ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Ying Chen,Lei Tian,Wen Liu,Yi Mei,Qiu-Ju Xing,Yi Mu,Ling-Ling Zheng,Qian Fu,Jian-Ping Zou,Daishe Wu
Dechlorination of chloropyridines can eliminate their detrimental environmental effects. However, traditional dechlorination technology cannot efficiently break the C–Cl bond of chloropyridines, which is restricted by the uncontrollable nonselective species. Hence, we propose the carbonate species-activated hydrogen peroxide (carbonate species/H2O2) process wherein the selective oxidant (peroxymonocarbonate ion, HCO4–) and selective reductant (hydroperoxide anion, HO2–) controllably coexist by manipulation of reaction pH. Taking 2-chloropyridine (Cl–Py) as an example, HCO4– first induces Cl–Py into pyridine N-oxidation intermediates, which then suffer from the nucleophilic dechlorination by HO2–. The obtained dechlorination efficiencies in the carbonate species/H2O2 process (32.5–84.5%) based on the cooperation of HCO4– and HO2– are significantly higher than those in the HO2–-mediated sodium hydroxide/hydrogen peroxide process (0–43.8%). Theoretical calculations confirm that pyridine N-oxidation of Cl–Py can effectively lower the energy barrier of the dechlorination process. Moreover, the carbonate species/H2O2 process exhibits superior anti-interference performance and low electric energy consumption. Furthermore, Cl–Py is completely detoxified via the carbonate species/H2O2 process. More importantly, the carbonate species/H2O2 process is applicable for efficient dehalogenation of halogenated pyridines and pyrazines. This work offers a simple and useful strategy to enhance the dehalogenation efficiency of halogenated organics and sheds new insights into the application of the carbonate species/H2O2 process in practical environmental remediation.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Tongtong Zhai,Luyao Zhang,Sipeng Tian,Zhangpeng Xu,Xiushuang Fan,Jing Li,Erkang Wang
Chemiluminescence (CL) as a powerful analytical tool has garnered increasing interest. However, traditional molecular-based CL luminophores suffer from low emission efficiency due to limited total CL photons emitted per luminophore, driving efforts to explore amplified strategies or novel probes to boost the emission. Although metal nanoclusters (NCs) as luminescent nanoprobes have been extensively studied for electrochemiluminescence and photoluminescence (PL) owing to their intriguing luminescent properties, the CL performance using metal NCs as emitters is often ignored. Herein, based on the synergistic effect within the bimetallic NCs, a series of glutathione-coated Au–Ag bimetallic NCs (GSH-AuAg NCs) were optimized by adjusting precursor ratios and achieved the maximum CL response at a Au:Ag molar ratio of 5:1. To our surprise, CL emission with GSH-AuAg NCs as emitters was triggered with oxidant reagents such as KMnO4, and bimetallic NCs display boosted CL emission (ca. 6.2-fold) compared to monometallic NCs owing to the synergistic effect on enhancing the emission efficiency. Surface-defect-involved CL was revealed by collecting the CL spectra with a maximum emission wavelength of around 750 nm and an obvious red shift of 140 nm compared to PL spectra. The mechanism reveals the KMnO4-injected hole into the valence band through redox reactions with GSH ligands, leading to CL emission by efficient radiative charge recombination with pre-existing electron. A sensing platform based on the GSH-AuAg NCs/oxidant system was constructed for sensing H2O2 and glucose, demonstrating the potential of GSH-AuAg NCs as CL emitters in analytical applications.
研究领域:
分析化学
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生物分析
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纳米材料科学
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DOI
PubMed
高影响因子
WATER RESEARCH
·
2018
·
IF 7.051
Wei Ding,Jing Xu,Tao Chen,Chengshuai Liu,Jinjun Li,Feng Wu
Previous studies have shown that the oxidation of Fe(II) by molecular oxygen can lead to the co-oxidation of As(III) at neutral pH. However, the mechanism of As(III) oxidation in the presence of Fe(II) with respect to the interaction between As(III) and Fe(II) is still unclear. In this work, we examined the oxidation of As(III) in the presence of Fe(II) in air-saturated water, which is affected by pH, co-existing phosphate, and scavengers ( tert -butanol, superoxide dismutase, catalase and dimethylsulfoxide). Results confirm that the formation of the Fe(II)–As(III) complex (formation constant, K Fe(II)–As(III) = 10 3.86 M –1 ) plays an extremely important role in the initial stage of As(III) oxidation at pH 7.25. The oxidation of Fe(II)–As(III) promotes the production of H 2 O 2 and colloidal ferric hydroxide. H 2 O 2 reacts with the Fe(II)–As(III) complex through oxidizing Fe(II) to Fe(IV), which then causes the partial oxidation (ca. 50%) of As(III). The other part of As(III) oxidation by H 2 O 2 occurs, in the form of Fe(III)–As(III) complex, through direct electron transfer from As(III) to H 2 O 2 but not through Fe(IV). This work provides new mechanistic insight into arsenic and iron redox chemistry in the environment and furthers our understanding of Fenton reactions at neutral pH.
研究领域:
环境化学
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氧化还原化学
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水处理
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DOI
PubMed
高影响因子
Journal of Physical Chemistry C
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2022
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IF 4.177
Chengyu Zhang,Zhaodong Nan
Nanoenzymes have been regarded as strong substitutes to natural enzymes in the last decades. However, high concentrations of substrates are always needed because of the low activity of nanozymes, which causes an increase of the cost and an increase in environmental pollution in practical applications. Thus, improved nanozymic activity is still urgent and vital to reduce the need for high concentrations of substrates. A series of binary metal sulfides (FexNi1–xS2), which exhibited intrinsic nanozymic activity, was first synthesized by a hydrothermal method. Among these samples, the nanosheet-shaped Fe0.8Ni0.2S2 showed the highest activity. Compared with those of FeS2, the catalytic constant (Kcat) and catalytic efficiency (Kcat/Km) of Fe0.8Ni0.2S2 increased about 1.9 and 3.6 times, respectively. The Michaelis–Menten constant (Km) of Fe0.8Ni0.2S2 is about 4.7-fold smaller than that of FeS2, and 193-fold smaller than that of natural enzyme horseradish peroxidase (HRP), indicating a stronger affinity to H2O2. The investigation on the mechanism indicated that Fe2+ and Fe3+ in Fe0.8Ni0.2S2 are the active sites. The synergistic effect between Ni2+ and Fe3+ accelerated the conversion from Fe3+ to Fe2+, which improved the nanozymic activity. In addition, Fe0.8Ni0.2S2 can be used as a nanozyme to detect H2O2 and ascorbic acid (AA) within 1 min at room temperature (25 °C). This work extends the development of binary metal sulfides as artificial enzymes.
研究领域:
生物化学
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材料科学
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催化反应
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DOI
高影响因子
Journal of Analysis and Testing
·
2019
·Vol. 3
·期 3
·238-245
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IF 0
Sun Shihao,Fan Yaofang,Du Jiaoyang,Song Zhilian,Zhao Huimin
Over the past few decades, the enzyme-mimicking activity of metal–organic frameworks (MOFs) accompanied with structural characteristics has aroused much attention. However, pure MOFs have low affinity with DNA. Here, iron-based MOFs with acidized carbon nanotubes (CNTs) via a simple hydrothermal process have been synthesized, named as MIL-88(NH 2 )-Fe@CNTs. CNTs can enhance the affinity between MOF and DNA, achieving flexible regulation of their catalytic activity benefiting from the strong π − π stacking between CNTs and DNA. Meanwhile, in comparison with conventional iron-based MOFs, the addition of CNTs, which contributes to the acceleration of electron transfer, endowing as-prepared nanocomposites remarkably enhanced peroxidase-like activity to achieve an ultrasensitive detection of H 2 O 2 with the LOD of 17.64 μg/L. Notably, the as-prepared nanocomposites with adsorbed DNA displayed excellent affinity towards both TMB (3, 3′, 5, 5′-tetramethylbenzidine) substrates and H 2 O 2 as well as high catalytic velocity. On the basis of their switchable peroxidase-like activity regulated by different length or sequence of ssDNA, it is believed that our-prepared MOF-based nanomaterials would be promising for fabricating versatile and sensitive label-free colorimetric assays for diverse targets.
研究领域:
生物化学
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纳米材料科学
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分析化学
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DOI
CELL BIOLOGY INTERNATIONAL
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2018
·Vol. 42
·期 11
·1584-1593
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IF 1.936
Bo Yu,Yanan Zhao,Hongli Zhang,Di Xie,Wei Nie,Kaiyao Shi
MicroRNA-143-3p (miR-143-3p) is involved in the initiation of inflammatory response and the progression of cardiovascular diseases. Myocardial hypertrophy is a common symptom in numerous cardiovascular diseases. In the current study, we attempted to demonstrate the role of miR-143-3p in the development of myocardial hypertrophy by focusing on its association with inflammation. Myocardial hypertrophy was induced by transverse aortic constriction (TAC) method in vivo and by H 2 O 2 administration in vitro. The expression status of miR-143-3p and downstream effectors were detected in animal heart tissues and H9c2 cells. Furthermore, the effect of miR-143-3p inhibition on H 2 O 2 -induced changes in ERK5/PPARδ/NF-κB axis was assessed. TAC induced oxidative stress and inflammation in rat heart tissues, which was associated with the increased expressions of miR-143-3p and p-ERK5. However, the up-regulated expression of miR-143-3p had no effect on the expression of ERK5, which was a direct target of miR-143-3p. The results of in vitro assays showed that H 2 O 2 administration increased the levels of miR-143-3p and p-EKR5 and induced the activation of NF-κB pathway. After the inhibition of miR-143-3p, the activation of EKR5 and NF-κB pathway was suppressed, whereas the expression of PPARδ was up-regulated. The current study demonstrated that miR-143-3p is crucial to the initiation of inflammatory response induced by myocardial hypertrophy. The activation of ERK5 following miR-143-3p up-regulation appears to be a complementary response to induce the subsequent anti-inflammatory signaling transduction, which needed further exploration.
研究领域:
心血管疾病
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分子生物学
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炎症
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DOI
PubMed
高影响因子
Advanced Composites and Hybrid Materials
·
2018
·Vol. 1
·期 3
·612-623
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IF 0
Chen Miaomiao,Zhu Jialong,Yang Baochan,Yao Xiuxiu,Zhu Xixi,Liu Qingyun,Lyu Xintian
In the present study, a facile method was proposed to prepare nickel sulfide (NiS) nanoparticles well-dispersed on the surface of montmorillonite/graphene oxide (MMT/GO). The NiS/MMT/GO nanocomposites were characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray diffraction (XRD), fluorescence spectrophotometry, etc. Significantly, the novel NiS/MMT/GO nanocomposites exhibited high peroxidase-like activity toward the typical chromogenic substrate, 3,3′,5,5′-tetramethylbenzidine (TMB). However, glutathione (GSH) could inhibit the peroxidase-like activity of NiS/MMT/GO along with a visible color variation. Based on the color change of the system of nanocomposites-H 2 O 2 -TMB, a novel colorimetric sensor was designed and conveniently used to quantitatively detect H 2 O 2 as well as GSH. The limit of detection (LOD) of H 2 O 2 and GSH is 9.73 and 0.5043 μM, respectively. The proposed H 2 O 2 sensor has potential application in the field of biosensing, food, and environment.
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研究领域:
纳米材料
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生物传感器
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分析化学
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DOI
Analytical Methods
·
2016
·Vol. 8
·期 9
·2097-2105
·
IF 1.915
Junrong Li,Liang Lv,Guannan Zhang,Xiaodong Zhou,Aiguo Shen,Jiming Hu
We herein present a simple and surfactant-free synthetic strategy for the preparation of core–shell Fructus Broussonetia-like Au@Ag@Pt nanoparticles (FBNPs) via a combination of galvanic replacement and reagent reduction, in which a chitosan (CS)-mediated epitaxial growth of Pt multi-branches occurs on cresyl violet labeled Au core–Ag shell nanoparticles (NPs) at room temperature. The as-prepared novel nanostructures exhibit an enzyme mimetic activity due to the formation of a Fructus Broussonetia-shaped Pt shell, the absence of surfactants and the positively charged CS molecules intertwined within the outermost Pt NPs. Relying on the high sensitivity of resonance-enhanced Raman scattering and the highly efficient intrinsic peroxidase-like activity of FBNPs, H2O2 was detected with a wide detection window from 10 pM to 100 μM when utilizing 3,3′,5,5′-tetramethylbenzidine (TMB) as the substrate. Based on the H2O2–TMB catalytic oxidation system a simple, sensitive, selective and universal platform has been extended for the detection of all peroxidase-related analytes. For example, glucose at a concentration range of 1 nM to 200 μM was detected in the presence of glucose oxidase with a limit of detection of 1 nM.
研究领域:
纳米材料
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生物分析化学
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医学诊断
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DOI
高影响因子
ANALYST
·
2019
·Vol. 145
·期 3
·873-879
·
IF 4.019
Minghan Wang,Junjie Liu,Xiaoli Qin,Xin Nie,Yifan Dong,Xu Liang,Zhiwei Zhu,Di Yang,Yuanhua Shao
In this work, an Au–Ag alloy nanourchin (Au–Ag alloy NU) based electrochemiluminescent (ECL) sensor for the measurement of cardiac troponin I (cTnI) was developed. The as-prepared Au–Ag alloy NUs exhibited higher specific surface area and better conductivity owing to their unique urchin-like morphology, which resulted in excellent electrocatalytic activity towards H2O2 in the luminol–H2O2 ECL system. We have found that the Au–Ag alloy NUs could enhance the ECL signal in the luminol–H2O2 solution. Based on these facts, a facile and label-free ECL immunosensor has been constructed for the analysis of cTnI, a cardiac biomarker, with a wide linear range of 3.5 pg mL−1–350 μg mL−1. This novel ECL immunosensor has good stability and reproducibility, showing potential application in clinical diagnostics. In addition, a non-enzymatic electrochemical sensor for H2O2 was also fabricated, with a wide linear detection range of 100 nM–200 μM, a low limit of detection of 45 nM and a fast response time (less than 2 s).
研究领域:
生物医学工程
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分析化学
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DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Rui Huang,Yi Zhou,Jiaxiang Hu
Latent fingerprints (LFPs) are important trace evidences found at crime scenes that assist forensic experts in human identification, and a growing number of studies show that LFPs have some medical value. Herein, as one of the common nanoenzymes, Fe 3 O 4 nanoparticles (Fe 3 O 4 NPs) was used for LFPs imaging due to its excellent superparamagnetic properties and for recognition of glucose/H 2 O 2 on LFPs because of its horseradish peroxidase-like activity, which makes it possible to diagnose diabetes non-invasively through LFPs. Furthermore, the intelligent qualitative and semi-quantitative analysis of glucose/H 2 O 2 on LFPs was achieved by designing the classifier based on the multi-channel convolutional neural network (MC-CNN) technology. The qualitative accuracy rate is over 97% and the semi-quantitative accuracy rate reaches 90%. This work offers the promise to facilitate cross-disciplinary studies between artificial intelligence methods and fingerprint development technique.
研究领域:
法医学
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纳米生物学
·
人工智能
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DOI
高影响因子
ANALYTICAL LETTERS
·
2022
·
IF 2.267
Miaomiao Tian,Liping Zhao,Ya Wang,Gang Liu,Peng Zhang
Bimetallic Pt/Ag nanoparticles (Pt/Ag NPs) were synthesized using 3-hydroxyphenyl-boronic acid as the reducing and stabilizing agent by a simple, one-step hydrothermal method. The bimetallic Pt/Ag NPs were demonstrated to possess intrinsic peroxidase mimetic catalytic activity for the luminol/H2O2 reaction to generate chemiluminescence (CL). The catalytic properties of the bimetallic Pt/Ag NPs were thoroughly investigated. The results showed that the combination of Pt and Ag greatly enhanced the chemiluminescence which is attributed to their synergy. Moreover, the prepared bimetallic Pt/Ag NPs exhibited superior peroxidase mimetic activity to horseradish peroxidase and were stable under a wide range of pH values and temperatures. Using the bimetallic Pt/Ag NPs as the catalyst, a novel chemiluminescence sensor was developed for the determination of glucose with a linear range from 1 to 500 µM and a detection limit of 0.35 µM. The developed method was successfully employed to determine glucose in human serum with satisfactory results. Bimetallic Pt/Ag NPs with peroxidase mimetic catalytic activity have promising applications for determination of glucose in clinical samples.
研究领域:
生物化学
·
纳米医学
·
分析化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Tianchang Miao,Ximeng Lv,Fangshuai Chen,Gengfeng Zheng,Qing Han
Achieving O 2 photoreduction to H 2 O 2 with high selectivity control and durability while using easily accessible catalyst requires new synthesis strategies. Herein, we propose an asymmteric Sb coordination active center strategy of introducing anthraquinone (AQ) and heptazine to form local N 3 − Sb − O coordination by a rapid and simple explosive crystallization approach, resulting in a mesoporous conjugated heptazine-amide-AQ polymer coordinated Sb (HAAQ-Sb). It is demonstrated that the N 3 − Sb − O coordination effectively suppresses the charge recombination and acts as the highly active site for O 2 adsorption. Moreover, as-introduced AQ units initiate low-barrier hydrogen transfer through a reversible redox process that triggers highly-efficient H 2 O 2 production. A superior apparent quantum yield of 20.2 % at 400 nm and a remarkable solar-to-chemical conversion efficiency of 0.71 % are achieved on the optimal HAAQ-Sb, which is the highest among C 3 N 4 -based photocatalysts at present. This asymmetric coordination concept and material design method provide new perspectives for the research of novel catalysts toward artificial photosynthesis.
研究领域:
材料科学
·
光催化
·
化学工程
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）