Citation: LI Wen-Zhe, WANG Li-Duo, GAO Rui, DONG Hao-Peng, NIU Guang-Da, GUO Xu-Dong, QIU Yong. Transforming Organic Ligands into a ZnS Protective Layer through the S^2- Intermediate State in ex situ CdSe Quantum Dot Devices[J]. Acta Physico-Chimica Sinica, ;2013, 29(11): 2345-2353. doi: 10.3866/PKU.WHXB201309242 shu

Transforming Organic Ligands into a ZnS Protective Layer through the S^2- Intermediate State in ex situ CdSe Quantum Dot Devices

1.
Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China

Received Date: 8 July 2013
Available Online: 24 September 2013
Fund Project: 国家自然科学基金(51273104) (51273104)国家重点基础研究发展规划项目(973)(2009CB930602)资助 (973)(2009CB930602)

In this paper, the tri-n-octylphosphine oxide (TOPO) ligand on CdSe quantum dots (QDs) are changed to ZnS coating layer through S^2- intermediate state. After ligand exchange, the Fourier transform infrared (FTIR) spectra indicate that the long chain organic ligands are replaced by S^2- ions. After ionic reaction, the generation of ZnS is confirmed by X-ray photoelectron spectroscopy (XPS) measurements. In addition the UV-Vis absorption peaks did not move and transmission electron microscopy (TEM) results show that the diameters of the quantum dots decrease. Electrochemical impedance spectroscopy (EIS) results show that the interface resistance between the TiO₂/QDs/electrolyte is reduced under illumination conditions, meaning that forward electron transport was enhanced. In addition, the intensity-modulated photovoltage spectroscopy (IMVS) and intensity-modulated photocurrent spectroscopy (IMPS) results reveal an increase in the electronic lifetime and diffusion rate increased. Finally, the conversion efficiency increases by 1.78 times from 0.98% (TOPO ligand) to 1.75% (ZnS coating).
- Quantum dot sensitized solar cell,
- Inorganic ligand,
- ZnS coating,
- Ligand exchange,
- Ionic reaction,
- CdSe quantum dot
1. [1]
  
  (1) O′Regan, B.; Grätzel, M. Nature 1991, 353, 737. doi: 10.1038/353737a0
2. [2]
  (2) Yella, A.; Lee, H.W.; Tsao, H. N.; Yi, C.; Chandiran, A. K.;Nazeeruddin, M. K.; Diau, E.W. G.;Yeh, C. Y.; Zakeeruddin, S.M.; Grätzel, M. Science 2011, 334, 629. doi: 10.1126/science.1209688
3. [3]
  (3) Vlachopoulos, N.; Liska, P.; Augustynski, J.; Grätzel, M. J. Am.Chem. Soc. 1988, 110, 1216. doi: 10.1021/ja00212a033
4. [4]
  (4) Watson, D. F. J. Phys. Chem. Lett. 2010, 1, 2299. doi: 10.1021/jz100571u
5. [5]
  (5) Sukhovatkin, V.; Hinds, S.; Brzozowski, L.; Sargent, E. H.Science 2009, 324, 1542. doi: 10.1126/science.1173812
6. [6]
  (6) Gao, R.; Tian, J.; Liang, Z.; Zhang, Q.;Wang, L.; Cao, G.Nanoscale 2013, 5, 1894. doi: 10.1039/c2nr33599a
7. [7]
  (7) Larson, D. R.; Zipfel,W. R.;Williams, R. M.; Clark, S.W.;Bruchez, M. P.;Wise, F.W.;Webb,W.W. Science 2003, 300,1434. doi: 10.1126/science.1083780
8. [8]
  (8) Kim, H.; Jeong, H.; An, T. K.; Park, C. E.; Yong, K. ACS Appl.Mater. Inter. 2012, 5, 268.
9. [9]
  (9) Gao, R.;Wang, L.; Ma, B.; Zhan, C.; Qiu, Y. Langmuir 2009,26, 2460.
10. [10]
  (10) Gao, R.;Wang, L.; Geng, Y.; Ma, B.; Zhu, Y.; Dong, H.; Qiu, Y.Phys. Chem. Chem. Phys. 2011, 13, 10635. doi: 10.1039/c0cp02820g
11. [11]
  (11) Gao, R.;Wang, L.; Geng, Y.; Ma, B.; Zhu, Y.; Dong, H.; Qiu, Y.J. Phys. Chem. C 2011, 115,17986. doi: 10.1021/jp204466h
12. [12]
  (12) Gao, R.; Niu, G.;Wang, L.; Geng, Y.; Ma, B.; Zhu, Y.; Dong,H.; Qiu, Y. Phys. Chem. Chem. Phys. 2012, 14, 5973. doi: 10.1039/c2cp24137d
13. [13]
  (13) Gao, R.; Ma, B. B.;Wang, L. D.; Shi, Y. T.; Dong, H. P.; Qiu, Y.Acta Phys. -Chim. Sin. 2011, 27, 413. [高瑞, 马蓓蓓, 王立铎, 史彦涛, 董豪鹏, 邱勇. 物理化学学报, 2011, 27, 413.]doi: 10.3866/PKU.WHXB20110234
14. [14]
  (14) Dong, H.;Wang, L.; Gao, R.; Ma, B.; Qiu, Y. J. Mater. Chem.2011, 21, 19389. doi: 10.1039/c1jm14191k
15. [15]
  (15) Shen, Q.; Kobayashi, J.; Diguna, L. J.; Toyoda, T. J. Appl. Phys.2008, 103, 084304.
16. [16]
  (16) Shalom, M.; Dor, S.; Ruühle, S.; Grinis, L.; Zaban, A. J. Phys.Chem. C 2009, 113, 3895.
17. [17]
  (17) Choi, H.; Nicolaescu, R.; Paek, S.; Ko, J.; Kamat, P. V. ACSNano 2011, 5, 9238. doi: 10.1021/nn2035022
18. [18]
  (18) Braga, A.; Giménez, S.; Concina, I.; Vomiero, A.; Mora-Seró, I.N. J. Phys. Chem. Lett. 2011, 2, 454. doi: 10.1021/jz2000112
19. [19]
  (19) Ning, Z.; Tian, H.; Qin, H.; Zhang, Q.; Ågren, H.; Sun, L.; Fu,Y. J. Phys. Chem. C 2010, 114, 15184. doi: 10.1021/jp102978g
20. [20]
  (20) Sambur, J. B.; Parkinson, B. A. J. Am. Chem. Soc. 2010, 132,2130. doi: 10.1021/ja9098577
21. [21]
  (21) Zhang, H.; Cheng, K.; Hou, Y. M.; Fang, Z.; Pan, Z. X.;Wu,W.J.; Hua, J. L.; Zhong, X. H. Chem. Commun. 2012, 48, 11235.doi: 10.1039/c2cc36526j
22. [22]
  (22) Deka, S.; Quarta, A.; Luo, M. G.; Falqui, A.; Boninelli, S.;Giannini, C.; Morello, G.; De Giorgi, M.; Lanzani, G.; Spinella,C.; Cin lani, R.; Pellegrino, T.; Manna, L. J. Am. Chem. Soc.2009, 131, 2948. doi: 10.1021/ja808369e
23. [23]
  (23) Xing, G.; Chakrabortty, S.; Ngiam, S.W.; Chan, Y.; Sum, T. C.J. Phys. Chem. C 2011, 115, 17711. doi: 10.1021/jp205238q
24. [24]
  (24) Xia, X.; Liu, Z.; Du, G.; Li, Y.; Ma, M. J. Phys. Chem. C 2010,114, 13414. doi: 10.1021/jp100442v
25. [25]
  (25) Justo, Y.; ris, B.; Kamal, J. S.; Geiregat, P.; Bals, S.; Hens, Z.J. Am. Chem. Soc.2012, 134, 5484. doi: 10.1021/ja300337d
26. [26]
  (26) Pan, Z.; Zhang, H.; Cheng, K.; Hou, Y.; Hua, J.; Zhong, X. ACSNano 2012, 6, 3982. doi: 10.1021/nn300278z
27. [27]
  (27) Murray, C. B.; Norris, D. J.; Bawendi, M. G. J. Am. Chem. Soc.1993, 115, 8706. doi: 10.1021/ja00072a025
28. [28]
  (28) Lee, H. J.; Yum, J. H.; Leventis, H. C.; Zakeeruddin, S. M.;Haque, S. A.; Chen, P.; Seok, S. I.; Graätzel, M.; Nazeeruddin,M. K. J. Phys. Chem. C 2008, 112, 11600. doi: 10.1021/jp802572b
29. [29]
  (29) Dibbell, R. S.; Youker, D. G.;Watson, D. F. J. Phys. Chem. C2009, 113, 18643. doi: 10.1021/jp9079469
30. [30]
  (30) Lokteva, I.; Radychev, N.;Witt, F.; Borchert, H.; Parisi, J. R.;Kolny-Olesiak, J. J. Phys. Chem. C 2010, 114, 12784. doi: 10.1021/jp103300v
31. [31]
  (31) Zillner, E.; Fengler, S.; Niyamakom, P.; Rauscher, F.; Köhler,K.; Dittrich, T. J. Phys. Chem. C 2012, 116, 16747. doi: 10.1021/jp303766d
32. [32]
  (32) Kovalenko, M. V.; Scheele, M.; Talapin, D. V. Science 2009,324, 1417. doi: 10.1126/science.1170524
33. [33]
  (33) Nag, A.; Kovalenko, M. V.; Lee, J. S.; Liu,W.; Spokoyny, B.;Talapin, D. V. J. Am. Chem. Soc. 2011, 133, 10612. doi: 10.1021/ja2029415
34. [34]
  (34) Kovalenko, M. V.; Bodnarchuk, M. I.; Zaumseil, J.; Lee, J. S.;Talapin, D. V. J. Am. Chem. Soc. 2010, 132, 10085. doi: 10.1021/ja1024832
35. [35]
  (35) Kovalenko, M. V.; Bodnarchuk, M. I.; Talapin, D. V. J. Am.Chem. Soc. 2010, 132, 15124. doi: 10.1021/ja106841f
36. [36]
  (36) Abel, K. A.; Qiao, H.; Young, J. F.; van Veggel, F. C. J. M.J. Phys. Chem. Lett. 2010, 1, 2334. doi: 10.1021/jz1007565
37. [37]
  (37) Dworak, L.; Matylitsky, V. V.; Breus, V. V.; Braun, M.; Basché,T.;Wachtveitl, J. J. Phys. Chem. C 2011, 115, 3949. doi: 10.1021/jp111574w
38. [38]
  (38) Jing, P.; Yuan, X.; Ji,W.; Ikezawa, M.;Wang, Y. A.; Liu, X.;Zhang, L.; Zhao, J.; Masumoto, Y. J. Phys. Chem. C 2010, 114,19256. doi: 10.1021/jp107524b
39. [39]
  (39) Kim, S.; Fisher, B.; Eisler, H. J.; Bawendi, M. J. Am. Chem.Soc. 2003, 125, 11466. doi: 10.1021/ja0361749
40. [40]
  (40) Mora-Seró, I. N.; Giménez, S.; Fabregat-Santia , F.; Gómez,R.; Shen, Q.; Toyoda, T.; Bisquert, J. Accounts Chem. Res.2009, 42, 1848. doi: 10.1021/ar900134d
41. [41]
  (41) Samanta, A.; Deng, Z.; Liu, Y. Langmuir 2012, 28, 8205. doi: 10.1021/la300515a
42. [42]
  (42) Wang, H.; Luan, C.; Xu, X.; Kershaw, S. V.; Rogach, A. L.J. Phys. Chem. C 2011, 116, 484.
43. [43]
  (43) Zhong, X.; Feng, Y.; Zhang, Y. J. Phys. Chem. C 2006, 111, 526.
44. [44]
  (44) Vogel, R.; Hoyer, P.;Weller, H. J. Phys. Chem. 1994, 98, 3183.doi: 10.1021/j100063a022
45. [45]
  (45) Niu, G.;Wang, L.; Gao, R.; Ma, B.; Dong, H.; Qiu, Y. J. Mater.Chem. 2012, 22, 16914. doi: 10.1039/c2jm32459h
46. [46]
  (46) Tachan, Z.; Shalom, M.; Hod, I.; Ruühle, S.; Tirosh, S.; Zaban,A. J. Phys. Chem. C 2011, 115, 6162. doi: 10.1021/jp112010m
47. [47]
  (47) Zhang, L.;Wang, Y.; Xu, Z.; Li, H. J. Phys. Chem. B 2009, 113,5978. doi: 10.1021/jp900139z
48. [48]
  (48) Li, H.; Brescia, R.; Krahne, R.; Bertoni, G.; Alcocer, M. J. P.;D′Andrea, C.; Scotognella, F.; Tassone, F.; Zanella, M.; DeGiorgi, M.; Manna, L. ACS Nano 2012, 6, 1637. doi: 10.1021/nn204601n
49. [49]
  (49) Li, H.; Zanella, M.; Genovese, A.; Povia, M.; Falqui, A.;Giannini, C.; Manna, L. Nano Letters 2011, 11, 4964. doi: 10.1021/nl202927a
50. [50]
  (50) Tang, J.; Kemp, K.W.; Hoogland, S.; Jeong, K. S.; Liu, H.;Levina, L.; Furukawa, M.;Wang, X.; Debnath, R.; Cha, D.;Chou, K.W.; Fischer, A.; Amassian, A.; Asbury, J. B.; Sargent,E. H. Nat. Mater. 2011, 10, 765. doi: 10.1038/nmat3118
51. [51]
  (51) Buckley, A. N.;Wouterlood, H. J.;Woods, R. Hydrometallurgy1989, 22, 39. doi: 10.1016/0304-386X(89)90040-6
52. [52]
  (52) Wang, D. H.;Wang, L.; Xu, A.W. Nanoscale 2012, 4, 2046.doi: 10.1039/c2nr11972b
53. [53]
  (53) Gimenez, S.; Mora-Sero, I.; Macor, L.; Guijarro, N.; Lana-Villarreal, T.; mez, R.; Diguna, L. J.; Shen, Q.; Toyoda, T.;Bisquert, J. Nanotechnology 2009, 20, 295204. doi: 10.1088/0957-4484/20/29/295204
54. [54]
  (54) Grätzel, M. Inorg. Chem. 2005, 44, 6841. doi: 10.1021/ic0508371
55. [55]
  (55) Kern, R.; Sastrawan, R.; Ferber, J.; Stangl, R.; Luther, J.Electrochimica Acta 2002, 47, 4213. doi: 10.1016/S0013-4686(02)00444-9
56. [56]
  (56) Stergiopoulos, T.; Karakostas, S.; Falaras, P. J. Photochem.Photobiol. A: Chem. 2004, 163, 331. doi: 10.1016/j.jphotochem.2004.01.002
57. [57]
  (57) Vittadini, A.; Selloni, A.; Rotzinger, F. P.; Grätzel, M. Phys. Rev.Lett. 1998, 81, 2954. doi: 10.1103/PhysRevLett.81.2954
58. [58]
  (58) Schlichthörl, G.; Huang, S. Y.; Sprague, J.; Frank, A. J. J. Phys.Chem. B 1997, 101, 8141. doi: 10.1021/jp9714126
59. [59]
  (59) Krüger, J.; Plass, R.; Grätzel, M.; Cameron, P. J.; Peter, L. M.J. Phys. Chem. B 2003, 107, 7536. doi: 10.1021/jp0348777
60. [60]
  (60) Dloczik, L.; Ileperuma, O.; Lauermann, I.; Peter, L. M.;Ponomarev, E. A.; Redmond, G.; Shaw, N. J.; Uhlendorf, I.J. Phys. Chem. B 1997, 101, 10281. doi: 10.1021/jp972466i
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Transforming Organic Ligands into a ZnS Protective Layer through the S2- Intermediate State in ex situ CdSe Quantum Dot Devices

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通讯作者: 陈斌, bchen63@163.com

Transforming Organic Ligands into a ZnS Protective Layer through the S^2- Intermediate State in ex situ CdSe Quantum Dot Devices