Effect of Anion-Directed Structural Tuning of Triazole-Containing Ag(I) Coordination Polymers for “Turn-on” Sensing of the Disulfide (−S–S−) Amino Acid over the Monosulfide (−SH) Form: Experiments and DFT Corroboration

IF 4.7 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Sourav Bej, Xintian Wang, Hongbiao Huang, Zhonghang Chen, Wei Shi, Xuemei Yang* and Peng Ren*, 
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Abstract

Identification of disulfide-peptide-bond-containing glutathione (GSSG) over the monosulfide form (GSH) remains a very challenging task because of their identical chemical properties. Although GSH detection has been well documented, selective detection of GSSG has rarely been reported. Here, four cationic Ag-based coordination polymers (Ag CPs) were synthesized using newly synthesized monotriazole linker 3-amino-5-(4H-1,2,4-triazol-4-yl)pyridine to selectively screen GSSG over GSH. The judicious choice of the counteranion in the metal salt changes the architecture, which affects the detection limit at the parts per million level. The restriction of the photoinduced electron transfer process is the driving reason for the enhancement of the fluorescence, owing to the favorable energy band gap match of the Ag CPs with GSSG over GSH. The de novo strategy for incorporating polar heteroatoms (N) into the CP network plays a pivotal role in the host–guest noncovalent interactions with donor–acceptor transfer of electrons, which was supported by X-ray photoelectron spectroscopy and density functional theory studies. The Ag CPs are thermochemically robust, recyclable, and work efficiently in a very short time (within ∼14–18 s) in different pH ranges. Additionally, detection of GSSG in serum samples was carried out with appreciable detection limits and recovery percentages (94.40–117.89%).

Abstract Image

阴离子定向结构调谐对含三唑银(I)配位聚合物对二硫(- S-S -)氨基酸在单硫(- SH)形式上的“开启”感应的影响:实验和DFT确证
由于含有二硫肽键的谷胱甘肽(GSSG)与单硫形式的谷胱甘肽(GSH)具有相同的化学性质,因此鉴定它们仍然是一项非常具有挑战性的任务。虽然谷胱甘肽检测已经有了很好的文献记载,但选择性检测GSSG很少有报道。本研究利用新合成的单三唑连接剂3-氨基-5-(4h -1,2,4-三唑-4-基)吡啶合成了4种银基阳离子配位聚合物(Ag CPs),以选择性筛选GSSG对GSH的影响。金属盐中反阴离子的合理选择会改变结构,从而影响百万分之一水平的检测限。由于Ag CPs与GSSG比GSH具有良好的能带隙匹配,光致电子转移过程的限制是其荧光增强的驱动原因。将极性杂原子(N)纳入CP网络的从头策略在主-客体非共价相互作用中起着关键作用,电子的供体-受体转移得到了x射线光电子能谱和密度泛函理论研究的支持。Ag CPs在不同的pH范围内具有热化学稳定性、可回收性,并且在很短的时间内(约14-18秒)有效地工作。此外,对血清样品进行了GSSG检测,检出限和回收率均在94.40 ~ 117.89%之间。
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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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