ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Mihebai Yilimulati,Jiyuan Jin,Xin Wang,Xiaomeng Wang,Dmitry Shevela,Bing Wu,Kai Wang,Lang Zhou,Yunlu Jia,Bingcai Pan,Govindjee Govindjee,Shujuan Zhang
Selective inhibition of photosynthesis is a fundamental strategy to solve the global challenge caused by harmful cyanobacterial blooms. However, there is a lack of specificity of the currently used cyanocides, because most of them act on cyanobacteria by generating nontargeted oxidative stress. Here, for the first time, we find that the simplest β-diketone, acetylacetone, is a promising specific cyanocide, which acts on Microcystis aeruginosa through targeted binding on bound iron species in the photosynthetic electron transport chain, rather than by oxidizing the components of the photosynthetic apparatus. The targeted binding approach outperforms the general oxidation mechanism in terms of specificity and eco-safety. Given the essential role of photosynthesis in both natural and artificial systems, this finding not only provides a unique solution for the selective control of cyanobacteria but also sheds new light on the ways to modulate photosynthesis.
研究领域:
环境科学
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微生物学
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植物生理学
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产品关联
DOI
PubMed
高影响因子
Journal of Functional Biomaterials
·
2022
·Vol. 13
·期 4
·220
·
IF 4.901
Wenhsuan Lu,Conglei Li,Jian Wu,Zhongshi Ma,Yadong Zhang,Tianyi Xin,Xiaomo Liu,Si Chen
Here, we developed a new synthetic method for the production of a new class of polymeric inorganic hybrid biomaterial that has potential for dental implant applications and, in general, other orthopedic applications owing to its excellent mechanical properties and biomechanical compatibility. The new hybrid biomaterial is a composite consisting of polyetherketoneketone (PEKK) and hydroxyapatite (HA). This hybrid material boasts several unique features, including its high HA loading (up to 50 wt%), which is close to that of natural human bone; the homogeneous HA distribution in the PEKK matrix without phase separation; and the fact that the addition of HA has no effect on the molecular weight of PEKK. Nanoindentation analysis was used to investigate the mechanical properties of the composite, and its nano/microstructure variations were investigated through a structural model developed here. Through nanoindentation technology, the newly developed PEKK/HA hybrid biomaterial has an indentation modulus of 12.1 ± 2.5 GPa and a hardness of 0.42 ± 0.09 GPa, which are comparable with those of human bone. Overall, the new PEKK/HA biomaterial exhibits excellent biomechanical compatibility and shows great promise for application to dental and orthopedic devices.Keywords:polyetherketoneketone;hydroxyapatite;composite;hybrid;dental;orthopedic;orthodontic;high performance;mechanical compatibility
研究领域:
生物医学工程
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材料科学
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牙科研究
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骨科研究
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DOI
PubMed
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Hengtao Tang,Zheng Zhou,Zhi Chen,Xin Ju,Liangzhi Li
Monosaccharides from biomass can be used as cost-effective raw materials to produce rare sugars which are valuable sweeteners. Enzymes play a pivotal role in such biomass biorefinery processes to develop novel synthetic routes, and improve the environmental friendliness of current routes. Here we propose a proof of concept biorefinery process to prepare useful rare sugars of D-xylulose and D-ribulose from D-xylose which was abundant in biomass. Ribose-5-phosphate isomerase B from Ochrobactrum sp. (OsRpiB) with a unique substrate scope was engineered to intensify the activity of transforming D-xylose to D-xylulose. A double mutant R94N/N137Q with 80% higher catalytic efficiency was identified, and kinetic and molecular dynamic studies were conducted to explore the mechanism underneath. The results revealed a correlation between enhancing stability and activity simultaneously. Then a one-pot enzyme cascade was constructed with OsRpiB and D-tagatose-3-epimerase from Pseudomonas cichorii and transformed D-xylulose further to D-ribulose. The conversions of D-xylose and D-xylulose in cascade reaction were 1.80-fold and 1.83-fold of that in separate reactions with the aid of process parameter adjustment. The presented work is the first reported enzyme cascade converting D-xylose to D-ribulose, and proves the promising role of monosaccharide isomerase platforms in the refinery of biomass.
研究领域:
生物化学
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酶工程
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生物质精炼
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产品关联
DOI
高影响因子
Science China-Chemistry
·
2021
·Vol. 64
·期 5
·770-777
·
IF 9.445
Qiao Xiaofeng,Lin Yuhan,Li Jiazhen,Ma Wanhong,Zhao Jincai
Both β- and γ- hydroxyketone structures are important units in biologically active molecules, synthetic drugs and fine chemicals. Although there are some routes available for their manufacture from pre-functionalized groups on one or two matrix molecule(s), the approaches to simply and simultaneously deposit two oxygen atoms from dioxygen into two specific C(sp 3 ) positions of pure saturated hydrocarbons have rarely succeeded because they are involved in the targeted activation of three inert C-H σ bonds all at once. Here, we show that a TiO 2 -CH 3 CN photocatalytic suspension system enables the insertion of dioxygen into one C(sp 3 )-C(sp 3 ) bond of strained cycloparaffin derivatives, by which difunctionalized hydroxyketone products are obtained in a one-pot reaction. With the cleavage event to release strain as the directional driving force, as-designed photocatalytic reaction systems show 21 examples of β-hydroxyketone products with 31%–76% isolated yields for three-membered ring derivatives and 5 examples of γ-hydroxyketone products with 30%–63% isolated yields for four-membered ring substrates. 18 O isotopic labeling experiments using 18 O 2 , Ti 18 O 2 and intentionally added H 2 18 O, respectively, indicated that both oxygen atoms of hydroxyketone products were exclusively from dioxygen, suggesting a previously unknown H + /TiO 2 -e − catalyzed arrangement pathway of the hydroperoxide intermediate to convert dioxygen into hydroxyketone units.
研究领域:
有机化学
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光催化化学
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药物化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2024
·Vol. 25
·期 2
·709
·
IF 4.9
Seungmee Lee,Hyeonmi Shin,Jihyun Bae,Taek Lee,Minji Kim,Heung Bae Jeon,Kang Hyun Lee,Hah Young Yoo,Chulhwan Park
Puerarin is a flavonoid known as a natural antioxidant found in the root ofPueraria robata. Its antioxidant, anticancer, and anti-inflammatory effects have attracted attention as a potential functional ingredient in various bioindustries. However, puerarin has limited bioavailability owing to its low lipid solubility and stability. Acylation is proposed as a synthesis method to overcome this limitation. In this study, lipase-catalyzed acylation of puerarin and various acyl donors was performed, and the enzymatic synthetic condition was optimized. Under the condition (20 g/L of Novozym 435, palmitic anhydride, 1:15, 40 °C, tetrahydrofuran (THF)), the synthesis of puerarin ester achieved a significantly high conversion (98.97%) within a short time (3 h). The molecule of the synthesized puerarin palmitate was identified by various analyses such as liquid chromatography–mass spectrometry (LC–MS), Fourier-transform infrared spectroscopy (FT-IR), and carbon-13 nuclear magnetic resonance (13C NMR). The lipid solubility and the radical scavenging activity were also evaluated. Puerarin palmitate showed a slight decrease in antioxidant activity, but lipid solubility was significantly improved, improving bioavailability. The high conversion achieved for puerarin esters in this study will provide the foundation for industrial applications.Keywords:antioxidant;flavonoid;puerarin;flavonoid ester;lipase;lipid solubility
研究领域:
生物化学
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制药工程
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Pengfei Yu,Zhongyu Guo,Jieqiong Wang,Yuchen Guo,Tingting Wang,Lilan Zhang
Methylisothiazolinone (MIT) and Benzisothiazolinone (BIT) are two widely used non-oxidizing biocides of isothiazolinones. Their production and usage volume have sharply increased since the pandemic of COVID-19, inevitably leading to more release into water environment. However, their photochemical behaviors in water environment are still unclear. Therefore, this study investigated photodegradation properties of MIT and BIT in natural water under simulated sunlight. The results demonstrated that direct photolysis was mainly responsible for their photodegradation which occurred through their excited singlet states rather than triplet states. The quantum yields of MIT and BIT photodegradation were 11 - 13.6 × 10 −4 and 2.43 - 5.79 × 10 −4 , respectively. pH had almost no effect on the photodegradation of MIT, while the photodegradation of BIT was significantly promoted under alkaline condition due to abundance of BIT in its deprotonated form (BIT- N − ). Cl − , NO 3 − and dissolved organic matter (DOM) in natural water inhibited the photodegradation of both MIT and BIT, with the light screening effect of DOM being the most significantly inhibitory factor. The addition of other isothiazolinones, which possibly coexisted with MIT and BIT in actual condition, slightly inhibited the photodegradation of MIT and BIT. The estimated half-life under natural sunlight at a 30°N latitude was estimated to be approximately 1.1 days. The photodegradation pathways of MIT and BIT are similar, primarily initiated from the ring-opening at the N-S bond, with Frontier electron densities (FED) calculations suggesting the likelihood of oxidation and ·OH addition reactions at the O, N, and S sites. While the photodegradation products exhibited significantly reduced acute toxicity compared to their parent compounds, they nonetheless posed substantial chronic toxicity. These insights are vital for assessing the ecological impacts of MIT and BIT in aquatic environments.
研究领域:
环境科学
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生态学
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产品关联
DOI
PubMed
高影响因子
ANALYST
·
2023
·Vol. 148
·期 15
·3518-3523
·
IF 4.2
Hao Gu,Guoxin Dai,Zhongqiu Teng,Lina Geng,Wei Xu
Liquid chromatography-tandem mass spectrometry (LC-MS/MS) is a universal method for the quantitative analysis of small molecular drugs in therapeutic drug monitoring (TDM). Alternatively, liquid chromatography-miniature mass spectrometry (LC-Mini MS) is a simple operating technique for quantitative analysis. However, the wide chromatographic peaks and long retention times of TDM samples using the LC-Mini MS system deteriorated the accuracy and efficiency of quantitative analysis. Here, an optimized electrospray ionization (ESI) interface setup with a splitter valve and a capillary needle (I.D. 30 μm and O.D. 150 μm) of the LC-Mini MS system was acquired. The chromatographic peaks were narrower and smoother and the retention time was shorter for TDM compounds. Furthermore, a quantitative analysis method for risperidone and the active metabolite 9-hydroxyrisperidone in plasma was developed based on this optimal LC-Mini MS setup. The results showed that the calibration curves of risperidone and 9-hydroxyrisperidone had good linear ranges of 2–100 ng mL−1 (R2 = 0.9931) and 2–100 ng mL−1 (R2 = 0.9915), respectively. Finally, the matrix effects, recoveries and stability of risperidone and 9-hydroxyrisperidone samples were analyzed. The results satisfied the requirements of quantitative validation in routine TDM procedures.
研究领域:
分析化学
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药学
·
医学
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产品关联
DOI
PubMed
高影响因子
POLYMER COMPOSITES
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2023
·
IF 5.2
Tianxiang Fan,Ziyan Zhou,Huiying Zhang,Xiaole Zhao,Ye Chen,Huaping Wang
Continuous fiber reinforced thermoplastic composites (CFRTPCs) prepared by fused deposition modeling (FDM) have gained great attention for the benefit of preparing products without molds. However, unexpected debonding and defects are derived from insufficient impregnation between fiber and matrix in 3D-printed samples, resulting in weak interfacial performance. In this work, a polyetherimide (PEI) sizing agent was used to improve the fiber-matrix interfaces, and the interlaminar shear strength (ILSS) of the continuous carbon fiber reinforced poly(ether-ketone-ketone) composites was increased to 27.1 MPa, 12.4% higher than that of unmodified composite. Meanwhile, the performance of CFRTPCs is affected by process parameters in FDM. Build orientation of FDM was discussed and PEI weakened the anisotropy of samples' mechanical properties because the performance variation caused by build orientation decreased from 86.8% to 65.2%, which may be beneficial for the forming freedom of in situ impregnated FDM. The addition of PEI makes sense to apply in situ impregnated FDM in high-tech fields. Highlights CCF/PEKK composites were prepared by in situ impregnated FDM. ILSS of flat-oriented CCF/PEKK was 86.8% higher than that of on-edge. 5 wt% PEI sizing agent promoted adhesion of CCF and PEKK to obtain the best mechanical properties. PEI weakened the anisotropy of samples' mechanical properties, which was conducive to forming freedom.
研究领域:
材料科学
·
增材制造
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Haixin Sun,Jianlei Qi,Jianfei Sun,Lin Li,Kunpeng Yu,Jintao Wu,Jianzhong Yin
As a common precursor for supercritical CO 2 (scCO 2 ) deposition techniques, solubility data of organometallic complexes in scCO 2 is crucial for the preparation of nanocomposites. Recently, metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials. In this study, the solubilities of iron(III) acetylacetonate (Fe(acac) 3 ) and nickel(II) acetylacetonate (Ni(acac) 2 ) were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data. Solubility was measured using a static weight loss method. The semi-empirical models proposed by Chrastil and Sung et al . were used to correlate the solubility data of Fe(acac) 3 and Ni(acac) 2 . The equations obtained can be used to predict the solubility of the same system in the experimental range.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Guifang Qin,Jie Lei,Sihui Li,Yongmei Jiang,Lei Qiao,Mengdie Ren,Qiong Gao,Changwei Song,Shaobin Fu,Jinquan Zhou,Shiji Xiao,Maosheng Zhang,Gang Wang
In this study, ultrasonic-assisted deep eutectic solvents (DESs-UAE) was applied for efficient and environmentally friendly extraction of amentoflavone (AME) and robustaflavone (ROB) from Selaginella uncinata. Firstly, proline-lactic acid (Pro-Lac) was screened as the optimal DES from the 30 DESs. The maximum extraction rates of AME and ROB were obtained adopting the response surface methodology (RSM). Under the optimal conditions of molar ratio of 1:4, water content of 33 %, and extraction time of 30 min, the extraction yields of AME and ROB were 709.72 ± 11.31 μg/g and 145.13 ± 9.77 μg/g, respectively. Compared with the traditional extraction methods, the DESs-UAE extraction could enhance the extraction rates and save extraction time. At the same time, 23 flavonoids were identified by UPLC-Q-TOF-MS, of which 6 components appeared for the first time in S. uncinata. In addition, three antioxidant experiments (DPPH method, ABTS method, and hydroxyl radical scavenging method) were carried out, and the results showed that the S. uncinata extracts had potential antioxidant activity. Furthermore, S. uncinata extracts exhibited obvious growth inhibitory effect on A549, HCT-116, HT-29, sw1990, HepG2 and HeLa cancer cells. In conclusion, deep eutectic solvent, as an promising solvent, is much more effective and simple extraction of bioactive constituents from S. uncinata with high safety and low toxicity.
研究领域:
药物化学
·
分析化学
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植物科学
·
生物技术
·
肿瘤学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shuling Zhang,Yuqing Zhang,Weixi Kong,Wanting Guo,Quan Yuan,Yanjun Jiang,Yunting Liu
Enzymatic reduction of (hetero)aryl ketones is an important reaction for the synthesis of industrially relevant chiral alcohols, but its preparative application remains restricted due to enzyme unavailability and substrate inhibition. Herein, we reported the identification of a ketoreductase and its mutant from Metabacillus lacus ( Ml KREDs) with high activity and wide substrate scope (50 examples) for the reduction of (hetero)aryl ketones by gene mining and protein engineering. During process development, we constructed a deep eutectic solvent (DES)-buffer system to relieve substrate inhibition, achieving the efficient conversion of high-concentration (up to 1.2 M) (hetero)aryl ketones to the corresponding chiral alcohols, some of which are key intermediates for pharmaceuticals. In addition, molecular dynamics simulations provided deeper insights into the substrate inhibition mechanism as well as the DES-induced enzyme activation and stabilization mechanisms. This work provides a green and reliable strategy for the preparative synthesis of pharmaceutical-related chiral (hetero)aryl alcohols.
研究领域:
生物化学
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制药工程
·
合成生物学
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产品关联
DOI
高影响因子
ChemSusChem
·
2017
·Vol. 10
·期 4
·711-719
·
IF 7.226
Shanshan Li,Fang Chen,Ning Li,Wentao Wang,Xueru Sheng,Aiqin Wang,Yu Cong,Xiaodong Wang,Tao Zhang
Graphical Green triketones : Renewable C 9 –C 12 triketones with repeating [COCH 2 CH 2 ] units are synthesized in high carbon yields (ca. 90 %) over a cost-effective and reusable Au/TiO 2 catalyst. The triketones as obtained can be used as feedstocks in the production of conducting or semi-conducting polymers. Furthermore, they can also be converted to diketones or jet-fuel range branched cycloalkanes with high densities and low freezing points. A series of renewable C 9 –C 12 triketones with repeating [COCH 2 CH 2 ] units were synthesized in high carbon yields (ca. 90 %) by the aqueous-phase hydrogenation of the aldol-condensation products of 5-hydroxylmethylfurfural (HMF) and ketones over an Au/TiO 2 catalyst. Compared with the reported routes, this new route has many advantages such as being environmentally friendly, having fewer steps, using a cheaper and reusable catalyst, etc. The triketones as obtained can be used as feedstocks in the production of conducting or semi-conducting polymers. Through a solvent-free intramolecular aldol condensation over solid-base catalysts, the triketones were selectively converted to diketones, which can be used as intermediates in the synthesis of useful chemicals or polymers. As another application, the tri- and diketones can also be utilized as precursors for the synthesis of jet-fuel range branched cycloalkanes with low freezing points (224–248 K) and high densities (ca. 0.81 g mL −1 ).
研究领域:
化学工程
·
可再生能源
·
催化化学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）