SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xinyang Xu,Jiawen Liu,Yixin Sun,Zhonghua Li
Among the various advanced photocatalytic materials, the organic conjugated microporous polymer (CMP) photocatalysts have garnered significant interest due to their exceptional efficiency in photogenerated electron transfer and their structural versatility. In this study, we developed two novel donor-acceptor 1 -acceptor 2 CMP systems through varying the electron donor unit. Pyrene (P) and triphenylamine (T) were acted as donor units (D), respectively, meanwhile dibenzothiophene-S,S-dioxide (BTDO, A 1 ) and 3,4-ethylenedioxythiophene (EDOT, A 2 ) as their acceptors to construct two D−A 1 −A 2 type CMP photocatalysts, P-BTDO-EDOT and T-BTDO-EDOT. Their photocatalytic performances were compared and studied through photocatalytic hydrogen production. The findings show that P-BTDO-EDOT possesses higher photocatalytic hydrogen production activity (87.21 mmol g −1 h −1 ) than T-BTDO-EDOT (66.25 mmol g −1 h −1 ) under visible light, attributing to its stable conjugated architecture, larger specific surface area, exceptional optoelectronic capability, wider light absorption, donor unit pyrene with strong electron-donating and efficient charge separation ability. This work not only highlights the potential for designing innovative CMP molecular structures with D−A 1 −A 2 system, but also opens up a new pathway for developing high-efficiency photocatalysts.
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Analytical Methods
·
2017
·Vol. 10
·期 1
·84-90
·
IF 1.9
Xia Lin,Shu Zhu,Qiao Xia,Jiao Ma,Yingzi Fu
Herein, an ultrasensitive and stereo-selective electrochemiluminescent (ECL) biosensor based on ECL signal amplification of luminol by the synergetic catalysis of a hemin-functionalized composite and gold–platinum nanowires (Au-PtNWs) has been designed for the detection of D-alanine (D-Ala). In the sensor design, D-amino acid oxidase (DAAO) was used to generate the ECL co-reactant (H2O2) for luminol in situ. The reduced graphene oxide-hemin-cysteine (rGO-H-Cys) composite and Au-PtNWs acted not only as amplification labels to amplify signals via synergetic catalysis, but also as an ideal nanocarrier to accelerate electron transfer. A great difference in ECL intensities toward D-Ala and L-Ala was obtained, and an obviously higher intensity was seen for D-Ala. Under optimal conditions, the ECL intensity had a linear relationship with the logarithm of the D-Ala concentration in the range from 1.0 × 10−9 to 5.0 × 10−3 M with a detection limit of 3.3 × 10−10 M (S/N = 3). This study provides a new method for the determination of D-Ala in food with high sensitivity, excellent selectivity, and good stability and reproducibility.
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 24
·12144-12148
·
IF 8.867
Qianqian Yang,Jie Zhou,Genqiang Zhang,Cong Guo,Meng Li,Yongchun Zhu,Yitai Qian
Sb nanoparticles encapsulated in 1-D N-doped porous carbon (denoted as Sb/NPC) have been fabricated by an in situ nanoconfined replacement reaction between SbCl3 and the intermediate Ni/NPC, in which Ni/NPC was obtained by annealing the hydrothermally synthesized nickel–nitrilotriacetic acid (Ni–NTA) precursor in an argon atmosphere. The Sb nanoparticles with a size of 10–20 nm were uniformly encapsulated in the 1-D N-doped porous carbon scaffolds. When the Sb/NPC composite was applied as an anode material in the batteries, it exhibited a high reversible capacity of 556 mA h g−1 at 200 mA g−1 after 100 cycles for Li-ion batteries (LIBs) and a reversible capacity of 400.9 mA h g−1 at 100 mA g−1 after 100 cycles for Na-ion batteries (NIBs). Such enhanced electrochemical performance of the designed Sb/NPC can be attributed to the synergistic effect between uniformly dispersed Sb nanoparticles and the 1-D N-doped porous carbon matrices.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xinyang Xu,Yixin Sun,Jiawen Liu,Zhonghua Li
Conjugated microporous polymers (CMPs) featuring donor–acceptor (D–A) structures have garnered significant attention for their potential in hydrogen production, primarily due to their excellent charge transfer efficiency and large specific surface area. However, the uncontrollable composition in D–A structure severely limits the improvement of photocatalytic activity. In this study, employing pyrene as the donor, dibenzothiophene-S-S-dioxide (BTDO, A 1 ) and 1-methyl-1,2,4-triazole (TAME, A 2 ) as acceptors, the innovative tri-component CMP photocatalysts featuring a donor–acceptor 1 –acceptor 2 (D–A 1 –A 2 ) configuration were developed and created. By regulating the ratio of D and A, as well as BTDO and TAME in the polymer backbone, the optimized copolymer Py-BTDO-TAME-2 exhibits superior hydrogen production activity (27.53 mmol g −1 h −1 ) in the absence of Pt co-catalyst under visible light, owing to the broad light absorption, high specific surface area and enhanced charge separation capability. The findings of this study indicate that utilizing a D–A 1 –A 2 structural design method can greatly improve the photocatalytic performance of CMP photocatalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Xiaoying Gao,Jiarui Zhu,Jiahui Zhao,Lei Zhao,Ying Sun,Jiazhen Lin,Mengli Hu,Yunjia Liu,Shenghong Yang,Jian Liu
A cascade colorimetric detection of salivary D-amino acids (DAAs) holds promise for the preliminary screening diagnosis of gastric cancer. Pursuing metal-organic complexes with high peroxidase-mimic (POD-mimic) activity is crucial to enhance diagnosis efficiency. In this work, we developed a straightforward strategy in a “one-pot” process to modulate the POD-mimic activity of CuX-trithiocyanuric acid (CuX-TTCA) complexes. By adjusting the molar ratios of CuX (Cl, Br, and I) and TTCA during synthesis to modify the coordination configuration of Cu(I) in CuX-TTCA, we easily tuned their POD-mimic activities. Among them, CuCl-TTCA-2 with a feeding molar ratio of 2:1 for CuCl:TTCA exhibited remarkable POD-mimic activity attributed to its exposed catalytic active sites and efficient mass transfer ability during catalysis. Long-lived 1 O 2 was identified as the primary reactive oxygen intermediate. A highly sensitive and selective cascade colorimetric detection platform was developed for two typical DAAs associated with gastric cancer, namely D-proline and D-alanine, achieving limit of detection values of 1.1 and 0.8 μM, respectively. As a proof-of-concept application, our cascade detection platform demonstrated excellent specificity in distinguishing saliva samples between gastric cancer patients and healthy individuals. The outstanding selectivity and reliable outcomes from DAAs assay make our detection platform highly promising for preliminary screening diagnosis of gastric cancer and patient self-detection applications. Our straightforward strategy for tuning POD-mimic activity provides an in-depth understanding on structure-activity relationship in nanozymes, offering valuable opportunities to advance enzyme-mimic optimization for other potential applications.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Yun Liu,Zhina Qiao,Hengwei Zhang,Xian Zhang,Yanan Li,Zhiming Rao
D-tagatose, a functional rare sugar, has physiological effects such as lowering blood sugar and anti-caries. However, research on the industrial production of D-tagatose has primarily focused on Escherichia coli , limiting application in the food field. In this study, a cell factory for efficient synthesis of D-tagatose was constructed using the GRAS strain Corynebacterium glutamicum . Firstly, the key enzyme L-arabinose isomerase from Lactobacillus fermentum was screened. Secondly, by rational design, the optimal mutant D390V/H339P significantly enhanced enzyme activity by 40.65 % and improved thermostability. Subsequently, a dual-enzyme coupled whole-cell system was established by regulating the ratio of β-galactosidase and L-arabinose isomerase by RBS optimization. After optimizing the catalytic system, 101.42 g/L D-tagatose was produced from 400 g/L lactose, and the conversion rate reached 25.12 % in 5 L fermenter, which is the highest yield using lactose as substrate and GRAS strain as chassis cells. This research laid a foundation for the industrial application of food-grade D-tagatose.
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Carbon Neutrality
·
2025
·Vol. 4
·期 1
·1-9
·
IF 12.5
Yang Delong,Dai Jinhang,Du Ziting,Cao Qingya,Chen Gang,Qi Ting,Wang Weilu,Li Fukun
Since 3-acetylamino-5-acetylfuran (3A5AF) has been regarded as a promising nitrogen-containing synthon, the conversion of renewable chitin and its monomer N-acetyl-D-glucosamine (NAG) to 3A5AF is of significance. In this paper, we compared the catalytic activity of several Cl-containing compounds and found that LiCl exhibited superior performance. The effects of solvent, catalyst dosage, reaction temperature, and reaction time on the synthesis of 3A5AF were investigated. Under the optimized conditions, about 60% yields of 3A5AF were obtained in N-methyl-2-pyrrolidone (NMP) or dimethylacetamide (DMA) medium. The spent LiCl and DMA could be recycled and reused, without obvious decrease of 3A5AF yield. Moreover, the formed 3A5AF could be purified by a facile procedure. Experiment results and density functional theory (DFT) calculations revealed that homogeneous Cl − was vital for 3A5AF formation. This study provides an example for the effective conversion of chitin biomass to value-added compounds.
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ACS Catalysis
·
2025
·
IF 13.1
Fang Huang,Aihao Xu,Xiangyu Chen,Huanhuan Sun,Siyu He,Dong Wei,Boran Wang,Anxiang Guan,Xucai Yin,Jing Xu,Huibing He
The direct electrocatalytic conversion of carbon dioxide to methane using water as a medium is a reliable way to store intermittent renewable energy and solve environmental problems. However, in such multielectron/proton transfer reactions, the role of water is often overlooked. Specifically, the sluggish kinetics of water dissociation limit the effective proton supply during methane formation. Here, we propose a copper-doped CeO2 catalyst with frustrated Lewis pairs (FLPs), which can effectively reduce carbon dioxide to methane. Combined experimental analysis and theoretical calculations reveal that the synergistic interaction between Cu and FLPs forms an f-p-d gradient orbital coupling system, which significantly promotes water dissociation to generate active protons and optimizes the adsorption behavior of the *H and *COOH intermediates. Even at the large current density of −273 mA cm–2, the Faraday efficiency of Cu/CeO2-FLPs for methane was as high as 78.0%, with a conversion frequency of 15784.1 h–1 in the flow cell. This work provides a strategy for the rational design of efficient multipoint catalytic systems.
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Molecular Medicine Reports
·
2017
·Vol. 16
·期 2
·1298-1306
·
IF 1.692
Yuyan Liang,Hai Niu,Limei Ma,Dan Du,Li Wen,Qing Xia,Wen Huang
Coreopsis tinctoria (snow chrysanthemum) has been reported to exert antihyperlipidemic effects. The present study aimed to identify the active compounds of Coreopsis tinctoria and to investigate the molecular mechanisms underlying its effects on lipid dysregulation by measuring lipid levels, reactive oxygen species, lipid peroxidation and fatty acid synthesis. The present results demonstrated that snow chrysanthemum aqueous extracts significantly reduced serum lipid levels and oxidative stress in vivo. The main compounds that were isolated were identified as flavanomarein (compound 1) and eriodictyol 7‑O‑β‑D glucopyranoside (compound 2). Compounds 1 and 2 demonstrated potent antioxidative properties, including free radical scavenging activity, inhibition of lipid peroxidation, as well as lipid‑lowering effects in human HepG2 hepatocellular carcinoma cells treated with free fatty acids (FFAs). Compound 2 was revealed to suppress the elevation of triglyceride levels and inhibit lipid peroxidation following FFA treatment. In addition, it was demonstrated to significantly reduce intracellular levels of reactive oxygen species and improve the mitochondrial membrane potential and adenosine triphosphate levels, thus protecting mitochondrial function in FFA‑treated HepG2 cells. Furthermore, compound 2 markedly suppressed the protein expression levels of disulfide‑isomerase A3 precursor and fatty acid synthase, thus suppressing FFA‑induced lipogenesis in HepG2 cells. In conclusion, the present study identified compound 2 as one of the main active compounds in Coreopsis tinctoria responsible for its lipid‑lowering effects. Compound 2 was revealed to possess antihyperlipidemic properties, exerted via reducing oxidative stress, protecting mitochondrial function and suppressing lipogenesis.
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高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2026
·Vol. 74
·期 29
·22965-22974
·
IF 6.7
Li Mengyu,Fu Chenchen,Zhuang Wei,Zhang Keke,Xu Jingliang,Wang Zhenfu
D-Amino acid oxidase (DAAO) catalyzes the oxidation of
D-phosphinothricin
(D-PPT) to produce optically pure L-PPT, but low catalytic efficiency
limits its industrial application. Here, a synergistic strategy combining
geometric remodeling and charge engineering was applied to enhance
the oxidation activity of our previously developed stable variant
TIF-DAAO (S18T/V7I/Y132F) toward D-PPT. Systematic analysis of the
active pocket-guided alanine and neutral hydrophilic (Ser/Thr/Tyr)
scanning mutagenesis revealed position-specific steric constraints.
Subsequent Arg/His scanning tailored the positively charged microenvironment
around D-PPT, leading to a triple mutant ATR (F58A/Q335T/P221R) with
improved electrostatic complementarity and spatial fit. ATR showed
a 10.7-fold increase in catalytic activity, a 35-fold improvement
in substrate affinity, and a 380-fold higher catalytic efficiency
( k cat / K M )
toward D-PPT. Molecular dynamics simulations provided mechanistic
insight. Our results demonstrate that the synergistic optimization
of substrate tunnel geometry and the electrostatic microenvironment
effectively boosts DAAO activity, offering a rational strategy for
engineering industrial biocatalysts.
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ANALYTICAL BIOCHEMISTRY
·
2015
·
IF 2.219
Fang Wang,Wencheng Gong,Lili Wang,Zilin Chen
Selective recognition of d -tryptophan ( d -Trp) in the presence of Cu(II) was investigated at poly- l -lysine (p-l-Lys) film using electrochemical impedance spectroscopy (EIS) and differential pulse voltammetry (DPV). p-l-Lys film was immobilized on a glassy carbon electrode (GCE) by cyclic voltammetry between 0.0 and 1.9 V in 20 mM phosphate buffer solution (pH 8.6). After the p-l-Lys/GCE electrode was incubated with d -Trp solution containing Cu(II) ions, obvious enhancement of electron transfer resistance and decrease of voltammetric current could be observed. If d -Trp was replaced by l -tryptophan (l-Trp), there was no apparent resistance and current changes. Moreover, no resistance and current changes could be found in the absence of Cu(II). It may be due to the formation of Cu complex with l -lysine and d -tryptophan. Finally, this method was successfully applied to monitoring enantiomeric composition of the d -Trp and l-Trp mixtures.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Fuping Wang,Xinyi Peng,Zhengpeng Zhong,Mingchen He,Qinyan Lu,Yifan Li,Huaiyang Liu,Wang Li,Guobao Chen,Bo Zhou,Zhongmin Chen
A non-isotopic methanol-releasing probe detects HCC early via breath. • Selectively cleaved by β-galactosidase in HCC for tumor-specific signal. • A low-cost dual-sensor array enables real-time exhaled methanol detection. • Distinguishes early-stage tumor-bearing mice from controls (< 2 mm). • Offers a portable, affordable screening tool for primary healthcare. Early detection is crucial for improving therapeutic outcomes in hepatocellular carcinoma (HCC), yet the widespread implementation of low-cost, accessible screening for high-risk populations remains a significant challenge. To address this issue, we investigated the β-galactosidase–methanol signaling axis using a hydrophilic, cell-membrane-impermeable probe, methyl-β-D-galactopyranoside (MGP). This probe is selectively hydrolyzed by β-galactosidase, which is overexpressed in the HCC microenvironment, releasing methanol—an easily volatile, non-isotopic, and metabolically inert volatile organic compounds (VOCs). Methanol levels in exhaled breath were quantified using a custom-designed sensor array. Through in vitro enzymatic assays, cellular studies, and animal experiments, we demonstrated that methanol concentrations in tumor-bearing mice (with tumor diameters <2 mm) were significantly elevated compared to healthy controls, and these levels positively correlated with tumor volume. Our findings highlight the potential of Me-β-Gal in addressing critical barriers to early HCC detection. With further validation, this approach could potentially improve clinical management for high-risk populations, including patients with liver cirrhosis.
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