ACS Applied Nano Materials
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2022
·
IF 6.14
Yifan Yu,Lu Ma,Linling Qin,Wenxiang Lu,Cheng Zhang,Shaolong Wu,Xiaofeng Li
Photoelectrochemical (PEC) biosensors show great potential in biochemical molecular detection due to the advantages of low background noise, high sensitivity, and easy integration. However, the current PEC glucose biosensors are subject to the deficiencies of the relatively large limit of detection, small detectable range of concentration, and requirement of an operation voltage. Herein, we construct an unbiased glucose biosensor both in three- and two-electrode configurations using a glucose oxidase (GOx)-modified Schottky junction comprised of Au nanoparticle (NP)-decorated TiO2-coated Al films. A wide detectable range of concentration (0.3–104 μM) is achieved at relatively zero bias versus the reference electrode in a three-electrode configuration under AM 1.5G illumination along with a fitted sensitivity of 3780 μA mM–1 cm–2 (in the concentration range of 0.3–1.0 μM) and a limit of detection down to 0.05 μM. The photocurrents corresponding to typical interfering substances (e.g., uric acid and ascorbic acid) are less than 10% of that to glucose. Moreover, the constructed sensor achieves almost no attenuation in photocurrent under light ON/OFF circular irradiation for 30 min and shows a photocurrent around 92% of the initial value after 30-day storage in air at room temperature. The satisfactory sensing performance is ascribed to the following three aspects: (1) the optical absorption is enhanced due to the formation of a plane-parallel resonance cavity and the reduced band gap of the TiO2 material, (2) the separation and extraction of the photogenerated carriers are facilitated due to the Al doping and the embedded Schottky junction, and (3) the carrier transfer from the photoelectrode surfaces into the electrolyte is boosted because of the Au NPs and nanostructured GOx decoration. This work provides an alternative route to prepare high-performance and self-powered glucose sensors for diabetes diagnosis.
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Journal of Physical Chemistry C
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2022
·
IF 4.177
Wei Liu,Hongpeng Liu,Yatian Liu,Zejian Dong,Langli Luo
In heterogeneous catalysis, specific surface planes of metals and/or supports have a prominent effect on the catalytic processes, i.e., adsorption, dissociation of reactants, and electron transfer behaviors. In addition, surface planes of oxide supports have a direct impact on the shape and dispersion of metal particles through a metal–support interaction. Herein, we synthesized ZnO nanoplates (p-ZnO) exposing mostly polar surfaces and ZnO nanorods (r-ZnO) exposing non-polar surfaces and used them as supports to prepare Au/ZnO catalysts. Then, the surface plane effect of ZnO was demonstrated by employing the CO oxidation reaction. We found that the activity of Au/p-ZnO is superior to that of Au/r-ZnO, which is due to more O2 activation sites on polar surfaces than on non-polar surfaces. Furthermore, Au can activate both polar and non-polar surfaces of ZnO by creating more oxygen vacancies for O2 activation. This study highlights the effects of different surface planes of oxides in catalytic reactions and provides new insights for the development of highly active metal-oxide catalysts.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Qingyi Wei,Qirong Dong,Da-Wen Sun,Hongbin Pu
Surface-enhanced Raman spectroscopy (SERS) substrates based on metal/semiconductors have attracted much attention due to their excellent photocatalytic activity and SERS performance. However, they generally exhibit low light utilization and photocatalytic efficiencies. Herein, molybdenum disulfide coated titanium dioxide modified with gold nanoparticles (MoS 2 @TiO 2 @Au) as a heterojunction-based recyclable SERS platform was fabricated for the efficient determination of fungicides. Results showed that the MoS 2 @TiO 2 @Au platform could rapidly degrade 90.7% crystal violet in 120 min under solar light irradiation and enable reproducible and sensitive SERS analysis of three fungicides (methylene blue, malachite green, and crystal violet) and in-situ monitor of the photodegradation process. The platform could also be reused five times due to the unique integrated merits of the MoS 2 @TiO 2 @Au heterojunction. Meanwhile, experiments in determining methylene blue in prawn protein solution achieved a limit of detection of 1.509 μg/L. Therefore, it is hoped that this work could expand detection applications of photocatalytic materials.
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FOOD CHEMISTRY
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2021
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IF 7.514
Zhihui Wu,Da-Wen Sun,Hongbin Pu,Qingyi Wei,Xuanran Lin
Mycotoxin B1 (AFB1) contamination in agricultural products pose a deadly danger to animal and human health and its rapid and reliable detection is thus very important. Herein, a ratiometric surface-enhanced Raman scattering (SERS) aptasensor for AFB1 detection was developed, in which 1,2-bis(4-pyridyl) ethylene (BPE) was used to trigger the assembly of Au nanoparticle dimers (AuNP dimers) and form intensive SERS “hot spots”, and MXenes nanosheets could load aptamer-modified AuNP dimers due to the hydrogen bonding and the chelation between the phosphate groups of aptamers and the Ti ion of MXenes. With the presence of AFB1 preferentially binding to AFB1 aptamer, AuNP dimers were separated from MXenes nanosheets, leading to a decrease in SERS intensity. Regression analysis in the range from 0.001 to 100 ng·mL −1 showed the limit of detection (LOD) being 0.6 pg·mL −1 in standard solution, indicating that the great prospects of the AuNP dimers/MXenes SERS substrate for detecting AFB1.
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Green Energy & Environment
·
2021
·
IF 8.207
Weiyao Yang,Mengchen Fu,Chenyu Yang,Yiwen Zhang,Chun Shen
Despite wide applications of noble metal-based catalysts in 5-hydroxymethylfurfural (HMF) oxidation, promoting the catalytic performance at low loading amounts still remains a significant challenge. Herein, a series of metal oxide modified MO x -Au/TiO 2 (M = Fe, Co, Ni) catalysts with low Au loading amount of 0.5 wt% were synthesized. Addition of transition metal oxides promotes electron transfer and generation of the Au δ − –O v –Ti 3+ interface. A combination study reveals that the dual-active site (Au δ − -O v -Ti 3+ ) governs the catalytic performance of the rate-determining step, namely hydroxyl group oxidation. Au δ − site facilitates chemisorption and activation of O 2 molecules. At the same time, O v -Ti 3+ site acts as the role of “killing two birds with one stone”: enhancing adsorption of both reactants, accelerating the activation and dissociation of H 2 O, and facilitating activation of the adsorbed O 2 . Besides, superoxide radicals instead of base is the active oxygen species during the rate-determining step. On this basis, a FDCA yield of 71.2% was achieved under base-free conditions, complying with the “green chemistry” principle. This work provides a new strategy for the transition metal oxides modification of Au-based catalysts, which would be constructive for the rational design of other heterogeneous catalysts.
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Yuting Hu,Shixing Wang,Libo Zhang
A novel Cu-based bisligand metal organic framework adsorbent (Cu-BMOF) was prepared by hydrothermal method using 5-methyl-2-thiophenecarboxylic acid and 4,4-azopyridine as organic linkers. The samples were analyzed by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD) and zeta potentiometry (Zeta). To investigate the adsorption performance of Cu-BMOF for Au(III), the effects of pH, temperature, adsorption time and initial concentration were explored. At 298 K and pH = 2, the maximum adsorption capacity of Cu-BMOF for Au(III) is 933 mg/g. Langmuir and quasi-second-order models can describe the adsorption process well. Au(III) adsorption on Cu-BMOF is a monolayer and irreversible chemisorption process. Thermodynamic studies show that the adsorption process of gold on Cu-BMOF is exothermic and spontaneous. The response surface method (RSM) was applied to optimize the adsorption efficiency. Under optimal conditions, the adsorption rate was 99.64%. X-ray photoelectron spectroscopy (XPS) results show that the adsorption mechanism of Cu-BMOF is the binding between Au (III) and the N, and S functional groups of Cu-BMOF. In addition, the affinity of Cu-BMOF for Au(III) is superior compared with that of coexisting ions in water. Cu-BMOF have promising applications in environmental protection and water purification .
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Plasmonics
·
2021
·Vol. 17
·期 2
·597-612
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IF 2.404
Li Jian-Jun,Qin Qiu-Xiang,Weng Guo-Jun,Zhu Jian,Zhao Jun-Wu
In this study, Au–Ag nanoboxes are converted into Au–Ag alloy nanocages by increasing the hole size. The extinction spectrum and the refractive index sensing characteristics of Au–Ag alloy nanocages with different geometric parameters are studied by using discrete dipole approximation method (DDA). With the increase of Au composition, the peak of local surface plasmon resonance (LSPR) shows approximately linear redshift and the sensitivity factor shows approximately linear decrease. The refractive index sensitivity can be effectively controlled by the Au–Ag ratio at large hole size because the hole and cavity surfaces distribute more environmental dielectric components. Therefore, increasing the hole size and decreasing the Au–Ag ratio can improve the refractive index sensitivity. These calculation results have also been verified experimentally. In order to illustrate the influence of alloy composition on the LSPR characteristics and the refractive index sensitivity, the local electric field distributions under different geometric parameters are plotted. We find that the electric field direction on the hole and cavity surfaces is controlled by the Au–Ag ratio and environmental dielectric constant. Moreover, the field vectors on the hole and cavity surfaces are formed by the superposition of the incident field, the electric field generated by the oscillating electrons on the outer surface, and the polarized field in the environmental dielectric constant.
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Journal of Physical Chemistry C
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2021
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IF 4.126
Chen Ding,Zijie Mao,Jia-Shun Liang,Xianxian Qin,Qing Zhang,Fan Yang,Qing Li,Wen-Bin Cai
The commercialization of proton exchange membrane fuel cells (PEMFCs) calls for the development of active and durable Pt-based catalysts for oxygen reduction reaction (ORR) by means of a cost-effective and environmentally benign protocol. We report herein an all aqueous phase preparation of carbon supported Au-modified Pt–Co alloy catalyst (Au/Pt–Co/C), which involves the dimethylamine borane co-reduction of aqueous Pt(II) and Co(II) precursors to form a Pt–Co/C catalyst and the ethanol reduction of an aqueous Au(III) precursor to form Au/Pt–Co/C. This Au/Pt–Co/C catalyst not only shows a greatly enhanced ORR activity like the homemade Pt–Co/C and state-of-art Pt–Co/C(com) catalysts as compared to the Pt/C catalyst but also exhibits a much higher durability over the Pt/C(com), homemade Pt–Co/C, and state-of-art Pt–Co/C(com) catalysts in accelerated degradation tests (ADTs) with both half-cell and single-cell configurations. Specifically, the maximum power density of a PEMFC involving the Au/Pt–Co/C cathode suffers only a 6% loss after 30 000 cycles of a standard ADT while that involving the state-of-art Pt–Co/C(com) suffers a 37% loss. This research provides an alternative route to prepare efficient and durable Pt-based ORR catalysts toward a widespread application of PEMFCs.
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LANGMUIR
·
2021
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IF 3.882
Mengjiao Yi,Lin Ma,Wenrong Zhao,Jie Zhao,Qi Fan,Jingcheng Hao
Cationic magnetic Gemini surfactants (mag-G-surfs), [C14H29(CH3)2N(CH2)2N(CH3)2C14H29]2+·2[XCl3Br]− (14-2-14·2X, X = Ce, Gd, or Ho), efficiently induce the aggregation of glutathione-protected Au nanoclusters (NCs) (GSH-Au NCs). These magnetic luminescent aggregates not only possess aggregation-induced emission (AIE) behavior but also display aggregation-induced magnetic enhancement. In particular, 14-2-14·2Ce and 14-2-14·2Gd have a better effect on boosting the luminescence intensity, quantum yield (QY), and luminescence lifetime (τ). The luminescent aggregates of GSH-Au NCs triggered by 14-2-14·2Gd or 14-2-14·2Ho exhibit more favorable paramagnetic behavior. Other Au NCs containing a Au(I)–thiolate complex shell also exhibit the obvious AIE phenomenon after introducing 14-2-14·2Gd, demonstrating the luminescence enhancement effect of mag-G-surfs. The luminescent aggregate 14-2-14·2Ce@GSH-Au NCs can serve as a “light up” fluorometric probe to detect cysteine selectively with the detection limit (DL) of 36 μM, and the magnetic luminescent aggregate 14-2-14·2Gd@GSH-Au NCs has the potential to be a novel contrast agent in T1-weighted magnetic resonance (MR) imaging due to its satisfactory contrasting ability.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 5
·1-10
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IF 5.833
Gu Ying,Hu Yuanling,Zhang Fuyuan,Yi Lunzhao,Shang Ying,Ren Dabing,Ge Zhenhua
A glucose (Glu) sensor was designed by introducing synthetic cyclic peptides (CPs) as recognition receptors and Au nanoparticles assisted graphitic carbon nitride (AuNPs/g-C 3 N 4 ) for electrochemiluminescence (ECL) enhancement. The synthetic CP receptor (cyclo-[−CNDNHCRDNDC−]) with natural active center of Glu binding protein can mimic the interactions between Glu and Glu binding protein to specifically capture Glu. The AuNPs were reduced on g-C 3 N 4 and formed a new nanohybrid that can be applied as an ECL emitter. The AuNPs/g-C 3 N 4 effectively ameliorated the ECL response of bare g-C 3 N 4 . The ECL enhancement mechanism was theoretically speculated through computer simulation. Glu quantification was conducted by recording ECL shifts induced by the binding of Glu to CPs. The linear detection range of the fabricated CPs-based ECL sensor was 1 to 100 mmol L −1 , and the detection limit (LOD) was 0.57 nmol L −1 (S / N = 3). The CP-based ECL sensor also showed good specificity, repeatability, stability, and favorable recoveries in sample analysis. This work offer a promising analytical method for Glu assay in clinical diagnostics and bioprocess monitoring. Graphical abstract
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2021
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IF 4.098
Kaiqiang Wang,Jinjie Li
The fabrication of sensitive and reliable interfacial plasmonic platform for measuring chemical contaminants in various phases is an exciting topic in the food industry and for environment monitoring. In this study, a high-performance surface-enhanced Raman spectroscopy (SERS) analytic platform was developed through self-assembly of the gold@4-mercaptobenzoic acid@silver nanoparticles (Au@4-MBA@Ag NPs) at the cyclohexane/water interface. By addition of the inducer ethanol, the Au@4-MBA@Ag NPs in aqueous phase was effectively migrated to the biphasic interface, forming a large-scale close-packed nanoparticle array. The average gap between adjacent nanoparticles was smaller than 3 nm, where intensive SERS “hot spots” were created for high-sensitive detection. Furthermore, using the sandwiched 4-MBA molecule as the internal standard to correct the Raman signal fluctuations, the point-to-point and batch-to-batch reproducibility of Au@4-MBA@Ag array were improved with lower relative standard deviation (RSD) values of 8.84% and 14.97%, respectively, and pesticides (thiram and thiabendazole) analysis in both aqueous and organic phases were achieved with higher accuracy (R 2 of 0.986 and 0.990) as compared with those without 4-MBA correction (R 2 of 0.867 and 0.974). The high-throughput fabrication of the self-assembled nanoparticle array is a promising approach for development of a sensitive and reliable SERS platform for chemical contaminants monitoring in multiphase.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 22
·13080-13086
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IF 12.732
Mei Zhang,You Xu,Shengqi Wang,Mengying Liu,Lianbang Wang,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
How to boost the electrocatalytic performance of non-Pt catalysts for the hydrogen evolution reaction (HER) to substitute Pt is an important research topic. Herein, by combining a one-pot wet-chemical method and the post surface functionalization, we successfully fabricated polyethylenimine (PEI)-modified bimetallic Au@Rh core–shell mesoporous nanospheres (Au@Rh@PEI MNs). Benefiting from the synergetic effects of Au@Rh core–shell mesoporous architectures and interfacial modification by PEI molecules, the resultant Au@Rh@PEI MNs exhibit excellent electrocatalytic activity and stability for the HER in all pH value solutions, which even surpass the benchmark commercial Pt/C catalyst. Our synthetic protocol may offer guidelines for the rational design of advanced catalysts for water splitting and other electrocatalytic applications.
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