JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Xiaohui Zhang,Qingqing Gu,Yanfu Ma,Qiaoqiao Guan,Rui Jin,Hengwei Wang,Bing Yang,Junling Lu
For supported metal catalysts, the underlying support not only disperses and stabilizes metal particles, but also modulates their electronic structures remarkably, and even directly participates in catalytic reactions. Here we report that Pd nanoparticles (NPs) supported on oxygen-functionalized carbon black (Pd/O-C) show an unexpected inverse trend of selectivity on Pd particle size in chemoselective hydrogenation of para -chloronitrobenzene ( p -CNB), compared to those on carbon black (Pd/C). In situ X-ray photoemission spectroscopy reveals that the Pd NPs are more positively charged with decrease of particle size in both samples, while the Pd NPs in Pd/O-C have relatively higher fractions of positive Pd δ+ species than those in Pd/C with similar sizes. Fourier transform infrared spectroscopy shows that the balance of positive Pd δ+ species strongly modulates the competitive adsorption of -NO 2 and -Cl group in p -CNB according to their different electronegativities. As a consequence, we, for the first time, demonstrate that a moderate positive charge of Pd NPs is essential to improve the p- chloroaniline ( p -CAN) selectivity, while too high or too low positive charge could impel the adsorption of the less negatively charged -Cl group, thus generating the dehalogenated aniline by-product. These findings suggest that precise tailoring of the electronic structures of metal NPs could be essential for design of high chemoselective metal catalysts.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
IONICS
·
2022
·Vol. 28
·期 9
·4321-4329
·
IF 2.961
Zhang Jin-Zhong,Wu Shuai,Shen Fengxia,Song Wenkang,Hua Yaxin,Wu Zhenyu,Zhang Xiao-Gang,Shi Jin
A novel gas diffusion electrode (GDE) electrolyzer has been constructed to convert CO 2 into CO, with chlorine (Cl 2 ) and sodium carbonate (Na 2 CO 3 ) produced as the by-products. Using this method, the product value yielded from CO 2 electrolysis can be increased substantially. In contrast to the conventional GDE electrolyzer, we use a cation-exchange membrane as the diaphragm to separate the cathode from the anode compartment, and use NaCl aqueous solution as the anolyte. During the electrolysis process, CO 2 is reduced to CO on the cathode, with CO 3 2− generated accompanied with CO formation. On the anode, Cl − is oxidized to Cl 2 . Na + in the anode chamber transfers through the cation-exchange membrane, and migrates into the catholyte. Thus, Na 2 CO 3 can be obtained owing to the co-existing of Na + and CO 3 2− in the catholyte. Using this method, CO 3 2− penetrating through the anion-membrane can be avoided. This problem has been considered as the crucial obstacle that impedes the practical utilization of the conventional GDE electrolyzer. Our designed GDE electrolyzer has a promising application perspective in the phosgene chemical industry.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Applied Bio Materials
·
2020
·
IF 0
Xiaojun He,Ziman Zheng,Feifan Zhang,Chuchu Xu,Wei Xu,Lisong Ye,Xiaoshuai Sun,Zhan Zhou,Jianliang Shen
Bioactive molecules play a vital role in the process of regulating the redox balance in the intracellular environment, especially in maintaining the function of organelles. To explore the association and function of bioactive molecules in organelles, it is essential to develop a chemosensor tool that uses multiresponse fluorescence signals to distinguish between and track two related bioactive molecules in organelles. However, the development of sensors with multiresponse functions is still a challenging task. Herein, we present a unique and practical single chemosensor (Mito-CTC) that can monitor HClO (as an oxidative substance) and H2S (as a reductive substance) in mitochondria (organelle targeting) with multiresponse fluorescence signals. The response of the sensor to HClO and H2S changes from red to green and blue channel emission simultaneously, respectively, thereby providing a specific signal response to reductive/oxidative substances in the mitochondria. Using a single chemosensor, we have realized multichannel bioimaging of the exogenous and endogenous HClO and H2S in cellular mitochondria. Additionally, the excellent properties of the sensor Mito-CTC can be used to reveal the relationship between HClO and H2S in mitochondria. Meanwhile, Mito-CTC has been endowed with the ability to image in bacteria and zebrafish attributed to the good permeability and low cytotoxicity. Expectantly, drug-induced liver injury (DILI) caused by fluoxetine (an antidepressant drug) and the degree of drug-induced toxicity to the liver were evaluated using Mito-CTC through discriminating and imaging HClO, indicating that Mito-CTC has the potential function of evaluating the toxicity of the drug to the liver.
研究领域:
生物化学
·
医学影像
·
药理学
✓ 已验证
DOI
PubMed
International Journal of Environmental Research and Public Health
·
2019
·Vol. 16
·期 9
·1629
·
IF 2.468
Jie-Xu Ye,Tong-Hui Lin,Jing-Tao Hu,Rabin Poudel,Zhuo-Wei Cheng,Shi-Han Zhang,Jian-Meng Chen,Dong-Zhi Chen
In this study, a water–silicone oil biphasic system was developed to enhance the biodegradation of monochlorobenzene (CB) byDelftia tsuruhatensisLW26. Compared to the single phase, the biphasic system with a suitable silicone oil fraction (v/v) of 20% allowed a 2.5-fold increase in the maximum tolerated CB concentration. The CB inhibition onD. tsuruhatensisLW26 was reduced in the presence of silicone oil, and the electron transport system activity was maintained at high levels even under high CB stress. Adhesion of cells to the water–oil interface at the water side was observed using confocal laser scanning microscopy. Nearly 75% of cells accumulated on the interface, implying that another interfacial substrate uptake pathway prevailed besides that initiated by cells in the aqueous phase. The 8-fold increase in cell surface hydrophobicity upon the addition of 20% (v/v) silicone oil showed that silicone oil modified the surface characteristics ofD. tsuruhatensisLW26. The protein/polysaccharide ratio of extracellular polymeric substances (EPS) fromD. tsuruhatensisLW26 presented a 3-fold enhancement. These results suggested that silicone oil induced the increase in the protein content of EPS and rendered cells hydrophobic. The resulting hydrophobic cells could adhere on the water–oil interface, improving the mass transfer by direct CB uptake from silicone oil.Keywords:waste gas;monochlorobenzene;biodegradation;silicone oil;cell adhesion
研究领域:
环境科学
·
微生物学
✓ 已验证
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
·
2022
·
IF 4.01
Chunhao Liu,Yongli Wang,Yihan Zhao,Xin Li,Na Wang,Xin Huang,Ting Wang,Hongxun Hao
In an attempt to understand the relationship between solution chemistry and polymorphic nucleation, the flexible molecule chlorpropamide is used as a model compound to study its cooling crystallization behavior in four solvent systems. Online ATR-FTIR spectra proved the existence of dimers and solvated monomers in the solution. 2D nuclear overhauser effect spectroscopy and molecular dynamics simulations further revealed the molecular preassembled species in the solution. The results show that, in ethanol, ethanol/n-heptane, and ethyl acetate/n-heptane solvents, the solute molecules exist in the form of solvated monomers in multiple conformations. The stable formation of metastable form γ in ethyl acetate/n-heptane shows that, compared to conformational flexibility, the desolvation process plays a crucial role in overall self-assembly during the nucleation process. While in ethyl acetate, the solute molecules mainly exist as dimers and the rearrangement of the “wrong conformation” dimers becomes a key step to the nucleation rate and leads to the formation of stable form α. As a result, the self-association mode and conformational distribution of chlorpropamide in the solution work together to affect the nucleation process and polymorphic outcome.
研究领域:
化学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Enguang Nie,Haiyan Wang,Yan Chen,Yuhui Lu,Kashif Akhtar,Muhammad Riaz,Sufen Zhang,Zhiyang Yu,Qingfu Ye
Triclosan is a widely used biocide against microorganisms and is ubiquitously distributed in the environment. Triclosan can be accumulated into plants from soil and hydroponic media. However, little information is currently available on the comparative fate of triclosan in plants under soil and hydroponics cultivation conditions and factors governing uptake. Therefore, this study was designed to comparatively elucidate the uptake mechanism of 14 C-triclosan in youdonger ( Brassica campestris subsp. Chinensis var. communis ) grown under different soils and hydroponics and clarify dominant uptake factors. Results showed that 77.2% of 14 C were accumulated in youdonger grown in a hydroponic system, while only 1.24%–2.33% were accumulated in the two soil-planting systems. In addition, the bioconcentration factor (BCF) of 14 C-triclosan in soil-plant systems was approximately 400-fold smaller than that in the hydroponics. In the soil-planting system, a strong linear correlation was found between concentrations of triclosan in soil pore water and youdonger plant (R 2 > 0.85, p < 0.01) at different incubation times. Therefore, triclosan in pore water might be a good indicator to estimate its accumulation in plants and is significantly affected by soil pH, clay, and organic matter contents. The estimated average dietary intakes of triclosan for youdonger grown in hydroponic and soil-planting systems were estimated to be 1.31 ng day −1 kg −1 and 0.05–0.12 ng day −1 kg −1 , respectively, much lower than the acceptable dietary intakes of triclosan (83 μg day −1 kg −1 ), indicating no significant human health risks from youdonger consumption. This study provided insights into uptake routes of triclosan into youdonger plants from both soil and hydroponic systems, bioavailability of triclosan in different soils, and further assessment of human exposure to triclosan from youdonger.
研究领域:
环境科学
·
植物学
✓ 已验证
DOI
高影响因子
Frontiers of Environmental Science & Engineering
·
2024
·Vol. 18
·期 9
·1-14
·
IF 6.1
Liao Xiaobin,Liu Xinyue,He Yueyun,Tang Xueping,Xia Ruanjunjie,Huang Yongjun,Li Wenhua,Zou Jing,Zhou Zhenming,Zhuang Mazhan
During the COVID-19 pandemic, most sewage treatment plants increased disinfectant dosages to inactivate pathogenic viruses and microorganisms more effectively. However, this approach also led to the production of more disinfection by-products (DBPs). To ensure both disinfection efficiency and a reduction in DBP formation, new disinfection protocols are required. In this study, the disinfection efficiency, DBP amounts, and toxicity changes resulting from ozone (O 3 ), ultraviolet (UV), chlorine (Cl 2 ), and their combined processes were examined. The results demonstrated that the O 3 /UV/Cl 2 combination achieved the highest disinfection efficiency. Chlorination produced the most DBPs, whereas UV treatment reduced the formation of trihalomethane (THM), halogenated ketones (HKs), haloacetic acids (HAA), dichloroacetonitrile (DCAN) and N-nitrosodimethylamine (NDMA) by 45.9%, 52.6%, 82.0%, 67.95%, and 47%, respectively. O 3 also significantly reduced their production by 99.1%, 91.1%, 99.5%, 100%, and 35%. Intracellular organic matter (IOM) was identified as the primary DBP precursors, producing 2.94 times more DBPs than extracellular organic matter (EOM). The increased DBP formation during chlorination was attributed to IOM leakage and cell membrane damage, which was verified using scanning electron microscopy (SEM). The toxicities of DBPs were evaluated for six disinfection methods, revealing inconsistent results. The overall toxicities were assessed using zebrafish embryo experiments. Both evaluations indicated that chlorination alone was the least favorable method. In addition, the toxicities followed a sequence: Cl 2 ≈ O 3 /Cl 2 > O 3 > O 3 /UV/Cl 2 > UV > UV/Cl 2 . These findings can serve as a reference for sewage treatment plants in selecting appropriate disinfection methods to manage the COVID-19 epidemic from comprehensive perspective.
研究领域:
环境科学
·
公共卫生
·
毒理学
✓ 已验证
DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 18
·5709-5717
·
IF 4.478
Yu Ying,Hu Jiaju,Zhao Xinyi,Liu Jiangchuan,Gao Ying
Photochemical vapor generation (PVG) of germanium (Ge) was first reported in this work. The synergistic effect from cobalt/chloride ions and air-liquid interfaces was found for the PVG of Ge. No obvious signal response was observed from the standard solution of Ge in 10% (v/v) formic acids (FAs) under UV irradiation. The addition of 300 mg L −1 of Co 2+ and 30 mmol L −1 of Cl − resulted in enhanced photochemical reduction for Ge, and the introduction of air-liquid interfaces proceeding and succeeding the sample solution caused another 4.6 folds of enhancement in signal response of Ge. Under the selected condition, the limit of detection (LOD, 3σ, n = 11) was obtained to be 0.008 ng mL −1 with inductively coupled plasma mass spectrometry (ICP MS) measurement. A good precision, expressed as a relative standard deviation (RSD, n = 7) of 2.0%, was found from replicated measurements of 2 ng mL −1 of Ge. The generation efficiency was found to be no better than 9 ± 2%. The PVG mechanism of Ge was investigated in this work. The new finding is useful for understanding the principle of PVG, and further exploring the analytical and environmental application of PVG. Graphical abstract
研究领域:
分析化学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Materials Au
·
2023
·
IF 0
Dongdong Li,Ning Zhang,Dandan Gao,Ziyu Zhuang,Dewen Zeng
Lithium aluminum layered double hydroxide chlorides (LADH-Cl) have been widely used for lithium extraction from brine. Elevation of the performances of LADH-Cl sorbents urgently requires knowledge of the composition–structure–property relationship of LADH-Cl in lithium extraction applications, but these are still unclear. Herein, combining the phase equilibrium experiments, advanced solid characterization methods, and theoretical calculations, we constructed a cyclic work diagram of LADH-Cl for lithium capture from aqueous solution, where the reversible (de)hydration and (de)intercalation induced phase evolution of LADH-Cl dominates the apparent lithium “adsorption–desorption” behavior. It is found that the real active ingredient in LADH-Cl type lithium sorbents is a dihydrated LADH-Cl with an Al:Li molar ratio varying from 2 to 3. This reversible process indicates an ultimate reversible lithium (de)intercalation capacity of ∼10 mg of Li per g of LADH-Cl. Excessive lithium deintercalation results in the phase structure collapse of dihydrated LADH-Cl to form gibbsite. When interacting with a concentrated LiCl aqueous solution, gibbsite is easily converted into lithium saturated intercalated LADH-Cl phases. By further hydration with a diluted LiCl aqueous solution, this phase again converts to the active dihydrated LADH-Cl. In the whole cyclic progress, lithium ions thermodynamically favor staying in the Al–OH octahedral cavities, but the (de)intercalation of lithium has kinetic factors deriving from the variation of the Al–OH hydroxyl orientation. The present results provide fundamental knowledge for the rational design and application of LADH-Cl type lithium sorbents.
研究领域:
材料化学
·
环境科学
✓ 已验证
DOI
Entropy
·
2022
·Vol. 24
·期 6
·765
·
IF 2.738
Haopeng Zeng,Yu Zhang,Lei Zhang,Zhaoyang Chen,Xiaosen Li
Depressurization combined with brine injection is a potential method for field production of natural gas hydrate, which can significantly improve production efficiency and avoid secondary formation of hydrate. In this work, the experiments of hydrate production using depressurization combined with brine injection from a simulated excess-water hydrate reservoir were performed, and the effects of NaCl concentration on hydrate decomposition, temperature change, and heat transfer in the reservoir were investigated. The experimental results indicate that there is little gas production during depressurization in a excess-water hydrate reservoir, and the gas dissociated from hydrate is trapped in pores of sediments. The high-water production reduces the final gas recovery, which is lower than 70% in the experiments. The increasing NaCl concentration only effectively promotes gas production rate in the early stage. The final cumulative gas production and average gas production rate have little difference in different experiments. The NaCl concentration of the produced water is significantly higher than that which is in contact with hydrate in the sediments because the water produced by hydrate decomposition exists on the surface of undissociated hydrate. The high concentration of NaCl in the produced water from the reactor significantly reduces the promoting effect and efficiency of NaCl solution on hydrate decomposition. The injection of NaCl solution decreases the lowest temperature in sediments during hydrate production, and increases the sensible heat and heat transfer from environment for hydrate decomposition. The changes of temperature and resistance effectively reflect the distribution of the injected NaCl solution in the hydrate reservoir.
研究领域:
能源科学
·
地质学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Mengjie Wang,Huanhuan Shi,Shuai Shao,Kun Lu,Hanyu Wang,Yun Yang,Zhimin Gong,Yuegang Zuo,Shixiang Gao
The photolysis of amlodipine (AML) as a ubiquitous pollutant in natural water has been extensively studied. Montmorillonite (MMT), a major component of suspended particles in surface aquifers, plays key roles in the natural transportation and transformation of organic contaminants in the environment. However, literature has scarcely focused on whether and how suspended particles affect the phototransformation of AML. This study systematically investigated the phototransformation behavior of AML in MMT suspensions under simulated sunlight. The results obtained showed that MMT significantly enhanced the photolysis of AML. The photodegradation of AML in 0.05 g/L MMT suspension reached 92.2 % after 3 h irradiation under the simulated sunlight. The photodecomposition followed the pseudo-first-order kinetic with a rate constant of 0.803 h −1 in the presence of 0.05 g/L MMT, which is about 19 times larger than that in the absence of MMT (0.0421 h −1 ). Further mechanistic investigation suggested that MMT accelerated the photolysis of AML by the formation of surface complexes between cationic amino groups of AML and the negatively charged sites on MMT surface, which greatly facilitated light absorption and electron transfer for the production of cationic radical AML +· . Meanwhile, the hydroxyl radicals generated by irradiated MMT also played an important role in the photocatalytic degradation of AML. The probable photodegradation pathways of AML in MMT suspension further supported the proposed mechanisms. The toxicity evaluation of phototransformation products of AML with ECOSAR program indicated that photolysis could reduce its potential threats. These findings reveal an important and previously overlooked phototransformation mechanisms of AML in the presence of MMT clays, which is of importance in assessing the environmental fate of other similar organic contaminants.
研究领域:
环境科学
·
污染控制
·
药学
✓ 已验证
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2020
·
IF 10.257
Hua Ma,Kaiwen Chen,Bo Song,Zhixin Tang,Yundi Huang,Ting Zhang,Huanan Wang,Wenping Sun,Jingli Yuan
Development of fluorescent/luminescent probes for rapid, selective and sensitive detection of reactive oxygen species (ROS) is of great significance for understanding the roles of ROS in pathophysiological processes. In the present research, a visible-light-excitable Eu 3+ complex-based probe, Eu(L) 3 (DPBT), is designed and synthesized for the time-gated luminescence (TGL) determination of hypochlorous acid (HClO) in vitro and in vivo . The proposed probe exhibits a rapid, selective and sensitive TGL response to HClO, and excellent localization of mitochondria in living cells with low cytotoxicity. These features allow the probe to be used for the TGL sensing and imaging of HClO formation in mimic inflammatory cells at a subcellular level, as well as in endotoxin-induced liver injury and rheumatoid arthritis in live mice. In addition, by immobilizing the probe in the PEG hydrogel, the smart sensor films with rapid response to HClO were prepared, and successfully used for the real-time monitoring of HClO generation in mouse wounds, in order to distinguish the infected wounds from acute ones. Overall, this study provides a useful tool for the clinical monitoring and treatment of wound diseases.
研究领域:
生物化学
·
医学影像学
·
分子生物学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）