. Z.; Yu, C. C.; Liu, Y.; Shen, S. K. Appl. Catal. A 1998, 174, 121.
9. [9]
  (9) Xu, J. G.; Froment, G. F. AICHE J. 1989, 35, 88.
10. [10]
  (10) Tang, S.; Lin, J.; Tan, K. L. Catal. Lett. 1998, 55, 83.
11. [11]
  (11) Rabe, S.; Nachtegaal, M.; Vogel, F. Phys. Chem. Chem. Phys. 2007, 9, 1461.
12. [12]
  (12) Liu, Y.; Huang, F. Y.; Li, J. M.;Weng,W. Z.; Luo, C. R.;Wang, M. L.; Xia,W. S.; Huang, C. J.;Wan, H. L. J. Catal. 2008, 256, 192.
13. [13]
  (13) Shustorovich, E.; Sellers, H. Surf. Sci. Rept. 1998, 31, 1.
14. [14]
  (14) Shustorovich, E. Adv. Catal. 1990, 37, 101.
15. [15]
  (15) Rhodin, T. N.; Ertl, G. In The Nature of the Surface Chemical Bond; North-Holland Publ.: Amsterdam, 1979; Tables 5.1.
16. [16]
  (16) Brennan, D.; Hayward, D. O.; Trapnell, B. M.W. Proc. R. Soc. London, Ser. A 1960, 256, 81.
17. [17]
  (17) In CRC Handbook of Chemistry and Physics; CRC Press: Boca Raton, Florida, 1984-1985; p F171.
18. [18]
  (18) Xia,W. S.; Sellers, H. Surf. Sci. 2003, 524, 15.
19. [19]
  (19) Wei, J.; Iglesia, E. J. Catal. 2004, 224, 370.
20. [20]
  (20) Hu, Y. H.; Ruckenstein, E. Catal. Lett. 1999, 57, 167.
21. [21]
  (21) Theron, J. N.; Dry, M. E.; Steen, E. V.; Fletcher, J. C. Q. Stud. Surf. Sci. Catal. 1997, 107, 455.
1. [1]
  Jiahong WANG , Zekun XU , Tianjiao LU , Jinming HUANG . Performance of N, Mn doped semi-coke activated carbon catalyzed ozone oxidation for the degradation of tetracycline hydrochloride in water. Chinese Journal of Inorganic Chemistry, 2025, 41(12): 2549-2560. doi: 10.11862/CJIC.20250120
2. [2]
  Shiyi WANG , Chaolong CHEN , Xiangjian KONG , Lansun ZHENG , Lasheng LONG . Polynuclear lanthanide compound [Ce₄^ⅢCe₆^Ⅳ(μ₃-O)₄(μ₄-O)₄(acac)₁₄(CH₃O)₆]·2CH₃OH for the hydroboration of amides to amine. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 88-96. doi: 10.11862/CJIC.20240342
3. [3]
  Haiqiang Lin , Weizheng Weng , Jingdong Lin , Mingshu Chen , Xueming Fang , Lefu Yang . Diverse Variables-Driven Catalytic Optimization: Experimental Enhancement and Instructional Design for Selective Methane Oxidation on Supported Nickel-based Catalysts. University Chemistry, 2025, 40(11): 327-336. doi: 10.12461/PKU.DXHX202505106
4. [4]
  Guang Huang , Lei Li , Dingyi Zhang , Xingze Wang , Yugai Huang , Wenhui Liang , Zhifen Guo , Wenmei Jiao . Cobalt’s Valor, Nickel’s Foe: A Comprehensive Chemical Experiment Utilizing a Cobalt-based Imidazolate Framework for Nickel Ion Removal. University Chemistry, 2024, 39(8): 174-183. doi: 10.3866/PKU.DXHX202311051
5. [5]
  Wen YANG , Didi WANG , Ziyi HUANG , Yaping ZHOU , Yanyan FENG . La promoted hydrotalcite derived Ni-based catalysts: In situ preparation and CO₂ methanation performance. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 561-570. doi: 10.11862/CJIC.20230276
6. [6]
  Kexin Yan , Zhaoqi Ye , Lingtao Kong , He Li , Xue Yang , Yahong Zhang , Hongbin Zhang , Yi Tang . Seed-Induced Synthesis of Disc-Cluster Zeolite L Mesocrystals with Ultrashort c-Axis: Morphology Control, Decoupled Mechanism, and Enhanced Adsorption. Acta Physico-Chimica Sinica, 2024, 40(9): 2308019-0. doi: 10.3866/PKU.WHXB202308019
7. [7]
  Yiting Huo , Xin Zhou , Feifan Zhao , Chenbin Ai , Zhen Wu , Zhidong Chang , Bicheng Zhu . Boosting photocatalytic CO₂ methanation through TiO₂/CdS S-scheme heterojunction and fs-TAS mechanism study. Acta Physico-Chimica Sinica, 2025, 41(11): 100148-0. doi: 10.1016/j.actphy.2025.100148
8. [8]
  Bo YANG , Gongxuan LÜ , Jiantai MA . Nickel phosphide modified phosphorus doped gallium oxide for visible light photocatalytic water splitting to hydrogen. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 736-750. doi: 10.11862/CJIC.20230346
9. [9]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1953-1964. doi: 10.11862/CJIC.20240028
10. [10]
  Meiran Li , Yingjie Song , Xin Wan , Yang Li , Yiqi Luo , Yeheng He , Bowen Xia , Hua Zhou , Mingfei Shao . Nickel-Vanadium Layered Double Hydroxides for Efficient and Scalable Electrooxidation of 5-Hydroxymethylfurfural Coupled with Hydrogen Generation. Acta Physico-Chimica Sinica, 2024, 40(9): 2306007-0. doi: 10.3866/PKU.WHXB202306007
11. [11]
  Hailang JIA , Pengcheng JI , Hongcheng LI . Preparation and performance of nickel doped ruthenium dioxide electrocatalyst for oxygen evolution. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1632-1640. doi: 10.11862/CJIC.20240398
12. [12]
  Changsheng An , Tao Liu . Decoding SEI chemistry at the lithium-metal potential. Acta Physico-Chimica Sinica, 2025, 41(9): 100101-0. doi: 10.1016/j.actphy.2025.100101
13. [13]
  Jiahong ZHENG , Jiajun SHEN , Xin BAI . Preparation and electrochemical properties of nickel foam loaded NiMoO₄/NiMoS₄ composites. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 581-590. doi: 10.11862/CJIC.20230253
14. [14]
  Feng Lin , Zhongxin Jin , Caiying Li , Cheng Shao , Yang Xu , Fangze Li , Siqi Liu , Ruining Gu . Preparation and Electrochemical Properties of Nickel Foam-Supported Ni(OH)₂-NiMoO₄ Electrode Material. University Chemistry, 2025, 40(10): 225-232. doi: 10.12461/PKU.DXHX202412017
15. [15]
  Yan LIU , Jiaxin GUO , Song YANG , Shixian XU , Yanyan YANG , Zhongliang YU , Xiaogang HAO . Exclusionary recovery of phosphate anions with low concentration from wastewater using a CoNi-layered double hydroxide/graphene electronically controlled separation film. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1775-1783. doi: 10.11862/CJIC.20240043
16. [16]
  Bizhu Shao , Huijun Dong , Yunnan Gong , Jianhua Mei , Fengshi Cai , Jinbiao Liu , Dichang Zhong , Tongbu Lu . Metal-Organic Framework-Derived Nickel Nanoparticles for Efficient CO₂ Electroreduction in Wide Potential Windows. Acta Physico-Chimica Sinica, 2024, 40(4): 2305026-0. doi: 10.3866/PKU.WHXB202305026
17. [17]
  Wang Wang , Yucheng Liu , Shengli Chen . Use of NiFe Layered Double Hydroxide as Electrocatalyst in Oxygen Evolution Reaction: Catalytic Mechanisms, Electrode Design, and Durability. Acta Physico-Chimica Sinica, 2024, 40(2): 2303059-0. doi: 10.3866/PKU.WHXB202303059
18. [18]
  Lianghong Ye , Junqing Ni , Zhongyi Yan , Zhanming Zhang , Can Zhu , Mo Sun . Chemical Fuel-Driven Non-Equilibrium Color Change. University Chemistry, 2025, 40(3): 349-354. doi: 10.12461/PKU.DXHX202406109
19. [19]
  Ronghao Zhao , Yifan Liang , Mengyao Shi , Rongxiu Zhu , Dongju Zhang . Investigation into the Mechanism and Migratory Aptitude of Typical Pinacol Rearrangement Reactions: A Research-Oriented Computational Chemistry Experiment. University Chemistry, 2024, 39(4): 305-313. doi: 10.3866/PKU.DXHX202309101
20. [20]
  Yi Li , Zhaoxiang Cao , Peng Liu , Xia Wu , Dongju Zhang . Revealing the Coloration and Color Change Mechanisms of the Eriochrome Black T Indicator through Computational Chemistry and UV-Visible Absorption Spectroscopy. University Chemistry, 2025, 40(3): 132-139. doi: 10.12461/PKU.DXHX202405154

Get Citation

PDF

XML

Metrics

PDF Downloads(999)
Abstract views(2953)
HTML views(28)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142