运用广义梯度密度泛函理论结合周期性平板模型方法研究了N2O在完整及负载Cu的四方相ZrO2(101)表面的吸附与解离.结果表明, N2O在完整ZrO2(101)表面的吸附均为物理吸附, Cu在其完整表面的次表层第一氧位为最稳定吸附位,且覆盖度为0.25 ML时的吸附最为稳定,吸附能为155.8 kJ/mol; N2O分子中O端弱物理吸附于Cu/ZrO2(101)表面,其N端及平行吸附方式得到的稳定吸附能分别为121.6和66.8 kJ/mol.频率及电荷布居计算表明,吸附后对称和反对称伸缩振动频率均发生红移,电子由Cu负载底物表面转移给N2O分子.对N2O分子的解离考虑了N端垂直吸附和平行吸附两种解离反应过程,发现平行吸附过程的解离更易发生.
参考文献
| [1] | Thiemens M H;Trogler W C .[J].Science,1991,251:932. |
| [2] | Kapteijn F;Rodriguez-Mirasol J;Moulijn J A .[J].Applied Catalysis B:Environmental,1996,9:25. |
| [3] | Dickinson R E;Cicerone R J .[J].Nature,1986,319:109. |
| [4] | Arai N .[J].Journal of the Institute of Energy,1994,67:61. |
| [5] | Satsuma A;Maeshima H;Watanabe K;Hattori T .[J].Energy Conversion and Management,2001,42:1997. |
| [6] | Perez-Ramirez, J .Prospects of N2O emission regulations in the European fertilizer industry[J].Applied Catalysis. B, Environmental,2007(26):31-35. |
| [7] | Russo N;Mescia D;Fino D;Saracco G;Specchia V .N2O decomposition over perovskite catalysts[J].Industrial & Engineering Chemistry Research,2007(12):4226-4231. |
| [8] | Martinez A;Goursot A;Coq B;Delahay G .[J].Journal of Physical Chemistry B,2004,108:8823. |
| [9] | Shimizu A;Tanaka K;Fujimori M .[J].Chemosphere-Global Change Science,2000,2:425. |
| [10] | Centi G;Generali P;dall'Olio L;Perathoner S Rak Z .[J].Industrial and Engineering Chemistry Research,2000,39:131. |
| [11] | Wójtowicz M A;Miknis F P;Grimes R W;Smith W W Se-rio M A .[J].Journal of Hazardous Materials,2000,74:81. |
| [12] | Shen Q;Li L D;Li J J;Tian H Hao Z P .[J].Journal of Hazardous Materials,2009,163:1332. |
| [13] | Asano K;Ohnishi C;Iwamoto S;Shioya Y;Inoue M .Potassium-doped CO3O4 catalyst for direct decomposition of N2O[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2008(3/4):242-249. |
| [14] | Ito T;Wang J X;Lin C H;Lunsford J H .[J].Journal of the American Chemical Society,1985,107:5062. |
| [15] | Russo N;Mescia D;Fino D;Saracco G;Specchia V .N2O decomposition over perovskite catalysts[J].Industrial & Engineering Chemistry Research,2007(12):4226-4231. |
| [16] | Nakamura M;Mitsuhashi H;Takezawa N .[J].Journal of Catalysis,1992,138:686. |
| [17] | Nakamura M;Fujita S;Takezawa N .[J].Catalysis Letters,1992,14:315. |
| [18] | Yamamoto H;Chu H Y;Xu M T;Shi C L Lunsford J H .[J].Journal of Catalysis,1993,142:325. |
| [19] | Hutchings G J;Scurrell M S;Woodhouse J R .[J].Chemical Society Reviews,1989,18:251. |
| [20] | Heyden A;Peters B;Bell A T;Keil F J .[J].Journal of Physical Chemistry B,2005,109:1857. |
| [21] | Nakamura M;Yanagibashi H;Mitsuhashi H;Takezawa N .[J].Bulletin of the Chemical Society of Japan,1993,66:2467. |
| [22] | Li Y J;Armor J N .[J].Applied Catalysis B:Environmental,1992,1:L21. |
| [23] | Ma Z Y;Yang C;Wei W;Li W H Sun Y H .[J].Journal of Molecular Catalysis A:Chemical,2005,227:119. |
| [24] | Centi G;Cerrato G;D'Angelo S;Finardi U Giamello E Morterra C Perathoner S .[J].Catalysis Today,1996,27:265. |
| [25] | Sun Y H;Sermon P A.[J].Journal of the Chemical Society,Chemical Communications,1993:1242. |
| [26] | Bianchi D;Chafik T;Khalfallah M;Teichner S J .[J].Applied Catalysis A:General,1994,112:219. |
| [27] | Ma Z Y;Xu R;Yang C;Dong Q N Wei W Sun Y H .[J].Studies in Surface Science and Catalysis,2004,147:625. |
| [28] | Saito M;Murata K .[J].Catalysis Surveys From Asia,2004,8:285. |
| [29] | Ko J B;Bae C M;Jung Y S;Kim D H .[J].Catalysis Letters,2005,105:157. |
| [30] | Ma ZY;Yang C;Wei W;Li WH;Sun YH .Catalytic performance of copper supported on zirconia polymorphs for CO hydrogenation[J].Journal of molecular catalysis, A. Chemical,2005(1/2):75-81. |
| [31] | Fellah M F;Pidko E A;van Santen R A;Onal I .[J].Journal of Physical Chemistry C,2011,115:9668. |
| [32] | Orita H;Kubo T;Matsushima T;Kokalj A .[J].Journal of Physical Chemistry C,2010,114:21444. |
| [33] | Stelmachowski P;Zasada F;Piskorz W;Kotarba A Paul J-F Sojka Z .[J].Catalysis Today,2008,137:423. |
| [34] | Zhang B;Lu Y A;He H;Wang J G Zhang C B Yu Y B Xue L .[J].Journal of Environmental Science,2011,23:681. |
| [35] | Manzhos S;Yamashita K .[J].Surface Science,2010,604:555. |
| [36] | Lü Y A;Zhuang G L;Wang J G;Jia Y B Xie Q .[J].Physical Chemistry Chemical Physics,2011,13:12472. |
| [37] | Hofmann A;Clark S J;Oppel M;Hahndorfk I .[J].Physical Chemistry Chemical Physics,2002,4:3500. |
| [38] | 曾庆松,陈文凯,戴文新,章永凡,李奕,郭欣.密度泛函理论研究CO和O_2在NiFeB_2/TiO_2表面的吸附[J].催化学报,2010(04):423-428. |
| [39] | 杜玉栋,郭欣,陈文凯,李奕,章永凡.甲醛在FeS2（100）完整与S-缺陷表面吸附的理论研究[J].催化学报,2011(06):1046-1050. |
| [40] | Du Y D;Chen W K;Zhang Y F;Guo X .[J].Journal of Natural Gas Chemistry,2011,20:60. |
| [41] | Delly B .[J].Journal of Chemical Physics,1990,92:508. |
| [42] | Delly B .[J].Journal of Chemical Physics,2000,113:7756. |
| [43] | Delly B .[J].Journal of Physical Chemistry,1996,100:6107. |
| [44] | Perdew J P;Wang Y .[J].Physical Review B:Condensed Matter,1992,45:13244. |
| [45] | Lide D R.CRC Handbook of Chemistry and Physics[M].Boca Raton:crc Press,2003:9. |
| [46] | Fellah M F;van Santen R A;Onal I .[J].Journal of Physical Chemistry C,2009,113:15307. |
| [47] | Walter E J;Lewis S P;Rappe A M .[J].Surface Science,2001,495:44. |
| [48] | Tang Q L;Liu Z P .[J].Journal of Physical Chemistry C,2010,114:8423. |
| [49] | Yang Y L;Chen W K;Guo X;Li Y Zhang Y F .[J].Chinese Journal of Structural Chemistry,2010,29:1021. |
| [50] | Wu, S.-Y.;Su, C.-H.;Chang, J.-G.;Chen, H.-T.;Hou, C.-H.;Chen, H.-L. .Adsorption and dissociation of N_2O molecule on Fe(1 1 1) surface: A DFT study[J].Computational Materials Science,2011(12):3311-3314. |
| [51] | Sun B Z;Chen W K;Wang X;Lu C H .[J].Applied Surface Science,2007,253:7501. |
| [52] | Herzberg G.Infrared and Raman Spectra and Molecular Structure[M].New York:D.Van Nostrand Company,Inc,1945 |
| [53] | Plíva J .[J].Journal of Molecular Spectroscopy,1964,12:360. |
| [54] | Ohno Y;Kimura K;Bi M;Matsushima T .[J].Journal of Chemical Physics,1999,110:8221. |
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