以DNA为模板的银纳米簇荧光检测及逻辑门的构建

doi:10.7503/cjcu20190385

摘要/Abstract

摘要：

以DNA为模板, 合成了具有荧光性质的银纳米簇(DNA-Ag NCs), 利用荧光光谱、紫外光谱和红外光谱等手段对其进行了表征. 基于DNA-Ag NCs与离子相互作用时产生的荧光变化可实现对离子浓度的检测. 实验结果表明, 在最佳实验条件下, Ni ²⁺及Hg ²⁺的浓度与DNA-Ag NCs荧光强度呈线性关系; 并验证了该荧光探针用于检测自来水样品中汞离子和镍离子的实用性. 由于以DNA为模板的DNA-Ag NCs能够响应多种刺激, 如Ni ²⁺, S ^2-, Hg ²⁺和pH等, 利用相应的荧光强度可构建多输入的DNA-Ag NCs逻辑门及其组合逻辑门. 当荧光输出强度(I_output)>初始荧光强度(I_origin)时, 设定输出为1, 采用各种刺激及其组合作为输入, 构建了YES, INH和组合的NOR与INH逻辑门. 而只有当I_output≥I_origin时定义为输出为1, 可建立NOT, NOR, 组合的IMP加上NOR与AND逻辑门. 基于DNA-Ag NCs可以构建响应多元输入的复杂逻辑门, 实现化学信息的转变和传输, 在构建新的分子器件方面有较大应用前景.

关键词: 荧光检测, DNA模板, 银纳米簇, 逻辑门

Abstract:

Fluorescent silver nanoclusters were synthesized using DNA as template(DNA-Ag NCs), and characterized by fluorescence, ultraviolet and infrared spectroscopy. According to the fluorescence changes generated by the interaction between DNA-Ag NCs and ions, relative concentration detections can be carried out. Under the optimal experimental conditions, the concentrations of Ni ²⁺ and Hg ²⁺ showed a linear relationship with the fluorescence intensity of DNA-Ag NCs. The practicability of this fluorescent probe in tap water samples is also verified. Since DNA-Ag NCs can respond to a variety of stimuli, including Ni ²⁺, S ^2-, Hg ²⁺ and H ⁺(pH=7.0), logic gates of multiple input and their combination can be constructed based on the corresponding fluorescence intensity. When definition of fluorescence output intensity(I_output)>initial fluorescence intensity(I_origin) as output=1 was adopted, the YES, INH and integrative NOR and INH logic gates were constructed. And if I_output≥I_origin is defined as output=1, the NOT, NOR and integrative IMP, NOR and AND logic gates can be established. Based on DNA-Ag NCs, complex logic gates involving multiple inputs can be constructed to realize the transformation and transmission of chemical information, which has great application prospects in constructing new molecular devices.

Key words: Fluorescence detection, DNA template, Silver nanoclusters, Logic gate

中图分类号:

O652

TrendMD:

肖周锐,黄东华,边孟孟,袁亚利,聂瑾芳. 以DNA为模板的银纳米簇荧光检测及逻辑门的构建. 高等学校化学学报, 2020, 41(1): 102.

XIAO Zhourui,HUANG Donghua,BIAN Mengmeng,YUAN Yali,NIE Jinfang. Fluorescence Detection Based on DNA-templated Silver Nanoclusters and the Construction of Multi-level Logic Gate ^†. Chem. J. Chinese Universities, 2020, 41(1): 102.

图/表 12

Fig.1 UV-Vis(a), fluorescence excitation(b) and emission(c) spectra of DNA-Ag NCs(A), infrared spectra of DNA(a) and DNA-Ag NCs(b)(B), TEM images of DNA-Ag NCs with different magnifications(C, D)

Fig.2 Fluorescence(A) and UV-Vis absorption spectra(B) of DNA-Ag NCs(a) with Ni2+(b) and Hg2+(c) Inset of (A): fluorescence intensity change of DNA-Ag NCs with the addition of Hg2+ and Ni2+, respectively.

Fig.3 Fluorescence intensities of DNA-Ag NCs with Hg2+(a) and Ni2+(b) at different time interval

Fig.4 Fluorescence spectra of DNA-Ag NCs with Hg2+(A) and Ni2+(B) Insets: linear relationship between fluorescence intensity and concentration of ions.

Table1 Determination of Hg2+ and Ni2+ in tap water samples(n=3)

Ion	Spiked/(μmol·L^-1)	Detected/(μmol·L^-1)	Recovery(%)	RSD(%)
Hg²⁺	0.02	0.018	90.0	4.7
	0.08	0.078	97.5	1.2
	0.14	0.160	114.2	4.3
Ni²⁺	0.04	0.044	110.0	1.1
	0.15	0.164	109.3	1.9
	0.29	0.299	103.1	2.0

Fig.5 Influence of different factors on fluorescence of DNA-Ag NCs a. Cd2+; b. Cr3+; c. Cu2+; d. Hg2+; e. Ni2+; f. pH=3.0; g. pH=7.0; h. S2-; i. Cl-; j. Pb2+; k. Al3+.

Fig.6 Ni2+ as unitary input YES logic gate (A) Fluorescence spectra of DNA-Ag NCs with different inputs; (B) fluorescence intensity of YES gate; (C) logic gates symbol; (D) truth table.

Fig.7 Ni2+ and Hg2+ as binary input INH logic gate (A) Fluorescence spectra of DNA-Ag NCs with different input; (B) fluorescence intensity of INH gate; (C) logic gates symbol; (D) truth table.

Fig.8 Ni2+, Hg2+ and S2- as ternary input integrative NOR and INH logic gate (A) Fluorescence spectra of DNA-Ag NCs with different inputs; (B) fluorescence intensity; (C) logic gates symbol; (D) truth table.

Fig.9 S2- as unitary input NOT logic gate (A) Fluorescence spectra of DNA-Ag NCs with different inputs; (B) fluorescence intensity of NOT gate; (C) logic gates symbol; (D) truth table.

Fig.10 Hg2+ and S2- as binary input NOR logic gate (A) Fluorescence spectra of DNA-Ag NCs with different inputs; (B) fluorescence intensity of NOR gate; (C) logic gates symbol; (D) truth table.

Fig.11 Ni2+, H+, Hg2+ and S2- as quaternary input integrative IMP, NOR and AND logic gate (A) Fluorescence spectra of DNA-Ag NCs with different input combinations; (B) fluorescence intensity; (C) logic gates symbol; (D) truth table.

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