ANALYTICA CHIMICA ACTA
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2019
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IF 5.256
Miao-Feng Fan,Hui-Min Wang,Li-Jiao Nan,Ai-Jun Wang,Xiliang Luo,Pei-Xin Yuan,Jiu-Ju Feng
A biomimetic assembly of per-O-methylated-cyclodextrin dimer with cobalt proto-porphyrin (Co III -PPIX@Py2CD) was achieved via covalent linkage between Co III of Co III -PPIX and pyridine N of Py2CD (primarily synthesized by the acyl chlorination reaction of two β-CDs monomers with 3,5-bis (bromomethyl) pyridine). Ultraviolet–visible (UV–vis) and circular dichroism (CD) absorption spectroscopy , and NMR hydrogen spectroscopy (H 1 -NMR) were adopted to carefully characterize the structure of Py2CD and its functional assembly with Co III -PPIX. X-ray photoelectron spectroscopy (XPS) was employed to affirm the binding of the as-obtained Co III -PPIX@Py2CD, whose electrochemical kinetics were extensively studied to validate the feasibility in the catalytic reduction of hydrogen peroxide (H 2 O 2 ). The developed sensor displayed the wide linear range for H 2 O 2 detection and the low detection limit of 2.47 × 10 −7 M. This work sheds some constructive lights on rational design and synthesis of preeminently biomimic carrier and high cost-effectiveness catalyst for (bio)analytical applications.
研究领域:
生物化学
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分析化学
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材料科学
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Di Cheng,Tuo Wang,Guangxue Zhang,Huimin Wu,He Mei
Cu x Co 3-x O 4 (x = 0.5, 1, 1.5, 2) are successfully synthesized through hydrothermal and calcination processes. A series of electrochemical tests reveal that all of them exhibit electrocatalytic activity towards glucose and H 2 O 2 . Among them, CuCo 2 O 4 (x = 1) has a unique double-shelled hollow structure and shows higher catalytic performance. The electrochemical sensor based on CuCo 2 O 4 displays a linear range from 2.5 μM to 7.9 mM, with a sensitivity of 400.0 μA mM −1 cm −2 for the detection of glucose. As for H 2 O 2 , it shows a linear range from 10.0 μM to 8.9 mM, with a sensitivity of 94.1 μA mM −1 cm −2 . The sensor also exhibits short response time (<3 s), good selectivity, reproducibility, and stability over 18 days. Thus, this novel non-enzyme sensor has potential application in glucose and H 2 O 2 detection.
研究领域:
生物化学
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材料科学
·
分析化学
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DYES AND PIGMENTS
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2021
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IF 4.889
Yingchao Zhang,Yunfei Xie,Mingjuan Zhou,Erik B. Berda,Danming Chao
The elegant electroswitchable color/emission properties of electrochromic/electrofluorochromic dual-functional materials motivates the exploration of their new applications. In this work, a new poly (urea-urethane) was synthesized via nucleophilic copolymerization of electroactive oligoaniline derivative, solid-emissive tetraphenylethylene groups, and alkyl isocyanate. The resultant poly (urea-urethane) exhibited good electroactivity and desirable aggregation-induced emission properties. High-performance electrochromic/electrofluorochromic behavior had been disclosed with a high optical contrast ratio of ΔT = 50.4%, a moderate fluorescence on/off ratio of 10.5, and high coloration efficiency of 503 cm 2 /C at 768 nm. A reflective/emissive dual-mode display device had also been manufactured based on the resultant poly (urea-urethane) and charge-balancing V 2 O 5 , exhibiting a reversible color change and tunable fluorescence conversion upon the electric stimulus. Furthermore, this polymer showed an interesting color/fluorescence response to H 2 O 2 , due to the linkage mechanism between its redox states and optical properties . The spray-coated poly (urea-urethane) test strips were employed in visualized dual-determination of H 2 O 2 with gradual color change from gray to dark green, along with an obvious fluorescence change from light blue to dark, which displays easy operation and rapid detection.
研究领域:
材料科学
·
化学
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FOOD CHEMISTRY
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2026
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IF 10.4
Yu Bai,Jian Xie,Ziwei Zhao,Zhongdong Zhang,Qinghua Xu,Yong Xu
Accurate detection of residual H 2 O 2 in food is essential for safety compliance, yet conventional methods rely on its oxidative reactivity and are susceptible to redox-active interferents. We report an alternative strategy based on perhydrolysis of activated aryl esters, which is enabled by common biological buffers as general base catalysts under near-neutral conditions. Mechanistic studies, including kinetics, product identification, and DFT calculations, reveal a concerted asynchronous pathway without a discrete HOO − intermediate. This oxidation-independent mechanism supports two practical assays: a fluorogenic FDA assay for trace quantification (LOD 1.3 μM) and a chromogenic NPA assay for rapid screening (LOD 7.3 μM). The FDA assay gave recoveries of 80–120% in spiked samples, while the NPA assay serves as a screening tool for moderate-to-high peroxide levels. They also outperform a standard HRP-based assay in complex matrices. This work establishes buffer-catalyzed perhydrolysis as a practical platform for interference-resistant H 2 O 2 monitoring in food safety. Download: Download high-res image (124KB) Download: Download full-size image
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Li Wang,Kun Ge,Jiaqi Duan,Xiaomeng Du,Guoqiang Zhou,Lili Ma,Shutao Gao,Jinchao Zhang
Chemodynamic therapy (CDT) based on hydroxyl radicals (•OH) to suppress tumor cells is a promising strategy due to its efficacy and safety. Nevertheless, in tumor cells, CDT still faces challenges such as insufficient •OH and weak killing effect of tumor cells under physiological conditions due to inadequate amounts of endogenous hydrogen peroxide (H 2 O 2 ) and heightened glutathione expression. These challenges limit the therapeutic potential of CDT. To improve the effects of CDT, combination treatment strategies have been developed. Here, we report a rationally designed nanocomposite (CaO 2 @Cu-LA) with self-supplying H 2 O 2 ability from calcium peroxide, and nitric oxide (NO) generation ability from l -arginine. NO molecules not only exhibit a strong killing effect, but also have the potential to transfer into the more cytotoxic substance peroxynitrite anion by reacting with reactive oxygen species. The results showed that CaO 2 @Cu-LA could significantly suppress tumor growth by increasing •OH radicals and NO molecules. Taken together, the strategy developed here provides a good application foreground to yield a remarkable synergistic antitumor effect of CDT and NO gas therapy.
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ACS ES&T Engineering
·
2023
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IF 7.1
Beiping Zhang,Chaoting Guan,Qin Guo,Run Huang,Jin Jiang
Electrochemical technologies and permanganate oxidation are two attractive strategies in water treatment due to their low cost, easy operation, good adaptability, and environmental friendliness. Interestingly, recent studies have demonstrated that the combination of electrolysis and Mn(VII) (E-Mn(VII) process) shows a synergetic effect on organic contaminants degradation. However, the underlying mechanism of the E-Mn(VII) process remains unclear. In this study, the enhanced removal of diclofenac (DCF) by the E-Mn(VII) process was also demonstrated, and the main reactive species were reidentified. It was found that H2O2 was considerably formed via the reduction of O2 on the cathode, and it played a key role in facilitating Mn(VII) transformation into MnO2. Increasing O2 concentration, working potential, and pH value were conducive to H2O2 formation as well as Mn(VII) transformation to MnO2. Higher Mn(VII) dosages did not impact H2O2 formation but also led to faster MnO2 formation. The enhanced formation of MnO2 was favorable for the fast degradation of DCF in the E-Mn(VII) process owing to the catalytic effect of MnO2 on Mn(VII) oxidation. This was confirmed by the observation that (i) the E-Mn(VII) process showed a similar pH-dependent oxidation trend to that of MnO2 catalytic oxidation of Mn(VII) (i.e., the reactivity was much stronger at lower pH); and (ii) the addition of MnO2 prepared ex situ had a significant enhancing effect on DCF oxidation by the E-Mn(VII) process. Moreover, the possible contribution of reactive manganese intermediates such as soluble free Mn(III), Mn(VI), and Mn(V) was ruled out by the results of the probe experiments, UV–visible spectrophotometry, and examining the reactivity of Mn(III) complexes prepared ex situ. Also, the results of radical scavenging experiments indicated the negligible contribution of HO•. Furthermore, for the practical application of the E-Mn(VII) process in water decontamination, suitable operating parameters (e.g., a moderate potential and relatively lower pH) should be determined to avoid the fast loss of Mn(VII) and the electrical energy consumption. Overall, this work brings new insights into the reaction mechanism of the E-Mn(VII) process as well as proposes an efficient, sustainable, and feasible strategy for water and wastewater treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Wei Gan,Xucheng Fu,Juncheng Jin,Jun Guo,Miao Zhang,Ruixin Chen,Chunsheng Ding,Yuqing Lu,Jianrou Li,Zhaoqi Sun
Developing efficient and facilitated recycling photocatalysts for H 2 O 2 formation is an ideal strategy for solar-to-chemical energy conversion. In this work, we synthesized ultrathin C 3 N 5 nanosheets through the process of thermal polymerization and polyvinylpyrrolidone (PVP)-assisted solvent exfoliation. Subsequently, the obtained ultrathin C 3 N 5 nanosheets were tightly attached to the surface of TiO 2-x arrays, resulting in an enhanced photocatalytic H 2 O 2 production rate. The density functional theory (DFT) calculations demonstrate that an internal electric field (IEF) is generated between the TiO 2-x array and the ultrathin C 3 N 5 due to the different work functions. The presence of IEF provides an additional driving force for carrier separation and transfer in the heterointerface. Benefitting from this unique strategy, the optimal heterojunction obtains the highest H 2 O 2 formation rate (2.93 μmol/L/min), which is about 4.1 times than that of TiO 2-x arrays. The rotating disk electrode (RDE) analysis manifests H 2 O 2 formation through 2e - -dominated oxygen reduction reaction (ORR). This research provides an innovative strategy for assembling a type-II heterojunction with a useful IEF for efficient photocatalytic H 2 O 2 production.
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Advanced Science
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2023
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IF 15.1
Yulu Xu,Xia Hu,Yuyuan Chen,Sijie Lin,Chen Wang,Faliang Gou,Xiaogang Yang,Weiwei Zheng,De-Kun Ma
Resorcinol-formaldehyde (RF) resin represents a promising visible-light responding photocatalyst for oxygen reduction reaction (ORR) toward H 2 O 2 production. However, its photocatalytic ORR activity toward H 2 O 2 generation is still unsatisfied for practical application. Herein, 3-hydroxythiophenol-formaldehyde (3-HTPF) resin microspheres synthesized through polycondensation reaction between 3-HTP and formaldehyde at room temperature and subsequent hydrothermal treatment exhibit enhanced photocatalytic ORR activity is reported. The experimental results show that the partial substitution of hydroxy group (─OH) by sulfhydryl one (─SH) through using 3-HTP to replace resorcinol could slow the rates of nucleation and growth of the resin particles and lead to strongly π -stacked architecture in 3-HTPF. The introduction of ─SH group can also improve adsorption ability of 3-HTPF to O 2 molecules and enhance ORR catalytic activity of the photocatalysts. Stronger built-in electric field, better adsorption ability to O 2 molecules, and increased surface catalytic activity collectively boost photocatalytic activity of 3-HTPF microspheres. As a result, H 2 O 2 production rate of 2010 µ m h −1 is achieved over 3-HTPF microspheres at 273 K, which is 3.4 times larger than that obtained using RF submicrospheres (591 µ m h −1 ). The rational substituent group modulation provides a new strategy for designing polymeric photocatalysts at the molecular level toward high-efficiency artificial photosynthesis.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Yu Cao,Huanhuan Shi,Yun Zheng,Zhongjian Tan,Zhihao Xie,Congxuan Zhang,Zhen Chen
The low concentration of respiratory H 2 O 2 requires high detection sensitivity and stability. In this work, a Polyaniline/Prussian Blue Nanolayer (nano-PANI/PB) coated electrode using a 30 nm porous alumina template was fabricated to enhance the roughness of the electrode surface to improve the sensitivity of H 2 O 2 detection. The limit of detection of 2.52 μM was realized within a detection range of 0–1 mM. In addition, a condensing device that uses microchannel with a secondary flow structure was designed with computational fluid dynamics to downsize the exhaled breath condensing device and improve the condensing efficiency. Increasing the contact area between exhaled breath and condensing materials in the microchannel can obviously increase the amount of condensate. The performance of the condensing device was visualized through the condensing of sodium fluorescein solution. A multichannel condensing device was integrated with screen printing electrode, three-electrode detection circuit and display module into a N95 mask to realize portable Exhaled breath condensate (EBC) detection and showed a favorable feasibility. The application of this portable exhaled breath measurement device could be expanded through modifying the specific biomarker probes on electrode, and may provide some inspirations for the development of wearable and portable non-invasive healthy monitoring devices.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2023
·Vol. 33
·期 10
·3237-3246
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IF 4
Zhu Xiaokang,Wang Xiuwu,Zhou Guiyang,Yin Hong,Qi Dongming,Deng Hangjun,Chen Tao
The preparation of polymer-metal complex is an effective way to achieve the bifunctionality of polymer and metal. In this study, temperature-sensitive polymer was synthesized from triethylene glycol methyl ether methacrylate (MEO 2 MA) and methacrylic acid N-hydroxysuccinimide ester (NMS) monomers via reversible addition-fragmentation chain transfer (RAFT) polymerization. 6-Aminohexanoic acid was introduced into the temperature-sensitive polymer using an activated ester strategy to obtain branched carboxyl-containing polymers. The carboxyl group in the polymer was coordinated with Fe(III), resulting in temperature-sensitive polymer-based iron complexes. The obtained iron complexes were used as homogeneous catalysts in the Fenton oxidation. Where, 97% and 96% decolorization of rhodamine B (RhB) and methylene blue (MB) could be achieved within 2 h for P(COOH 10 - co -MEO 2 MA 41 )-Fe 3+ , and the catalytic activities increased with the increase of the COOH content of polymer. In addition, the recycling of the catalyst can be achieved by the heating-centrifugal precipitation method using the temperature-sensitive nature of the polymer. Graphical Abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yanqing Cong,Shiyi Zhang,Qiuang Zheng,Xinyue Li,Yi Zhang,Shi-Wen Lv
Photocatalytic oxygen reduction is regarded as the cleanest approach for the production of hydrogen peroxide (H 2 O 2 ). Herein, oxygen-modified graphite carbon nitride (g-C 3 N 4 ) with nitrogen-defect (namely g-C 3 N 4 -ND4-OM3) was synthesized by a feasible method. Owing to the existence of nitrogen vacancy and oxygen-containing functional group, the absorption bands derived from n → π* and π → π* electronic transitions were enhanced, thereby enlarging the visible light response range of catalysts. Interestingly, nitrogen-defect can capture electron and effectively suppress the recombination of photoinduced electrons and holes. More importantly, the introduction of oxygen-containing functional groups can improve the hydrophilicity of g-C 3 N 4 , which was beneficial for the adsorption of dissolved oxygen. The electrostatic potential distributions of g-C 3 N 4 -based photocatalyst structural unit were also changed after introducing nitrogen vacancy and oxygen-containing functional group, and the electron-donating ability of g-C 3 N 4 was improved. As a result, the evolution rate of H 2 O 2 catalyzed by g-C 3 N 4 -ND4-OM3 was as high as 146.96 μmol/g/L under visible light irradiation. The photocatalytic H 2 O 2 generation was completed through the direct 2-e − oxygen reduction. In short, current work will share novel insights into photocatalytic H 2 O 2 generation over g-C 3 N 4 -based catalyst.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Jing Zhang,Miaoqi Liu,Bo Pang,Chun Liu,Junjun Ma,Jianrui Niu,Ruina Zhang
Microbubble ozonation combined with electro-generated H 2 O 2 process ( E H 2 O 2 -MB-O 3 ) was applied to degrade ciprofloxacin (CIP) as a typical antibiotic in wastewater in this study. The results showed that the performance of CIP degradation and mineralization in E H 2 O 2 -MB-O 3 process was more efficient than other related processes. Microbubble ozonation and electro-generated H 2 O 2 showed obvious synergistic effect on enhanced CIP removal in E H 2 O 2 -MB-O 3 process. The O 3 dosage, applied current and initial pH in E H 2 O 2 -MB-O 3 process were optimized as 12.5 mg/min, 50 mA and 7.0 (uncontrolled). Under the optimal conditions, CIP could be degraded completely within 60 min and the TOC removal efficiency of 28.85% could be achieved within 90 min in E H 2 O 2 -MB-O 3 process. The corresponding ozone utilization efficiency was close to 100%. More efficient ROS generation was observed in E H 2 O 2 -MB-O 3 process, especially •OH, compared with other related processes. The contribution rates of •OH, 1 O 2 , O 3 and O 2 .- to CIP removal were determined as 66.79%, 23.57%, 6.67% and 2.98% in E H 2 O 2 -MB-O 3 process, respectively. The electro-generated H 2 O 2 was clarified to contribute to not CIP removal but ROS generation. Three CIP degradation pathways were proposed according to identified degradation intermediates, which indicated that pyridone structure of quinoline and piperazine ring in CIP molecule could be destroyed more easily than benzene ring of quinoline, and the hydroxylation seemed to prevail in these CIP degradation pathways due to •OH electrophilic addition reaction probably. The removal of other antibiotics in E H 2 O 2 -MB-O 3 process also depended on not ozone direct oxidation but •OH oxidation mainly.
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