Cu/N表面沉积共掺杂TiO2光催化剂作用机理的理论研究

李宗宝; 王霞; 樊帅伟

doi:10.7498/aps.63.157102

摘要

本文采用基于周期性密度泛函理论研究了Cu/N表面沉积共掺杂对锐钛矿相TiO2（001）面的修饰作用. 计算了Cu在不同位置掺杂TiO2（101）面和（001）面的形成能，并在此基础上计算N不同位置掺杂TiO2（001）面及Cu/TiO2（001）面的形成能，通过形成能的比较获得了表面共掺杂的最优化结构. 在此基础上计算了最稳定结构的能带结构及态密度，并与S单掺杂TiO2（001）面最稳定结构进行了对比. 通过对结果的分析发现：Cu/N在（001）表面的沉积共掺杂有效降低了TiO2 的禁带宽度，并在表面形成CuO2 相，更利于提高其光催化活性.

关键词:

Abstract

First principles density functional theory calculations are carried out to investigate the interactions between implanted copper and nitrogen atoms at the anatase TiO2 (001) surface. The doped configurations and formation energies of Cu on TiO2 (001) and TiO2 (101) surfaces, N on TiO2 (001) and Cu/TiO2 (001) surfaces have been considered, and the perfected structures are obtained. Compared with the S/TiO2 (001) perfected structure, the analyses of the band structure and density of states of Cu/N-TiO2 (001) show that the band gap is decreased obviously when the CuO2 state occurrs; this could improve the photocatalytic activity significantly.

Keywords:

作者及机构信息

1.
铜仁学院物理与应用工程系, 贵州省教育厅材料制备新技术和与应用特色重点实验室, 铜仁 554300;

2.
铜仁学院生物与化学工程系, 铜仁 554300;

3.
三峡大学理学院, 宜昌 443002

基金项目: 贵州省教育厅自然科学基金重点项目（批准号：黔教合KY字[2013]182号）和贵州省自然科学基金（批准号：黔科合J字LKT[2012]17号）资助的课题.

Authors and contacts

1.
Department of Physics and Application Engineering & Key Laboratory of New Material Manufacture and Application, the Department of Education of Guizhou Province, Tongren University, Tongren 554300, China;

2.
Department of Biological and Chemical Engineering, Tongren University 554300, China;

3.
College of Science, China Three Gorges University, Yichang 443002, China

Funds: Project supported by the Natural Science Foundation of Guizhou Province, China (Grant Nos. KY[2013]182, LKT[2012]17).

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施引文献

[1]	Wang P, Grätze M 2003 Nat. Mater. 21 402
[2]
[3]	Hagfeldt A, Grätzel M 1995 Chem. Rev. 95 49
[4]
[5]	Mills A, Hunte S L 1997 J. Photoch. Photobio. A 08 1
[6]
[7]
[8]	Li Z B, Wang X, Jia L C, Chi B 2014 J. Mol. Str. 1061 160
[9]
[10]	Yang K S, Dai Y, Huang B B 2009 Chem. Phys. Chem. 10 2327
[11]	Zhu Y T, Wei W, Dai Y, Huang B B 2012 Appl. Surf. Sci. 258 4806
[12]
[13]	Wang Y J, Wang C Y, Wang S Y 2013 Chin. Phys. B 03 364
[14]
[15]	Li W, Wei S H, Duan X M 2014 Chin. Phys. B 02???? 465
[16]
[17]	Maeda M, Yamada T 2007 J. Phys.:Conf. Ser. 61 755
[18]
[19]
[20]	Sreethawong T, Yoshikawa S 2005 Photocatalys. Catal. Commun. 6 661
[21]
[22]	Rodríguez J A, Evans J, Graciano J, Park J B, Liu P, Hrbek J, Sanz J F 2009 J. Phys. Chem. C 113 7364
[23]
[24]	Karunakaran C, Abiramasundari G, Gomathisankar P 2010 J. Colloid Interf. Sci. 352 68
[25]	Zhao X W, Xi H P, Liao Q W 2013 Acta Phys. -Chim. Sin. 29 2232
[26]
[27]
[28]	Li Z B, Wang X, Jia L C 2013 Acta Phys. Sin. 62 203103 [李宗宝, 王霞, 贾礼超 2013 物理学报 62 203103]
[29]
[30]	Sakthivel R, Ntho T, Witcomb M, Scurrell M S 2009 Catal. Lett. 130 341
[31]
[32]	Zhang X J, Zhang G F, Jin H X, Zhu L D, Liu Q J 2013 Acta Phys. Sin. 62 017102 [张学军, 张光富, 金辉霞, 朱良迪, 柳清菊 2013 物理学报 62 017102]
[33]
[34]	Liu C, Tang X H, Mo C H, Qiang Z M 2008 J. Solid State Chem. 181 913
[35]
[36]	Obata K, Irie H, Hashimoto K 2007 Chem. Phys. 339 124
[37]	Yang G D, Jiang Z, Shi H H, Jones M O, Xiao T C, Edwards P P, Yan Z F 2010 Appl. Catal. B 96 458
[38]
[39]	Morikawa T, Irokawa Y, Ohwaki T 2006 Appl. Catal. A 314 123
[40]
[41]
[42]	Song K, Zhou J, Bao J, Feng Y 2008 J. Am. Ceram. Soc. 91 1369
[43]	Wang C, Hu Q Q, Huang J Q 2014 Appl. Surf. Sci. 292 161
[44]
[45]
[46]	Pham T D, Lee B K 2014 Appl. Surf. Sci. 296 15
[47]	Finazzi E, Valentin C D, Selloni A, Pacchioni G 2007 J. Phys. Chem. C 111 9275
[48]
[49]	Lee J H, Hevia D F, Selloni A 2013 Phys. Rev. Lett. 110 5
[50]
[51]	Perdew J P, Burke K M 1996 Phys. Rev. Lett. 77 3865
[52]
[53]
[54]	Dudarev S L, Botton G A, Savarsov S Y 1998 Phys. Rev. B 57 1505
[55]	Jia L C, Wu C C, Han S, Yao N, Li Y Y, Li Z Z, Chi B, Pu J, Li J 2011 J. Alloy. Compd. 509 6067
[56]
[57]	Kresse G, Furthermuller J 1996 Phys. Rev. B 54 11169
[58]
[59]	Monkhorst H J, Pack J D 1998 Phys. Rev. B 13 5188
[60]
[61]	Zhao X W, Xi H P, Liao Q W 2013 Acta Phys.-Chim. Sin. 29 2232
[62]
[63]	Liu Y M, Liang W, Zhang W G, Zhang J J, Han P D 2013 Solid State Commun. 164 27

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