Alloyed AuPt nanoframes loaded on h-BN nanosheets as an ingenious ultrasensitive near-infrared photoelectrochemical biosensor for accurate monitoring glucose in human tears
Introduction
Glucose biosensors have attracted extensive research due to their potential application in clinical diagnostic biology, fuel cell, biotechnology and food monitoring, etc. (Yoo et al., 2010; Basu et al., 2010; Barman et al., 2012; Adriaenssens et al., 2019). Especially, the highly sensitive biosensors with rapid response and excellent reliability, can realize the precise assessment of glucose concentration in human body, playing a critical role in the diagnosis and treatment of diabetes mellitus (DM) (Kownacka et al., 2018; Salsali and Nathan, 2006; Han et al., 2020). Some alternative glucose biosensors based on saliva (Arakawa et al., 2016), sweat (Han et al., 2020; Toi et al., 2019), tear (Romeo et al., 2018; Yao et al., 2011) and urine (Karim et al., 2018) have recently garnered considerable interest, since they can effectively reduce inconveniences during the invasive method of blood sampling with needle bleeding. In particular, glucose monitoring in tear fluid with a typical glucose range of around 0.1–0.6 mM (Yao et al., 2011) has been regarded as an appealing way to indirectly reflect the situation of blood glucose. Up to now, numerous glucose detection techniques were already proposed, such as electrochemistry, chemiluminescence, spectrophotometry and colorimetry, etc. (Wang, 2008; Li et al., 2017; Yamakoshi et al., 2006; Huang et al., 2016). Especially, the electrochemical sensing can be served as one of the most promising methods owing to fast response, high stability, sensitivity, repeatability, high precision, low power consumption and cost-effectiveness (Chen et al., 2020; Chiu et al., 2020; Nantaphol et al., 2017). Besides the electrocatalysis, the oxidation of glucose molecules through photocatalysis is also a feasible method, which is usually applied in the field of photon energy conversion (Madriz et al., 2020; Zhou et al., 2016; Iervolino et al., 2018). Therefore, the novel photo-electro-chemical (PEC) reaction can simultaneously take advantage of both photocatalytic reaction via the utilization of photon energy and the electrocatalytic oxidation through extra electric field (Yang et al., 2020; Wang et al., 2017; Li et al., 2012). Compared to the mere electrochemical or photocatalytic technique, the ingenious PEC biosensor can possess higher applicability for ultrasensitive glucose monitoring in diverse fields.
As for the PEC biosensor, it should not only exhibit superior electrocatalytic performance towards the reactions occurring at both anode and cathode, but also have the effective plasmonic effect with the high capacity of harvesting light in the broad wavelength range to induce the oscillation charge carriers (Li et al., 2021; Chao et al., 2019; Linic et al., 2015). In this way, plasmonic Au-based nanocomposites (NCs) have been frequently used in direct plasmon-accelerated electro-oxidation and constructed a plasmon-improved glucose electrochemical sensor (Wang et al., 2017, 2019). For instance, Au/NiAu multilayered nanowire (Wang et al., 2018) and AuNi nanodendrite arrays (Wang et al., 2019) as well as the Au–NiO1–x (0 < x < 1) hybrid nanowire (Wang et al., 2020) were proposed as novel plasmon aided non-enzymatic glucose biosensors. In addition, the local surface enhanced resonance (LSPR) of Au NCs can still be stimulated by monochrome blue or green LED illumination, improving the sensitivity of glucose biosensor (Hsu et al., 2017). On the other hand, despite numerous great achievements in the construction of PEC biosensors, there is still an urgent issue to be considered in this field. Most of pervious works merely focused on the shorter wavelength (violet-visible) light-accelerated PEC glucose monitoring, while the near infrared (NIR) light is seldomly involved in PEC biosensors. The main reason is that the simple and discontinuous Au nanoparticles (NPs) with inherent LSPR peak at ~520 nm are usually adopted in glucose biosensors, determining the PEC reactions were restricted to violet-visible light excitation with higher photon energy. It is well known that the excellent NIR response-harvest-conversion can be effectively realized by construction of diverse anisotropic Au-based nanostructures (nanorods (Yoshii et al., 2019; Yoshii et al., 2021), nanostars (Peng et al., 2018), nanoporous (Lu et al., 2018), nanodendrites (Wang et al., 2019), etc.). Compared with ultraviolet or visible light, the NIR light that accounts for over 50% of solar energy (Liu et al., 2019) can be served as a biological tissue optical window, reaching a maximum depth in biological tissue with low photo-damage and having minimum interference from background autofluorescence in living biosystems (Cao et al., 2020; Liu et al., 2020). Therefore, superior to shorter wavelength excitation, the anticipated NIR-PEC glucose biosensor with multiple fascinating features is more suitable for practical glucose monitoring in diagnose, surgery and therapy.
Herein, we rationally proposed an appealing NIR-PEC glucose biosensor by loading alloyed Pt/Au nanoframes on 2D h-BN nanosheets, which can be effectively used to achieve broadband light response-harvest-conversion from visible to NIR region. Obviously, the obtained h-BN/Au5Pt9 nanoproducts with Au/Pt ratio of 5/9 after appropriate annealing at 200 °C for 2 h possess a remarkable higher PEC activity under visible-NIR light excitation, as compared to the other as-prepared h-BN/AuPt references. Adopting 808 nm NIR excitation, the optimal h-BN/Au5Pt9 nanoframes served as a novel NIR-PEC biosensor can provide accurate and ultrasensitive glucose monitoring of human tears, reaching a detection concentration range of 0.03–100 μM and a low detection limit of 0.406 nM. The corresponding schematic diagram was shown in Scheme S1 in Supporting Information (SI). Moreover, the excellent selectivity, reproductivity and long-term stability of h-BN/Au5Pt9-based NIR-PEC glucose biosensor will be favorable for ultrasensitive NIR-PEC glucose monitoring of clinical diagnostics in the near future.
Section snippets
Experimental setup
The experimental chemicals, characterization and experimental methods are provided in SI.
Characterization of h-BN/AuPt NCs
The h-BN/Pt (Section S1 in SI) can be used as the precursors for overgrowth of bimetallic Pt/Au core-shell structure via the galvanic replacement reaction. Then, the structural characterizations of the obtained h-BN/Pt/Au are measured by transmission electron microscopy (TEM) in Fig. 1(a). The Pt/Au on h-BN supports have obvious solid cores with darker contrasting light images and thick shell architectures, which are randomly bonded to each other on the 2D surfaces. Besides the fringe distance
Conclusion
An interesting NIR-PEC biosensor based on alloyed h-BN/Au5Pt9 nanoframes has been established for ultrasensitive glucose monitoring in human tears. The h-BN/Au5Pt9 nanoframes with enhanced intermetallic synergetic effect provide a significantly improved electrocatalytic performance. Moreover, the uniform alloyed framework-like feature enables the h-BN/Au5Pt9 nanoframes to exhibit a broader and stronger absorption across visible-NIR region, which can further improve the catalytic activity upon
CRediT authorship contribution statement
Yue Tian: Methodology, Data curation, Formal analysis, Investigation, Writing – original draft. Qingqiang Cui: Methodology, Data curation. Linlin Xu: Data curation, Investigation. Anxin Jiao: Data curation, Investigation. Hui Ma: Data curation, Investigation. Chang Wang: Data curation, Investigation. Mengya Zhang: Data curation, Investigation. Xuelin Wang: Data curation, Investigation. Shuang Li: Supervision, Writing – review & editing, Funding acquisition. Ming Chen: Supervision,
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgments
This work was financially supported by the National Natural Science Foundation of China (NSFC) (Nos. 11905115 and 11575102), Shandong Jianzhu University XNBS Foundation (No. 1608) and Fundamental Research Fund of Shandong University (No. 2018JC022).
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