(Wuli Huaxue Xuebao) Acta Phys. -Chim. Sin., 2010, 26(2) , ; 2

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1 February (Wuli Huaxue Xuebao) Acta Phys Chim Sin (2) [Article] wwwwhxbpkueducn DNA 1* 2* 2 ( ; ) (SERS) (DNA) (ClO4 ) ClO 4 ClO4 ClO4 SERS ClO4 Cl NO3 SO 2 4 ClO4 ClO4 ; ; DNA ; O647 SurfaceEnhanced Raman Spectroscopic Study on the Coadsorption of DNA Bases with Perchlorate CUI Li 1* REN Bin 2* TIAN ZhongQun 2 ( 1 Institute of Urban Environment Chinese Academy of Sciences Xiamen Fujian Province P R China; 2 State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen Fujian Province P R China) Abstract Coadsorption with molecules that strongly adsorb on metallic surfaces is beneficial in improving the surfaceenhanced Raman spectroscopy (SERS) detection sensitivity of some weakly adsorbed molecules or ions In this paper the coadsorption of four deoxyribonucleic acid (DNA) bases: adenine guanine cytosine and thymine with ClO4 was studied Factors like adsorption ability applied potentials and coexisting anions were examined to illustrate how they affect coadsorption We found that the four DNA bases in their protonated forms could coadsorb with ClO4 Among them thymine with the weakest adsorption ability on Au showed the weakest coadsorption ability with ClO 4 In addition repulsion from both negative potentials and reduced SERS enhancements of Au substrates at relatively positive potentials led to a decrease in the SERS intensity of ClO 4 Moreover anions such as Cl NO 3 and SO 2 4 were shown to influence the coadsorption of ClO 4 with adenine based on a dynamic and reversible competitive coadsorption process The above results are very helpful in optimizing the SERS detection sensitivity of weakly adsorbed ions or molecules via the coadsorption method Key Words Coadsorption; Surfaceenhanced Raman spectroscopy; DNA bases; ClO 4 ( surface enhanced Raman spectroscopy SERS) [1] Received: August ; Revised: September ; Published on Web: December * Corresponding authors bren@xmueducn lcui@iueaccn; Tel: The project was supported by the National Natural Science Foundation of China ( ) and Natural Science Foundation of Fujian Province China (2009J05032) ( ) (2009J05032) 鬁 Editorial office of Acta PhysicoChimica Sinica

2 398 Acta Phys Chim Sin 2010 Vol26 SERS [27] SERS SERS ClO4 SERS SERS ClO [ ] 4 [20] [56812] DNA ClO [1314] 11 (NaClO 4 980%1020% Alfa Aesar) (C 5 H 5 N 5 99% Alfa Aesar) (C 5 H 5 N 5 O > [15] 99% Acros) (C 4 H 5 N 3 O >98% Alfa Aesar) (ClO4 [58] ) SERS (C 5 H 6 N 2 O 2 99% Sigma) (HAuCl 4 ClO 4 4H 2 O) (C 6 H 5 Na 3 O 7 2H 2 O) (thiourea) (methyl thiourea) (allyl 12 SERS [21] (cystamine dihydrochloride) 2 Frens (2dimethylaminoethanethiol hydrochloride) (imidazole) [581618] Gu [5] 065 ml 1% ClO4 60 nm ClO 4 ClO ml 001% SERS mol L 1[5] 2 ClO mol L 1 SERS LabRam I [8] ( Dilor ) 6328 nm ClO4 Olympus 50 ( mm) XHDII (SERS) ( ) [58] TcO 4 UO [69] mol L mol L ClO4 ClO 4 1 a ClO4 1 mmol L mol L 1 NaClO 4 ClO4 SERS ClO4

3 No2 DNA ph ClO4 SERS Fig1 SERS spectra of adenine and ClO 4 in solutions with different ph values and anions (a) 1 mmol L 1 adenine+01 mol L 1 NaClO 4; (b) 1 mmol L 1 adenine+01 mol L 1 HClO 4; (c) 1 mmol L 1 adenine+ 01 mol L 1 HClO 4+05 mol L 1 H 2SO cm 1 ph=1 (1 mmol L mol L 1 HClO 4 ) ClO 4 ph pk a (38) [22] 933 cm 1 ClO4 NaClO 4 ( 1 b) ClO4 ClO 4 (01 mol L 1 ) SERS 933 cm 1 ClO4 ClO4 SERS 05 ClO4 mol L 1 H 2 SO 4 1 c SERS SERS ClO4 933 cm cm 1 SO 2 4 SO 2 DNA : 2 DNA ph=1 933 cm 1 ClO4 ph=1 ClO4 DNA ClO 4 DNA [2326] ClO4 ClO 4 Gu [58] ClO 4 SERS 4 ClO4 22 ClO4 SO 2 4 ClO4 933 cm cm 1 ClO 4 SERS (c) ph 1 ph 7 Fig2 2 (a) (b) (c) SERS SERS spectra of guanine (a) cytosine (b) and thymine (c) on gold surfaces in acid and neutral solutions (a) 1 mmol L 1 guanine+01 mol L 1 ClO 4; (b) 1 mmol L 1 cytosine+01 mol L 1 ClO 4; (c) 10 mmol L 1 thymine+01 mol L 1 ClO 4

4 400 Acta Phys Chim Sin 2010 Vol26 Fig3 3 SERS Potential dependent SERS spectra of adenine adsorbed on gold surfaces in neutral and acid solutions (a) 1 mmol L 1 adenine+01 mol L 1 NaClO 4; (b) 1 mmol L 1 adenine+01 mol L 1 HClO 4 02 V 23 ClO4 06 V ClO4 ClO4 ph ClO4 ClO 4 Cl NO 3 SO 2 4 ClO 4 ClO4 5(A) 04 V 01 mol L 1 HClO mmol L 1 ClO 4 01 mol L 1 HCl+01 mol L 1 NaClO ClO4 mmol L cm 1 ClO4 ClO4 Cl ClO4 01 mol L 1 HClO mmol L 1 ClO4 SERS 4(b) SERS HNO 3 HCl 5(B) 02 V 0 V ClO cm 1 ClO cm 1 0 V NO 3 01 mol L 1 HClO V 06 V ClO4 mmol L 1 ClO4 H 2 SO 4 5(C) 933 cm 1 SERS 980 cm 1 01 mol L 1 HClO 4 + Fig4 4 SERS Potential dependent SERS spectra of guanine in neutral and acid solutions (a) 1 mmol L 1 guanine+01 mol L 1 NaClO 4; (b) 1 mmol L 1 guanine+01 mol L 1 HClO 4

5 No2 DNA mmol L cm 1 (1) ClO4 ClO4 ClO4 SERS SO 2 4 NO3 Cl ClO4 Gu [16] 2 ClO 4 Cl NO 3 SO 2 4 (2) ClO4 PO 3 4 ClO 4 ClO 4 ClO 4 23 ClO 4 SERS SERS SO 2 4 ClO 4 (3) Cl NO3 SO 2 4 ClO4 ClO 4 ( / ) SO 2 4 ClO4 SO 2 4 NO 3 Cl ClO 4 ph ClO4 DNA SERS ClO4 References 3 Fig5 5 SERS SERS spectra of adenine in different solutions 15 mmol L 1 adenine+01 mol L 1 ClO4 (AC a c) with different competitive anions: (A b) 01 mol L 1 HCl (B b) 01 mol L 1 HNO 3 (C b) 01 mol L 1 H 2SO 4 DNA ClO4 ClO4 1 Pieczonka N P W; Aroca R F Chem Soc Rev (5): Costa J C S; Sant Ana A C; Corio P; Temperini M L A Talanta (5): Goeller L J; Riley M R Appl Spectrosc (7): Mahajan S; Richardson J; Brown T; Bartlett P N J Am Chem Soc (46): 15589

6 402 Acta Phys Chim Sin 2010 Vol26 5 Ruan C; Wang W; Gu B Anal Chim Acta (1): Ruan C; Luo W; Wang W; Gu B Anal Chim Acta (1): 80 7 Han X X; Kitahama Y; Tanaka Y; Guo J; Xu W Q; Zhao B; Ozaki Y Anal Chem (17): Gu B H; Ruan C M; Wang W Appl Spectrosc (1): 98 9 Gu B; Ruan C Anal Chem (6): Cao P G; Yao J L; Ren B; Gu R N; Tian Z Q J Phys Chem B (39): Tian Z Q; Li W H; Mao B W; Gao J S J Electroanal Chem (12): Tan S; Erol M; Sukhishvili S; Du H Langmuir (9): Gu B H; Coates J D Perchlorate environmental occurence interactions and treatment New York: Springer Kirk A B; Martinelango P K; Tian K; Dutta A; Smith E E; Dasgupta P K Environ Sci Technol (7): Zhang K J; Gao Y N; Sui H M; Lu N Sichuan Environment (6): 562] 17 Cao P G; Gu R A; Tian Z Q J Phys Chem B (3): Gu R A; Yao J L; Yuan Y X; Zhong Q L; Tian Z Q Acta Chim Sin (7): 692 [ (7): 692] 19 Zheng J Z; Ren B; Wu D Y; Tian Z Q J Electroanal Chem (2): Frens G Nat Phys Sci : Puppels G J; Otto C; Greve J; RobertNicoud M; ArndtJovin D J; Jovin T M Biochemistry (11): Ostblom M; Liedberg B; Demers L M; Mirkin C A J Phys Chem B (31): KimuraSuda H; Petrovykh D Y; Tarlov M J; Whitman L J J Am Chem Soc (30): Demers L M; Oestblom M; Zhang H; Jang N H; Liedberg (1): 91 [ B; Mirkin C A J Am Chem Soc (38): (1): 91] 26 Gourishankar A; Shukla S; Ganesh K N; Sastry M J Am 16 Zhong Q L; Wang D Q; Liu F M; Su X Q; Shi C H; Tian Chem Soc (41): Z Q Acta Phys Chim Sin (6): 562 [