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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Synergistic effect of Z-scheme junction and core–shell architecture over NH2-MIL-125@Ag@AgCl ternary heterojunction for cooperative CO and H2O2 production

Haopeng Jiang,Xiaohui Yu,Jinhe Li,Lele Wang,Weikang Wang,Chunxia Wu,Liyong Tang,Qinqin Liu

Herein, a NH 2 -MIL-125(Ti)@Ag@AgCl (NM@Ag@AgCl) stacked core–shell heterojunction with Z-scheme carrier transfer mechanism was developed to fulfil the goal of synchronous reactions of CO 2 reduction and H 2 O oxidation. In detail, the NM@Ag@AgCl was obtained by in-situ loading the AgCl as the shell-inorganic semiconductor on the octahedral NM as the core-organic semiconductor, followed by in-situ transforming part of the AgCl shell into the plasmonic Ag nanoparticles using a photo-reduction method. As a result, the interface effects of core–shell architecture majorized by the Ag electronic mediator can favor the transmission of photogenerated carriers and reduce electron transport resistance; while the plasmonic Ag mediated Z-scheme mode with a giant internal electronic field provided a strong driving force to recombine the carriers with weak redox ability, reserving the carrier with strong redox ability on the NH 2 -MIL-125-core and AgCl-shell for the simultaneous reactions. The CO and H 2 O 2 yields of the optimal NM@Ag@AgCl were 6.02 and 5.43 μmol⋅g −1 ⋅h −1 , which were 3.31 and 4.02 times that of the NM, respectively. This study furnishes a novel thread for the design of core–shell organic–inorganic heterojunction with high interfacial charge transfer for realizing the simultaneous reactions.

CAS / MDL: 10312-55-7 7761-88-8
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ANALYTICAL CHEMISTRY · 2021 · IF 6.986

Self-Terminated Electroless Deposition of Surfactant-Free and Monodispersed Pt Nanoparticles on Carbon Fiber Microelectrodes for Sensitive Detection of H2O2 Released from Living Cells

Yuxi Tong,Lifen Wang,Jiajia Song,Mengyue Zhang,Hetong Qi,Shujiang Ding,Honglan Qi

We report a self-terminated electroless deposition method to prepare surfactant-free and monodispersed Pt nanoparticle (NP)-modified carbon fiber microelectrodes (Pt NP/CFEs) for electrochemical detection of hydrogen peroxide (H2O2) released from living cells. The surfactant-free and monodispersed Pt NPs with a uniform size of 65 nm are spontaneously deposited on a CFE surface by immersing an exposed carbon fiber (CF) of CFE in the PtCl42– solution, in which an exposed CF can be used as the reducing agent and stabilizer. A self-terminated electroless deposition method is demonstrated, in which the density and size of Pt NPs on a CFE surface do not increase when the reaction time increases from 20 to 60 min. The self-terminated electroless deposition process not only can effectively avoid any manual electrode modification and thus largely minimize person-to-person and electrode-to-electrode deviations but also can avoid the use of any extra reductant or surfactant in the fabrication process. Therefore, Pt NPs/CFEs, with good reproducibility and sensitivity, not only exhibit high electrocatalytic activity toward the oxidation of H2O2 but also maintain the spatial resolution of CFEs. Moreover, Pt NPs/CFEs can detect H2O2 with a wide linear range of 0.5–80 μM and a low detection limit of 0.17 μM and then can be successfully applied in the monitoring of H2O2 released from RAW 264.7 cells. The self-terminated electroless deposition method can also be extended to selectively prepare other metal NP-modified CFEs, such as Au NPs/CFEs or Ag NPs/CFEs, by choosing the metal ions with higher reduction potential as precursors. This work provides a simple, straightforward, and general method for the preparation of small, surfactant-free, and monodispersed metal NP-modified CFEs with high sensitivity, reproducibility, and spatial resolution.

CAS / MDL: 10025-99-7 7761-88-8
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

FeS nanoparticles embedded in 2D carbon nanosheets as novel nanozymes with peroxidase-like activity for colorimetric and fluorescence assay of H2O2 and antioxidant capacity

Chan Song,Haibo Liu,Linlin Zhang,Jie Wang,Chenglong Zhao,Qinyuan Xu,Cheng Yao

Nanozymes with high catalytic performance play a vital role in the construction of advanced biosensors for the signal detection and analysis of complicated biological samples. Herein, FeS nanoparticles (NPs) embedded in 2D carbon nanosheets (denoted as [email protected] ) are demonstrated to serve as excellent nanozymes with high catalytic activity . Notably, the introduction of mesoporous carbon substrate could effectively improve the enzymatic peroxidase-like catalytic ability of embedded FeS nanozymes, especially in the fluorescence catalytic system . Based on the high peroxidase-like activity of proposed [email protected] nanozymes, a facile method was then designed for H 2 O 2 assay with detection limit as low as 0.78 μM and 0.86 μM for the colorimetric and fluorescence method , respectively. The oxidation of the colorimetric and fluorescence substrates could be ascribed to the hydroxyl radical (·OH) produced by catalytic reaction of H 2 O 2 with [email protected] nanozymes. Thus, the [email protected] nanozymes-based H 2 O 2 sensing platform was further constructed to evaluate the antioxidant capacity of glutathione (GSH), cysteine (Cys), and gallic acid (GA). Notably, [email protected] nanozymes can keep the functionality in a broad pH range (2.0 ~ 9.0) for catalytic reaction, delivering a great potential in the fabrication of advanced biosensors.

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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2021 · IF 4.464

Ultrasensitive prostate specific antigen monitoring based on electrochemiluminescent immunesystem with synergistic signal amplification effect of resonance energy transfer coupling with K2S2O8-H2O2 dual coreactants

Zhimin Liu,Jie Wang,Yilei Lu,Chen Cui,Limei Zheng,Leqian Hu

In this work, an effective signal amplification strategy was used for the fabrication of the ultrasensitive sandwich-typed electrochemiluminescence (ECL) immunosensing platform. The combining of K 2 S 2 O 8 -H 2 O 2 dual coreactants with the localized surface plasmon resonance of silver nanoparticles (AgNPs) resulted in the remarkable increase of ECL response. Noticeably, because of the perfect overlap between the plasmon spectra of AgNPs and the ECL emission spectra of graphitic carbon nitride quantum dots (g-CNQDs), a plasmon-enhanced ECL phenomenon was proved in g-CNQDs/AgNPs system result from high efficient energy transfer. Besides, the ECL signal of the ECL immunosensor was greatly improved in the presence of K 2 S 2 O 8 -H 2 O 2 dual coreactants. Consequently, this synergistic amplified ECL sensing platform was applied for the specific prostate specific antigen (PSA) analysis. Under the optimum conditions, the immunoassay strategy demonstrated excellent sensing performance with a wide linear concentration of PSA from 1.0 × 10 − 5 ng mL −1 to 500 ng mL −1 and a detection limit of 0.0046 pg mL −1 (S/N = 3). Considering the favorable analytical feedback in actual serum samples assay, the developed strategy indicated an enormous potential for biomarkers analysis.

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TALANTA · 2024 · IF 5.6

Target-driven functionalized DNA hydrogel capillary sensor for SARS-CoV-2 dual-mode detection

Jing-bo Jiao,Qing Kang,Shu-xin Cui,Jiang-li Cao,Tong Lin,Chen-jing Ma,Ze-hui Xiao,Ting Du,Nan Wang,Xin-jun Du,Shuo Wang

Coronavirus disease caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) has caused secondary pandemic, which still poses a serious threat to physical health and economic development. Herein, the target-driven functionalized DNA hydrogel capillary sensor based on cascade signal amplification and carbon coated cobalt manganese modified by prussian blue and platinum nanoparticles (MnCo@C-Pt-PB NPs) has been successfully developed for dual-mode detection of SARS-CoV-2. The cascade signal amplification triggered by target RNA causes the permeability of the DNA hydrogel loaded in the capillary to be destroyed, thereby releasing the embedded MnCo@C-Pt-PB NPs as signal molecules into 3,3′,5,5′-tetramethylbenzidine/hydrogen peroxide (TMB/H 2 O 2 ) solution under the driving of capillarity. The colorless TMB is then catalyzed to blue oxidation products (oxTMB) due to peroxidase-like activity of MnCo@C-Pt-PB NPs, and MnCo@C-Pt-PB NPs and oxTMB with photothermal properties synergistically increase the system temperature under near-infrared irradiation, which are recorded by portable devices to achieve dual-mode detection. Signals intensity are proportional to the logarithm of T-RNA concentration in a wide detection range (100 aM-100 pM), with a detection limit of 100 aM. Moreover, the reliability of the developed method in oropharyngeal swabs samples has also been validated. The signal conversion and amplification function of functionalized DNA hydrogel enhances the convenience, sensitivity and versatility of the developed method, which is promising to be applied in environmental safety, molecular diagnostic assays and disease prevention.

研究领域: 生物技术 · 分析化学 · 纳米技术 · 医学诊断 · 公共卫生
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BIOSENSORS & BIOELECTRONICS · 2016 · IF 7.476

Ultrasensitive electrochemical DNA biosensor based on functionalized gold clusters/graphene nanohybrids coupling with exonuclease III-aided cascade target recycling

Wei Wang,Ting Bao,Xi Zeng,Huayu Xiong,Wei Wen,Xiuhua Zhang,Shengfu Wang

In this work, a novel and ultrasensitive electrochemical biosensor was constructed for DNA detection based on functionalized gold clusters/graphene nanohybrids (AuNCs/GR nanobybrids) and exonuclease III (Exo III)-aided cascade target recycling. By utilizing the capacity of GR as universal template, different metal nanoclusters including AuNCs/GR nanobybrids and PtNCs/GR nanohybrids were synthesized through convenient ultrasonic method. Exo III-aided cascade recycling was initiated by target DNA, generating the final cleavage product (S2), which acted as a linkage between capture probe and the functionalized metal nanoclusters/GR conjugates in the construction of the biosensor. The AuNCs/GR-DNA-enzyme conjugates acted as interfaces of enzyme-catalyzed silver deposition reaction, achieving DNA detection ranging from 0.02 fM to 20 pM with a detection limit of 0.057 fM. In addition, PtNCs/GR-DNA conjugates presented peroxidase-like activity and the functionalized PtNCs/GR nanohybrids-based electrochemical biosensor also realized DNA detection by catalyzing the 3,3′,5,5′-tetramethylbenzidine-hydrogen peroxide (TMB-H 2 O 2 ) system to produce electrochemical signal. This metal clusters/GR-based multiple-amplified electrochemical biosensor provided an universal method for DNA detection.

研究领域: 生物化学 · 纳米技术 · 分析化学 · 分子生物学
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JOURNAL OF ENVIRONMENTAL ENGINEERING · 2020 ·Vol. 146 ·期 4 ·04020019 · IF 1.264

Supercritical Fenton Oxidation: New Advanced Oxidation Technology

Junru Bu,Xinkai Zhou,Huan Liu,Chunmian Lin

The roles of H2O2 in supercritical water oxidation (SCWO) were investigated. The results showed that some of the H2O2 could persist for a short time in SCW, and organic pollutants were mainly oxidized by the O2 generated from the H2O2 in SCWO. However, the introduction of Fe2+ into the SCWO system with H2O2 formed a new Fenton oxidation environment, i.e., supercritical Fenton oxidation (SCFO), which showed the cooperative effect of Fenton oxidation and SCWO. Comparative experiments of phenol and p-aminophenol (PAP) in SCWO and SCFO, respectively, were carried out. The results showed that, in the SCFO system, the CO2 yield from the oxidative degradation of phenol-simulated wastewater (766.0  mg/L) in 45s could reach 73.3%, much higher than that in the SCWO (49.2%) under the same conditions. After 8 min, the CO2 yield in SCFO (97.4%) was also significantly higher than that in SCWO (89.4%). The degradation efficiency of PAP-simulated wastewater (272.5  mg/L) in the SCFO system exceeded 94.3%, especially under acidic conditions, and the degradation efficiency reached 97.4%, much higher than that in the SCWO system (86.2%).

研究领域: 环境工程 · 化学工程 · 水处理技术 · 高级氧化工艺 · 污染控制
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ACS Nano · 2019 · IF 13.903

Differential Diagnosis and Precision Therapy of Two Typical Malignant Cutaneous Tumors Leveraging Their Tumor Microenvironment: A Photomedicine Strategy

Peiru Wang,Weitao Yang,Shuzhan Shen,Chao Wu,Long Wen,Qian Cheng,Bingbo Zhang,Xiuli Wang

Elevated hydrogen peroxide (H2O2) in biological tissues is generally recognized to be relevant to the carcinogenesis process that regulates the proliferative activity of cancer cells and the transformation of malignant features. Inspired by this observation, it can be hypothesized that imaging H2O2 in the tumor microenvironment (TME) could help diagnose tumor types and malignancy, and even guide precise therapy. Thus, in this study, a noninvasive photomedicine strategy is demonstrated that leverages the different levels of H2O2 in the TME, and two representative skin cancers, malignant melanoma (MM, clinically higher incidence of metastasis and recurrence) and cutaneous squamous cell carcinoma (cSCC, relatively less dangerous), are differentially diagnosed. The working probe used here is one we previously developed, namely, intelligent H2O2 responsive ABTS-loaded HRP@Gd nanoprobes (iHRANPs). In this study, iHRANPs have advantages over ratiometric imaging due to their bimodal imaging elements, in which the inherent magnetic resonance imaging (MR) mode can be used as the internal imaging reference and the H2O2 responsive photoacoustic (PA) imaging modality can be used for differential diagnosis. Results showed that after intravenous injection of iHRANPs, the tumor signals on both MM and cSCC are obviously enhanced without significant difference under the MR modality. However, under the PA modality, MM and cSCC can be easily distinguished with obvious variations in signal enhancement. Particularly, guided by PA imaging, photothermal therapy (PTT) can be precisely applied on MM, and a strong antitumor effect was achieved owing to the excessive H2O2 in the TME of MM. Furthermore, exogenous H2O2 was injected into cSCC to remedy H2O2 deficiency in the TME of cSCC, and an evident therapeutic efficacy on cSCC can also be realized. This study demonstrated that MM can be differentially diagnosed from cSCC by noninvasive imaging of H2O2 in the TME with iHRANPs; meanwhile, it further enabled imaging-guided precision PTT ablation, even for those unsatisfactory tumor types (cSCC) through exogenously delivering H2O2.

研究领域: 肿瘤学 · 光医学 · 生物医学工程 · 分子影像 · 诊疗一体化
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Applied Materials Today · 2021 · IF 10.041

Porous selenium nanozymes targeted scavenging ROS synchronize therapy local inflammation and sepsis injury

Xu Chen,Xufeng Zhu,Youcong Gong,Guanglong Yuan,Jieqiong Cen,Qiaoshan Lie,Yida Hou,Gang Ye,Shengming Liu,Jie Liu

Excessive reactive oxygen species (ROS) is the main factor leading to high mortality in local inflammation and sepsis. Therefore, developing efficient ROS scavenger in pro-inflammatory immune cells is an urgent strategy for therapy local inflammatory and sepsis injury. Herein, we constructed a novel mesoporous selenium-hyaluronic acid nanoenzyme therapeutic system (MSe-HA NPs) for therapy local inflammatory and sepsis injury by targeting eliminate ROS in inflammatory macrophage. In detail manners, the high specific surface area of mesoporous selenium nanoenzyme exhibited ultra-high activity like glutathione peroxidase (GPx), which catalytic speed of H 2 O 2 scavenging was increasing to 2.02 times compare with solid Se NPs. Moreover, the broad spectrum of ROS eliminating capacity further promoted ability of MSe NPs in eliminating various ROS. More interestingly, we found that choose HA as the modification not only endowed the MSe NPs targeting to inflammatory macrophage, but the ROS degradable property of HA could enhance the MSe NPs to eliminating ROS. In vivo , MSe-HA NPs after injection showed that simultaneously cured the local inflammation and sepsis induced with LPS by quickly eliminating excessive ROS. Especially in sepsis mouse models, the survival rate and the organic dysfunction significantly improved after treated with MSe-HA NPs. Thus, this novel mesoporous nanozyme provides an effective strategy for the design of nanomedicine and the treatment of inflammation-related diseases.

CAS / MDL: 50-81-7 9004-61-9
研究领域: 纳米技术 · 药学 · 免疫学 · 炎症研究 · 败血症治疗
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BIOSENSORS & BIOELECTRONICS · 2014 · IF 6.451

Visual detection of melamine based on the peroxidase-like activity enhancement of bare gold nanoparticles

Pengjuan Ni,Haichao Dai,Yilin Wang,Yujing Sun,Yan Shi,Jingting Hu,Zhuang Li

In this study, a facile method to sensitively detect melamine and highly improve the peroxidase-like activity of bare gold nanoparticles (Au NPs) at the same time is proposed for the first time. It is interesting to find that the addition of melamine could improve the peroxidase-like activity of Au NPs. By coupling with 3,3′,5,5′-tetramethlybenzidine (TMB)–H 2 O 2 chormogenic reaction, a novel method for colorimetic detection of melamine is developed. The detection limit of this method is as low as 0.2   nM with the help of UV–vis spectroscopy and 0.5   µM by naked-eye observation, both which are far below the US food and Drug Administration estimated melamine safety limit of 20   µM. In addition, the present method is successfully applied for the detection of melamine in raw milk and milk powder. More importantly, the proposed method could also improve the peroxidase-like activity of Au NPs, which may not only provide a new approach to develop effective nanomaterials-based mimetic enzyme , but also irradiative to develop new applications for Au NPs in varieties of cost-effective and simple sensors in medicine, biotechnology and environmental chemistry.

CAS / MDL: 64-19-7 54827-17-7
研究领域: 分析化学 · 纳米技术 · 食品科学 · 环境化学
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RSC Advances · 2020 ·Vol. 10 ·期 11 ·6647-6653 · IF 3.119

An electrochemical aptasensor for lead ion detection based on catalytic hairpin assembly and porous carbon supported platinum as signal amplification

Huali Jin,Di Zhang,Yong Liu,Min Wei

An electrochemical aptasensor is fabricated for lead ion (Pb2+) detection based on catalytic hairpin assembly as signal amplification. Biomass porous carbon derived from soybean straw (PCs) is used to load platinum nanoparticles (PtNPs), which are introduced as mimetic enzymes to catalyze the hydroquinone–H2O2 system. In the presence of Pb2+, the complementary DNA (cDNA) releases from aptamer-cDNA and hybridizes with hairpin DNA1 (HP1) on the electrode surface. After bio-hairpin DNA2 (bio-HP2) is added, hybridization between HP1 and bio-HP2 further releases cDNA, which participates in the next cycle and triggers amplification, eventually forming a large number of bio-HP2/HP1 on the electrode surface. Then PtNPs@PCs immobilize on the electrode surface by specific binding of streptavidin with biotin, and catalyze the oxidation of hydroquinone in the presence of H2O2. The produced electrochemical signal depends on the concentration of Pb2+. The developed biosensor exhibits a wide linear range from 50 pM to 1000 nM with a detection limit of 18 pM, and high selectivity for Pb2+ over other environmentally relevant metal ions at concentration ratios of 100. The recoveries of Pb2+ in real samples were 93.5–108%. Thus, the proposed biosensor can provide an efficient method for sensitive and selective detection of Pb2+ in real samples.

CAS / MDL: 1633-78-9
研究领域: 分析化学 · 电化学 · 生物传感器 · 环境科学
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Nanoscale · 2024 ·Vol. 16 ·期 16 ·8162-8176 · IF 5.8

Electrochemical control of the morphological evolution of PEDOT on a Ni–Co(OH)2/carbon cloth surface to modulate the performance of wearable H2O2 sensors

Xinmeng Zhang,Mingyue Bai,Lei Ge,Yuanyuan Yao

The slow redox rate of hydrogen peroxide (H2O2) in neutral environments makes the H2O2 sensor inadequate for the detection of low levels of signalling molecules. The aim of this study is to fabricate a flexible sensing electrode by hydrothermally loading micro-nanometer Ni and Co(OH)2 on carbon cloth (CC) and electrochemically depositing poly(3,4-ethylenedioxythiophene) (PEDOT) on the surface of the electrode. The sensor presented high sensitivity (10.43 mA mM−1 cm−2), a wide detection range (0.033–120.848 mM), a low detection limit (0.92 nM), high stability, and excellent anti-interference performance in neutral solutions. Ni–Co(OH)2 provides abundant active sites while CC solves their agglomeration phenomenon and conductivity. The PEDOT film offers heightened conductivity, hydrophilicity, interfacial stability, and an electrochemically active surface area (ECSA). The side area of the chrysanthemum petal like PEDOT is 39 ± 7 times the bottom area, and PEDOT increases the ECSA of the composite to six times that of CC. Electrochemical precise control of PEDOT morphology to improve sensor performance provides a new strategy for the application of PEDOT in sensors.

CAS / MDL: 7791-03-9
研究领域: 材料科学 · 生物医学工程 · 分析化学
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