Citation: YIN Yueqi, JIANG Mengxu, LIU Chunguang. DFT Study of POM-Supported Single Atom Catalyst (M₁/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-) for Activation of Nitrogen Molecules[J]. Acta Physico-Chimica Sinica, ;2018, 34(3): 270-277. doi: 10.3866/PKU.WHXB201707071 shu

DFT Study of POM-Supported Single Atom Catalyst (M₁/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-) for Activation of Nitrogen Molecules

Institute of Functional Material Chemistry, College of Chemical Engineering, Northeast Electric Power University, Jilin 132012, Jilin Province, P. R. China

Corresponding author: LIU Chunguang, liucg407@163.com
Received Date: 22 May 2017
Revised Date: 30 June 2017
Accepted Date: 30 June 2017
Available Online: 7 March 2017
Fund Project: The project was supported by the Natural Science Foundation of China (21373043)the Natural Science Foundation of China 21373043

Molecular geometries, electronic structure, and infrared spectroscopy of a series of polyoxometalate (POM)-supported single atom catalyst (SACs) (M₁/POM (M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-) have been studied based on density factional theory (DFT) combined with natural bond orbital (NBO) analysis method. The results show that Pt₁/POM has a higher reactivity for activation of N₂ relevant to the others. The interaction between the isolated Pt atom and N₂ arises from an orbital mixture, which is formed by the d_xz and d_yz orbital of Pt atom and the π* anti-bond orbit of N₂ molecule. The electron transfer from Pt atom to the nitrogen molecule leads to a weakened N≡N bond. The N≡N bond distance increases when compared with the free N₂ molecule. All results indicate an effective activation of the nitrogen molecules. For DFT-derived IR spectra, the four characteristic peaks of Keggin-type POM split into five because of introduction of the isolated metal atom.
- Single atom catalyst,
- Artificial nitrogen fixation,
- Density functional theory,
- Electronic structure,
- Infrared spectroscopy
1. [1]
  Burris, R. H. J. Biol. Chem. 1991, 266, 9339.
2. [2]
  Shah, V. K.; Brill, W. J. Proc. Natl. Acad. Sci. U. S. A. 1977, 74, 3249. doi: 10.1073/pnas.0507853103 doi: 10.1073/pnas.0507853103
3. [3]
  Chakrabarti, P.; Woo, D.; Kornuc, J. J.; Rees, D. C. Science 1992, 257, 1653. doi: 10.1126/science.1529353 doi: 10.1126/science.1529353
4. [4]
  Kirn, J.; Rees, D. C. Nature 1992, 360, 553. doi: 10.1038/360553a0 doi: 10.1038/360553a0
5. [5]
  Kirn, J.; Rees, D. C. Science 1992, 257, 1677. doi: 10.1126/science.1529354 doi: 10.1126/science.1529354
6. [6]
  Chan, M. K.; Kirn, J.; Rees, D. C. Science1993, 260, 792. doi: 10.1126/science.8484118 doi: 10.1126/science.8484118
7. [7]
  Kirn, J.; Woo, D.; Rees, D. C. Biochemistry1993, 32, 7104. doi: 10.1021/bi00079a006 doi: 10.1021/bi00079a006
8. [8]
  Kirn, J.; Rees, D. C. Biochemistry 1994, 33, 389. doi: 10.1021/bi00168a001 doi: 10.1021/bi00168a001
9. [9]
  Jia, H. P.; Quadrelli, E. A. Chem. Soc. Rev. 2014, 43, 547. doi: 10.1039/c3cs60206k doi: 10.1039/c3cs60206k
10. [10]
  MacKay, B. A.; Fryzuk, M. D. Chem. Rev. 2004, 104, 385. doi: 10.1021/cr020610c doi: 10.1021/cr020610c
11. [11]
  Yandulov, D. V.; Schrock, R. R. Science 2003, 301, 76. doi: 10.1126/science.1085326 doi: 10.1126/science.1085326
12. [12]
  Arashiba, K.; Miyake, Y.; Nishibayashi, Y. Nat. Chem. 2011, 3, 120. doi: 10.1038/nchem.906 doi: 10.1038/nchem.906
13. [13]
  Anderson, J. S.; Rittle, J.; Peters, J. C. Nature 2013, 501, 84. doi: 10.1038/nature12435 doi: 10.1038/nature12435
14. [14]
  Allen, A. D.; Harris, R. O.; Loescher, B. R.; Stevens, J. R.; Whiteley, R. N. Chem. Rev. 1973, 73, 11. doi: 10.1021/cr60281a002 doi: 10.1021/cr60281a002
15. [15]
  Hoffman, B. M.; Lukoyanov, D.; Yang, Z. Y.; Dean, D. R.; Seefeldt, L. C. Chem. Rev. 2014, 114, 4041. doi: 10.1021/cr400641x doi: 10.1021/cr400641x
16. [16]
  Qiao, B.; Wang, A.; Yang, X.; Allard, L. F.; Jiang, Z.; Cui, Y.; Liu, J.; Li, J.; Zhang, T. Nat. Chem. 2011, 3, 634. doi: 10.1038/nchem.1095 doi: 10.1038/nchem.1095
17. [17]
  Yang, X. F.; Wang, A.; Qiao, B.; Li, J.; Liu, J.; Zhang, T. Acc. Chem. Res. 2013, 46, 1740. doi: 10.1021/ar300361m.Epub 2013 Jul1 doi: 10.1021/ar300361m.Epub2013Jul1
18. [18]
  Thomas, J. M. Nature2015, 525, 325. doi: 10.1038/525325a doi: 10.1038/525325a
19. [19]
  Liu, J. ACS Catal.2017, 7, 34. doi: 10.1021/acscatal.6b01534 doi: 10.1021/acscatal.6b01534
20. [20]
  Wei, H.; Liu, X. Y.; Wang, A.; Zhang, L.; Qiao, B. T.; Yang, Y. F.; Huang, Y. Q.; Miao, S.; Liu, J.; Zhang, T. Nat. Commun. 2013, 5, 5634. doi: 10.1038/ ncomms6634 doi: 10.1038/ncomms6634
21. [21]
  Liu, P.; Zhao, Y.; Qin, R.; Mo, S.; Chen, G.; Gu, L.; Chevrier, D. M.; Zhang, P.; Guo, Q.; Zang, D.; Wu, B.; Fu, G.; Zheng, N. Science 2016, 352, 797. doi: 10.1126/science.aaf5251 doi: 10.1126/science.aaf5251
22. [22]
  Katsoulis, D. E. Chem. Rev. 1998, 98, 359. doi: 10.1021/cr960398a doi: 10.1021/cr960398a
23. [23]
  Dolbecq, A.; Dumas, E.; Mayer, C. R.; Mialane, P. Chem. Rev. 2010, 110, 6009. doi: 10.1021/cr1000578 doi: 10.1021/cr1000578
24. [24]
  Hill, C. L. Chem. Rev.1998, 98, 1. doi: 10.1021/cr960395y doi: 10.1021/cr960395y
25. [25]
  Izarova, N. V.; Pope, M. T.; Kortz, U. Angew. Chem., Int. Ed. 2012, 51, 2. doi: 10.1038/srep25154 doi: 10.1038/srep25154
26. [26]
  Dablemont, C.; Hamaker, C. G.; Thouvenot, R.; Sojka, Z.; Che, M.; Maatta, E. A.; Proust, A. Chem. -Eur J. 2006, 12, 9150. doi: 10.1002/chem.200600934 doi: 10.1002/chem.200600934
27. [27]
  Besson, C.; Musaev, D. G.; Lahootun, V.; Cao, R.; Chamoreau, L. M.; Villanneau, R.; Villain, F.; Thouvenot, R.; Geletii, Y. V.; Hill, C. L.; Proust, A. Chem. Eur. J. 2009, 15, 10233. doi: 10.1002/chem.200900965 doi: 10.1002/chem.200900965
28. [28]
  Lahootun, V.; Besson, C.; Villanneau, R.; Villain, F.; Chamoreau, L. M.; Boubekeur, K.; Blanchard, S.; Thouvenot, R.; Proust, A. J. Am. Chem. Soc. 2007, 129, 7127. doi: 0.1021/ja071137t
29. [29]
  Sokolov, M. N.; Adonin, S. A.; Mainichev, D. A.; Sinkevich, P. L.; Vicent, C.; Kompankov, N. B.; Gushchin, A. L.; Nadolinny, V. A.; Fedin, V. P. Inorg. Chem. 2013, 52, 9675. doi: 10.1021/ic401492q doi: 10.1021/ic401492q
30. [30]
  Liu, C. G.; Liu, S.; Zheng, T. Inorg. Chem. 2015, 54, 7929. doi: 10.1021/acs.inorgchem.5b01002 doi: 10.1021/acs.inorgchem.5b01002
31. [31]
  Coperet, C.; Comas-Vives, A.; Conley, M. P.; Estes, D. P.; Fedorov, A.; Mougel, V.; Nagae, H.; Nunez-Zarur, F.; Zhizhko, P. A. Chem. Rev. 2016, 116, 323. doi: 10.1002/chin.201615211 doi: 10.1002/chin.201615211
32. [32]
  Zhang, B.; Asakura, H.; Zhang, J.; Zhang, J.; De, S.; Yan, N. Angew. Chem. Int. Ed. 2016, 55, 8319–8323. doi: 10.1002/anie.201602802 doi: 10.1002/anie.201602802
33. [33]
  Zhang, B.; Asakura, H.; Yan, N. Ind. Eng. Chem. Res. 2017, 56, 3578. doi: 10.1021/acs.iecr.7b00376 doi: 10.1021/acs.iecr.7b00376
34. [34]
  Zhao, Y.; Truhlar, D. G.J. Chem. Phys. 2006, 125, 194101. doi: 10.1063/1.2370993 doi: 10.1063/1.2370993
35. [35]
  Hay, P. J.; Wadt, W. R. J. Chem. Phys. 1985, 82, 270. doi: 10.1063/1.448799 doi: 10.1063/1.448799
36. [36]
  Hay, P. J.; Wadt, W. R. J. Chem. Phys. 1985, 82, 299. doi: 10.1063/1.448975 doi: 10.1063/1.448975
37. [37]
  Tomasi, J.; Mennucci, B.; Cammi, R. Chem. Rev. 2005, 105, 2999. doi: 10.1021/cr9904009 doi: 10.1021/cr9904009
38. [38]
  Glendening, A. E.; Carpenter, J. E.; Weinhold, F. NBO Version 3.1.
39. [39]
  Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; et al. Gaussian 09, Revision D.01; Gaussian, Inc.: Wallingford, CT, 2009.
40. [40]
  Zhang, B.; Asakura, H.; Zhang, J.; Zhang, I.; De, S.; Yan, N. Angew. Chem. Int. Ed. 2016, 55, 1. doi: 10.1002/anie.201602801 doi: 10.1002/anie.201602801
1. [1]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
2. [2]
  Zhenming Xu , Mingbo Zheng , Zhenhui Liu , Duo Chen , Qingsheng Liu . Experimental Design of Project-Driven Teaching in Computational Materials Science: First-Principles Calculations of the LiFePO₄ Cathode Material for Lithium-Ion Batteries. University Chemistry, 2024, 39(4): 140-148. doi: 10.3866/PKU.DXHX202307022
3. [3]
  Xiaochen Zhang , Fei Yu , Jie Ma . 多角度数理模拟在电容去离子中的前沿应用. Acta Physico-Chimica Sinica, 2024, 40(11): 2311026-. doi: 10.3866/PKU.WHXB202311026
4. [4]
  Kun WANG , Wenrui LIU , Peng JIANG , Yuhang SONG , Lihua CHEN , Zhao DENG . Hierarchical hollow structured BiOBr-Pt catalysts for photocatalytic CO₂ reduction. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1270-1278. doi: 10.11862/CJIC.20240037
5. [5]
  Maitri Bhattacharjee , Rekha Boruah Smriti , R. N. Dutta Purkayastha , Waldemar Maniukiewicz , Shubhamoy Chowdhury , Debasish Maiti , Tamanna Akhtar . Synthesis, structural characterization, bio-activity, and density functional theory calculation on Cu(Ⅱ) complexes with hydrazone-based Schiff base ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1409-1422. doi: 10.11862/CJIC.20240007
6. [6]
  Asif Hassan Raza , Shumail Farhan , Zhixian Yu , Yan Wu . 用于高效制氢的双S型ZnS/ZnO/CdS异质结构光催化剂. Acta Physico-Chimica Sinica, 2024, 40(11): 2406020-. doi: 10.3866/PKU.WHXB202406020
7. [7]
  Fei Xie , Chengcheng Yuan , Haiyan Tan , Alireza Z. Moshfegh , Bicheng Zhu , Jiaguo Yu . d带中心调控过渡金属单原子负载COF吸附O₂的理论计算研究. Acta Physico-Chimica Sinica, 2024, 40(11): 2407013-. doi: 10.3866/PKU.WHXB202407013
8. [8]
  Wei Zhong , Dan Zheng , Yuanxin Ou , Aiyun Meng , Yaorong Su . K原子掺杂高度面间结晶的g-C₃N₄光催化剂及其高效H₂O₂光合成. Acta Physico-Chimica Sinica, 2024, 40(11): 2406005-. doi: 10.3866/PKU.WHXB202406005
9. [9]
  Jizhou Liu , Chenbin Ai , Chenrui Hu , Bei Cheng , Jianjun Zhang . 六氯锡酸铵促进钙钛矿太阳能电池界面电子转移及其飞秒瞬态吸收光谱研究. Acta Physico-Chimica Sinica, 2024, 40(11): 2402006-. doi: 10.3866/PKU.WHXB202402006
10. [10]
  Wenlong LI , Xinyu JIA , Jie LING , Mengdan MA , Anning ZHOU . Photothermal catalytic CO₂ hydrogenation over a Mg-doped In₂O_3-x catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 919-929. doi: 10.11862/CJIC.20230421
11. [11]
  Xuyang Wang , Jiapei Zhang , Lirui Zhao , Xiaowen Xu , Guizheng Zou , Bin Zhang . Theoretical Study on the Structure and Stability of Copper-Ammonia Coordination Ions. University Chemistry, 2024, 39(3): 384-389. doi: 10.3866/PKU.DXHX202309065
12. [12]
  Juntao Yan , Liang Wei . 2D S-Scheme Heterojunction Photocatalyst. Acta Physico-Chimica Sinica, 2024, 40(10): 2312024-. doi: 10.3866/PKU.WHXB202312024
13. [13]
  Yuanyin Cui , Jinfeng Zhang , Hailiang Chu , Lixian Sun , Kai Dai . Rational Design of Bismuth Based Photocatalysts for Solar Energy Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2405016-. doi: 10.3866/PKU.WHXB202405016
14. [14]
  Dan Li , Hui Xin , Xiaofeng Yi . Comprehensive Experimental Design on Ni-based Catalyst for Biofuel Production. University Chemistry, 2024, 39(8): 204-211. doi: 10.3866/PKU.DXHX202312046
15. [15]
  Quanliang Chen , Zhaohui Zhou . Research on the Active Site of Nitrogenase over Fifty Years. University Chemistry, 2024, 39(7): 287-293. doi: 10.3866/PKU.DXHX202310133
16. [16]
  Zhanggui DUAN , Yi PEI , Shanshan ZHENG , Zhaoyang WANG , Yongguang WANG , Junjie WANG , Yang HU , Chunxin LÜ , Wei ZHONG . Preparation of UiO-66-NH₂ supported copper catalyst and its catalytic activity on alcohol oxidation. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 496-506. doi: 10.11862/CJIC.20230317
17. [17]
  Juan WANG , Zhongqiu WANG , Qin SHANG , Guohong WANG , Jinmao LI . NiS and Pt as dual co-catalysts for the enhanced photocatalytic H₂ production activity of BaTiO₃ nanofibers. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1719-1730. doi: 10.11862/CJIC.20240102
18. [18]
  Yonghui ZHOU , Rujun HUANG , Dongchao YAO , Aiwei ZHANG , Yuhang SUN , Zhujun CHEN , Baisong ZHU , Youxuan ZHENG . Synthesis and photoelectric properties of fluorescence materials with electron donor-acceptor structures based on quinoxaline and pyridinopyrazine, carbazole, and diphenylamine derivatives. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 701-712. doi: 10.11862/CJIC.20230373
19. [19]
  Guoxian Zhu , Jing Chen , Rongkai Pan . Enhancing the Teaching Quality of Atomic Structure: Insights and Strategies. University Chemistry, 2024, 39(3): 376-383. doi: 10.3866/PKU.DXHX202305027
20. [20]
  Jin Jia , Shangda Jiang . Is the z Axis Special in Atomic Structure?. University Chemistry, 2024, 39(6): 400-404. doi: 10.12461/PKU.DXHX202403091

Get Citation

PDF

XML

Metrics

PDF Downloads(20)
Abstract views(349)
HTML views(21)

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

DFT Study of POM-Supported Single Atom Catalyst (M1/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW12O40]3-) for Activation of Nitrogen Molecules

Metrics

通讯作者: 陈斌, bchen63@163.com

DFT Study of POM-Supported Single Atom Catalyst (M₁/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-) for Activation of Nitrogen Molecules