NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 20
·9595-9601
·
IF 3.925
Hongbo Wu,Yingjie Xu,Ruyan Xie,Mingyu Tang,Lihua Chen,Fengyu Qu,Changhong Guo,Fang Chai
Facile and accurate detection of dopamine (DA) in biological samples is crucial for diagnostic needs. This study reports a portable colorimetric fluorescent probe for the tracing of DA based on orange-red emitting Au nanoclusters (AuNCs). The AuNCs were reduced and stabilized with L-methionine by strictly controlling the reaction conditions. The resultant L-methionine capped AuNCs (M-AuNCs) exhibit bright and stable orange-red emission with a quantum yield of 31.08%. The excitation/emission wavelength is located at 420 nm/610 nm, and the large Stoke's shift of 190 nm endows the M-AuNCs with great potential as a late-model sensing probe for life studies and environmental science. The M-AuNCs exhibit unique specificity and excellent sensitivity for tracing DA by an “on–off” strategy with a lower limit of detection (LOD) of 3.96 nM (S/N = 3) within a linear range of 10–100 nM. Notably, the colorimetric detection results can be explored as a visual sensor for sensitive, reliable and real-time/on-site detection of DA with the assistance of a smartphone. The LOD can be determined as 81.94 nM within a wide linear range of 0.1–1.0 μM by a smartphone. Furthermore, the M-AuNCs as a late-model potable probe allow simple and rapid discrimination of DA in serum, and the cellular imaging of the M-AuNCs indicated that the detection of DA can also be achieved in living cells, demonstrating their great feasibility for the tracing of DA in real samples.
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LANGMUIR
·
2022
·
IF 4.331
Xin Kou,Yutian Ma,Congming Pan,Yong Huang,Yulai Duan,Ying Yang
Ionic polymers have been proven to be promising adsorbents in recovering Au(III) due to their advantages of simple synthesis and high adsorption efficiency. However, the unclarity of the relationship between the adsorption ability of ionic polymers and their cationic structures hinders further optimization of their adsorption performance. This study synthesized a series of ionic polymers with pyridinium, imidazolium, piperidinium, pyrrolidinium, and triethylammonium cations to discover the effects of the cationic structure on their adsorption properties. Experimental results show that the existence of anion−π interaction between aromatic cations and [AuCl4]− makes the aromatic cations–anion interaction stronger, which does not enhance the adsorption performance of the aromatic-based ionic polymer. This is due to the charge delocalization in the aromatic ring, resulting in a lower electrostatic potential (ESP) of aromatic cations than that of aliphatic cations with a localized charge. The higher the ESP of cations, the better the adsorption performance of the corresponding ionic polymer. This study serves as a deep understanding of the cationic structure–adsorptive performance relationship of the ionic polymer at the molecular level and further provides a theoretical guidance to optimize the adsorption performance of ionic polymers.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2022
·
IF 7.129
Dandan Kong,Xinyue Li,Yang Tang,Ming Sui,Jinping Li,Yonggui Ma,Gaofeng Wang,Wei Gu,Xuegang Guo,Meihua Yang
Environmental pollution and medicine safety have aroused increasing public concerns due to human health. Amongst various contaminants, mercury is of special attention owing to their environmental persistence and biogeochemical recycling and ecological risks. Herein, a simple and highly parallel electrochemical biosensor for Hg determination was designed and investigated. The proposed biosensor was prepared and compared between (1) DTT/MB-DNA/Au with configuration occupation approach and (2) MCH/MB-DNA/Au with passivation approach. According to the combined results of scanning electrochemical microscope (SECM) and Randles-Sevcik equation, the DTT modified electrode exhibited high uniformity on DNA distribution and superb stability on electron transfer in Hg 2+ detection. Evidentially, the response value of proposed DTT/MB-DNA/Au was increased from 57.518% to 97.607%, while RSD% between duplicate runs had dropped from 22.658% to 0.223% (n = 3). Moreover, the increased proportion of effective working area was 467.380% compared with general sensors. Besides, DTT concentration, DNA concentration as well as assembly time were optimized, utilizing electrochemical impedance spectroscopy (EIS), Cyclic Voltammetry (CV) and Square Wave Anode Stripping Voltammetry (SWASV). This optimized biosensor exhibited an excellent selectivity toward Hg 2+ over Cu 2+ , As 2+ , Cd 2+ , Pb 2+ , Cr 3+ , Ni 2+ and Zn 2+ etc., and the stability of DTT/MB-DNA/Au were at least two times better even after 3 days under room temperature. Also, a linear relation was observed between the peak current and Hg 2+ concentrations in a range from 0.25 nM to 2.00 μM with a detection limit of 53.00 pM under optimal conditions. Finally, DTT/MB-DNA/Au was applied for plants and medical products analysis. In all, this optimized DTT/MB-DNA/Au with advantages of high repeatability and sensitivity would provide a new insight into the design and application of biosensor for reliable sensing in safeguarding plant protection and medicinal safety.
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Nanoscale
·
2022
·Vol. 14
·期 12
·4538-4547
·
IF 8.307
Yanjun Yang,Chunyuan Song,Jingjing Zhang,Jie Chao,Hoang Mai Luong,Yiping Zhao,Lianhui Wang
To sensitively detect multiple and cross-species disease-related targets from a single biological sample in a quick and reliable manner is of high importance in accurately diagnosing and monitoring diseases. Herein, a surface-enhanced Raman scattering (SERS) sensor based on a functionalized multiple-armed tetrahedral DNA nanostructure (FMTDN) immobilized silver nanorod (AgNR) array substrate and Au nanoparticle (AuNP) SERS tags is constructed to achieve both multiplex detection and enhanced sensitivity using a sandwich strategy. The sensor can achieve single, dual, and triple biomarker detections of three lung cancer-related nucleic acid and protein biomarkers, i.e., miRNA-21, miRNA-486 and carcinoembryonic antigen (CEA) in human serum. The enhanced SERS signals in multiplex detections are due to the DNA self-assembled AuNP clusters on the silver nanorod array during the assay, and the experimentally obtained relative enhancement factor ratios, 150 for AuNP dimers and 840 for AuNP trimers, qualitatively agree with the numerically calculated local electric field enhancements. The proposed FMTDN-functionalized AgNR SERS sensor is capable of multiplex and cross-species detection of nucleic acid and protein biomarkers with improved sensitivity, which has great potential for the screening and clinical diagnosis of cancer in the early stage.
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LAB ON A CHIP
·
2023
·Vol. 23
·期 14
·3207-3216
·
IF 6.1
Ganggang Zhang,Xiaocui Lai,Weihua He,Liu Su,Gan Zhang,Weihua Lai,Shengliang Deng
Lateral flow assays (LFAs) are widely used in screening analysis. However, the detection flux and sensitivity of LFAs are unsatisfactory because of the ‘one-to-one’ read mode and the ordinary performance conventional probe. In this work, a high-flux smartphone-integrated LFA (sLFA) based on chrysanthemum-like Au@polydopamine (AuNC@PDA) for the detection of enrofloxacin (ENR) in milk was established. The smartphone-integrated device was developed and applied in the LFA, giving rise to a reading maximum of 64 samples with only two photos in less than 2 min compared to a ‘one-to-one’ read mode of a conventional LFA in more than 14 min with a 36.4% deviation. For ENR detection, the limits of detection of sLFA based on AuNC@PDA (33.78 pg mL−1) had 5.0-fold and 6.4-fold reduction compared with those based on AuNP (169.99 pg mL−1, conventional probe) and vvAuNP (216.47 pg mL−1, commercial probe), respectively. This study provides an effective technical means for screening ENR in large quantities of milk samples.
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TALANTA
·
2023
·
IF 6.1
Chen Cui,Xinyao Lin,Jie Lv,Hang Guo,Lu Shen,Guoqiang Xiang,Wenjie Zhao,Dechen Jiang
Designing innovative electrochemiluminescence (ECL) immunosensors is critical for the detection of biomarkers with a low concentration and the precise evaluation of clinical diseases. Herein, a Cu 3 (hexahydroxytriphenylene) 2 (Cu 3 (HHTP) 2 ) nanoflake-based sandwich-type ECL immunosensor was constructed for C-Reactive Protein (CRP) detection. The Cu 3 (HHTP) 2 nanoflake , an electronically conductive metal–organic framework (MOF), has a periodically arranged porous structure with a cavity size of 2 nm, which not only accommodates a large amount of Ru(bpy) 3 2+ but also confines the spatial diffusion of active species. Therefore, the Ru(bpy) 3 2+ -loaded Cu 3 (HHTP) 2 nanocomplex (Ru@CuMOF) as an ECL emitter exhibits an enhanced ECL efficiency. The ECL resonance energy transfer (ECL-RET) was accomplished by combining Ru@CuMOF used as a donor with gold nanoparticles-functionalized graphene oxide nanosheets (GO-Au) utilized as an acceptor. This should be ascribed to the fact that the ECL emission spectrum of Ru@CuMOF shows the strongest signal intensity at 615 nm, overlapping with the absorption spectrum of GO-Au at 580–680 nm. Targeted detection of CRP in human serum samples was achieved by the sandwich-type immunosensor based on the ECL-RET mechanism with a 0.26 pg mL −1 detection limit. The electro-activated hybrids of Cu 3 (HHTP) 2 and ECL emitters provide a new sensing strategy for the high-sensitivity detection of disease markers.
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TALANTA
·
2023
·
IF 6.1
Chaonan Jiao,Ying Zhu,Tongkai Ji,Xingwei Cai,Jing Wang
For yolk-shell structured nanoreactors , multiple active components can be precisely positioned on core and/or shell that can afford more exposed accessible active sites, and the internal voids can guarantee sufficient contact of reactants and catalysts. In this work, a unique yolk–shell structured nanoreactor [email protected] 3 O 4 /CeO 2 @mSiO 2 was fabricated and applied as nanozyme for biosensing. The [email protected] 3 O 4 /CeO 2 @mSiO 2 exhibited superior peroxidase-like activity with a lower Michaelis constant ( K m ) and a higher affinity to H 2 O 2 . The enhanced peroxidase-like activity was attributed to the unique structure and the synergistic effects between the multiple active components. Colorimetric essays were developed based on [email protected] 3 O 4 /CeO 2 @mSiO 2 for the ultra-sensitive sensing of glucose in the range of 3.9 nM–1.03 mM with the limit of detection as low as 3.2 nM. In the detection of glucose-6-phosphate dehydrogenase (G6PD), the cooperation between G6PD and [email protected] 3 O 4 /CeO 2 @mSiO 2 triggered the redox cycling between NAD + and NADH, thereby achieving the amplification of the signal and enhancing the sensitivity of the assay. The assay showed superior performance as compared to other methods with linear response of 5.0 × 10 −3 –15 mU mL −1 and lower detection limit of 3.6 × 10 −3 mU mL −1 . The fabricated novel multi-enzyme catalytical cascade reaction system allowed rapid and sensitive biodetection, demonstrating its potential in biosensors and biomedical applications.
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ACS Nano
·
2021
·
IF 15.881
Yang Yu,Guojian Yang,Shengrui Zhang,Mo Liu,Shujue Xu,Chunyu Wang,Minjie Li,Sean Xiao-An Zhang
Circular dichroism (CD) chiral sensing is very promising to meet the ever-increasing demands for high-throughput chiral analysis in asymmetric synthesis. However, it is still very challenging to sensitively quantify the composition of enantiomers in a wide concentration range because the existing sensing systems show either linear CD response resultant from stoichiometric chiral transfer or nonlinear CD response resultant from amplified chiral transfer and thus have the drawbacks of low sensitivity and narrow quantification range, respectively. Herein, we propose a sensing system of two-dimensional (2D) Au(I)-thiolate nanosheets. The disordered interligand interactions on the confined surfaces of nanosheets enable the formation of discrete amplified chiral domains around the adsorbed chiral analytes, resulting in a linearly amplified chiral transfer behavior, which provides a solution for highly sensitive and wide-range quantification of enantiomer compositions. Taking (1R, 2R)-(−)- and (1S, 2S)-(+)-1,2-diamino cyclohexanes as example analytes, the concentration and full-range enantiomeric excess (ee) values have been quickly determined by adsorbing them on the surface of Au(I)-MPA (MPA: 3-mercaptopropionic acid) nanosheets in the concentration range of 1.0 × 10–6 to 4.0 × 10–5 M. By engineering the surface functional groups, Au(I)-thiolate nanosheets can be extended to sense other types of analytes, and several polyols with multiple chiral centers have been sensed by boronic acid functionalized nanosheets at the 10–7 M level. The high performances, good extendibility, and one-pot high-yield aqueous synthesis ensure these Au(I)-thiolate nanosheets can be developed as a practical and powerful chiral sensing platform.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Xiaoming Liu,Suqing Wang,Fang Yang,Yinchu Zhang,Liushui Yan,Kexin Li,Huiqin Guo,Jiajun Yan,Jun Lin
In this paper, a novel Au/g-C 3 N 4 /ZnIn 2 S 4 plasma photocatalyst heterojunction composite with 3D hierarchical microarchitecture has been successfully constructed by integrating Au/g-C 3 N 4 plasmonic photocatalyst composite with 3D ZnIn 2 S 4 nanosheet through a simple hydrothermal process. The Au nanoparticles were firstly anchored on the surface of pristine g-C 3 N 4 material to get Au/g-C 3 N 4 plasmonic photocatalyst. Ascribing to the surface plasmon resonance of Au nanoparticles , the obtained Au/g-C 3 N 4 plasmonic photocatalyst shows a significant improved photocatalytic activity toward hydrogen production from water with visible light response comparing with pristine g-C 3 N 4 . Further combining Au/g-C 3 N 4 plasmonic photocatalyst with 3D ZnIn 2 S 4 nanosheet to construct a heterojunction composite. Owing to the synergistic effect of the surface plasmon resonance of Au nanoparticles in Au/g-C 3 N 4 and the heterojunction structure in the interface of Au/g-C 3 N 4 and ZnIn 2 S 4 , the prepared Au/g-C 3 N 4 /ZnIn 2 S 4 plasma photocatalyst heterojunction composite shows an excellent photocatalytic activity toward hydrogen production from water with visible light response, which is around 7.0 and 6.3 times higher than that of the pristine C 3 N 4 and Znln 2 S 4 nanosheet, respectively. The present work might provide some insights for exploring other efficient heterojunction photocatalysts with excellent properties.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2021
·Vol. 38
·期 1
·200-208
·
IF 1.307
Wang Yue,Wang Xiaoxue,She Ping,Guan Dehui,Song Lina,Xu Jijing
D esign and fabrication of functional porous air cathode materials with superior catalytic activity is still the key point for non-aqueous lithium-oxygen(Li-O 2 ) batteries. Herein, inspired by the self-standing three-dimensional(3D) structure of the natural spinach leaves, a unique binder-free and self-standing porous Au/spinach cathode for high-performance Li-O 2 batteries has been developed. The carbonized spinach leaves serve as a superconductive current collector and an ideal porous host for accommodating catalysts. The Au/spinach cathode could offer enough spaces for accommodating the discharge products, shorten the distance of the oxygen and electrolyte diffusion, and promote the oxygen reduction reaction(ORR) and oxygen evolution reaction (OER) processes. This optimized Au/spinach cathode achieved a high specific area capacity of 7.23 mA·h/cm 2 at a current density of 0.05 mA/cm 2 and exhibited excellent stability(280 cycles at 0.05 mA/cm 2 with a fixed capacity of 0.2 mA·h/cm 2 ). The superior performance encourages the construction of more advanced cathode architectures by the use of bio-composites for Li-O 2 batteries.
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MICROCHIMICA ACTA
·
2023
·Vol. 191
·期 1
·1-12
·
IF 5.7
Liu Xinyu,Yu Yang,Xie Tianhua,Cao Zijin,Li Zhiyan,Li Yuejing,Gu Yingqiu,Han Caiqin,Yang Guohai,Qu Lulu
Monolayer g-C 3 N 4 -modified Au/Ag nanorods (g-C 3 N 4 /Au/Ag NRs) array is fabricated as a dual-function platform with high surface-enhanced Raman scattering (SERS) response and excellent photocatalytic degradation ability for bisphenol A (BPA) residues. FDTD simulation results of Au/Ag NRs proves that the electromagnetic field intensity is significantly enhanced at the gap of Ag NRs and Au NPs and the protrusion of Au NPs, which endows the arrays with excellent SERS activity. The arrays exhibit high sensitivity for rhodamine 6G (R6G) (LOD = 1.1 × 10 -11 mol/L) and high SERS enhancement (EF = 9.2 × 10 7 ). In addition, the g-C 3 N 4 /Au/Ag NRs could degrade ˃90% of BPA adsorbed on the substrate surface within 140 min under visible light irradiation, and maintains its SERS activity after repeated use for 4 times. The dual-function platform with high SERS response and excellent recycling capability is proved to be reliable and is very promising for monitoring of BPA residues in food. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Qi Xu,Gong Chen,Han Hu,Zhimin Mo,Wenqiu Chen,Qianyuan He,Zushun Xu,Xiaofang Dai
Non-centrosymmetric tetragonal barium titanate nanocrystals have the potential to serve as piezoelectric catalysts in cancer therapy. When exposed to ultrasound irradiation, BaTiO 3 can generate reactive oxygen species with a noninvasive and deep tissue-penetrating approach. However, the application of BaTiO 3 in cancer nanomedicine is limited by their biosafety, biocompatibility, and dosage efficiency. To explore the potential application of BaTiO 3 in nanomedical cancer treatment, we introduced ultra-small Au nanoparticles onto the surface of BaTiO 3 to enhance the piezoelectric catalytic performance. Additionally, we also coated the BaTiO 3 with polydopamine to improve their biosafety and biocompatibility. This led to the preparation of a novel multifunctional BaTiO 3 -based nanoplatform called BTAPs. In vitro and in vivo experiments demonstrated that the incorporation of Au dopants and polydopamine coating successfully improved the piezoelectric catalysis properties and biocompatibility of BaTiO 3 . Compared with unmodified BaTiO 3 , BTAPs achieved a similar piezoelectric catalytic effect at a low dose (0.3 mg ml −1 in vitro and 10 mg kg −1 in vivo ). Moreover, BTAPs also exhibited enhanced properties in computed tomography imaging and photothermal effects in vivo . Therefore, BTAPs offer valuable insights into the advantages and limitations of piezoelectric catalytic nanomedicine in cancer treatment.
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