Analytical Methods
·
2023
·Vol. 15
·期 30
·3642-3649
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IF 3.1
Kai Zhang,Xiaoyuan Zhang,Yanqin Rong,Qingfang Niu,Pengyue Jin,Xuewen Ma,Cheng Yang,Wenting Liang
Ractopamine (RAC) is universally known for improving lean meat percentage in livestock and thus is widely introduced as a feed additive. However, it is difficult to eliminate the RAC residue in animal tissues from the biological system and will inevitably harm human health. Hence, detecting RAC molecules in biological samples is extremely significant. Herein, a novel strategy of supramolecular recognition-enhanced electrochemical sensing is presented. This platform was constructed by coupling β-cyclodextrin (β-CD) with palladium nanoparticles (Pd NPs)-functionalized three-dimensional reduced graphene oxide (3D-rGO) to form a nanocomposite (3D-rGO/Pd/β-CD), which was further used to modify a glassy carbon electrode (GCE) for RAC detection. Benefiting from the attractive electrical conductivity and catalytic activity of 3D-rGO/Pd, as well as the unique small-molecule-recognition ability of β-CD demonstrated by 1H NMR spectrum, which revealed the 1 : 2 binding mode of RAC with β-CD, increased peak current signals of RAC were observed in the cyclic voltammetry (CV) test. Under optimized conditions, the wide linear concentration range spanned 1–95 μM, along with a relatively low detection limit of 0.12 μM (S/N = 3), as evidenced by the differential pulse voltammetry (DPV) approach. The platform also exhibited satisfactory stability and fine reproducibility, as well as high selectivity and good anti-interference capability. Moreover, this as-obtained sensor was efficiently applied in pork samples with a high recovery rate (96.44–103.99%), which provides a promising view of its electrochemical biosensing ability in practical applications.
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PubMed
高影响因子
FOOD CONTROL
·
2022
·
IF 6.652
Chengyuan Wu,Xiangchuan Wu,Fan Hou,Lina Wu,Guangxia Liu
An ultrasensitive electrochemical aptasensor was established based on metalloporphyrin metal organic frameworks ( [email protected] ) with peroxidase-like activity and exonuclease III-assisted recycling magnification for the detection of ochratoxin A (OTA). [email protected] showed well peroxidase-like activities due to Fe-tetrakis (4-carboxyphenyl) porphyrin (Fe-TCPP) as a heme-like ligand and in situ supported with palladium nanoparticle, which could be used for the label of ssDNA instead of nature enzyme. The designed exonuclease III-assisted recycling magnification further improve the sensitivity for the detection. Based on this, the proposed aptasensor showed a well linear relationship within the scope of 1 × 10 −5 ng mL −1 to 10 ng mL −1 and a low detection limit of 6.79 fg mL −1 . Additionally, the application in the real spiked oil samples confirmed the dependability and veracity of the aptasensor. Hence, the designed aptasensor has comprehensive application prospects for the detection of OTA in food .
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International Journal of Nanomedicine
·
2023
·
IF 8
Yan Zhou,Zekun Zhou,Xiaojuan Wu,Zefeng Wang,Wangdan Qi,Jing Yang,Liming Qing,Juyu Tang,Le Deng
Purpose We aimed to develop an oxidative-stress-activated palladium-copper nanozyme to reduce bacterial’s heat sensitivity by down-regulating heat shock proteins to overcome the shortcomings of conventional photothermal antimicrobial therapy and achieve mild photothermal bactericidal efficacy.Methods We first synthesized palladium-copper nanozymes (PC-NPs) by hydration and used transmission electron microscopy, X-ray diffraction, and Fourier transform infrared spectroscopy to demonstrate their successful preparation. Their photothermal therapy (PTT) and chemo-dynamic therapy (CDT) activities were then determined by a series of photothermal performance tests and peroxidase-like performance tests, and the destruction of heat shock proteins by reactive oxygen species (ROS) was verified at the protein level by Western Blotting tests, providing a basis for the effective bacteria-killing by the mild-temperature photothermal treatment subsequently applied. We also validated this promising programmed and controlled antimicrobial treatment with palladium-copper nanozymes by in vivo/in vitro antimicrobial assays. A hemolysis assay, MTT cytotoxicity test and histopathological analysis were also performed to assess the in vivo safety of PC-NPs.Results In the micro-acidic environment of bacterial infection, PC-NPs showed peroxidase-like activity that broke down the H2O2 at the wound into hydroxyl radicals and down-regulated bacterial heat shock proteins. The application of PC-NPs increased bacteria’s sensitivity to subsequent photothermal treatment, enabling the elimination of bacteria via mild photothermal treatment.Conclusion The programmed synergistic catalytic enhancement of CDT and mild photothermal therapy achieves the most efficient killing of bacteria and their biofilms, which brings future thinking in the relationship between heat shock proteins and oxidative stress damage in bacteria.
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PubMed
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Journal of Environmental Sciences
·
2023
·
IF 6.9
Anqi Lu,Xiaokang Xiang,Ming Lei,Shuangshuang Huang,Bingbing Liang,Siyu Zhao,Lihua Zhu,Heqing Tang
The reduction of nitrobenzene to aniline is very important for both pollution control and chemical synthesis. Nevertheless, difficulties still remain in developing a catalytic system having high efficiency and selectivity for the production of aniline. Herein, it was found that PdO nanoparticles highly dispersed on TiO 2 support (PdO/TiO 2 ) functioned as a highly efficient catalyst for the reduction of nitrobenzene in the presence of NaBH 4 . Under favorable conditions, 95% of the added nitrobenzene (1 mmol/L) was reduced within 1 min with an ultra-low apparent activation energy of 10.8 kJ/mol by using 0.5%PdO/TiO 2 as catalysts and 2 mmol/L of NaBH 4 as reductants, and the selectivity to aniline even reached up to 98%. The active hydrogen species were perceived as dominant species during the hydrogenation of nitrobenzene by the results of isotope labeling experiments and ESR spectroscopic. A mechanism was proposed as follows: PdO activates the nitro groups and leads to in-situ generation of Pd, and the generated Pd acts as the reduction sites to produce active hydrogen species. In this catalytic system, nitrobenzene prefers to be adsorbed on the PdO nanoparticles of the PdO/TiO 2 composite. Subsequently, the addition of NaBH 4 results in-situ generation of a Pd/PdO/TiO 2 composite from the PdO/TiO 2 composite, and the Pd nanoclusters would activate NaBH 4 to generate active hydrogen species to attack the adsorbed nitro groups. This work will open up a new approach for the catalytic transfer hydrogenation of nitrobenzene to aniline in green chemistry.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ningfan Song,Zihan Chen,Jinghua Shi,Dezhi Shi,Li Gu
In the present study, a Pd/Cu bimetallic catalyst supported on a chelating resin (TP207) was prepared in order to selectively reduce nitrate to N 2 with ZVI (zero valent iron) as a reductant. The effects of Pd/Cu mass ratio, temperature, and initial solution pH on the removal of nitrate and TN were then examined. The highest nitrate (63.2%) removal was obtained under neutral conditions at a ratio of Pd/Cu 2:1, in which 57.8% of TN was removed and N 2 accounted for more than 90% of the final products. Additional ammonia (30–40%) were formed when the reaction was conducted at a higher temperature (313 K) compared to when performed at 303 K. The mechanism study for nitrate reduction indicated that this catalyst could broaden the suitable pH range and improve the selectivity of N 2 without the generation of other intermediate compounds or by-products in comparison to ZVI and its combination with a non-supported Pd/Cu catalyst. The slow rate of ZVI corrosion, high Fe(Ⅱ) proportion in corrosion products and high N/H ratio at neutral pH conditions may serve as reasons for the high N 2 selectivity. The chelating resin also played a key role via its load capacity and dispersion ability to Pd/Cu particles in enhancing N 2 selectivity. Accordingly, the proposed method may have great potential application for nitrate reduction to N 2 , which warrants further study.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 23
·6659-6668
·
IF 5.726
Jie Yang,Haochen Yu,Yanbing Wang,Fuyuan Qi,Haodong Liu,Lan-Lan Lou,Kai Yu,Wuzong Zhou,Shuangxi Liu
Four types of Ca–Mn oxides, CaMnO3, CaMn2O4, CaMn3O6 and Ca2Mn3O8, have been prepared and used as supports for Pd nanoparticles. The oxygen activation capacity of these oxides and the catalytic activity of the oxide supported Pd nanocatalysts have been investigated using the aerobic oxidation of 5-hydroxymethyl-2-furfural as a model reaction. It is found that the local coordination environment of lattice oxygen sites plays a crucial role on their redox properties and charge transfer ability from Pd nanoparticles to the support. In particular, the Ca–Mn oxide with lower oxygen coordination number, weaker metal–oxygen bonds and tunnel crystal structure, e.g. CaMn2O4, exhibits promoted oxygen activation capacity, and stronger electron transfer ability. Consequently, Pd/CaMn2O4 exhibits the highest catalytic activity among these catalysts, providing a promising yield of 2,5-furandicarboxylic acid. This work may shed light on future investigations on the design of local structure of active oxygen sites in oxides or oxide supported catalysts for redox reactions.
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RSC Advances
·
2015
·Vol. 5
·期 50
·40227-40235
·
IF 3.84
Fangyuan Yi,Fugui Xu,Yong Gao,Huaming Li,Daoyong Chen
In this study, the preparation of styrene/divinylbenzene-based macrocellular polymers of high internal phase emulsions (polyHIPEs) with interconnected open-cell structure as well as their application as support for Pd nanoparticles are presented. Firstly, water in oil high internal phase emulsions (HIPEs) were generated by adding the water stepwise to the oil phase (styrene and divinylbenzene) containing Janus polymer nanoparticles that consist of a linear poly(methyl methacrylate) “tail” and a cross-linked poly(4-vinylpyridine) “head”. The generated water in oil HIPEs stabilized solely by Janus polymer nanoparticles were then converted to polyHIPEs foams by polymerizing the external continuous oil phase, followed by the extraction with methanol and the drying under the reduced press. Scanning electron microscopy observation revealed that the as-produced macrocellular polyHIPEs were foam structure with closed and/or partially open-cells. Partial cells covered by a thin polymer film were peeled off during the post-treatment. Some key factors influencing the polyHIPEs morphologies, including emulsifier particles content, the mole ratio of styrene to divinylbenzene and the internal phase volume fraction were investigated, and macrocellular polyHIPEs with interconnected open-cell morphologies could be achieved under optimal conditions. Benefited from the strong interaction between the emulsifier particles embedded in the polyHIPEs and H2PdCl4 precursor, Pd nanoparticles were facilely supported in situ within the macrocellular polyHIPEs without any functional monomers or post-functionalization requirement. The obtained Pd@macrocellular polymer hybrid foams were then applied for the heterogeneous Suzuki–Miyaura carbon–carbon coupling reactions between iodobenzene and benzeneboronic acid, and a high catalytic activity with a good recyclability were demonstrated.
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CATALYSIS LETTERS
·
2024
·Vol. 155
·期 1
·1-15
·
IF 2.3
Gao Qing,Yu Yingxue,Wang Chengyun,Xiang Rui,Lu Hao
Designing an efficient Pd-based catalyst with high atom utilization efficiency is a pressing priority, presenting a significant challenge for the practical deployment of electrocatalytic hydrodechlorination (EHDC), a promising method for degrading hazardous chlorophenols (CPs). Herein, a hybrid Pd/Co(OH) 2 /NF electrode for the dechlorination of 2,4- dichlorophenol (2,4-DCP) is fabricated by a newly developed etching-deposition approach. Physical characterizations demonstrate that ultra-fine Pd nanoparticles (1.57 ± 0.29 nm) accompany with Pd 2+ hydroxides are uniformly deposited on the surface of Co(OH) 2 nanowire arrays. EHDC tests on Pd/Co(OH) 2 /NF show an impressive catalytic performance with a 94.5% removal efficiency within 2 h, fast reaction kinetics (0.024 min − 1 ) and remarkable current efficiency (55.4%), highly competitive with literature reports. Mechanism investigations indicate that the even distribution of Pd nanoparticles and coexistence of Pd 2+ sites facilitate the production of active H * and activation of C-Cl, contributing to the improvement of activity.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Siqi Wu,Jianshan Chen,Rong Guo,Haoyi Tong,Shanshan Zong,Zhifang Diao,Yeyan Qin,Yuangen Yao
Efficient production of dimethyl carbonate (DMC) from methyl nitrite (MN) carbonylation based on PdCu/NaY zeolite catalysts is highly desired for industrial applications. The introduction of boron species into the initial gels of NaY synthesis is a cost-effective modification strategy for boosting the catalytic performance. It not only introduces trace amounts of framework boron but also regulates the distribution of framework aluminum (Al F ) species. Most importantly, the synergistic effect of framework boron and Al-rich region significantly enhanced the metal − support interaction, thus promoting more electrons to be transferred from metal to support. This strategy allows the palladium active species to remain in an electron-deficient state more easily. The carbon monoxide (CO) adsorption and the critical intermediate species *CH 3 COO are more easily formatted on PdCu/NaBY catalyst, which leads to superior weight-time yields (WTY DMC up to 1507·g·kg cat − 1 ·h − 1 ), and CO conversion to DMC (C CO up to 83 %). Our design is of great importance for developing metal-zeolites catalysts, which motivates the industrial application of Pd-based catalysts in the MN carbonation of DMC field.
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Food Bioscience
·
2025
·
IF 5.9
Yixuan Wang,Songyu Yang,Shengbin Chen,Yingbing Zuo,Xiaoyu Mu,Hongmei Zhou,Yufei Yao,Xiaoping Peng,Wenjuan Li
This study aimed to explore the anti-tumor activity and mechanisms of the ethanol-soluble acidic components (ESAC) of Camellia oleifera cake through a combination of network pharmacology, in vitro and in vivo studies, and metabolomics based on UPLC-Q-TOF/MS. Additionally, the potential application of ESAC in combination with PD-1 inhibitors was explored. In this work, our results demonstrated that ESAC exhibited anti-tumor activities mediated by regulated cell death (RCD), which were associated with apoptosis, pyroptosis, and ferroptosis. UPLC-Q-TOF/MS-based serum metabolomics revealed that metabolic disorders were occurred in tumor group when compared to control group. In contrast, ESAC significantly inhibited abnormal energy metabolism including glycolysis, tricarboxylic acid cycle, and amino acid metabolism. Consequently, hexokinase and malate dehydrogenase, key enzymes of energy metabolism, were determined, and data showed that treatment of tumor mice with ESAC significantly suppressed activities of these metabolic enzymes when compared to tumor group, confirming that mitigating metabolic disorders contributed to the anti-tumor activities of ESAC. Moreover, ESAC could also reduced PD-L1 expression in tumor tissue, which was similar to the effect of PD-1 inhibitor. Furthermore, combination treatment with ESAC and PD-1 inhibitor was superior to either treatment alone, and it enhanced pyroptosis through the NLRP3/Caspase-1/GSDMD pathway. Together, we concluded that metabolic correction and PD-L1 inhibition were the critical mechanisms to exert anti-tumor activities of ESAC.
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JOURNAL OF CONTROLLED RELEASE
·
2025
·
IF 11.5
Yali Wu,Wenjuan Chen,Jingjing Deng,Xingyu Zhou,Jiangbin Chen,Zimo Yang,Xinghui Cao,Jiatong Liu,Qi Tan,E. Zhou,Minglei Li,Mengfei Guo,Yang Jin
Cancer immunotherapy has transformed cancer treatment, demonstrating the potential for lasting responses in multiple solid and hematologic malignancies and thus has revolutionized cancer treatment in clinic. However, the intricate tumor microenvironment (TME), characterized by a rigid extracellular matrix (ECM) and robust immunosuppressive environment, presents substantial hurdles to the effectiveness of cancer immunotherapy. Thus, cancer-associated fibroblasts (CAFs), the most abundant stromal cells that mediate ECM remodeling and participate in immune suppression, represent promising therapeutic targets for combination immunotherapy. In this study, by using and analyzing single-cell RNA-sequencing (scRNA-seq) in the public datasets, we have identified the elevated expression of glucose transporter 1 (GLUT1) in activated CAF subgroups within tumor sites compared to normal tissues. Moreover, the recent literature has also demonstrated that CAFs undergoing high metabolic levels have been identified to show a better response to immunotherapy. Furthermore, extracellular vesicles (EVs) secreted by CAFs remain unexplored, and their role in drug transport systems and targeting efficiency towards tumorous cells remains uninvestigated. Herein, we identified the elevated expression of glucose transporter 1 (GLUT1) as a prognostic indicator for cancer associated with poor prognosis and investigated the vulnerability of lung tumor cell lines and CAFs to pharmacological GLUT1 inhibition with BAY-876. Based on the possibility of targeting the intrinsic TME-associated metabolism by GLUT1 inhibition, we have firstly employed CAFs-derived extracellular vesicles (cEVs) as a carrier for targeted delivery of BAY-876 into GLUT1-high CAFs and tumor cells. The cEV-BAY-876 (cEV B6) treatment significantly resulted in glucose-rich, low-lactate TME, reversed the activated CAFs phenotype, enabled stromal reprogramming, decreased ECM stiffness and enhanced the infiltration of CD3 + CD8+ T cells in tumor core, thereby achieving an excellent anti-tumor efficiency. Moreover, cEV-B6 treatment synergized anti-programmed death ligand 1 (antiPD-L1) to reinvigorate the exhausted lymphocytes and exerted strong anticancer effects against mice lung tumors. Our study provides the first evidence that tumor stroma-specific therapies by targeting glucose metabolism present a promising strategy of remodeling the extracellular matrix to reverse CAFs into normal type and potentiate cytotoxic T lymphocytes (CTLs) infiltration thereby improving anticancer immunotherapy.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Xingjie Yang,Xubao Jiang,Muhammad Sohail Bashir,Xiang Zheng Kong
Polyurethanes (PUNs) have been widely used in many fields. However, there are few reports on their microsphere preparation through precipitation polymerization. Herein, uniform PUN microspheres are prepared by precipitation polymerization of toluene diisocyanate and trimethylolpropane, without any surfactant and stabilizer. Under optimized conditions, monomers are fully polymerized within 2 h at a monomer concentration as high as 25.0 wt %, with a high yield of the microspheres (96.9%). By loading Pd on their surface, composite microspheres Pd@PUN are obtained and used as catalysts. 4-Nitrophenol is completely reduced within 1 min, with a kinetic constant of 4.96 min–1, significantly higher than many reported Pd-loaded catalysts, and with comparable reusability. Used in degradation of dye molecules, the catalytic performance is practically unchanged after 20 recycled uses. This work provides a simple method for the preparation of highly uniform PUN microspheres with a high yield and their Pd-loaded catalysts, both of great potential for various applications.
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