ACS Applied Materials & Interfaces
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2017
·
IF 7.504
Jiao Li,Yalan Liu,Xiaoqian Zhu,Gang Chang,Hanping He,Xiuhua Zhang,Shengfu Wang
Electrochemical sensors now play an important role in analysis and detection of nucleic acids. In this work, we present a novel double-signal technique for electrochemically measuring the sequence and length of the d(CAG)n repeat. The double-signal technique used an electrochemical molecular beacon (a hairpin DNA labeled with ferrocene), which was directly modified on the surface of a gold electrode, while a reporter probe (a DNA sequence labeled with horseradish peroxidase) was hybridized to the target DNA. First a simple single-signal sensor was characterized in which d(CAG)n repeats were detected using a short reporter DNA strand labeled with horseradish peroxidase. To obtain a reliable signal that was dependent on repeat number, a double-signal biosensor was created in which the single strand capture DNA in single-signal sensor was replaced by an electrochemical molecular beacon labeled with ferrocene. When the hairpin DNA hybridized to the target–reporter DNA complex, it opened, resulting in a decreased ferrocene current. Both electrochemical biosensors exhibited high selectivity and sensitivity with low detection limits of 0.21 and 0.15 pM, respectively, for the detection of d(CAG)n repeats. The double-signal sensor was more accurate for the determination of repeat length, which was measured from the ratio of signals for HRP and ferrocene (H/F). A linear relationship was found between H/F and the number of repeats (n), H/F = 0.1398n + 9.89788, with a correlation coefficient of 0.974. Only 10 nM of target DNA was required for measurements based on the value of H/F in the double-signal technique. These results indicated that this new double-signal electrochemical sensor provided a reliable method for the analysis of CAG trinucleotide repeats.
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Journal of Functional Foods
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2018
·
IF 3.47
Cuicui Duan,Yujuan Zhao,Cheng Huang,Zijian Zhao,Lei Gao,Chunhua Niu,Chao Wang,Xiaoxiao Liu,Chuan Zhang,Shengyu Li
Acute liver failure (ALF) is a life-threatening clinical condition resulting from massive apoptosis of hepatocytes. This study aims to examine the protective effects of Lactobacillus plantarum C88 on LPS/D-GalN-induced ALF and elucidate its underlying molecular mechanisms in mice. The results showed that L. plantarum C88 pretreatment significantly reduced the levels of plasma ALT and AST in mice with LPS/D-GalN–induced liver injury. L. plantarum C88 pretreatment decreased the secretion of inflammatory cytokines. In addition, L. plantarum C88 remarkably increased the expression levels and nuclear translocations of Nrf2 mRNA in liver tissues, but inhibited NF-κB nuclear translocations and P65, P38 phosphorylation levels. Moreover, L. plantarum C88 enhanced the intestinal mucosal barrier by upregulating the expressions of tight junction proteins as well as HIF-1α. These results suggest that L. plantarum C88 protects against ALF associated with Nrf2 and the MAPK/NF-κB signaling pathways.
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MATERIALS CHEMISTRY AND PHYSICS
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2024
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IF 4.3
YanXiao Zhang,XiaoNing Gao,Nan Ma,Hong Zhou,Lu Feng
Diosgenin is an indispensable intermediate in the production of various steroid drugs. Conventional hydrolysis of sulfuric acid produces large amounts of acidic wastewater and has always faced stringent restrictions from environmental requirements. Here, UiO-66-NH 2 and its derivative of UiO-66-NH 2 -AT (AT = 3-amino-1,2,4-triazole) were synthesized, and these two compounds were further grafted with high-concentration CF 3 SO 3 H molecules to obtain the MOF-based solid superacids, namely UiO-66-NH 2 -[SO 3 CF 3 ] and UiO-66-NH 2 -AT-[SO 3 CF 3 ], respectively. They have been applied to the alcoholysis of total saponins to extract diosgenin, and the alcoholysis conditions, including the solid acid dosage, extraction temperature and extraction time, have been optimized by single-factor experiments. Subsequently, the alcoholysis conditions of UiO-66-NH 2 -AT-[SO 3 CF 3 ] with more prominent catalytic performance and cycle stability were further optimized by the response surface method, and under the optimum conditions, the diosgenin yield reached 20.8 %, which was close to the predicted value of 21.3 % and was superior to the conventional hydrolysis of sulfuric acid and our previously reported solid acids. Additionally, the alcoholysis pathways and alcoholysis mechanism of the total saponins catalyzed by UiO-66-NH 2 -AT-[SO 3 CF 3 ] have been proposed by the analysis of high-resolution electrospray mass spectrometry.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Hongfang Zhao,Jianrong Wang,Hongxia Li,Xiaohui Niu,Hui Xu,Kunjie Wang
The enantioselective recognition and separation of racemic tryptophan are of significant importance in the fields of medicine, pharmaceutics, and biochemistry. However, conventional methods are costly, energy intensive, and environmentally unfriendly. In this case, l-Cys with amino (−NH2) and sulfhydryl (−SH) groups was chosen to modify β-CD with a chiral cavity to achieve self-assembly via hydrogen bonding, which not only serves as an electrochemical chiral sensor with enhanced chiral sites at the sensing interface but also achieves a higher enantioselectivity for d-tryptophan enantiomers through hydrogen bonding between the host and guest. Moreover, the d-tryptophan enantiomers were subsequently degraded under catalytic conditions simulating visible light, which was a new approach to introduce chiral properties in photocatalysis without organic synthesis. The use of inclusion-complex formation with β-CD combined with simple electrochemical technology and photocatalytic degradation techniques to efficiently and rapidly identify and degrade harmful d-type amino acid enantiomers offers new avenues, which would have great potential in future studies.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Qianxi Zhou,Hao Zhang,Tianyu Zeng,Jiahua Yang,Qizhi Liang,Hai Shi,Yongmei Yin,Genxi Li
The dynamic variation of D-amino acids (D-AAs) in human saliva has great potential as the indicator for individual physiological states and disease progression; however, enantiospecific profiling of D-AAs is a great challenge. In this work, a nanoreactor based on mesoporous hydrogen-bonded organic framework (MHOF) has been fabricated for the enantiospecific profiling of D-AAs. The nanoreactor is prepared by using MHOFs as the scaffold to organize the biocatalytic cascade of D-AA oxidase (DAAO) and horseradish peroxidase (HRP). In the meanwhile, the large, stable, and robust transport channels of MHOFs allow the unimpeded transport of the involved biocatalytic substrates. Once D-AA substrates efficiently transport into MHOFs, the chromogenic reactions of 3,3′,5,5′-tetramethylbenzidine (TMB) and H 2 O 2 can be activated. So, using this MHOF nanoreactor, enantiospecific and visual detection of D-AAs can be achieved. Moreover, the stable nanoreactor can be operated in complex solution and utilized for the profiling of D-AA levels in saliva samples collected from gastric cancer patients, suggesting that D-AAs may be a powerful fingerprint for the diagnosis of gastric cancer. Therefore, the fabricated MHOF-based nanoreactor may provide an emerging tool for the enantiospecific profiling of D-AAs and supports the D-AA fingerprint as the indicator of gastric cancer diagnosis.
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Materials
·
2017
·Vol. 10
·期 8
·879
·
IF 2.654
Tao Chen,Cong Zhang,Yuemei Qin,Haiguan Yang,Peng Zhang,Fanggui Ye
A cationic porous framework with mobile anions (MIL-101(Cr)-Cl) was easily and successfully synthesized by utilizing the stronger affinity of F−to Al3+than Cr3+in the charge-balanced framework of MIL-101(Cr). The structure, morphology and porosity of MIL-101(Cr)-Cl were characterized. The obtained new materials retain the high surface area, good thermostability, and structure topology of MIL-101(Cr). With the mobile Cl−anion, MIL-101(Cr)-Cl can be used as an ion-exchange material for anionic organic pollutions. In this work, 2,4-dichlorophenoxyacetic acid (2,4-D) was used as a model to test the absorption performance of this new material. This new material exhibited improved adsorbability compared to that of the original metal-organic frameworks (MOFs). At the same time, this material also shows high anti-interference performance with changing solution pH.Keywords:adsorption;2,4-dichlorophenoxyacetic acid;ion exchange;metal-organic frameworks
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CARBOHYDRATE POLYMERS
·
2017
·
IF 4.811
Guoguang Wei,Alei Zhang,Kequan Chen,Pingkai Ouyang
This study presents an efficient pretreatment of crayfish shell using high pressure homogenization that enables N -acetyl- d -glucosamine (GlcNAc) production by chitinase. Firstly, the chitinase from Serratia proteamaculans NJ303 was screened for its ability to degrade crayfish shell and produce GlcNAc as the sole product. Secondly, high pressure homogenization, which caused the crayfish shell to adopt a fluffy netted structure that was characterized by Scanning electron microscope (SEM), Fourier transform infrared spectrometer (FT-IR), X-ray diffraction (XRD), was evaluated as the best pretreatment method. In addition, the optimal conditions of high pressure homogenization of crayfish shell were determined to be five cycles at a pressure of 400 bar, which achieved a yield of 3.9 g/L of GlcNAc from 25 g/L of crayfish shell in a batch enzymatic reaction over 1.5 h. The results showed high pressure homogenization might be an efficient method for direct utilization of crayfish shell for enzymatic production of GlcNAc.
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ACS Catalysis
·
2024
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IF 11.3
Ruilin Liu,Chao Wang,Yong Yan,Ruzhi Wang,Ge Chen
The direct hydrogen peroxide (H2O2) product from H2 and O2 is a promising anthraquinone replacement because it is environmentally friendly and has a high atom efficiency. Experimental and theoretical studies have proven that optimizing the adsorption of the critical intermediate OOH* on the metal site significantly promotes the further protonation of this intermediate and inhibits the O–O bond cleavage, thus enhancing the activity and selectivity. Redistributing the charge density of active sites to tuning the d-band center of the metal could effectively modulate the intermediates adsorption, and thus regulate the catalytic efficiency. Herein, we show that a Lewis acid (ZnCl2 solution) induces abundant oxygen vacancies (Ovs) on the TiO2 surface, which results in a reversal of charge transfer from TiO2–Ov support to the Pd atom, generating an electron-rich Pd configuration. Compared with pristine Pd/TiO2, Pd/TiO2–Ov possesses higher H2O2 selectivity and productivity, with values of 80.7% and 186 mol kgcat–1 h–1, respectively. In addition, Pd/TiO2–Ov maintains stability during the six cycles reaction due to its high resistance to the leaching of Pd species. Theoretical calculations reveal that the reversed charge transfer downshifts the d-band center of Pd, which promotes O2 adsorption on the Pd surface and weakens the OOH* intermediates adsorption. Thus, the energy barrier for the hydrogenation of the OOH* intermediate is significantly decreased, and the O–O band cleavage is inhibited. This study reports a reversal of charge transfer tuning the d-band center of the active site for efficient direct H2O2 synthesis, which may provide insight for designing high-performance catalysts.
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Biology-Basel
·
2025
·Vol. 14
·期 3
·226
·
IF 3.5
Zonghan Jiang,Leisheng Sun,Yuanyuan Li,Haoyu Li,Yu Fu,Jiyun Li,Zhiliang Sun
Simple SummaryEscherichia coliis a ubiquitous pathogen, with certain strains causing severe diarrhea and intestinal illnesses, which pose significant health risks to both children and animals. As antimicrobial resistance continues to rise, traditional antibiotics are increasingly ineffective, highlighting the urgent need for novel therapeutic strategies. In this study, we investigated the antimicrobial peptide D-CONGA-Q7, aiming to evaluate its efficacy and underlying mechanism against drug-resistantE. colistrains. Our results demonstrate that D-CONGA-Q7 effectively disrupts bacterial cell membranes, leading to bacterial death, and exhibits comparable activity against polymyxin- and meropenem-resistant strains. In vivo experiments revealed that D-CONGA-Q7 significantly alleviated intestinal inflammation, reduced inflammatory cytokine levels, and promoted the repair of damaged intestinal tissues. Furthermore, D-CONGA-Q7 displayed good stability. These findings suggest that D-CONGA-Q7 not only represents a promising new approach to combat drug-resistant bacterial infections but also holds potential for clinical application.Escherichia coli(E. coli) is a zoonotic bacterium widespread in the environment, highly transmissible, and responsible for significant economic losses and millions of cases of illness annually. The rise of multidrug-resistant (MDR) strains has rendered last-line antibiotics such as polymyxin and meropenem ineffective, making the development of new antibiotics urgent. Although D-CONGA-Q7 has broad-spectrum bactericidal activity, its underlying mechanism remains poorly understood. In this study, we used in vitro and in vivo experiments to demonstrate that D-CONGA-Q7 effectively kills both antibiotic-sensitive and multidrug-resistant strains ofE. coli. D-CONGA-Q7 disrupts the cell membranes of Gram-negative bacteria, and the treatment ofE. colistrainLN175with D-CONGA-Q7 resulted in a significant up-regulation of theMlacgene, suggesting that D-CONGA-Q7 may interact with phospholipids in the cell membrane. Furthermore, in treatingK88-induced bacterial enteritis in the small intestine, D-CONGA-Q7 significantly reduced intestinal inflammation. In conclusion, this study provides a novel approach to combat drug-resistantE. coli.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Liu Hong-Zhi,Shu Xiao-Xuan,Huang Mingjie,Wu Bing-Bing,Chen Jie-Jie,Wang Xi-Sheng,Li Hui-Lin,Yu Han-Qing
Polymerization-driven removal of pollutants in advanced oxidation processes (AOPs) offers a sustainable way for the simultaneous achievement of contamination abatement and resource recovery, supporting a low-carbon water purification approach. However, regulating such a process remains a great challenge due to the insufficient microscopic understanding of electronic structure-dependent reaction mechanisms. Herein, this work probes the origin of catalytic pollutant polymerization using a series of transition metal (Cu, Ni, Co, and Fe) single-atom catalysts and identifies the d -band center of active site as the key driver for polymerization transfer of pollutants. The high-valent metal-oxo species, produced via peroxymonosulfate activation, are found to trigger the pollutant removal via polymerization transfer. Phenoxyl radicals, identified by the innovative spin-trapping and quenching approaches, act as the key intermediate in the polymerization reactions. More importantly, the oxidation capacity of high-valent metal-oxo species can be facilely tuned by regulating their binding strength for peroxymonosulfate through d -band center modulation. A 100% polymerization transfer ratio is achieved by lowering the d -band center. This work presents a paradigm to dynamically modulate the electronic structure of high-valent metal-oxo species and optimize pollutant removal from wastewater via polymerization.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Shaorou Ke,Yajing Zhao,Xin Min,Xinyu Zhu,Xin Li,Bozhi Yang,Fan Yang,Xiaowen Wu,Ruiyu Mi,Yangai Liu,Zhaohui Huang,Minghao Fang
Platinum-based bimetallic catalysts exhibit superior hydrogen evolution reaction performance compared to single platinum catalysts. Most studies on platinum bimetallic catalysts have focused on changing the metals used, with not much attention on how the d-band theory affects the catalyst's performance. Herein, we investigated the additional of different transition metals alters the d-band center for better hydrogen evolution. A method combining the ultrasound processing and in-situ reduction was designed, resulting in the alloys with different stacking orders. As the d-band of transition metal elements in the alloy shifts upwards, the lower the energy of the alloy's d-band center, the better the stability of the adsorption bonding exhibited by the alloy. The PtCu/C, with a hexagonal-close-packed structure and a d-band center at −1.823 eV, has an 84 mV overpotential at 100 mA cm −2 , lower than PtNi/C (89 mV) and PtCo/C (91 mV). It also has 4.75 times the mass activity of commercial Pt/C. As a cathode catalyst, PtCu/C provides improved water-splitting at 2.31 V vs. 2.55 V for commercial Pt/C (at 1 A cm −2 ). This analytical strategy through the d-band center advances the design of platinum-based bimetallic catalysts and offers a new direction for the optimization and development of hydrogen evolution reaction electrocatalysts.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 38
·e55968
·
IF 2.7
Meili Li,Xiancheng Meng,Zaizai Tong
Poly( L -lactic acid) (PLLA), as a green, biodegradable polymer material, has garnered considerable attention due to its ease of processing and exceptional properties. However, the inherent slow crystallization rate and brittleness of PLLA substantially restrict its extensive applications across various domains. In present work, PLLA and poly( D -lactide) (PDLA)-modified cellulose nanocrystals (CNCs), referred as CNC- g -L and CNC- g -D, are serving as nano-fillers to enhance the crystallization rate of PLLA. Our findings demonstrate that both nano-fillers could enhance the crystallization rate of PLLA, but the CNC- g -D shows a more efficient nucleation agent compared with its counterpart, CNC- g -L. Isothermal crystallization analysis indicates that CNC- g -D substantially increases nucleation density of PLLA, with pronounced crystallization at an elevated temperature of 155°C as confirmed by differential scanning calorimetry (DSC) and polarized optical microscopy (POM). Wide-angle x-ray diffraction (WAXD) analysis shows the preformation of stereocomplex crystals on the CNC- g -D surface may result in a fast crystallization rate. Meanwhile, after incorporation of different nano-fillers, the toughness property of PLLA has also been significantly enhanced. Our result has shown the CNC- g -D could serve as an efficient nucleation agent toward PLLA and also facilitate to aiding in establishing comprehensive structure–property relationships of polymer materials.
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