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浙江工业大学化学工程学院 绿色化学合成技术国家重点实验室培育基地, 浙江 杭州 310032
纸质出版日期:2017-4-5,
收稿日期:2016-10-27,
修回日期:2017-1-23,
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聂永惠, 李盼, 刘文涵等. 表面增强拉曼光谱研究胞嘧啶在银胶上的吸附行为[J]. 发光学报, 2017,38(4): 543-551
NIE Yong-hui, LI Pan, LIU Wen-han etc. Adsorption Behavior of Cytosine on Silver Colloid Investigated by Surface Enhanced Raman Scattering[J]. Chinese Journal of Luminescence, 2017,38(4): 543-551
聂永惠, 李盼, 刘文涵等. 表面增强拉曼光谱研究胞嘧啶在银胶上的吸附行为[J]. 发光学报, 2017,38(4): 543-551 DOI: 10.3788/fgxb20173804.0543.
NIE Yong-hui, LI Pan, LIU Wen-han etc. Adsorption Behavior of Cytosine on Silver Colloid Investigated by Surface Enhanced Raman Scattering[J]. Chinese Journal of Luminescence, 2017,38(4): 543-551 DOI: 10.3788/fgxb20173804.0543.
为探讨胞嘧啶(Cytosine'Cy)在基底银表面的吸附特性和规律'采用表面增强拉曼散射(SERS)光谱对其吸附行为进行分析'并结合量子化学密度泛函理论(DFT)/B3LYP计算方法对Cy分子的常规拉曼光谱(NRS)及Cy与Ag团簇吸附的SERS光谱进行计算'与测定结果进行比对且对其拉曼峰进行系统指认及归属'理论计算结合实测值探讨了Cy在基底Ag上的增强效应和吸附行为。考察了Cy分子在Ag纳米粒子上的不同吸附时间、浓度、pH等条件对SERS光谱的影响及优化'发现pH影响最大'在中性和强碱性条件下的增强效应明显优于酸性。Cy分子存在2种不同的异构体和3种不同的存在形态'并随酸度变化相互转化而达动态平衡。基于Cy在不同pH时的形态分布和相应的SERS变化规律'结合DFT算得的Cy分子中的电荷分布及在银基底表面的吸附机制'详细探讨了酸碱对Cy分子的SRES光谱影响的内因和吸附机理'指出在中性和弱碱性时'是Cy中的N
3
和O与Ag形成配位吸附;在pH大于11时'N与Ag形成配位吸附'而O与Ag形成共价吸附。
The adsorption characteristics and regularity of cytosine (Cy) on the silver substrate surface were analyzed by the means of surface enhanced Raman scattering (SERS) combing with quantum chemistry density functional theory (DFT). The normal Raman spectrum (NRS) of Cy and Cy-Ag
n
complex (
n
=1
3
5) SERS spectra were calculated by DFT/B3LYP method
which were further compared with the measured results to identify and assign the spectral peaks. The SERS spectra of Cy molecules on silver colloid nanoparticles were recorded at different adsorption time
concentration and pH. The results show that pH value has the greatest influence on its SERS signal
especially at neutral and strong alkaline conditions. It is inferred that there are two different isomers of Cy molecules and three kinds of existing forms
and all of them keep dynamic balance in the solution. The adsorption mechanism of Cy on the surface of silver substrate was further discussed in detail based on the morphological distribution of Cy at different pH by their corresponding SERS changes combining with the DFT calculation of charge distribution in Cy molecules. In conclusion
the N
3
and O in Cy are coordinated to Ag at the neutral and weakly alkaline conditions. N and Ag form coordinated adsorption and O and Ag form covalent adsorption
when the pH is greater than 11.
胞嘧啶表面增强拉曼光谱吸附行为DFT
cytosinesurface-enhanced Raman scatteringadsorption behaviorDFT
刘燕德, 靳昙昙. 拉曼光谱技术在农产品质量安全检测中的应用[J].光谱学与光谱分析, 2015,35(9):2567-2572. LIU Y D, JIN T T. Application of Raman spectroscopy technique to agricultural products quality and safety determination[J]. Spectrosc. Spect. Anal., 2015, 35(9):2567-2572. (in Chinese)
SHADI I T, CHOWDHRY B Z, SNOWDEN M J, et al.. Semi-quantitative analysis of alizarin and purpurin by surface-enhanced resonance Raman spectroscopy (SERRS) using silver colloids[J]. J. Raman Spectrosc., 2004, 35(8-9):800-807.
BILLINGHURST B E, LOPPNOW G R. Excited-state structural dynamics of cytosine from resonance Raman spectroscopy[J]. J. Phys. Chem. A, 2006, 110(7):2353-2359.
LI M J, DIAO L, KOU L, et al.. Hydroxyl radical reaction with the guanine-cytosine base pair:a density functional theory study[J]. Acta Phys. Chim. Sinica, 2015, 31(6):1007-1014.
MORARI C I, MUNTEAN C M. Numerical simulations of Raman spectra of guanine-cytosine Watson-Crick and protonated Hoogsteen base pairs[J]. Biopolymers, 2003, 72(5):339-344.
吴元菲, 李剑锋, 吴德印, 等. 胞嘧啶吸附在粗糙银和金电极上的表面增强拉曼光谱[J]. 光散射学报, 2006, 18(4):297-301. WU Y F, LI J F, WU D Y, et al.. Surface-enhanced Raman spectra of cytosine adsorbed on a roughened gold electrode[J]. J. Light Scatt., 2006, 18(4):297-301. (in Chinese)
郝艳玲, 张星, 方炎. 3种核酸碱基(胞嘧啶,胸腺嘧啶,尿嘧啶)在银电极表面的吸附形态[J]. 光谱实验室, 2011, 28(4):2019-2024. HAO Y L, ZHANG X, FANG Y. Adsorption distributions of three nucleic acid bases (cytosine, thymine, uracil) on silver electrode surface[J]. Chin. J. Spect. Lab, 2011, 28(4):2019-2024. (in Chinese)
LEE P C, MEISEL D. Adsorption and surface-enhanced Raman of dyes on silver and gold sols[J]. J. Phys. Chem., 1982, 86(17):3391-3395.
马枫茹, 刘琨, 张毅, 等. 以新型银胶为衬底的超低浓度R6G的拉曼光谱检测[J]. 光散射学报, 2007, 19(1):11-15. MA F R, LIU K, ZHANG Y, et al.. A novel silver colloid as substrate for detection of single-molecular level of R6G[J]. J. Light Scatt., 2007, 19(1):11-15. (in Chinese)
CARDINI G. MUNIZ-MIRANDA M. Density functional study on the adsorption of pyrazole onto silver colloidal particles[J]. J. Phys. Chem. B, 2002, 106(27):6875-6880.
TIAN Z Q, REN B. Proceedings of the International Symposium on Progress in Surface Raman Spectroscopy:Theory, Techniques and Applications[M]. Xiamen:China Xiamen University Press, 2000.
LIU S, ZHAO X, LI Y, et al.. Density functional theory study on Herzberg-Teller contribution in Raman scattering from 4-aminothiophenol-metal complex and metal-4-aminothiophenol-metal junction[J]. J. Chem. Phys., 2009, 130(23):234509.
SHAO Y, LI C, FENG Y, et al.. Surface-enhanced Raman scattering and density functional theory study of 1,4-benzenedithiol and its silver complexes[J]. Spectrochim. Acta Part A:Mol. Biomol. Spectrosc., 2013, 116:214-219.
ALONSO J L, VAQUERO V, PEA I, et al.. All five forms of cytosine revealed in the gas phase[J]. Angew. Chem., 2013, 125(8):2387-2390.
HAYNES W M. CRC Handbook of Chemistry and Physics[M]. Boca Raton:CRC Press, 2014.
刘文涵, 马苏珍, 滕渊洁, 等. 巯基苯并咪唑在银电极表面的自组装吸附特性及表面增强拉曼光谱[J]. 发光学报, 2015, 36(1):106-112. LIU W H, MA S Z, TENG Y J, et al.. Self-assembly behavior of 2-mercaptobenzimidazole on silver electrode investigated by surface enhancement Raman scattering[J]. Chin. J. Lumin., 2015, 36(1):106-112. (in Chinese)
司民真, 徐媛, 武荣国, 等. 正电性胶态纳米银中加入凝聚剂后的表面增强拉曼光谱[J]. 光谱学与光谱分析, 2006, 26(12):2251-2253. SI M Z, XU Y, WU R G, et al.. SERS of positive silver colloids with addition of aggregating agent[J]. Spectrosc. Spect. Anal., 2006, 26(12):2251-2253. (in Chinese)
陈林, 杨晓刚, 郑旭明, 等. 噻菌灵在纳米银胶表面吸附的表面增强拉曼光谱研究[J]. 光谱学与光谱分析, 2013, 33(12):3244-3248. CHEN L, YANG X G, ZHENG X M, et al.. Surface-enhanced Raman scattering of thiabendazole adsorbed on silver nanoparticles[J]. Spectrosc. Spect. Anal., 2013, 33(12):3244-3248. (in Chinese)
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