Dual-Fermi-level hydrogel SERS substrates for synergistic chemical and physical enhancement

IF 4.6 2区 化学 Q1 SPECTROSCOPY
Jiadan Zhang , Baiwen Wei , Jingwen Zhang , Pengzhao Wang , Jiefeng Rong , Fengfu Fu , Zhenyu Lin , Yongqiang Dong
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Abstract

Surface enhanced Raman scattering (SERS) hydrogel substrates face limitations in chemical enhancement (CM) due to the single-metal Fermi level, restricting analyte detection. Herein, negatively charged silver nanoparticles (AgNPs) and positively charged gold nanoparticles (AuNPs) were engineered into bimetallic hydrogel substrates (AgNPs@AuNPs-chips). The obtained AgNPs@AuNPs-chips exhibited a strong localized surface plasmon resonance (LSPR) peak matching the 785 nm laser for significant electromagnetic (EM) enhancement, while the dual Fermi levels (−4.26 eV for Ag, −5.10 eV for Au) enabled more photo-induced charge transfer (PICT) pathways for CM. Compared to monometallic AgNPs-chips with similar LSPR properties, the bimetallic chips demonstrated better synergistic EM/CM effects for some molecules. When applied to detect maleic hydrazide (MH), the chips achieved a limit of quantitation of 10 ppb, surpassing prior AgNPs-chip methods (100 ppb). Successful quantitative analysis of MH in real-world samples with good recovery demonstrated the substrate's practicality. This work pioneers dual-Fermi-level colloidal interfacial design, expanding SERS applicability in food safety.

Abstract Image

双费米水平水凝胶SERS底物的协同化学和物理增强
由于单金属费米能级的限制,表面增强拉曼散射(SERS)水凝胶底物在化学增强(CM)方面受到限制,限制了分析物的检测。在这里,带负电的银纳米粒子(AgNPs)和带正电的金纳米粒子(AuNPs)被设计成双金属水凝胶底物(AgNPs@AuNPs-chips)。获得的AgNPs@AuNPs-chips显示出与785 nm激光相匹配的强局部表面等离子体共振(LSPR)峰,具有显著的电磁(EM)增强,而双费米能级(Ag为- 4.26 eV, Au为- 5.10 eV)为CM提供了更多的光诱导电荷转移(PICT)途径。与具有相似LSPR性能的单金属agnps芯片相比,双金属agnps芯片对某些分子具有更好的EM/CM协同效应。当用于检测马来酰肼(MH)时,芯片达到了10 ppb的定量限制,超过了先前的agnps芯片方法(100 ppb)。实际样品中MH的定量分析成功,回收率高,证明了底物的实用性。这项工作开创了双费米能级胶体界面设计,扩大了SERS在食品安全中的适用性。
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来源期刊
CiteScore
8.40
自引率
11.40%
发文量
1364
审稿时长
40 days
期刊介绍: Spectrochimica Acta, Part A: Molecular and Biomolecular Spectroscopy (SAA) is an interdisciplinary journal which spans from basic to applied aspects of optical spectroscopy in chemistry, medicine, biology, and materials science. The journal publishes original scientific papers that feature high-quality spectroscopic data and analysis. From the broad range of optical spectroscopies, the emphasis is on electronic, vibrational or rotational spectra of molecules, rather than on spectroscopy based on magnetic moments. Criteria for publication in SAA are novelty, uniqueness, and outstanding quality. Routine applications of spectroscopic techniques and computational methods are not appropriate. Topics of particular interest of Spectrochimica Acta Part A include, but are not limited to: Spectroscopy and dynamics of bioanalytical, biomedical, environmental, and atmospheric sciences, Novel experimental techniques or instrumentation for molecular spectroscopy, Novel theoretical and computational methods, Novel applications in photochemistry and photobiology, Novel interpretational approaches as well as advances in data analysis based on electronic or vibrational spectroscopy.
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