SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Hongwei Luo,Qianqian Cheng,Dongqin He,Ganning Zeng,Jianqiang Sun,Jun Li,Xiangliang Pan
Methylmercury (MeHg) is a neurotoxin that bioaccumulates in organisms and it forms strong complexes with reduced sulfur-containing ligands in dissolved organic matter (DOM). In the present study, the influences of solar radiation and sulfide addition reaction of humic acids (HA) on MeHg binding to HA were investigated using synchronous fluorescence and FT-IR two-dimensional correlation spectroscopic (2DCOS) analysis. Results showed that the complexation of fluorescent fractions of HA and sulfur-reacted HA (S-HA) with MeHg was not significantly affected by photoreaction treatments and the affinity of fluorescent fractions followed the order of protein-like fractions > humic-like fractions > fulvic-like fractions for both HA and S-HA. FT-IR 2DCOS analysis showed that the affinity of various binding sites in DOM for MeHg changed under different photoreaction treatments. Under dark treatment, small molecular compounds with low humification degree such as aromatic amino acids may be the site with the strongest binding ability to MeHg in HA, whereas aliphatic amino acids and sulfur-containing groups from sulfide addition reactions play a role in complexing of S-HA and MeHg. Under BS treatment (irradiation of DOM before MeHg binding), aliphatic compounds in HA preferentially bind to MeHg and aliphatic amino acids are the components with the strongest complexing ability; but for S-HA binding to MeHg, unsaturated functional groups and aromatic groups are more sensitive (alkenes > alkanes, phenols > alcohols). Under AS treatment (irradiation of DOM after MeHg binding), unsaturated bonds and aromatic compounds in HA preferentially bind to MeHg and aromatic amino acids show the strongest complexing ability; but for S-HA binding to MeHg, aliphatic groups show the strongest complexing ability (alkanes, alkenes > aromatics). These findings help us to better understand the complexation mechanisms between MeHg and DOM.
研究领域:
环境科学
·
毒理学
✓ 已验证
DOI
高影响因子
TALANTA
·
2025
·
IF 6.1
Yifei Ma,Lijie Zhang,Hong Yang,Shanshan Zhu,Jinhua Liu
Highly selective and sensitive determination of dopamine (DA) from multiple sources remains a persistent and significant challenge. Here, we develop an imidazole-triggered in situ fluorescence reaction system for highly selective and sensitive determination of DA from various sources (human, horse, dog, rabbit, and mouse). The system operates by catalyzing the oxidation of DA with 1,5-Dihydroxynaphthalene (1,5-DHA) through a Lewis base formed by imidazole, leading to the rapid generation of yellow azamonardine fluorescent compounds (AFC). Notably, the system demonstrates minimal background noise and a high signal-to-noise ratio of up to 300-fold with a determination limit of 33.33 pM, making it 10-100 times more sensitive than conventional enzyme-linked immunosorbent assay (ELISA) methods. Moreover, selectivity tests reveal that our system can effectively distinguish between several common interfering substances, even at concentrations as low as 10 nM. The developed system shows promising results in detecting DA from diverse sources (humans, horses, dogs, rabbits, and mice), including urine samples from clinical patients, exhibiting good agreement with traditional ELISA kits. Therefore, the established in situ fluorescence reaction system holds great potential for the determination of DA-related disorders due to its impressive analytical capabilities.
研究领域:
分析化学
·
神经生物学
·
医学检测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2022
·
IF 4.331
Shizhong Zhang,Chuanbiao Zhang,Yang Fu,Linhai Li,Chuanbing Huang,Yang Lin,Chongqin Zhu,Joseph S. Francisco,Zhiyuan He,Xin Zhou,Jianjun Wang
Ice affects many chemical reactions in nature, which greatly influences the atmosphere, climate, and life. However, the exact mechanism of ice in these chemical reactions remains elusive. For example, it is still an open question as to whether ice can act as a catalyst to greatly enhance the reactivity and selectivity, which is essential for the production of some natural compounds in our planet. Here, we discover that ice can lead to high efficiency and stereoselectivity of the [2 + 2] photodimerization of coumarin and its derivatives. The conversion of the [2 + 2] photodimerization of coumarins enhanced by ice is dozens of times higher than that in the unfrozen saturated solution, and the reaction displays a high syn-head-head stereoselectivity (>95%) in comparison with those in the absence of the ice. Note that almost no reaction occurs in the crystal powder and melt of the coumarins, indicating that the role of ice in the photodimerization reaction is not simply due to the usual mechanisms found in the freezing concentration. We further reveal that the reaction rate is found to be proportional to the total area of the ice surface and follows Michaelis–Menten-like kinetics, indicating that the ice surface catalyzes the reaction. Molecular dynamics simulations demonstrate that ice surfaces can induce reactants to form a two-dimensional liquid-crystal-ordered layer with a suitable intermolecular distance and unique side-by-side packing, facilitating stereoselective photodimerization for syn-head-head dimers. These findings give evidence that ice-surface-induced molecular assembly may play an important role in atmospheric heterogeneous photoreaction processes.
研究领域:
化学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Liuqing Xiao,Yuxing Huang,Yu Luo,Bo Yang,Yizhen Liu,Xuechang Zhou,Junmin Zhang
Cotton fiber is an abundant natural material, which has a long history of application in human daily life. However, a report on using such material in catalysis for organic synthesis is rare. We envisaged that the hydroxyl groups on the surface of cotton fiber could be utilized for functionalization and further immobilization of organic catalysts. In this report, we demonstrate the facile functionalization of cotton fiber by growing polymer brushes on its surface and further anchoring of Rose Bengal (RB) organic photocatalyst. This novel composite cotton photocatalyst demonstrated high efficiency in catalyzing cross-dehydrogenative coupling reactions and N-demethylation reactions with irradiation of visible light. The catalytic reaction can be facilely scaled up by a homemade circulating flow reactor.
研究领域:
化学工程
·
材料科学
·
有机合成
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
·
2020
·
IF 0.936
Jia-Hui ZHAO,Guo-Yong LIU,Shuang WANG,Sha-Sha LU,Jian SUN,Xiu-Rong YANG
Dopamine is a crucial monoamine neurotransmitter involved in multiple cognitive functions and pathological processes. Herein, we described a rapid chromogenic and fluorogenic reaction between dopamine and naphthoresorcinol under ambient conditions, and found that the product possessed intense visible absorbance and high fluorescence quantum yield (78%) in aqueous solution. Through electrospray ionization-mass spectrometry (ESI-MS) and nuclear magnetic resonance (NMR) analysis, the plausible reaction mechanism between dopamine and naphthoresorcinol was deduced, and the structure of the reaction product was confirmed. Inspired by the explicit mechanism and accessible reaction conditions, a straightforward and selective assay for dopamine concentration was developed with colorimetric and fluorescent dual-modal signals based on the in situ reaction.
研究领域:
生物化学
·
分析化学
·
神经科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jianyong Zhao,Xiangchao Meng
A novel slant perforated mesh-plate photoreactor (SPPR) was designed and fabricated. The central assembly of SPPR was an array of slant perforated mesh-plate coated with TiO 2 (P25). The performance of SPPR in water detoxification was evaluated with regard to the degradation of phenol as the target pollutant. The effects of slant plate tilt angle (α) and perforated plate opening aperture diameter on SPPR performance were investigated and analyzed. The photocatalytic performance of SPPR increased with decreasing α. The SPPR with an α of 15° and a pore size of 1 mm showed the best performance with 9.17 h required to reach 80% of phenol degradation (4-L, initial concentration: 15 mg/L). The mass transfer was introduced into the kinetic reaction model, and mass transfer coefficients were calculated for SPPRs with different structures. Flow rate and initial pollutant concentration were investigated for their effects on degradation efficiency. In addition, the activity of SPPR under natural sunlight has also been tested to explore its potential to be applied in practice.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chemical Engineering and Processing-Process Intensification
·
2019
·
IF 3.031
Suqi Zhang,Jie Zhang,Jian Sun,Zhiyong Tang
A novel capillary microphotoreactor (MPR) packed with TiO 2 -coated glass beads was developed in this work and its photocatalytic performance was evaluated using degradation of methylene blue (MB) as a model reaction. As compared to conventional wall-coated MPR, the use of glass beads as packing material not only provides a larger surface area for catalyst immobilization and shortens the mass transfer route, but also introduces flow perturbation. An appropriate size of glass beads should be chosen for packing because there is a tradeoff between increased catalysts coating area and decreased light penetration. It was found out that nearly 100 % degradation efficiency could be achieved in 80# glass beads packed MPR within short residence time (20 s), which was more than 2 orders of magnitude larger than value obtained in wall-coated MPR under the same operational conditions. Moreover, the packed MPR showed good durability, which declined by about 17 % after 6 h of operation and then remained stable for next 19.5 h.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Journal of Flow Chemistry
·
2021
·Vol. 12
·期 1
·41-49
·
IF 2.786
Lan Zhou,Lu Yangcheng
Benzyl iodide, an important organic synthesis intermediate, has high reaction activity as well as high commercial value due to its weakest carbon-halogen bond. However, the development of direct iodination of toluene for benzyl iodide is limited by the fact that the C-I bond is easily decomposed under heat or light. In this work, the photoiodination of toluene to synthesize benzyl iodide in the I 2 /PhI(OAc) 2 / t BuOH system was carefully investigated in the flow photoreactor under LEDs irradiation. The reaction window suitable for the reaction kinetic characteristics recognition was revealed with the considerations of the effects of various parameters including light color, light intensity, reaction temperature, residence time, and usage of each substrate. And an optimized result is to achieve 95.83 % of yield and over 99 % of selectivity under a red light with 2.05 mW/cm 2 of light intensity at 80 o C after 15 min reaction. The reaction kinetic model coupling the iodination reaction (photo and thermal reaction) with the decomposition reaction is established, which fits well the experimental results and provides fundamentals for process design and optimization. Graphical abstract
研究领域:
有机化学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL PAPERS
·
2022
·Vol. 76
·期 7
·4235-4244
·
IF 2.146
Ding Yu,Yang Li-Hong,Shen Ji-Wei,Wei Yin-Mao,Wang Chao-Zhan
In this work, simple, cost efficient, highly selective and sensitive assay methods for dopamine (DA) concentration and tyrosinase (TYR) activity were established based on a benzoyl peroxide (BPO) facilitated in situ “turn-on” fluorogenic reaction between resorcinol (RS) and DA, in which BPO was introduced in the system to accelerate DA oxidation, thereby realizing a faster reaction with RS to form the fluorescent substance, azamonardine, which was verified by HPLC, 1 H NMR, 13 C NMR and high resolution mass spectrometry. The introduction of BPO remarkably improved the sensitivity, linearity range and response speed for assay of DA and TYR. For the determination of DA concentration, the concentration has a good linear relationship in the range of 4.0–1.2 μM, and the detection limit is as low as 0.8 nM, and it was successfully applied to measuring DA in human urine and serum samples. In addition, a fluorescent method for determining the TYR activity was further established based on the enzymatic oxidation of tyramine to DA, the detection limit is 0.0013 U mL −1 . And the method was used to determine TYR in human serum and screening of TYR inhibitors.
研究领域:
生物化学
·
医学检验
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2021
·
IF 3.247
Liping Liang,Weishou Tan,Yanyan Dong,Feng Gu,Xu Meng
A cotton fabric with special wettability was prepared in two simple steps. The surface of the fabric was grafted with silicon-oxygen group using 3-(methacryloyloxy) propyl trimethoxysilane (MSPMA) as the reagent, and then (3-mercaptopropyl)triethoxysilane (MPTES) was used to react with the grafted fabric under ultraviolet light according to the principle of thiolene reaction. Meanwhile, the modified cotton fabrics with various pore sizes were obtained via modifying the cotton fabric with different pore size under the same experimental conditions. The as-prepared fabric had a better hydrophobic and lipophilic effect, whose water contact angle could be up to 146.7° and the separation efficiency for different kinds of oil/water mixtures was better than 94%. In addition, the pore sizes of cotton fabrics had a great effect on the rate of oil/water separation, which increased with the increase of the pore size.
研究领域:
材料科学
·
环境工程
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Tan Meng,Xiao Su,Peizhe Sun,Wenjun Sun,Domenico Santoro,Hong Yao,Hui Wang
UV-based advanced oxidation processes (UV-based AOPs) via photolysis of radical precursor chemicals (RPCs) are among the most effective technologies for eliminating trace organic contaminants in water treatment facilities. However, mathematical discussions on the kinetics and energy consumption for the engineering photoreactor set-up of UV-based AOPs, especially the newly proposed UV-based AOPs (e.g., UV/persulfate, UV/chlorine and UV/chloramine), are scarce. In this study, a photoreactor with reflective sleeves was mathematically characterized and validated using clean and complex water matrices, and approaches for measuring effective light absorbance by RPC ( I RPC ) and the reflectance of the photoreactor wall ( η ) were proposed. By applying I RPC and η , and employing geosmin as a model compound, energy optimization of the UV-based AOPs was conducted based on an updated kinetic model . A new equation was derived for UV/H 2 O 2 to obtain the most cost-effective RPC dose regarding EE/O ( electric energy required for one order of contaminant removal ) ( C opt-EE/O ). This equation was then successfully extended to other UV-based AOPs (including UV/persulfate, UV/chlorine, and UV/chloramine). The balance between the treatment goals and operational costs was also discussed. Overall, the new concepts and approaches proposed in this study may aid in the energy optimization and reduce RPC consumption of various UV-based AOPs for engineering applications .
研究领域:
环境科学
·
水处理工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Jintao An,Qianrui Lv,Yuchao Wang,Wenbo Yang,Shengyang Tao,Lijing Zhang,Alexander A. Miskevich,Valery A. Loiko
Accurate, stable, and reproducible photocatalytic reaction systems remain a major challenge when performing photocatalytic mechanism studies. In this paper, we designed and built a standard photocatalytic reactor to realize the precise adjustment of each parameter related to the photoreaction to meet the demand for the accurate study of photochemical reaction mechanisms and can realize the personalized settings for different photochemical reactions. Based on this standard reactor, the influence of each independent parameter on the conversion rate of the reaction was studied based on the model reaction of 9,10-diphenylanthracene oxidation, and a mathematical model of the coupling influence of multiple factors to the photochemical reaction was obtained using the dimensionless data processing method. The mathematical model can help to carry out the coordinated selection of various parameters of photochemical reactions, reduce the reaction cost, and improve the reaction efficiency. Furthermore, we demonstrate the simplicity and accuracy of this reactor in measuring and calculating the quantum efficiency of photochemical reactions. This work is of great guidance to exploring the basic principles of photochemical reactions, the selection of reaction parameters, and the construction of photochemical reactors.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）