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染料敏化太阳能电池(dye-sensitized solar cells, DSCs)因其制备工艺简单、成本低廉以及优异的光学性质在近年来引起了大家的广泛关注. 为了获得更优的光电性能, 利用球磨法制备了一系列不同含量纳米结构SiO2@Au和固定含量石墨烯协同掺杂的复合光阳极薄膜, 并制备了相应的DSCs. 研究了纳米结构SiO2@Au和石墨烯联合掺杂对光阳极及其相应DSCs光电转换性能的影响. 金纳米颗粒因其局域表面等离子体共振效应能够有效提高DSCs的短路电流密度. 而石墨烯作为典型的二维材料, 具有较大的比表面积以及高导电性等优异性质, 有利于增加薄膜的比表面积. 当纳米结构SiO2@Au和石墨烯协同掺杂至光阳极薄膜内部, 且SiO2@Au掺杂量为1.5%时, 相应电池的短路电流密度为15.59 mA·cm–2, 光电转换效率为6.68%, 相比基于传统纯TiO2光阳极电池的性能分别提高了15.67%和8.8%. 研究表明, 基于不同含量复合纳米结构SiO2@Au和固定量石墨烯共掺的DSCs性能的提高, 主要归因于复合纳米结构SiO2@Au的掺入, 其中分布较为均匀的金纳米颗粒作为光学天线可以将光局域到颗粒表面, 增强表面电磁场强度, 有效增强光与物质的相互作用, 优化了染料的光吸收能力, 增加薄膜内部光生载流子数量. 而石墨烯的引入则改善了光阳极薄膜的比表面积, 增加了薄膜整体对染料的吸附量, 且石墨烯良好的导电性能加快了光生载流子的传输, 两者协同作用实现了DSCs的光电转换性能的优化.
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关键词:
- 纳米结构SiO2@Au /
- 石墨烯 /
- 染料敏化太阳能电池
Attributed to facile fabrication, low production costs and outstanding photoelectric properties, dye-sensitized solar cells (DSCs) have attracted widespread attention in recent years. In order to achieve better photoelectric conversion efficiency of the DSCs, a series of TiO2 nanocomposite photoanodes co-doped with different amounts of hybrid SiO2@Au nanostructures and certain amount of graphene are prepared by a mechanical ball milling method. The influence of SiO2@Au nanostructures and graphene on the performance of the photoanodes and their DSCs were investigated. The Au nanoparticles can remarkably enhance the short-circuit current density (Jsc) due to the local surface plasmon resonance effect of the noble metal nanoparticles. As a unique two-dimensional material, graphene has several amazing characteristics, such as high specific surface area and excellent conductivity. Studies showed that by introducing both SiO2@Au nanostructures and graphene, the light-absorbing, electron mobility and dye loading of the photoanodes were remarkably increased. Experimental results indicated that in comparison with those DSCs based with pure TiO2 photoanode, the DSCs with photoanodes incorporated with SiO2@Au nanostructures and graphene showed the optimal performance with short-circuit current density (Jsc ) of 15.59 mA/cm2 and photoelectric conversion efficiency (PCE) of 6.68%, increasing significantly by 15.67% and 8.8%, respectively. This significant enhancement in Jsc and PCE of DSCs are mainly attributed to the increase in light-absorption and dye-loading of the photoanodes due to the hybrid SiO2@Au nanostructures and graphene. -
Keywords:
- hybrid SiO2@Au nanostructure /
- graphene /
- dye-sensitized solar cells
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图 1 (a) SiO2球TEM图; (b) SiO2@Au复合结构TEM图; (c) 金纳米颗粒EDS图; (d) 纯金纳米颗粒光吸收谱图
Fig. 1. (a) TEM image of the SiO2 sphere; (b) TEM image of the SiO2@Au; (c) EDS image of the Au nanoparticles; (d) absorption spectra of pure Au nanoparticles.
图 2 SiO2@Au不同掺杂含量TiO2薄膜的紫外-可见光谱测试曲线 (a)吸收光谱; (b)漫反射光谱; (c)透射光谱; (d)染料脱吸附光谱
Fig. 2. (a) UV-vis absorption spectra; (b) diffuse reflectance spectra; (c) transmittance spectra; (d) spectra of the dyes desorbed from the TiO2 films containing different amounts of SiO2@Au.
图 3 复合结构SiO2@Au不同掺杂含量相应的DSCs (a) J-V性能曲线; (b) 电化学阻抗谱
Fig. 3. (a) J-V curves; (b) the Nyquist plots of EIS of the DSCs varying with the concentration of SiO2@Au.
表 1 不同光阳极的DSCs光电性能参数
Table 1. Photoelectric performance parameters of the DSCs with different photoanodes.
DSCs Jsc/mA·cm–2 Voc /mV FF η Pure 13.478 680 0.67 6.14 0.5% 15.436 678 0.58 6.07 1.0% 15.442 679 0.61 6.40 1.5% 15.59 680 0.63 6.68 2.0% 14.79 682 0.62 6.25 
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[1] Kong F T, Dai S Y, Wang K J 2007 Adv. Opto. Electron. 13 75384
[2] Hagfeldt A, Boschloo G, Sun L, Kloo L, Pettersson H 2010 Chem. Rev. 110 6595
Google Scholar
[3] Jena A, Mohanty S P, Kumar P, Naduvath J, Gondane V, Lekha P, Das J, Narula H K, Mallick S, Bhargava P 2012 T. Indian Ceram. Soc. 71 1
Google Scholar
[4] Zhang S, Yang X, Numata Y, Han L 2013 Energy Environ. Sci. 61 443
[5] O'regan B, Grätzel M 1991 Nature 1991 353
[6] Yin J F, Velayudham M, Bhattacharya D, Lin H C, Lu K L 2012 Coordin. Chem. Rev. 256 23
[7] Zhang Q, Cao G 2011 Nano Today 6 91
Google Scholar
[8] Chandiran A K, Comte P, Humphry-baker R, Kessler F, Yi C Y, Nazeeruddin M K, Grätzel M 2013 Adv. Funct. Mater. 23 2775
Google Scholar
[9] Liu B, Aydil E S 2009 J. Am.Chem. Soc. 131 3985
Google Scholar
[10] Cozzoli P D, Kornowski A, Weller H 2003 J. Am. Chem. Soc. 125 14539
Google Scholar
[11] Qin X, Wang H C, Li J L, Chen Q 2015 Talanta 139 56
Google Scholar
[12] Gurvinder S, Antonius T J, Sulalit B, Sondre V, Jens-Petter A, Wilheim R G 2014 Appl. Surf. Sci. 311 780
Google Scholar
[13] Zhang L, Niu W X, Xu G B 2012 Nano Today 7 586
Google Scholar
[14] Sun Z H, Yang Z, Zhou J H, Yeung M H, Ni W H, Wu H K, Wang J F 2009 Angew. Chem. 48 2881
Google Scholar
[15] Chen H J, Shao L, Li Q, Wang J F 2013 Chem. Sov. Rev. 42 2679
Google Scholar
[16] Liu X L, Liang S, Nan F, Yang Z J, Yu X F, Zhou L, Hao Z H, Wang Q Q 2013 Nanoscale 5 5368
Google Scholar
[17] Tapan K S, Catherine J M 2004 J. Am. Chem. Soc 126 8648
Google Scholar
[18] Suljo L, Phillip C, David B I 2011 Nat. Mater. 10 1038
[19] Subramanian V, Wolf E E, Kamat P V 2003 J. Phys. Chem. B 107 7479
Google Scholar
[20] Subramanian V, Wolf E E, Kamat P V 2004 J. Am. Chem. Soc. 126 4943
Google Scholar
[21] Chen S, Ingran R S, Hostetler M J, Pietron J J, Murray R W, Schaaff T G 1998 Science 280 2098
Google Scholar
[22] Pietron J J, Hicks J F, Murray R W 1999 J. Am. Chem. Soc. 121 5565
Google Scholar
[23] Fang X L, Li M Y, Guo K M, Liu X L, Zhu Y D, Sebo B, Zhao X Z 2014 Sol. Energy 101 176
Google Scholar
[24] He Z M, Phan H, Liu J, Nguyen T Q, Tan T Y 2013 Adv. Mater. 5 6900
[25] Brown M D, Suteewong T, Kumar R S S, D’Innocenzo V, Petrozza A, Lee M M, Wiesner U, Snaith H 2011 Nano lett. 11 438
Google Scholar
[26] Du L C, Furube A, Yamamoto K, Hara K, Katoh R, Tachiya M 2009 J. Phys. Chem. C 113 6454
Google Scholar
[27] Hägglund C, Zäch M, Kasemo B 2008 Appl. Phys. Lett. 92 013113
Google Scholar
[28] Qi J F, Dang X N, Hammond P T, Belcher A M 2011 ACS Nano 5 7108
Google Scholar
[29] Geim A K 2009 Science 324 1530
Google Scholar
[30] Luoshan M D, Li M Y, Liu X L, Guo K M, Bai L H, Zhu Y D, Sun B L, Zhao X Z 2015 J. Power Sources 287 231
Google Scholar
[31] Luoshan M D, Bai L H, Bu C H, Liu X L, Zhu Y D, Guo K M, Jiang R H, Li M Y, Zhao X Z 2016 J. Power Sources 307 468
Google Scholar
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