二元铜族团簇负离子催化CO氧化反应机理

doi:10.3866/PKU.WHXB20110226

Abstract

Abstract:

The detailed mechanisms of CO oxidation catalyzed by AuAg^-, AuCu^-, and AgCu^- were investigated using density functional theory at the B3LYP level. The computational results indicate that the adsorption site of CO onto the mixed clusters decreases as follows: Cu>Au>Ag. Copper is the preferred adsorption site for O₂ on the binary clusters. The adsorption of O₂ onto gold was found to be the weakest. Three reaction pathways exist for CO oxidation catalyzed by AuAg^-, AuCu^-, and AgCu^-. The most feasible pathway for CO oxidation catalyzed by AuAg^- is CO insertion into the Ag―O bond of AuAgO₂^- to produce the [Au―AgC(O―O)O]^- intermediate, which then decomposes into CO₂ and AuAgO^-, or another CO molecule attacks [Au―AgC(O―O)O]^- to form two CO₂ molecules and AuAg^- anion. A feasible pathway for CO oxidation catalyzed by AuCu^- or AgCu^- is initiated by the co-absorption of CO and O₂ onto the clusters followed by the formation of a four-membered ring intermediate to produce the corresponding products. The cooperation effect of the second CO is very weak. The catalytic activities of AuAg^- and AuCu^- toward CO oxidation are stronger than that of Au₂^- . Doping the Au clusters with Ag and Cu increases the catalytic activity. These results are in agreement with the previous experimental results.

Key words: Density functional theory, CO oxidation, Binary copper group cluster anion, Reaction mechanism

HU Jian-Ping, WANG Jun, TANG Dian-Yong, FU Qin-Chao, ZHANG Yuan-Qin. Reaction Mechanisms of CO Oxidation Catalyzed by Binary Copper Group Cluster Anions[J].Acta Phys. -Chim. Sin., 2011, 27(02): 329-336.

References

1 Min, B. K.; Friend, C. M. Chem. Rev. 2007, 107, 2709, and references therein.
2 Zhang, X.; Xu, B. Q. Acta Chim. Sin. 2005, 63, 86.
[张鑫, 徐柏庆. 化学学报, 2005, 63, 86.]
3 Shao, J. J.; Zhang, P.; Song, W.; Huang, X. M.; Xu, Y. D.; Shen, W. J. Acta Chim. Sin. 2007, 65, 2007.
[邵建军, 张平, 宋巍, 黄秀敏, 徐奕德, 申文杰. 化学学报, 2007, 65, 2007.]
4 Chen, M.; Goodman, D. W. Acc. Chem. Res. 2006, 39, 739.
5 Bowker, M. Chem. Soc. Rev. 2008, 37, 2204.
6 Campbell, C. T. Science 2004, 306, 234.
7 Reveles, J. U.; Johnson,G. E.; Khanna, S. N.; Castleman, A. W., Jr. J. Phys. Chem. C 2010, 114, 5438.
8 Xue, W.; Wang, Z. C.; He, S. G.; Xie, Y.; Bernstein, E. R. J. Am. Chem. Soc. 2008, 130, 15879.
9 Wang, A. Q.; Liu, J. H.; Lin, S. D.; Lin, T. S.; Mou, C. Y. J. Catal. 2005, 233, 186.
10 Wang, A. Q.; Chang, C. M.; Mou, C. Y. J. Phys. Chem. B 2005, 109, 18860.
11 Liu, X.; Wang, A. Q.; Wang, X.; Mou, C. Y.; Zhang, T. Chem. Commun. 2008, No. 27, 3187.
12 Yen, C. W.; Lin, M. L.; Wang, A.; Chen, S. A.; Chen, J. M.; Mou, C. Y. J. Phys. Chem. C 2009, 113, 17831.
13 Wang, A. Q.; Hsieh, Y. P.; Chen, Y. F.; Mou, C. Y. J. Catal. 2006, 237, 197.
14 Liu, J. H.; Wang, A. Q.; Chi, Y. S.; Lin, H. P.; Mou, C. Y. J. Phys. Chem. B 2005, 109, 40.
15 Liu, X.; Wang, A. Q.; Yang, X. F.; Zhang, T.; Mou, C. Y.; Su, D. S.; Li, J. J. Chem. Mater. 2009, 21, 410.
16 Wittstock, A.; Neumann, B.; Schaefer, A.; Dumbuya, K.; Kübel, C.; Biener, M. M.; Zielasek, V.; Steinrück, H. P.; Gottfried, J. M.; Biener, J.; Hamza, A.; B?umer, M. J. Phys. Chem. C 2009, 113, 5593.
17 Bernhardt, T. M.; Socaciu-Siebert, L. D.; Hagen, J.; Wöste, L. Appl. Catal. A-Gen. 2005, 291, 170.
18 Mitri?, R.; Burda, J.; Bona?i?-Koutecký, V.; Fantucci, P. Euro. Phys. J. D 2003, 24, 41.
19 Chang, C. M.; Cheng, C.; Wei, C. M. J. Chem. Phys. 2008, 128, 124710.
20 Gao, Y.; Shao, N.; Pei, Y.; Zeng, X. C. Nano Lett. 2010, 10, 1055.
21 Kimble, M. L.; Moore, N. A.; Johnson, G. E.; Castleman, A. W. J. Chem. Phys. 2006, 125, 204311.
22 Tang, D. Y.; Zhang, Y. Q.; Hu, C. W. Acta Chim. Sin. 2008, 66, 1501.
[唐典勇, 张元勤, 胡常伟. 化学学报, 2008, 66, 1501.]
23 Tang, D. Y.; Hu, J. P., Zhang, Y. Q., Hu, C. W. Acta Chim. Sin. 2009, 67, 1859.
[唐典勇, 胡建平, 张元勤, 胡常伟. 化学学报, 2009, 67, 1859.]
24 Dholabhai, P. P.; Wu, X.; Ray, A. K. J. Mol. Struct.-Theochem 2005, 723, 139.
25 Tang, D. Y.; Hu, J. P.; Zhang, Y. Q.; Hu, C. W. Acta Chim. Sin. 2010, 68, 1379.
[唐典勇, 胡建平, 张元勤, 胡常伟. 化学学报, 2010, 68, 1379.]
26 Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; et al. Gaussian 03, Revision E.01; Gaussian Inc.: Pittsburgh, PA, 2004.
27 Couty, M.; Hall, M. B. J. Comput. Chem. 1996, 17, 1359.
28 Ehlers, A. W.; Dapprich, B. S.; Gobbi, A.; Hollwarth, A.; Jonas, V.; Kohler, K. F.; Stegmann, R.; Veldkamp, A.; Frenking, G. Chem. Phys. Lett. 1993, 208, 111.
29 Ojifinni, R. A.; Gong, J.; Froemming, N. S.; Flaherty, D. W.; Pan, M.; Henkelman, G.; Mullins, C. B. J. Am. Chem. Soc. 2008, 130, 11250.
30 Wang, F.; Zhang, D.; Xu, X.; Ding, Y. J. Phys. Chem. C 2009, 113, 18032.

[1]	Fengyu Gao, Hengheng Liu, Xiaolong Yao, Zaharaddeen Sani, Xiaolong Tang, Ning Luo, Honghong Yi, Shunzheng Zhao, Qingjun Yu, Yuansong Zhou. Spherical Mn_xCo_3−xO_4−ƞ Spinel with Mn-Enriched Surface as High-Efficiency Catalysts for Low-Temperature Selective Catalytic Reduction of NO_x by NH₃ [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2212003-0.
[2]	. A DFT Study on S-Scheme Heterojunction Consisting of Pt Single Atom Loaded G-C₃N₄ and BiOCl for Photocatalytic CO₂ Reduction [J]. Acta Phys. -Chim. Sin., 2023, 39(6): 2212026-0.
[3]	Tianjie Wang, Yaowei Wang, Yuhui Chen, Jianpeng Liu, Huibing Shi, Limin Guo, Zhiwei Zhao, Chuntai Liu, Zhangquan Peng. Toward Practical Lithium-Air Batteries by Avoiding Negative Effects of CO₂ [J]. Acta Phys. -Chim. Sin., 2022, 38(8): 2009071-.
[4]	Ruoning Li, Xue Zhang, Na Xue, Jie Li, Tianhao Wu, Zhen Xu, Yifan Wang, Na Li, Hao Tang, Shimin Hou, Yongfeng Wang. Hierarchical Self-Assembly of Ag-Coordinated Motifs on Ag(111) [J]. Acta Phys. -Chim. Sin., 2022, 38(8): 2011060-.
[5]	Haoran Lu, Yaqing Wei, Run Long. Charge Localization Induced by Nanopore Defects in Monolayer Black Phosphorus for Suppressing Nonradiative Electron-Hole Recombination through Time-Domain Simulation [J]. Acta Phys. -Chim. Sin., 2022, 38(5): 2006064-.
[6]	Yishun Yang, Min Zhou, Yanxia Xing. Symmetry-Dependent Transport Properties of γ-Graphyne-based Molecular Magnetic Tunnel Junctions [J]. Acta Phys. -Chim. Sin., 2022, 38(4): 2003004-.
[7]	Xianhong Chen, Pengchao Ruan, Xianwen Wu, Shuquan Liang, Jiang Zhou. Crystal Structures, Reaction Mechanisms, and Optimization Strategies of MnO₂ Cathode for Aqueous Rechargeable Zinc Batteries [J]. Acta Phys. -Chim. Sin., 2022, 38(11): 2111003-.
[8]	Ying Li, Xueqi Lai, Jinpeng Qu, Qinzhi Lai, Tingfeng Yi. Research Progress in Regulation Strategies of High-Performance Antimony-Based Anode Materials for Sodium Ion Batteries [J]. Acta Phys. -Chim. Sin., 2022, 38(11): 2204049-.
[9]	Mengting Li, Xingqun Zheng, Li Li, Zidong Wei. Research Progress of Hydrogen Oxidation and Hydrogen Evolution Reaction Mechanism in Alkaline Media [J]. Acta Phys. -Chim. Sin., 2021, 37(9): 2007054-.
[10]	Peng Chen, Ying Zhou, Fan Dong. Advances in Regulation Strategies for Electronic Structure and Performance of Two-Dimensional Photocatalytic Materials [J]. Acta Phys. -Chim. Sin., 2021, 37(8): 2010010-.
[11]	Xingang Fei, Haiyan Tan, Bei Cheng, Bicheng Zhu, Liuyang Zhang. 2D/2D Black Phosphorus/g-C₃N₄ S-Scheme Heterojunction Photocatalysts for CO₂ Reduction Investigated using DFT Calculations [J]. Acta Phys. -Chim. Sin., 2021, 37(6): 2010027-.
[12]	Dong Liu, Shengtao Chen, Renjie Li, Tianyou Peng. Review of Z-Scheme Heterojunctions for Photocatalytic Energy Conversion [J]. Acta Phys. -Chim. Sin., 2021, 37(6): 2010017-.
[13]	Yunfei Wang, Jianhua Liu, Mei Yu, Jinyan Zhong, Qisen Zhou, Junming Qiu, Xiaoliang Zhang. SnO₂ Surface Halogenation to Improve Photovoltaic Performance of Perovskite Solar Cells [J]. Acta Phys. -Chim. Sin., 2021, 37(3): 2006030-.
[14]	Junjie Shi, Ziqi Hu, Yihao Yang, Yuxiang Bu, Zujin Shi. Stability and Formation Mechanism of Endohedral Metal Carbonitride Clusterfullerenes [J]. Acta Phys. -Chim. Sin., 2021, 37(10): 1907077-.
[15]	Xuezhu Xiao, Xiaofang Cao, Dongbo Zhao, Chunying Rong, Shubin Liu. Quantification of Molecular Basicity for Amines: a Combined Conceptual Density Functional Theory and Information-Theoretic Approach Study [J]. Acta Physico-Chimica Sinica, 2020, 36(11): 1906034-.

Reaction Mechanisms of CO Oxidation Catalyzed by Binary Copper Group Cluster Anions

PDF

Like

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Metrics

Recommended 0