First principle study of electronic structures and optical absorption properties of O and S doped graphite phase carbon nitride (g-C3N4)6 quantum dots

Zhai Shun-Cheng; Guo Ping; Zheng Ji-Ming; Zhao Pu-Ju; Suo Bing-Bing; Wan Yun

doi:10.7498/aps.66.187102

Abstract

Graphite phase carbon nitride (g-C3N4) quantum dots have received much attention due to its good stability, water solubility, biological compatibility, non-toxicity as well as strong fluorescence characteristics. In order to enhance the light absorption and improve photocatalytic activities of the g-C3N4 quantum dots, theoretical studies are carried out on the O and S atoms doped (g-C3N4)6 quantum dots. First-principles calculations based on the density functional theory and time dependent density functional theory are performed to investigate the geometries, electronic structures and ultraviolet visible absorption spectra of O and S atoms doped (g-C3N4)6 quantum dots. The results show that the highest electron occupied molecular orbital-the lowest electron unoccupied molecular orbital (HOMO-LUMO) energy gap of doped (g-C3N4)6 quantum dots is significantly reduced though the CN bond lengths closely related to the impurities only change slightly. The calculated formation energies indicate that the O-doped (g-C3N4)6 quantum dots are more stable, and the O atom tends to substitute for N atom at the N3-site, while the S atoms prefer to substitute for N atom at the N8-site. The simulated spectra indicate that the doping of O and S in (g-C3N4)6 could improve the light absorption. Not only the absorption peaks are extended from the UV to the infrared region (e.g. 200-1600 nm), but also the corresponding absorption intensities are enhanced significantly by doping the O or S atoms with the appropriate concentration. The increase of proper impurity concentration will lead to a pronounced red shift in light absorption. The effect of doping site on the optical absorption property of (g-C3N4)6 quantum dots shows that the absorption intensity is mainly affected in the visible range, however, besides the influence on the absorption intensity, the light absorptions of some structures are also affected beyond 800 nm. Overall, the O atoms and S atoms have a substantially similar effect on the light absorption of the (g-C3N4)6 quantum dots, while the effects of these impurity atoms are different in the long wavelength region. Oxygen doping is better than sulfur doping in the absorption of (g-C3N4)6 quantum dots by comparing the doping of O and S. These first-principles studies give us a method to effectively improve the light absorption of g-C3N4 quantum dots, and could provide a theoretical reference for tuning its electronic optical properties and applications.

Keywords:

Authors and contacts

1.
School of Physics, Northwest University, Xi'an 710069, China;
2.
Institute of Photonics and Photon-Technology, Northwest University, Xi'an 710069, China;
3.
Institute of Modern Physics, Northwest University, Xi'an 710069, China

Corresponding author: Guo Ping, 1121074564@qq.com;guoping@nwu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 21673174), the Natural Science Foundation of Shanxi Province, China (Grant No. 2014JM2-1008), and the State Key Laboratory of Transient Optics and Photonic Technology 2015 Natural Open Fund, China (Grant No. SKLST200915).

Supplements

187102-20171006suppl(1).pdf

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[30]	Ma X G, Lu B, Li D, Shi R, Pan C S, Zhu Y F 2011 J. Phys. Chem. C 115 4680
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[32]	Huang Z F, Pan L, Zou J J, Zhang X, Wang L 2014 Nano Scale 6 14044

Cited By

[1]	Fujishima A, Honda K 1972 Nature 238 37
[2]	Ong W J, Tan L L, Chai S P, Yong S T, Mohamed A R 2014 Chem. Sus. Chem. 7 690
[3]	Tan L L, Ong W J, Chai S P, Mohamed A R 2014 Chem. Commun. 50 6923
[4]	Chen Y, Wang B, Lin S, Zhang Y, Wang X 2014 J. Phys. Chem. C 118 29981
[5]	Ye C, Li J X, Li Z J, Li X B, Fan X B, Zhang L P, Chen B, Tung C H, Wu L Z 2015 ACS Catal. 5 6973
[6]	Zhang S L, Wang J X, Huang Y, Zeng M, Xu J 2015 J. Mater. Chem. A 3 10119
[7]	Umebayashi T, Yamaki T, Itoh H, Asai K 2002 Appl. Phys. Lett. 81 454
[8]	Zhao W, Ma W H, Chen C C, Zhao J C, Shuai Z G 2004 J. Am. Chem. Soc. 126 4782
[9]	Huang Z F, Song J, Pan L, Wang Z, Zhang X, Zou J J, Mi W, Zhang X, Wang L 2015 Nano Energy 12 646
[10]	Dong G, Zhao K, Zhang L 2012 Chem. Commun. 48 6178
[11]	Ma T Y, Ran J, Dai S, Jaroniec M, Qiao S Z 2015 Angew. Chem. Int. Ed. 54 4646
[12]	Xu C, Han Q, Zhao Y, Wang L, Li Y, Qu L J 2015 J. Mater. Chem. A 3 1841
[13]	Lu C, Chen R, Wu X, Fan M, Liu Y, Le Z, Jiang S, Song S 2016 Appl. Surf. Sci. 360 1016
[14]	Li Y, Hu Y, Zhao Y, Shi G Q, Deng L, Hou Y B, Qu L T 2011 Adv. Mater. 23 776
[15]	Zheng Y, Liu J, Liang J, Jaroniec M, Qiao S Z 2012 Energy Environ. Sci. 5 6717
[16]	Zhang Z P, Zhang J, Chen N, Qu L T 2012 Energy Environ. Sci. 5 8869
[17]	Cao L, Sahu S, Anikumar P, Bunker C E, Xu J, Fernanodo K A S, Wang P, Guliants E A, Tackett K N, Sun Y P 2011 J. Am. Chem. Soc. 133 4754
[18]	Song Z P, Lin T R, Lin L H, Lin S, Fu F F, Wang X C, Guo L Q 2016 Angew. Chem. Int. Ed. 55 2773
[19]	Chan M H, Chen C W, Lee I J, Chan Y C, Tu D T, Hsiao M, Chen C H, Chen X Y, Liu R S 2016 Inorg. Chem. 55 10267
[20]	Fageria P, Uppala S, Nazir R, Gangopadhyay S, Chang C H, Basu M, Pande S 2016 Langmuir 32 10054
[21]	Wang X, Maeda K, Thomas A, Takanabe K, Xin G, Carlsson J M, Domen K, Antonietti M 2009 Nat. Mater. 8 76
[22]	Zhou J, Yang Y, Zhang C Y 2013 Chem. Commun. 49 8605
[23]	te Velde G, Bickelhaupt F M, Baerends E J, Fonseca G C, vanGisbergen S J A, Snijders J G, Ziegler T 2001 J. Comput. Chem. 22 931
[24]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865
[25]	Perdew J P, Chevary J A, Vosko S H, Jackson K A, Pederson M R, Singh D J, Fiolhais C 1992 Phys. Rev. B 46 6671
[26]	Casida M E 2009 J. Mol. Struct:Theochem. 914 3
[27]	Casida M E, Huix-Rotllant M 2012 Rev. Phys. Chem. 63 287
[28]	Schipper P R T, Gritsenko O V, van Gisbergen S J A, Baerends E J 2000 J. Chem. Phys. 112 1344
[29]	Liu G, Niu P, Qing L G, Cheng H M 2010 J. Am. Chem. Soc. 132 11642
[30]	Ma X G, Lu B, Li D, Shi R, Pan C S, Zhu Y F 2011 J. Phys. Chem. C 115 4680
[31]	Zhang J, Zhang G, Chen X, Lin S, Mohlmann L, Dołega G, Lipner G, Antonietti M, Blechert S, Wang X 2012 Angew. Chem. Int. Ed. 51 3183
[32]	Huang Z F, Pan L, Zou J J, Zhang X, Wang L 2014 Nano Scale 6 14044

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Vol. 66, Issue 18 - 2017-09-20

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