ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Junyi Zeng,Caiping Ding,Liang Chen,Bing Yang,Ming Li,Xiaoyuan Wang,Fengmei Su,Chuntai Liu,Youju Huang
Most enzyme catalysts are unable to achieve effective oxidation resistance because of the monotonous mimicking function or production of secondary reactive oxygen species (ROS). Herein, the Au@Cu2O heterostructure with multienzyme-like activities is deigned, which has significantly improved antioxidant capacity compared with pure Cu2O for the scavenging of highly cell-damaging secondary ROS, i.e.,·OH. Experiments and theoretical calculations show that the heterostructure exhibits a built-in electric field and lattice mismatch at the metal–semiconductor interface, which facilitate to generate abundant oxygen vacancies, redox couples, and surface electron deficiency. On the one hand, the presence of rich oxygen vacancies and redox couple can enhance the adsorption and activation of oxygen-containing ROS (including O2·– and H2O2). On the other hand, the electron transfer between the electron-deficient Au@Cu2O surface and electron donor would promote peroxide-like activity and avoid producing ·OH. Importantly, endogenous ·OH could be eliminated in both acidic and neutral conditions, which is no longer limited by the volatile physiological environment. Therefore, Au@Cu2O can simulate superoxide dismutase (SOD), catalase (CAT), peroxidase (POD), and glutathione peroxidase (GPx) to form a complete antioxidant system. The deigned nanoenzyme is explored in the real sample world such as A549 cells and zebrafish. This work provides theoretical and practical strategies for the construction of a complete antioxidant enzyme system.
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Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
An-qi Yang,Wentong Zheng,Xiaoyang Chen,Jiayin Wang,Shuang Zhou,Hongzhi Gao
In this paper, we demonstrate a surface-enhanced Raman spectroscopy (SERS) biosensor based on the self-assembly of gold nanorods (AuNRs) for the specific detection of airway inflammatory factors in diluted sputum. The AuNR surface was modified with an antibody that was able to specifically recognize an airway inflammatory factor, interleukin-5 (IL-5), so that a end-to-end self-assembly system could be obtained, resulting in an order of magnitude amplification of the Raman signal and greatly improved sensitivity. Meanwhile, the outer layer of the biosensor was coated with silicon dioxide, which improved the stability of the system and facilitated its future applications. When the detected concentration was in the range of 0.1–50 pg/mL, the SERS signal generated by the sensor showed a good linear relationship with the IL-5 concentration. Moreover, it had satisfactory performance in diluted sputum and clinical subjects with asthma, which could achieve sensitive detection of the airway inflammatory factor IL-5. Overall, the developed biosensor based on the SERS effect exhibited the advantages of rapid and sensitive detecting performance, which is suitable for monitoring airway inflammatory factors in sputum.
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MOLECULES
·
2023
·Vol. 28
·期 13
·5116
·
IF 4.6
Rongyu Tang,Yang Song,Lizhi Zhang,Ziliang Shi
Herein, we demonstrate the supramolecular assemblies from a bifunctional ligand on Au(111), towards engineering two-dimensional (metal-) organic multilevel nanostructures. The bifunctional ligand employed, including two Br atoms and one carboxylic terminal, offers multiple bonding motifs with different configurations and binding energies. These bonding motifs are highly self-selective and self-recognizable, and thus afford the formation of subunits that contribute to engineering multilevel self-assemblies. Our scanning tunneling microscopy experiments, in combination with the density functional theory calculations, revealed various hydrogen, halogen and alkali-carboxylate bonding motifs dictating the different levels of the assemblies. The multilevel assembly protocol based on a judicious choice of multiple bonding motifs guarantees a deliberate control of surface-confined (metal-) organic nanostructures. Our findings may present new opportunities for the fabrication of complex two-dimensional (metal-) organic nanostructures with potential in applications of functionally diverse nanomaterials.Keywords:two-dimensional supramolecular self-assembly;metal-organic coordination;surface;scanning tunneling microscopy;density functional theory
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ACS Sensors
·
2022
·
IF 9.618
Hongting Ma,Peihao Cheng,Chuanrui Chen,Xiaodong Geng,Kaizhou Yang,Fengjuan Lv,Junlin Ma,Yue Jiang,Quanli Liu,Yan Su,Jian Li,Nan Zhu
Unhealthy alcohol inhalation is among the top 10 causes of preventable death. However, the present alcohol sensors show poor selectivity among alcohol homologues. Herein, Pt-coated truncated octahedron Au (Ptm@Auto) as the electrocatalyst for a highly selective electrochemical sensor toward alcohol homologues has been designed. The alcohol sensor is realized by distinguishing the electro-oxidation behavior of methanol (MeOH), ethanol (EtOH), or isopropanol (2-propanol). Intermediates from alcohols are further oxidized to CO2 by Ptm@Auto, resulting in different oxidation peaks in cyclic voltammograms and successful distinction of alcohols. Ptm@Auto is then modified on wearable glove-based sensors for monitoring actual alcohol samples (MeOH fuel, vodka, and 2-propanol hand sanitizer), with good mechanical performance and repeatability. The exploration of the Ptm@Auto-based wearable alcohol sensor is expected to be suitable for environmental measurement with high selectivity for alcohol homologues or volatile organic compounds.
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Biomaterials Advances
·
2022
·
IF 0
Hua Tian,Jixuan Hong,Changgui Li,Yuheng Qiu,Mengting Li,Ziyu Qin,Reza A. Ghiladi,Xueqiong Yin
As bacterial infections continue to pose a significant challenge to healthcare globally, new therapeutic strategies, interventions, and complementary approaches that address both infection prevention and treatment are needed. As one such strategy, photothermal therapy (PTT) as a non-chemotherapeutic approach is considered a safe and potentially efficient strategy to combat bacterial infections, particularly for antibiotic-resistant pathogens given that PTT operates via a temperature-dependent process against which the development of bacterial resistance is unlikely. Here, we prepared Au@CDs composite nanoparticles (Au@CD) comprised of gold nanoparticles (AuNPs) and carbon dots (N,S-CDs), and investigated their use as a photothermal agent in PTT. The presence of the CDs as surface decorations conferred improved photothermal conversion efficiency, photostability, and biocompatibility to the Au@CD when compared to the parent AuNPs. To investigate if the Au@CD could serve as a PTT wound dressing and accelerate tissue repair, they were embedded within a PVA membrane via electrospinning. The resultant Au@CD membrane exhibited excellent biocompatibility and photothermal antimicrobial activity. In vitro photothermal antibacterial inactivation studies confirmed their efficacy against S. aureus and E. coli (99 + % inactivation of both pathogens under NIR irradiation). Moreover, in vivo studies employing Kunming male mice with S. aureus -infected wounds on their backs were chosen as a trauma model, with the Au@CD membranes serving as wound dressings. The results showed that a local temperature increased up to 50 °C upon NIR irradiation could effectively eradicate bacteria at the wound site, reduce the risk of bacterial infection, suppress inflammation as well as improve collagen deposition and angiogenesis, all of which together facilitated wound closure and resulted in a better therapeutic effect than the controls. Taken together, this work confirms that NIR-irradiated Au@CD-based membranes and related materials are promising photothermal antimicrobial platforms for wound dressings and related healthcare applications.
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Nanomaterials
·
2022
·Vol. 12
·期 18
·3221
·
IF 5.719
Wanzhen Meng,Yunrui Zhao,Dujuan Dai,Qianqian Zhang,Zeyan Wang,Yuanyuan Liu,Zhaoke Zheng,Hefeng Cheng,Ying Dai,Baibiao Huang,Peng Wang
Efficient and low-cost degradation of ethylene has always been a difficult problem in the storage and transportation of fruits and vegetables. Although photocatalysis is considered to be a feasible and efficient solution for ethylene degradation, the low degradation ability of conventional catalysts for small non-polar molecules limits its application. TiO2has the advantage of tunable microstructure, but it also has the defects of wide band gap and low utilization of sunlight. The surface plasmon resonance (SPR) effect of noble metals can effectively improve the visible light absorption range of catalysts, and the synergy of noble metals further enhances the photocatalytic ability. Herein, we developed a series of AuPt catalysts through the photo-deposition method. Benefited from the SPR effect and the synergy of Au and Pt, the efficiency of AuPt–TiO2was 19.9, 4.64 and 2.42 times that of TiO2, Au–TiO2and Pt–TiO2, and the photocatalytic degradation ability of AuPt–TiO2was maintained in five cyclic stability tests. Meanwhile, the transient photocurrent spectra and PL spectra proved that the light absorption capacity and carrier separation efficiency of AuPt–TiO2were enhanced. This work provides a new direction for enhancing non-polar small-molecule photodegradation of semiconductors.Keywords:surface plasmon resonance;Au–Pt nanoparticles;synergy;non-polar small molecules;photodegradation
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Nanomaterials
·
2022
·Vol. 12
·期 17
·2977
·
IF 5.719
Xiaoying Zhang,Xin Wang,Mengling Ning,Peng Wang,Wen Wang,Xiaozhou Zhang,Zhiming Liu,Yanjiao Zhang,Shaoxin Li
The biochemical composition of sweat is closely related to the human physiological state, which provides a favorable window for the monitoring of human health status, especially for the athlete. Herein, an ultra-simple strategy based on the surface-enhanced Raman scattering (SERS) technique for sweat analysis is established. Metal–phenolic network (MPN), an outstanding organic-inorganic hybrid material, is adopted as the reductant and platform for the in situ formation of Au-MPN, which displays excellent SERS activity with the limit of detection to 10−15M for 4-mercaptobenzoic acid (4-MBA). As an ultrasensitive SERS sensor, Au-MPN is capable of discriminating the molecular fingerprints of sweat components acquired from a volunteer after exercise, such as urea, uric acid, lactic acid, and amino acid. For pH sensing, Au-MPN/4-MBA efficiently presents the pH values of the volunteer’s sweat, which can indicate the electrolyte metabolism during exercise. This MPN-based SERS sensing strategy unlocks a new route for the real-time physiological monitoring of human health.Keywords:surface-enhanced Raman scattering;metal–phenolic network;sweat;molecular fingerprint;pH
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Dan Liu,Ismail Nadia,Chaohe Fang,Kuan He,Binghui Ge,Hailong Chen,Zhuo Chen
Hydrogenation of nitroaromatics to the corresponding amines plays a central role in the drug, fine chemical, and petrochemical industry. However, realizing hydrogenation through highly effective and environment-friendly methods remains a significant challenge. Here we demonstrated photo-enhanced catalytic activity for hydrogenation of nitrobenzene using Pt-Au/TiO 2 heterojunction as catalyst and hydrogen as reducing agent. The catalytic reaction rate improved 6.5 times under the simulated sunlight compared to the counterpart without light irradiation, and the TOF value of the catalytic reaction achieved as high as 7315 h −1 under light irradiation, better than the previously reported results. Further mechanism investigations indicate that light illumination can promote the activation of hydrogen and nitrobenzene molecules so that the catalytic performance improves significantly. This finding not only develops a green approach for the hydrogenation of nitroaromatics but also opens an avenue for designing high-efficiency photocatalysts.
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ACS Omega
·
2022
·
IF 4.132
Shenyi Ding,Jixiang Zhang,Cui Liu,Nian Li,Shudong Zhang,Zhenyang Wang,Min Xi
Gold nanospheres (Au NSs) and gold nanorods (Au NRs) are traditional noble metal plasmonic nanomaterials. Particularly, Au NRs with tunable longitudinal plasmon resonance from the visible to the near-infrared (NIR) range were suitable for highly efficient photothermal applications due to the extended light-receiving range. In this work, we synthesized Au NRs and Au NSs of similar volumes and subsequently developed them into Au NR/poly(vinylidene fluoride) (PVDF) and Au NS/PVDF nanofilms, both of which exhibited excellent solar photothermal performance evaluated by solar photothermal experiments. We found that the Au NR/PVDF nanofilm showed a higher solar photothermal performance than the Au NS/PVDF nanofilm. Through detailed analysis, such as morphological characterization, optical measurement, and finite element method (FEM) modeling, we found that the plasmonic coupling effects inside the aggregated Au NR nanoclusters contributed to the spectral blue shifts and intensified the photothermal performance. As compared to Au NS/PVDF nanofilms, the Au NR/PVDF nanofilm exhibited a higher efficient light-to-heat conversion rate because of the extended light-receiving range and high absorbance, as a result of the strong plasmonic interactions inside nanoclusters, which was further validated by monochromatic laser photothermal experiments and FEM simulations. Our work proved that the Au NRs have huge potential for plasmonic solar photothermal applications and are envisioned for novel plasmonic applications.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Yingnan Sun,Yuhan Song,Haohan Sun,Qingqing Tian,Qian Wang,Yongshu Liu,Shusheng Zhang
The efficient development of reliable surface-enhanced Raman scattering (SERS)-active plasmonic substrates containing hot spots via an extremely facile, simple, cost-effective method remains challenging in terms of batch-to-batch reproducibility and large-scale homogeneity. Herein, a universal, single-step strategy to transform superhydrophobic (SH) surfaces to large, label-free SERS substrates using Au nanoparticles (NPs) is developed. The transformed superhydrophobic (TSH) substrate with SERS characteristics was named as TSH-SERS platform. Three-dimensional (3D) stacked Au NPs with double-nanoareole structures are mounted on the 3D quasi-network with micro-/nanostructures, which serves as a skeleton. The SH surface with typical 3D quasi-network with micro-/nanostructures serves as a skeleton to tailor complex hierarchical structures for Au NP deposition. As the 3D stacked Au NPs with double-nanoareole structures did not alter the overall morphology of the SH surface at the micrometer level, the TSH-SERS substrates not only provided uniform, dense hot spots but also enabled the homogenized concentration of the diluted analytes with the aid of surface hydrophobility. In this work, only 5 μL of pure analyte is used in label-free SERS assay, and the final spot is uniformly distributed on the 3D plasmonic film without a “coffee-ring” effect during evaporative enrichment. TSH-SERS is evaluated through the quantitative SERS detection of Raman probes, bioanalytes, and pesticides in a serial concentration gradient to the picomolar level. Our strategy provides versatile routes for the facile transformation of various SH substrates into large, efficient 3D plasmonic films with double-nanoareole structures as cost-effective SERS platforms. The reliable detection also demonstrates the applicability of the TSH-SERS platform for the emerging demands for sensitive and high-throughput detection in practical applications, including biological sensing and environmental pollution monitoring.
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Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 25
·4789-4799
·
IF 7.571
Hao Chen,Yongxin Jiang,Tingting Xu,Jiangmei Xu,Jun Yu,Zhaoyou Chu,Yechun Jiang,Yongbo Song,Hua Wang,Haisheng Qian
The persistent progression of synovial inflammation and cartilage destruction contributes to the crosstalk between pro-inflammatory macrophages and activated fibroblast-like synoviocytes (FLSs) in a synovial microenvironment. In this work, structurally well-defined Au25 nanoclusters were synthesized to induce phenotypic polarization of pro-inflammatory macrophages and apoptosis of activated FLSs for enhanced rheumatoid arthritis treatment. These ultra-small nanoclusters significantly modulated phenotypic polarization of a pro-inflammatory M1 phenotype to an anti-inflammatory phenotype M2 for relieving inflammation. Additionally, Au25 nanoclusters can efficiently activate reactive oxygen species (ROS)-mediated apoptotic signaling pathways by inactivating thioredoxin reductase (TrxR), resulting in imbalance of the cellular redox homeostasis and initiation of FLS apoptosis. In an adjuvant-induced arthritis rat model, Au25 nanoclusters efficiently ameliorated the hyperplasia of the synovium and reduced inflammatory cell infiltration with negligible side effects. This study provided a new insight into Au nanoclusters for treating rheumatoid arthritis.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Ziqiong Yang,Xun Liu,Shiying Xia,Qiong Ding,Haiyan Liu,Zhengxi Wang,Long Zhang,Haibo Zhang
The discharges from urban industries and domestic sewages have caused severe environmental pollution problems. Specifically, dyes are among the pollution sources that are relatively difficult to treat. In this study, Au/CB6-BOFs (BOFs namely closo -dodecaborate-based supramolecular organic frameworks) were successfully synthesized using a simple method. The sample was used as adsorbent and degradation agents on Congo red (CR) and methyl orange (MO). The adsorption effect of Au/CB6-BOFs on CR is excellent with the adsorption capacity reaching as high as 2178.36 mg g −1 . Experiments, including adsorption kinetics , isothermal adsorption, and adsorption thermodynamics, were conducted on Au/CB6-BOFs to verify its performance, which confirmed that the adsorption type is monolayer chemical adsorption and that the reaction proceeds spontaneously. Au/CB6-BOFs can lead to catalytic degradation of dye molecules in aqueous solution with the addition of sodium borohydride. The adsorption/degradation ability of Au/CB6-BOFs can be maintained for at least five times without significant attenuating. FT-IR spectroscope and XRD were used to investigate Au/CB6-BOFs changes before and after experiments, there has been no obvious change observed in the FT-IR and XRD results. The catalytic mechanism was also proposed based on the degradation performance. In previous reports, it is might impossible to see similar nanomaterials that combine dye adsorption and dye degradation . If our material does either of them alone, it has a good effect. Considering that Au/CB6-BOFs have two functions at the same time, the initial concentrations of dyes that we set are relatively high, which is beyond the relevant literature reports. Therefore, it has certain reference value and impelling function to shorten the subsequent industrial treatment process of dye wastewater. This study provides a simple method to design and synthesis adsorption/degradation agents, which may open a new path for dye wastewater treatment .
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