INTERNATIONAL IMMUNOPHARMACOLOGY
·
2026
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IF 5.6
Shangmin Yu,Jiaqi Liu,Shan Liu
Background Atherosclerosis (AS) is a chronic inflammatory vascular disease. Macrophage reprogramming plays a crucial role in the progression of AS. Ophiopogonin D (OP-D), a bioactive constituent of Ophiopogon japonicus , has exhibited potent anti-atherosclerotic property. However, whether OP-D exerts its atheroprotective effect via reprogramming macrophage remains unclear. This study aimed to investigate the effect of OP-D on AS and elucidate its underlying mechanism. Methods The atheroprotective effect of OP-D on atherosclerotic mice was evaluated by histological and molecular assays. The crucial role of macrophage in OP-D's atheroprotective effect was detected by flow cytometry and verified through macrophage depletion/infusion. The direct effect of OP-D on macrophages were assessed in vitro by RT-qPCR, flow cytometry, and immunofluorescence. RNA sequencing and amino acid-targeted metabolomics analysis were employed to identify the associated amino acid metabolic pathways. In addition, PPM1K deficient was established to validate the role of branched-chain amino acids (BCAAs) in macrophage reprogramming and OP-D's therapeutic effect. Results Our results demonstrated that OP-D attenuated the progression of AS and directly prevented the M1-like polarization of macrophages. Meanwhile, the therapeutic benefits of OP-D were abolished after macrophages depletion, suggesting macrophage was a crucial mediator of OP-D's therapeutic effect. Further mechanistic studies revealed that dysregulated BCAAs metabolism-mediated macrophage polarization underlay the anti-atherosclerotic effect of OP-D. Conclusion This study elucidated that OP-D reprogrammed the polarization of macrophages through modulating BCAAs catabolism to delay atherogenesis. These findings will deepen the understanding of OP-D's atheroprotective mechanisms and provide a potential therapeutic target for AS.
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ACS Catalysis
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2026
·
IF 13.6
Xing Yu,Peng Deng,Sheng Gu,Bu-Bing Zeng,Hui-Lei Yu,Jian-He Xu,Zhi-Jun Zhang
Direct asymmetric α-C−H bond amination of carboxylic acids is an attractive route to optically active α-amino acids from inexpensive, renewable starting materials. However, traditional chemical methods suffer from expensive catalysts and environmental concerns, while recently developed multienzyme cascades are limited by complex auxiliary enzyme requirements and narrow substrate scope. Here, we report an engineered P450 peroxygenase (P450CLA-M5) with enhanced overoxidation promiscuity that enables the direct conversion of fatty acids to α-keto acids. Coupling this enzyme with d-amino acid dehydrogenase and formate dehydrogenase establishes a biocatalytic cascade for the C−H amination of fatty acids to d-amino acids. Saturated, unsaturated, and aromatic fatty acids were converted to the corresponding d-amino acids with yields up to 94% and >99% ee. Specifically, the yield of d-2-aminodecanoic acid represents a 15-fold improvement over previous biocatalytic approaches. This work demonstrates how engineering increased enzyme promiscuity can enhance cascade efficiency for the synthesis of valuable chiral d-amino acids from renewable feedstocks.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2026
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IF 3.9
Zhu Jianxiang,Li Jiahui,Shen Runqiu,Song Yuwei,Xie Yuanyuan,Duan Hongliang,Su An
The development of efficient and sustainable amide-bond-forming
processes, together with their quantitative kinetic characterization,
is of major significance to the fine chemical and pharmaceutical industries.
In this study, the aminolysis of d -(−)-pantolactone
(DPL) with pyrrolidine (Pyr), catalyzed by 1,5,7-triazabicyclo[4.4.0]dec-5-ene
(TBD), was investigated in a continuous-flow microreactor equipped
with inline Fourier transform infrared (FTIR) spectroscopy. For the
first time, a flow-rate-ramp transient kinetic method was applied
to an organobase-catalyzed aminolysis system. A multiresponse FTIR–PLS
quantitative model was developed using Latin hypercube sampling (LHS)
for calibration-set design, thereby effectively reducing the collinearity
inherent in conventional calibration samples distributed along the
reaction stoichiometric line. An analytical mapping between experimental
time and the actual residence time of fluid elements under dynamic
flow conditions was established, making it possible to extract continuous
kinetic data over a residence-time range of 2–40 min from just
one 83.1 min flow-rate-ramp experiment. The reaction orders with respect
to DPL, Pyr, and TBD were determined to be 1, 1, and 0.85, respectively,
via the isolation and initial-rate methods. An explicit analytical
expression for DPL conversion was derived based on a plug-flow reactor
model. Arrhenius analysis yielded an activation energy of 26.26 kJ·mol –1 and a pre-exponential factor of 2.96 × 10 5 L 1.85 ·mol –1.85 ·min –1 . The resulting model demonstrated good predictive
accuracy when applied to temperatures and initial concentrations outside
the fitting range. This work provides a reliable kinetic basis for
the design and scale-up of continuous DPL aminolysis processes and
offers a rapid and resource-efficient strategy for kinetically characterizing
related metal-free organocatalytic systems.
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Science Advances
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2022
·Vol. 8
·期 50
·
IF 14.957
Qingxun Guo,Liang Wang,Longbo Yang,Jiashun Duan,Hainan Du,Guoqi Ji,Nian Liu,Xue Zhao,Chao Chen,Ling Xu,Liang Gao,Jiajun Luo,Jiang Tang
Next-generation wide color gamut displays require the development of efficient and toxic-free light-emitting materials meeting the crucial Rec. 2020 standard. With the rapid progress of green and red perovskite light-emitting diodes (PeLEDs), blue PeLEDs remain a central challenge because of the undesirable color coordinates and poor spectra stability. Here, we report Cs 3 CeBr x I 6− x ( x = 0 to 6) with the cryolite-like structure and stable and tunable color coordinates from (0.17, 0.02) to (0.15, 0.04). Further encouraged by the short exciton lifetime (26.1 ns) and high photoluminescence quantum yield (~76%), we construct Cs 3 CeBr x I 6− x -based rare-earth LEDs via thermal evaporation. A seed layer strategy is conducted to improve the device’s performance. The optimal Cs 3 CeI 6 device achieves a maximum external quantum efficiency of 3.5% and a luminance of 470 cd m −2 with stable deep-blue color coordinates of (0.15, 0.04). Our work opens another avenue to achieving efficient and spectrally stable deep-blue LEDs.
研究领域:
材料科学
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光电子学
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固态照明
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无机化学
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显示技术
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
·
IF 4.831
Yuanjie Teng,Zhenni Wang,Shaohua Zuo,Xin Li,Yinxin Chen
Universal and fast antibiotic residues detection technology is imperative for the control of food safety in aquatic products. However, accurate surface-enhanced Raman scattering (SERS) quantitative detection of complicated samples is still a challenge. A recognition method powered by deep learning and took advantage of the unique fingerprint information merits of SERS was proposed. Herein, the spectra were collected by Ag nanofilm SERS substrate prepared by self-assembly of Ag nanoparticles on water/oil interface. A SERS-based database of commonly used antibiotics in aquatic products was set up, which is suitable for employed as input data for learning and training. The results show that the five types of antibiotics are successfully distinguished through principal component analysis (PCA) and each antibiotic in every type was successfully distinguished. Furthermore, one-dimensional convolutional neural networks (1-D CNN) was used to distinguish the antibiotics, and the results show that all the test samples were correctly predicted by 1-D CNN model. The results of this research suggest the great potential of the combination of SERS spectra with deep learning as a method for rapid and highly accurate identification of antibiotic residues in aquatic products.
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ACS Catalysis
·
2023
·
IF 12.9
Jialin Wang,Yu-Cheng Huang,Yiqing Wang,Hao Deng,Yuchuan Shi,Daixing Wei,Mingtao Li,Chung-Li Dong,Hui Jin,Samuel S. Mao,Shaohua Shen
A variety of atomically dispersed transition-metal-anchored nitrogen-doped carbon (M–N–C) electrocatalysts have shown encouraging electrochemical CO2 reduction reaction (CO2RR) performance, with the underlying fundamentals of central transition-metal atom determined CO2RR activity and selectivity yet remaining unclear. Herein, a universal impregnation-acid leaching method was exploited to synthesize various M–N–C (M: Fe, Co, Ni, and Cu) single-atom catalysts (SACs), which revealed d-orbital electronic configuration-dependent activity and selectivity toward CO2RR for CO production. Notably, Ni–N–C exhibits a very high CO Faradaic efficiency (FE) of 97% at −0.65 V versus RHE and above 90% CO selectivity in the potential range from −0.5 to −0.9 V versus RHE, much superior to other M–N–C (M: Fe, Co, and Cu). With the d-orbital electronic configurations of central metals in M–N–C SACs well elucidated by crystal-field theory, Dewar–Chatt–Duncanson (DCD) and differential charge density analysis reveal that the vacant outermost d-orbital of Ni2+ in a Ni–N–C SAC would benefit the electron transfer from the C atoms in CO2 molecules to the Ni atoms and thus effectively activate the surface-adsorbed CO2 molecules. However, the outermost d-orbital of Fe3+, Co2+, and Cu2+ occupied by unpaired electrons would weaken the electron-transfer process and then impede CO2 activation. In situ spectral investigations demonstrate that the generation of *COOH intermediates is favored over Ni–N–C SAC at relatively low applied potentials, supporting its high CO2-to-CO conversion performance. Gibbs free energy difference analysis in the rate-limiting step in CO2RR and hydrogen evolution reaction (HER) reveals that CO2RR is thermodynamically favored for Ni–N–C SAC, explaining its superior CO2RR performance as compared to other SACs. This work presents a facile and general strategy to effectively modulate the CO2-to-CO selectivity from the perspective of electronic configuration of central metals in M–N–C SACs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Sundaram Chandrasekaran,Tingting Ma,Zhichang Hu,Qianying Liu,Chao Zhan,Yan Li,Chris Bowen,Huidan Lu,Yongping Liu
Chevrel-phase metal sulfides are known to be promising materials for energy conversion and storage applications. However, a detailed understanding of the intrinsic kinetic mechanisms of electrocatalytic bifunctional hydrogen and oxygen evolution reactions (HER/OER) on NiMo 3 S 4 -based Chevrel-phases is lacking. Herein, novel ultrathin self-assembled nanosheets of NiMo 3 S 4 are coupled with transition metal atoms (M/N-NiMo 3 S 4 ; where M = Co, Fe, and Cu) were formed by a facile hydrothermal approach. Notably, the Co/N-NiMo 3 S 4 electrocatalyst exhibits excellent performance in terms of ultralow overpotentials of 78, 208, 282, and 307 mV at 10, 100, 500, and 1000 mA cm −2 for the HER; and 186, 204, and 225 mV at 50, 100, and 300 mA cm −2 for the OER, respectively. Experimental and first principle calculations demonstrate that Co atoms coupling with edge Ni atoms results in d‐electron delocalization on Co/N-NiMo 3 S 4 , signifying the efficient charge transfer to improve overall water electrolysis. In addition, an upshift in the d‐band center of Co/N-NiMo 3 S 4 can optimize the free energies of a variety of reaction intermediates for water adsorption and dissociation; thereby facilitating the robust alkaline overall water electrolysis at 1.47 V. This work therefore greatly deepens the understanding of the bifunctional hydrogen and oxygen evolution reaction of Chevrel-phase electrocatalysts.
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Nano Research
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2023
·Vol. 16
·期 8
·10748-10755
·
IF 9.9
Li Junhua,Jiang Yi,Zhang Xu,Huo Yidan,Du Fanglin,Tuo Yongxiao,Guo Zhiyan,Chen Dawei,Chen Shenghua
The electrooxidation of the alcohol and aldehyde molecules instead of water coupled with H 2 production has been proven to be effective for producing high-value fine chemicals under alkaline conditions. It is also noteworthy that under acidic conditions, the stability of non-noble metal water oxidation catalysts remains a great challenge due to the lattice oxygen mechanism. Hence, we coupled the biomass-derived glucose oxidation for high-value D-glucaric acid (GRA) with ultra-durable hydrogen in acid solution over a Yb-MnO 2 catalyst. The Mn 3+ regulated by Yb atoms doped in MnO 2 can effectively optimize the adsorption and desorption processes of the alcohol and aldehyde group and improve the intrinsic activity but cannot for H 2 O. The catalyst exhibited extremely high activity and stability after 50 h for glucose oxidation, inhibiting the lattice oxygen process and MnO 4− formation, while the activity was quickly lost within 0.5 h for water oxidation. Density functional theory (DFT) calculations further demonstrated that glucose oxidation reaction proceeds preferentially due to the oxidation of aldehyde group with lower adsorption-free energy (−0.4 eV) than water (Δ G > 0 eV), avoiding the lattice oxygen mechanism. This work suggests that biomass-derived glucose oxidation not only provides a cost-effective approach for high-value chemicals, but also shows an extremely potential as an alternative to acidic oxygen evolution reaction (OER) for ultradurable H 2 production.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2022
·
IF 3.571
Baole Zhang,Wanglong Xu,Chuanlong Yin,Yangming Tang
Under the guideline issued by Food and Drug Administration (FDA), ANDAs for Certain Highly Purified Synthetic Peptide Drug Products That Refer to Listed Drugs of rDNA Origin Guidance for Industry , a synthetic Semaglutide that is intended to be a “generic” of the approved rDNA origin Semaglutide is under exploring. Thus, each peptide-related impurity that is 0.10% of the drug substance or greater need to be identified for Semaglutide covered by this guidance. Among others, characterization of the low-level D -amino acid (D form) isomeric impurities are always the most challenging ones. Reverse-phase high-performance liquid chromatography (RP-UPLC) was used to separate the impurities, followed by high resolution mass spectrometry (HRMS) to determine the molecular weight of the impurities that existed in both formulations. Following the targeted D form isomers off-line collection, the samples went through lyophilization, deuterated hydrochloric acid ( D -HCl) hydrolyzation with low level D/L form shifting suppression substrates, chiral derivatization and RP-UPLC tandem mass spectrometry analysis of different amino acids by comparing with standards. Herein, we reported an accurate, straightforward characterization method with low limit of detection for the low-level D -Ser 8 , D -His 1 and D -Asp 9 Semaglutide impurities in Semaglutide formulations. The developed UPLC tandem HRMS method entails a valuable step forward in the detection of trace levels of the D -isomers of Semaglutide and other peptide products.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Shaochun Su,Li Hao,Huayao Chen,Xinhua Zhou,Hongjun Zhou
Sustainable food consumption is intertwined with sustainable agriculture development, which focuses on the production and protection of agricultural crops in a safe and effective fashion. Herein, amphiphilic functionalized chitosan oligosaccharide nanoparticles (CSD) were formed by a Schiff base reaction grafted with salicylaldehyde and D-(+)-galactose ( D -Gal). Avermectin (AVM) was used as a model pesticide and self-assembled onto CSD to obtain AVM@CSD nanoparticles with an encapsulation efficiency of 74.94%. AVM@CSD nanocarrier exhibited excellent anti-UV property to retain more AVM, due to their Schiff base structure and salicylaldehyde for UV shielding. Compared with bare AVM and commercial AVM emulsifiable concentrates, AVM@CSD preserved high insecticidal activity after UV irradiation . Additionally, CSD carrier promoted cucumber seed germination and seedling growth. These data suggested the potential utilization of the amphiphilic chitosan oligosaccharide as carriers for pesticides to improve their delivery and release properties and opens a novel avenue towards the application of water-dispersible and biological CSD in the field of pest management and plant growth.
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TALANTA
·
2022
·
IF 6.556
Yi Wu,Keren Lu,Fubin Pei,Yanghao Yan,Shasha Feng,Qingli Hao,Mingzhu Xia,Wu Lei
The wide clinical application of d -penicillamine (D-PA) makes it inevitably accumulates in the environment, seriously threatening human health and the ecological environment. To better supervisory control D-PA, a highly sensitive and reliable photoelectrochemical (PEC) sensor based on gold nanoparticles (Au NPs) loaded on graphitic carbon nitride sheet and hexagonal NH 2 -UiO-66 composite (g-C 3 N 4 /Au/NH 2 -UiO-66) was synthesized. Tactfully using the strong bonding between D-PA and Au NPs and the effective carrier separation of Z-scheme heterojunction, the designed g-C 3 N 4 /Au/NH 2 -UiO-66 PEC sensor without an extra recognition unit exhibited a selective and sensitive photocurrent to D-PA. With the aid of UV diffuse reflectance spectra (UV-DRs), electron paramagnetic resonance (EPR) characterization, and free radical capture experiments, the electron transfer path of the PEC sensing system was deduced. The proposed g-C 3 N 4 /Au/NH 2 -UiO-66 PEC-based sensor achieved a low detection limit of 0.0046 μM (S/N = 3) with a wide linear response ranging from 10 nM to 400 μM. In addition, its good stability and selectivity also laid a good foundation for practical applications.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2022
·
IF 4.831
Xianghan Zhang,Zhiqing Gao,Yuqiong Xia,Qunyan Dong,Yutian Cao,Qian Jia,Fang Sun,Zheng Li,Chu Tang,Jie Yu
Nitroreductase (NTR) detection in tumor is critical because NTR level is correlated with hypoxia degree and cancer prognosis. With the feature of high sensitivity and selectivity, fluorescence organic probes for NTR detection exhibited a promising future for tumor hypoxia detection. However, the discovery and design of such probes have been impeded due to the lack of the understanding of spatial match and mismatch of these probes with NTR. Here, we have developed two new nitrophenyl-functionalized trimethincyanine (Cy3) probes with para- or meta- positions of nitro-group in phenyl ring. Para-nitrophenyl substituted Cy3 (pNP-Cy3) exhibited a remarkable response to NTR (20-fold fluorescence enhancement) with good selectivity and sensitivity. Experimental and theoretical analysis verified that the substituent position of nitro group on phenyl ring of dyes altered the spatial arrangement of nitro-substituent group, thereby modulated the spatial match and mismatch between Cy3 dyes and binding domain of NTR, and consequently led to a different fluorescent turn-on response. In tumor-bearing mice model, hypoxia status of A549 xenografted tumor of mice was successfully delineated by using pNP-Cy3. These results may provide a clue for designing new cyanine-derived NTR probe to monitor NTR-overexpressed hypoxia cancer cells.
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