电化学表面增强拉曼光谱的量子化学研究

doi:10.7503/cjcu20150747

高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (11): 2087.doi: 10.7503/cjcu20150747

电化学表面增强拉曼光谱的量子化学研究

庞然¹, 金曦¹, 赵刘斌², 丁松园¹, 吴德印¹(), 田中群¹

1. 厦门大学化学化工学院化学系, 固体表面物理化学国家重点实验室, 厦门 361005
2. 西南大学化学化工学院, 重庆 400715

收稿日期:2015-09-25 出版日期:2015-11-10 发布日期:2015-10-28
作者简介:联系人简介: 吴德印, 男, 博士, 教授, 主要从事光谱电化学研究. E-mail:dywu@xmu.edu.cn
基金资助:
国家自然科学基金(批准号: 21373712, 21321062, 21533006)、国家重点基础研究项目(批准号: 2015CB932303)和厦门大学固体表面物理化学国家重点实验室开放基金(批准号: 201416)资助

Quantum Chemistry Study of Electrochemical Surface-enhanced Raman Spectroscopy^†

PANG Ran¹, JIN Xi¹, ZHAO Liubin², DING Songyuan¹, WU Deyin^1,^*(), TIAN Zhongqun¹

1. State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
2. School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China

Received:2015-09-25 Online:2015-11-10 Published:2015-10-28
Contact: WU Deyin E-mail:dywu@xmu.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.21373712, 21321062, 21533006), the National Basic Research Program of China(No.2015CB932303), and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, China(No.201416)

摘要/Abstract

摘要：

对于在分子水平上研究电化学表面吸附和反应过程, 表面增强拉曼光谱(SERS)显示出了其独到的优势, 提供了有力的技术方法, 但对于其表面增强机理仍有待深入研究. 本文总结了将量子化学计算应用于电化学表面增强拉曼光谱(EC-SERS)分析的研究, 以电化学界面分子吸附、电化学反应以及光电化学反应的研究体系为模型, 提取EC-SERS光谱所蕴藏的物理化学信息. 通过对吡啶在电化学表面的吸附、水的吸附及其电化学反应、以及对巯基苯胺的电化学表面催化偶联反应等体系的研究, 揭示了电化学表面吸附、反应和光电化学过程的本质.

关键词: 量子化学, 表面增强拉曼光谱, 电荷转移态, 表面等离激元共振, 电化学

Abstract:

Considering the study of electrochemical surface adsorption and reaction processes at the molecular level, Surface-enhanced Raman spectroscopy(SERS) shows its particular merits and provides a powerful technical method for this study. However, the mechanism of enhancement needs to be further explored. This review summarizes the systematic work on electrochemical SERS(EC-SERS) by combining quantum chemistry calculations. On the basis of these studies, we can make deep insight for extracting the physical and chemical information in EC-SERS spectra. Focusing on adsorption of pyridine on the electrochemical surface, adsorption and reactional process of water on the surface, and surface coupling reaction for p-aminothiophenol, we had illustrated the nature of the adsorption and photochemical reactions on the electrochemical surface.

Key words: Quantum chemistry, Surface-enhanced Raman spectroscopy, Charge transfer state, Surface plasmon resonance, Electrochemistry

中图分类号:

O643

TrendMD:

庞然, 金曦, 赵刘斌, 丁松园, 吴德印, 田中群. 电化学表面增强拉曼光谱的量子化学研究. 高等学校化学学报, 2015, 36(11): 2087.

PANG Ran, JIN Xi, ZHAO Liubin, DING Songyuan, WU Deyin, TIAN Zhongqun. Quantum Chemistry Study of Electrochemical Surface-enhanced Raman Spectroscopy^†. Chem. J. Chinese Universities, 2015, 36(11): 2087.

图/表 8

Fig.1 Schematic diagrams of the influence of applied potentials to EC-SERS systems[3] Copyright from the Royal Society of Chemistry.

Fig.2 Schematic diagram of theoretical simulation for EC-SERS

Fig.3 Raman spectra of liquid pyridine, SERS spectra of pyridine adsorbed on silver electrode at open circuit potential and the peak potential at -0.6 V(vs. SCE)(A)[3], SERS spectra of pyridine on different electrodes at open circuit potentials(B), simulated SERS spectra of pyridine(C) and effect of the charge transfer excited state on resonance Raman spectra of the pyridine-silver complex(D)[32] Ref.[3] copyright from the Royal Society of Chemistry; ref.[32] copyright from Elsevier.

Table 1 Huang-Rhys factors(s) and vibrational frequencies(ω) of totally symmetry modes for the ground and excited states of Py-Ag2, calculated at the B3LYP/6-311+G**/LANL2DZ level*

Mode	ν₂	ν₁₃	ν_20a	ν_8a	ν_19a	ν_9a	ν_18a	ν₁₂	ν₁	ν_6a
s	0	0	0.001	0.288	0.021	0.339	0.052	0.035	0.309	0.152
ω_{Ground state}/cm^-1	3097.2	3076.5	3067.7	1605.4	1485.4	1217.2	1071.7	1030.8	1005.6	623.9
ω_{Excited state}/cm^-1	3054.8	3100.5	3077.9	1579.0	1435.3	1189.0	985.2	1019.4	937.6	613.8

Fig.4 Adsorded directions of water changed with the surface charges upon more negative potential(A) and SERS spectra of water molecules adsorded on Pt, Pd and Au nanoparticles(B)[60] Copyright from the Royal Society of Chemistry.

Fig.5 Calculated structures and SERS spectra from cluster models for a water molecule adsorbed on negatively charged Auδ10(δ=-1, -2)[44] Copyright from the Royal Society of Chemistry. (A) Simulated Raman spectrum of free water molecule; (B) simulated raman spectrum of H2O…Au through the interaction between O and Au atoms; (C) simulated Raman spectrum of HOH…Au- through the interaction between H atom and Au anion; (D) [Au10-H2O]δ(δ=-1, -2) clusters; (E) simulated Raman spectrum of Au10-H2O- complex; (F) simulated Raman spectrum of Au10-H2O2- complex.

Fig.6 Calculated Raman spectra of PATP-Ag5(A) and Ag5-DMAB-Ag5(B) on Ag clusters[67] Copyright from the Royal Society of Chemistry.

Fig.7 Schematic diagrams of the mechanisms of surface plasmon enhanced photoelectrochemical reaction (A) Oxygen activation at solid-gas interfaces; (B) hole oxidization at electrode-electrolyte interfaces.

参考文献 72

[1]	Fleischmann M., Hendra P. J., Mcquillan A., J. Chem. Phys. Lett., 1974, 26, 163—166
[2]	Jouanne M., Beserman R., Balkanski M., Jain K. P., Solid State Communications, 1974, 15(2), 251—253
[3]	Wu D. Y., Li J. F., Ren B., Tian Z. Q., Chem. Soc. Rev., 2008, 37(5), 1025—1041
[4]	Tian Z.Q., Ren B., Li J. F., Yang Z. L.,Chem. Commun., 2007, (34), 3514—3534
[5]	Nie S. M., Emery S. R., Science, 1997, 275(5303), 1102—1106
[6]	Tian Z. Q., Ren B., Wu D. Y., J. Phys. Chem. B, 2002, 106(37), 9463—9483
[7]	Tian Z. Q., Ren B., Annu. Rev. Phys. Chem., 2004, 55, 197—229
[8]	Abdelsalam M., Bartlett P. N., Russell A. E., Baumberg J. J., Calvo E. J., Tognalli N. G., Fainstein A., Langmuir, 2008, 24(13), 7018—7023
[9]	Ding S. Y., Yi J., Li J. F., Tian Z. Q., Surf. Sci., 2015, 631, 73—80
[10]	Lombardi J. R., Birke R. L., Lu T., Xu J., J. Chem. Phys., 1986, 84, 4174—4180
[11]	Otto A. J., Raman Spectrosc., 2005, 36(6/7), 497—509
[12]	Ding S. Y., Wu D. Y., Yang Z. L., Ren B., Xu X., Tian Z. Q., Chem. J. Chinese Universities, 2008, 29(12), 2569—2581
	(丁松园, 吴德印, 杨志林, 任赋, 徐昕, 田中群. 高等学校化学学报, 2008, 29(12), 2569—2581)
[13]	Tian Z.Q., Wu D. Y., Unified Theory of Surface Enhanced Spectroscopy, 10000 Selected Problems in Sciences: Chemistry, Science Press, Beijing, 2009, 210
	(田中群, 吴德印. 表面增强光谱学的统一理论, 10000个科学难题, 化学卷, 北京: 科学出版社, 2009, 210)
[14]	Lombardi J. R., Birke R. L., J. Phys. Chem. C, 2008, 112(14), 5605—5617
[15]	Wu D. Y., Liu X. M., Huang Y. F., Ren B., Xu X., Tian Z. Q., J. Phys. Chem. C, 2009, 113(42), 18212—18222
[16]	Su S., Huang R., Zhao L. B., Wu D. Y., Tian Z. Q., Acta Phys. Chim. Sin., 2011, 27(4), 781—792
[17]	Wang A., Huang Y. F., Sur U. K., Wu D. Y., Ren B., Rondinini S., Amatore C., Tian Z. Q., J. Am. Chem. Soc., 2010, 132(28), 9534—9536
[18]	Ding S. Y., Liu B. J., Jiang Q. N., Wu D. Y., Ren B., Xu X., Tian Z. Q., Chem. Commun., 2012, 48, 4962—4964
[19]	Wu D. Y., Hayashi M., Chang C. H., Liang K. K., Lin S. H., J. Chem. Phys., 2003, 118(9), 4073—4085
[20]	Huang R., Yang H. T., Cui L., Wu D. Y., Ren B., Tian Z. Q., J. Phys. Chem. C, 2013, 117(45), 23730—23737
[21]	Tao S., Yu L. J., Pang R., Huang Y. F., Wu D. Y., Tian Z. Q., J. Phys. Chem. C, 2013, 117(37), 18891—18903
[22]	Krishnan R., Binkley J. S., Seeger R., Pople J. A., J. Chem. Phys., 1980, 72(1), 650—654
[23]	Kendall R. A., Dunning T. H., Harrison R. J., J. Chem. Phys., 1992, 96(9), 6796—6806
[24]	Hay P. J., Wadt W. R., J. Chem. Phys., 1985, 82(1), 299—310
[25]	Wu D. Y., Hayashi M., Shiu Y. J., Liang K. K., Chang C. H., Yeh Y. L., Lin S. H., J. Phys. Chem. A, 2003, 107(45), 9658—9667
[26]	Wu D. Y., Ren B., Xu X., Liu G. K., Yang Z. L., Tian Z. Q., J. Chem. Phys., 2003, 119(3), 1701—1709
[27]	Liu J. L., Guo Y., Xue Y., Yan G. S., Chem. J. Chinese Universities, 2009, 30(1), 100—105
	(刘靖丽, 郭勇, 薛英, 鄢国森, 高等学校化学学报, 2009, 30(1), 100—105)
[28]	Xue Y., Xie D. Q., Yan G. S., Int. J. Quantum Chem., 2000, 76(6), 686—699
[29]	Wu D. Y., Ren B., Jiang Y. X., Xu X., Tian Z. Q., J. Phys. Chem. A, 2002, 106(39), 9042—9052
[30]	Wu D. Y., Liu X. M., Duan S., Xu X., Ren B., Lin S. H., Tian Z. Q., J. Phys. Chem. C, 2008, 112(11), 4195—4204
[31]	Wu D. Y., Duan S., Liu X. M., Xu Y. C., Jiang Y. X., Ren B., Xu X., Lin S. H., Tian Z. Q., J. Phys. Chem. A, 2008, 112(6), 1313—1321
[32]	Wu D. Y., Hayashi M., Lin S. H., Tian Z. Q., Spectroc. Acta Pt. A: Molec. Biomolec. Spectr., 2004, 60(1/2), 137—146
[33]	Lee M. T., Wu D. Y., Tian Z. Q., Lin S. H., J. Chem. Phys., 2005, 122(9), 094719
[34]	Bruckbauer A., Otto A., J. Raman Spectrosc., 1998, 29(8), 665—672
[35]	Billmann J., Otto A., Solid State Commun., 1982, 44(2), 105—107
[36]	Osamura Y., Yamaguchi Y., Schaefer H. F., J. Chem. Phys., 1982, 77(1), 383—390
[37]	Nakai H., Nakatsuji H., J. Chem. Phys., 1995, 103(6), 2286—2294
[38]	Rubim J. C., Corio P., Ribeiro M. C. C., Matz M., J. Phys. Chem., 1995, 99(43), 15765—15774
[39]	Zhao L. L., Jensen L., Schatz G. C., J. Am. Chem. Soc., 2006, 128(9), 2911—2919
[40]	Kambhampati P., Child C. M., Foster M. C., Campion A., J. Chem. Phys., 1998, 108(12), 5013—5026
[41]	Avouris P., Demuth J. E., J. Chem. Phys., 1981, 75, 4783—4794
[42]	Fang Y., Liu Z., Science China Chemistry, 2010, 53(3), 543—552
[43]	Jinnouchi R., Anderson A. B., Physical Review B, 2008, 77(24)
[44]	Li J. F., Huang Y. F., Duan S., Pang R., Wu D. Y., Ren B., Xu X., Tian Z. Q., Phys. Chem. Chem. Phys., 2010, 12(10), 2493—2502
[45]	Pang R., Yu L. J., Wu D. Y., Mao B. W., Tian Z. Q., Electrochim. Acta, 2013, 101, 272—278
[46]	Creighton J.A., Eds.: Tian Z. Q., Ren B., Progress in Surface Raman Spectros Copy Theory, Techniques & Applications, University Press: Xiamen, 2000, 11—16
[47]	Klots T. D., Spectroc. Acta Pt. A: Molec. Biomolec. Spectr., 1998, 54(10), 1481—1498
[48]	Schlucker S., Singh R. K., Asthana B. P., Popp J., Kiefer W., J. Phys. Chem. A, 2001, 105(43), 9983—9989
[49]	Creighton J. A., Surface Science, 1986, 173(2/3), 665—672
[50]	Jensen L., Zhao L. L., Schatz G. C., J. Phys. Chem. C, 2007, 111(12), 4756—4764
[51]	Wu D. Y., Zheng J. Z., Ren B., Xu X., Tian Z. Q., Spectrosc. Spectr. Anal., 2005, 25(3), 365—368
[52]	Ingram J. C., Pemberton J. E., Langmuir, 1992, 8(8), 2034—2039
[53]	Arenas J. F., Tocon I. L., Otero J. C., Marcos J. I., J. Phys. Chem., 1996, 100(22), 9254—9261
[54]	Islampour R., Hayashi M., Lin S. H., J. Raman Spectrosc., 1997, 28(5), 331—338
[55]	Xie Y., Wu D. Y., Liu G. K., Huang Z. F., Ren B., Yan J. W., Yang Z. L., Tian Z. Q., J. Electroanal. Chem., 2003, 554/555, 417—425
[56]	Clark J. H., Dines T., J. Angew. Chem. Int. Ed., 1986, 25, 131—158
[57]	Matz D. L., Pemberton J. E., J. Phys. Chem. C, 2012, 116(21), 11548—11555
[58]	Toney M. F., Howard J. N., Richer J., Borges G. L., Gordon J. G., Melroy O. R., Wiesler D. G., Yee D., Sorensen L. B., Nature, 1994, 368(6470), 444—446
[59]	Velasco-Velez J. J., Wu C. H., Pascal T. A., Wan L. F., Guo J., Prendergast D., Salmeron M., Science, 2014, 346(6211), 831—834
[60]	Jiang Y. X., Li J. F., Wu D. Y., Yang Z. L., Ren B., Hu J. W., Chow Y. L., Tian Z. Q., Chem. Commun., 2007, 43(44), 4608—4610
[61]	Gao P., Gosztola D., Weaver M. J., J. Phys. Chem., 1988, 92(25), 7122—7130
[62]	Sun S., Birke R. L., Lombardi J. R., Leung K. P., Genack A. Z., J. Phys. Chem., 1988, 92(21), 5965—5972
[63]	Matsuda N., Yoshii K., Ataka K., Osawa M.,Chem. Lett., 1992, 1385—1388
[64]	Osawa M., Matsuda N., Yoshii K., Uchida I., J. Phys. Chem., 1994, 98(48), 12702—12707
[65]	Hill W., Wehling B., J. Phys. Chem., 1993, 97(37), 9451—9455
[66]	Yang X. M., Tryk D. A., Hashimoto K., Fujishima A., J. Raman Spectroscopy, 1998, 29(8), 725—732
[67]	Wu D. Y., Zhao L. B., Liu X. M., Huang R., Huang Y. F., Ren B., Tian Z. Q., Chem. Commun., 2011, 47(9), 2520—2522
[68]	Huang Y. F., Zhu H. P., Liu G. K., Wu D. Y., Ren B., Tian Z. Q., J. Am. Chem. Soc., 2010, 132(27), 9244—9246
[69]	Zhao L. B., Zhang M., Huang Y. F., Williams C. T., Wu D. Y., Ren B., Tian Z. Q., J. Phys. Chem. Letters, 2014, 5(7), 1259—1266
[70]	Huang Y. F., Zhang M., Zhao L. B., Feng J. M., Wu D. Y., Ren B., Tian Z. Q., Angew. Chem. Int. Ed., 2014, 53(9), 2353—2357
[71]	Zhao L. B., Huang Y. F., Liu X. M., Anema J. R., Wu D. Y., Ren B., Tian Z. Q., Phys. Chem. Chem. Phys., 2012, 14(37), 12919—12929
[72]	Sun M., Xu H., Small, 2012, 8(18), 2777—2786

电化学表面增强拉曼光谱的量子化学研究

Quantum Chemistry Study of Electrochemical Surface-enhanced Raman Spectroscopy^†

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电化学表面增强拉曼光谱的量子化学研究

Quantum Chemistry Study of Electrochemical Surface-enhanced Raman Spectroscopy†

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Quantum Chemistry Study of Electrochemical Surface-enhanced Raman Spectroscopy^†