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La-O小团簇上超氧物种与过氧物种间的连接途径
DOI: 10.1016/S1872-2067(12)60694-9
Keywords: 氧 ,超氧 ,过氧 ,氧化镧 ,密度泛函理论
Abstract:
？采用密度泛函理论方法考察了La-O团簇上超氧物种与过氧物种间转化的连接途径.单重态下,团簇上单个超氧物种可通过一系列臭氧物种转化为过氧物种,且转化能垒较高;三重态下,单个超氧物种则并无与过氧物种间连接的途径.然而,La-O团簇上两超氧物种间的相互作用及其转化也具单重态和三重态两条途径.三重态下,超氧物种可很容易地转化为过氧物种(O2-+O2-？O22-+O2),超氧物种与过氧物种处于快速的交换状态之中;单重态下,超氧物种转化为过氧物种则需较高的活化能垒,表明在单重态下这些氧物种具有较高的稳定性.
References
[1 ] Zanthoff H W, Buchholz S A, Pantazidis A, Mirodatos C. Chem Eng Sci, 1999, 54: 4397 [2 ] Ferreira V J, Tavares P, Figueiredo J L, Faria J L. Ind Eng Chem Res, 2012, 51: 10535 [3 ] Wan H L, Zhou X P, Weng W Z, Long R Q, Chao Z S, Zhang W D, Chen M S, Luo J Z, Zhou S Q. Catal Today, 1999, 51: 161 [4 ] Shvets V A, Vorotyntsev V M, Kazanskii V B. Kinet Katal, 1969, 10: 356 [5 ] Kazanskii V B. Kinet Katal, 1977, 18: 43 [6 ] Au C T, He H, Lai S Y, Ng C F. J Catal, 1996, 163: 399 [7 ] Palmer M S, Neurock M, Olken M M. J Am Chem Soc, 2002, 124: 8452 [8 ] Valentin C D, Pacchioni G, Abbet S, Heiz U. J Phys Chem B, 2002, 106: 7666 [9 ] Louis C, Chang T L, Kermarec M, Le Van T, Tatibouet J M, Che M. Catal Today, 1992, 13: 283 [10 ] Louis C, Chang T L, Kermarec M, Le Van T, Tatibouet J M, Che M. Colloids Surf A, 1993, 72: 217 [11 ] Diwald O, Knozinger E. J Phys Chem B, 2002, 106: 3495 [12 ] Fujita S, Suzuki K, Ohkawa M, Mori T, Iida Y, Miwa Y, Masuda H, Shimada S. Chem Mater, 2003, 15: 255 [13 ] Chen H Y, El-Malki E M, Wang X, van Santen R A, Sachtler W M H. J Mol Catal A, 2000, 162: 159 [14 ] El-Malki E M, Werst D, Doan P E, Sachtler W M H. J Phys Chem B, 2000, 104: 5924 [15 ] Cotton F A, Wilkinson G, Murillo C A, Bochmann M. Advanced Inorganic Chemistry. Sixth ed. New York: John Wiley & Sons, 1999. 465-471 [16 ] Gao Z X, Kim H S, Sun Q, Stair P C, Sachtler W M H. J Phys Chem B, 2001, 105: 6186 [17 ] Willson S P, Andrews L. J Phys Chem A, 1999, 103: 3171 [18 ] Wang Z C, Yin S, Bernstein E R. J Phys Chem A, 2013, 117: 2294 [19 ] Frisch M J, Trucks G W, Schlegel H B, Scuseria G E, Robb M A, Cheeseman J R, Zakrzewski V G, Montgomery J A, Jr., Stratmann R E, Burant J C, Dapprich S, Millam J M, Daniels A D, Kudin K N, Strain M C, Farkas O, Tomasi J, Barone V, Cossi M, Cammi R, Mennucci B, Pomelli C, Adamo C, Clifford S, Ochterski J, Petersson G A, Ayala P Y, Cui Q, Morokuma K, Malick D K, Rabuck A D, Raghavachari K, Foresman J B, Cioslowski J, Ortiz J V, Stefanov B B, Liu G, Liashenko A, Piskorz P, Komaromi I, Gomperts R, Martin R L, Fox D J, Keith T, Al-Laham M A, Peng C Y, Nanayakkara A, Gonzalez C, Challacombe M, Gill P M W, Johnson B G, Chen W, Wong M W, Andres J L, Head-Gordon M, Replogle E S, Pople J A. Gaussian 98, revision A.11, 1998, Gaussian, Inc. [20 ] Vosko S H, Wilk L, Nusair M. Can J Phys, 1980, 58: 1200 [21 ] Becke A D. J Chem Phys, 1993, 98: 5648 [22 ] Perdew J P, Wang Y. Phys Rev B, 1992, 45: 13244 [23 ] Hay P J, Wadt W R. J Chem Phys, 1985, 82: 299 [24 ] Hehre W J, Ditchfield R, Pople J A. J Chem Phys, 1972, 56: 2257 [25 ] Krupenie P H. J Phys Chem Ref Data, 1972, 1: 423 [26 ] Fourier R, De Pristo A E. J Chem Phys, 1992, 96: 1183 [27 ] Shimanouchi T. Table of Molecular Vibrational Frequencies, Consolidated Vol. 1 National Standard Reference Data Series 39. Washington, D C: National Bureau of Standards, 1972 [28 ] Weng W Z, Wan H L, Li J M, Cao Z X. Angew Chem Int Ed, 2004, 43: 975 [29 ] Jing X L, Chen Q C, He C, Zhu X Q, Weng W Z, Xia W S, Wan H L. Phys Chem Chem Phys, 2012, 14: 6898 [30 ] Huacuja R, Graham D J, Fafard C M, Chen C H, Foxman B M, Herbert D E, Alliger G, Thomas C M, Ozerov O V. J Am Chem Soc, 2011, 133: 3820 [31 ] Cho J, Woo J, Nam W. J Am Chem Soc, 2010, 132: 5958 [32 ] Osada Y, Koike S, Fukushima T, Ogasawara S, Shikada T, Ikariya T. Appl Catal, 1990, 59: 59 [33 ] Hermans I, Spier E S, Neuenschwander U, Turra N, Baiker A. Top Catal, 2009, 52: 1162 [34 ] Xia W, Li J H, Weng W Z, Wan H L. Chem Phys Lett, 2006, 423: 427 [35 ] Ervin K M, Anusiewicz I, Skurski P, Simons J, Lineberger W C. J Phys Chem A, 2003, 107: 8521 [36 ] Kantorovich L N, Gillan M J. Surf Sci, 1997, 374: 373
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