Journal of Physical Chemistry Letters
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2026
·
IF 4.6
Meiqi Wang,Chen Yin,Yuxuan Du,Huan Liu,Bin Sun
Large-sized lead sulfide (PbS) colloidal quantum dots (CQDs) face significant stability challenges in near-infrared applications due to increased surface active sites. While traditional halogen ligands achieve preliminary passivation, they are prone to dissociation under high-temperature operating conditions, leading to rapid device performance degradation. This study proposes an aromatic bidentate ligand passivation strategy based on 2-picolinic acid (2-PCA). The device demonstrates an external quantum efficiency (EQE) of 35% at 1650 nm wavelength, with responsivity and normalized detectivity reaching 0.46 A/W and 3.58 × 1011 jones, respectively representing a 2.33-fold improvement over conventional halogen-passivated devices. Under thermal stress at 180 °C for 2 h, devices with 2-PCA ligands retain approximately 90% of their initial normalized EQE, marking a 15-fold improvement in stability compared to devices using halogen ligands (PbX2, X = Br–, I–), which undergo nearly complete failure. This aromatic bidentate ligand passivation strategy provides a new pathway for developing high-performance infrared photodetectors with enhanced thermal stability.
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Food Science & Nutrition
·
2023
·Vol. 11
·期 5
·2277-2287
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IF 3.9
Shuyuan Cao,Shengjie Hu,Ping Jiang,Zhan Zhang,Lei Li,Qian Wu
Sulforaphane (SFN) is a promising phytochemical with a wide range of antitumor activities. A comprehensive understanding of the effects of SFN on breast cancer based on the metabolome and microbiome is limited. Thus, we treated MCF-7 cell-transplanted nude mice with 50 mg/kg SFN. SFN inhibits breast cancer cell proliferation. SFN increased the levels of sulfate-related metabolites and glutathione-related metabolites and decreased tryptophan metabolites and methyl-purine metabolites in urinary metabolic profile. SFN indirectly affected the activation of aryl hydrocarbon receptor by tryptophan metabolism. The ratio of SAM to methionine was decreased by SFN while the global DNA methylation was downregulated in tumor tissue. SFN decreased the sulfate-reducing bacterium Desulfovibrio , which is related to reduced methylation capacity, and increased the genus Lactobacillus related to tryptophan metabolites with antitumor activities. In conclusion, we provide a perspective on the metabolome and microbiome to elucidate the antitumor activities of SFN.
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MOLECULES
·
2023
·Vol. 28
·期 9
·3650
·
IF 4.6
Jing Zhu,Lei Hu,Xiangying Meng,Feng Li,Wenjuan Wang,Guiyang Shi,Zhongxia Wang
Carbon-based nanoprobes, with excellent physicochemical performance and biocompatibility, are a kind of ideal nanomaterial for biosensing. Herein, we designed and prepared novel oxygen-doped nitrogen-enrichment carbon nanoribbons (ONCNs) with an excellent optical performance and uniform morphology, which could be used as a dual-mode fluorescence probe for the detection of Ag+ion and captopril (Ctl) based on the synergism of photo-induced electron transfer and aggregation-induced quenching mechanisms. By recording the changes in fluorescent intensities of ONCNs, the Ag+ion and Ctl concentrations can be easily tested in real samples. The results displayed that two good linear relationships existed between the change in fluorescent intensity of ONCNs and the concentrations of Ag+ion and Ctl in the ranges of 3 μM to 30 μM and 1 μM to 30 μM, with the detection limit of 0.78 µM and 74 nM, respectively. The proposed sensing platform has also been successfully applied for the Ctl analysis in commercial tablet samples based on its high selectivity, proving its value in practical applications.Keywords:carbon-based nanoprobe;photo-induced electron transfer;aggregation-induced quenching;metal ion detection;drug analysis
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Qiuyang Huang,Xiaoling Zang,Zhiwei Zhang,Hang Yu,Baoyan Ding,Zhuangzhuang Li,Simin Cheng,Xin Zhang,Mustafa R.K. Ali,Xue Qiu,Zhihua Lv
The discovery of new anti-cancer drugs targeting the PD-1/PD-L1 pathway has been a research hotspot in recent years. In this study, biological affinity ultrafiltration (BAU), UPLC-HRMS, molecular dynamic (MD) simulations and molecular docking methods were applied to search for endogenous active compounds that can inhibit the binding of PD-L1 to PD-1. We screened dozens of potential cancer related endogenous compounds. Surprisingly, cyclic adenosine monophosphate (cAMP) was found to have a direct inhibitory effect on the PD-1/PD-L1 binding with an in vitro IC 50 value of about 36.4 ± 9.3 μM determined by homogeneous time-resolved fluorescence (HTRF) assay. cAMP could recover the proliferation of Jurkat T cells co-cultured with DU-145 cells and may suppress PD-L1 expression of DU-145 cells. cAMP was demonstrated to bind and induce PD-L1 dimerization by FRET assay, and also predicted by MD simulations and molecular docking. The finding of cAMP as a potential inhibitor directly targeting the PD-1/PD-L1 interaction could advance our understanding of the activity of endogenous compounds regulating PD-L1.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2023
·
IF 6.8
Xina Liu,Taozhong Shi,Chenyang Xu,Meiqing Zhu,Yi Wang
Cu 2+ is an essential trace element for the organism, but its excess can also cause irreversible damage to the organism. As such, a “Turn-Off” fluorescent probe DPAP for the specific detection of Cu 2+ was successfully constructed. DPAP exhibits large Stokes shift (120 nm), fast reaction speed (1 min), low detection limit (15.2 nM), low toxicity, and good cell permeability. Cu 2+ quenches the fluorescence of DPAP by blocking its intramolecular charge transfer process to achieve the detection of Cu 2+ and has been confirmed by HRMS, 1 H NMR and DFT calculations. Excitingly, the five-cycle detection of Cu 2+ and the successful recovery of trace Cu 2+ in environmental water samples fully demonstrate the potential of DPAP for practical applications. In particular, DPAP can observe the distribution and translocation patterns of exogenous Cu 2+ in HeLa cells and zebrafish in real-time. This research concept has offered important theoretical support for the study of the environmental behavior of heavy metal ions.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2022
·Vol. 23
·期 19
·11087
·
IF 6.208
Zhuangzhuang Li,Baoyan Ding,Mustafa R. K. Ali,Lizhen Zhao,Xiaoling Zang,Zhihua Lv
Abnormal tryptophan metabolism is linked to cancer and neurodegenerative diseases, and tryptophan metabolites have been reported as potential prostate cancer (PCa) biomarkers. However, little is known about the bioactivities of tryptophan metabolites on PCa cell growth. In this study, MTT and transwell assays were used to study the cytotoxicities of 13 major tryptophan metabolites on PCa and normal prostate epithelial cell lines. Ultraperformance liquid chromatography–high resolution mass spectrometry (UPLC–HRMS) was used to analyze metabolic changes in cells treated with tryptamine. Flow cytometry, confocal imaging, and Western blot were used to test the apoptosis induced by tryptamine. It was shown that tryptamine had obvious inhibitory effects on PCa cell lines PC-3 and LNCaP, stronger than those on the normal prostate cell line RWPE-1. Tryptamine was further shown to induce apoptosis and inhibit PC-3 cell migration. Metabolic changes including amino acid metabolism related to cell proliferation and metastasis were found in PC-3 cells treated with tryptamine. Furthermore, a PC-3 xenograft mouse model was used to study the effect of tryptamine in vivo. The intratumoral injection of tryptamine was demonstrated to significantly reduce the tumor growth and tumor sizes in vivo; however, intraperitoneal treatment resulted in increased tumor growth. Such dual effects in vivo advanced our understanding of the bioactivity of tryptamine in regulating prostate tumor development, in addition to its major role as a neuromodulator.Keywords:tryptamine;prostate cancer (PCa);cell proliferation;apoptosis;cell migration;xenograft model antitumor assays
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Hai-Fang Mao,Hong-Qing Fu,Ji-Bo Liu,Yun Zhao
A novel iron-pyridine-based chelate Fe-PYPA was synthesized via a facile and green strategy. The chelate served as a highly efficient catalyst toward CO 2 cycloaddition . A 95.7% PO conversion and a 98.4% PC selectivity were achieved under moderate conditions. Even under solvent-free conditions, Fe-PYPA could achieve a 93.6% conversion and 98.2% selectivity, acting as a robust and efficient catalyst toward CO 2 cycloaddition. Moreover, the as-prepared catalyst showed desirable catalytic activity , good recyclability , remarkable thermo-stability and ideal compatibility to a variety of epoxy substrates. In-situ ATR-IR spectroscopy was used as a powerful tool to gain process understanding for the whole conversion from CO 2 to cyclic carbonate under atmospheric pressure in the presence of TBAI. The process of PO’s ring opening, activation and insertion of CO 2 and the formation of cyclic carbonate were illuminated explicitly through the change of characteristic absorption peaks, providing direct and visual evidence for the mechanism proposed. The present work paves a new way for theoretical and experimental explorations on novel catalyst design and process understanding for highly-efficient greenhouse gas re-utilization.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 5
·13739-13754
·
IF 5.19
Wu Hao,Bao Yuling,Yan Tongtong,Huang Hui,Jiang Ping,Zhang Zhan,Li Lei,Wu Qian
Epidemiological studies have shown that PAHs may exert adverse effects on childhood asthma. However, the underlying molecular mechanism remains to be fully elucidated. This study aimed to investigate this process in view of metabolic pathways, especially one-carbon metabolism and tryptophan metabolism. Fifty asthmatic children and 50 control subjects were recruited for this study. Serum IgE and IL-17A levels were detected by ELISA. Serum PAH concentrations were measured by GC-MS. One-carbon-related metabolites and tryptophan metabolites were determined by UPLC-Orbitrap-MS. DNA methylation was analyzed by bisulfite sequencing PCR. ChIP assays were used to examine H3K4me3 enrichment on IL-17A gene. Multivariable linear regression was performed to evaluate the association between PAHs and childhood asthma mediated by intermediators. HE staining in lung tissue, IgE and IL-17A in BALF, metabolic profiles in urine, and Ahr , Il-17a , and Cyp1a1 gene expression were determined in PAH-exposed mice. Serum Fla level was associated with childhood asthma (OR = 1.380, 95% CI: 1.063–1.792), and had a great effect on one-carbon metabolites, especially SAH, SAM, and Ser, which exerted significant mediation effects on the relationship between the Fla concentration and asthma. Moreover, we did find significant mediation effects between serum Fla and asthma by LINE-1 DNA methylation and H3K4me3 levels in the IL-17A promoter region. The differential Trp metabolites, such as Trp, tryptamine, IA, IAA, indole, IAld, and IAAld, indicated that asthmatic children had increased indole-AhR pathway. Mediation analysis failed to show a mediator effect of Trp metabolites in the association between PAHs and childhood asthma. An animal study confirmed that PAH exposure increased methylation levels, and altered Trp metabolite-AhR-IL-17A axis, which may be influenced by gender. PAHs disturbed one-carbon metabolism to influence the methyl group refilling DNA methylation and histone methylation, and disturbed tryptophan metabolism to regulate Th17-cell differentiation, which may elevate serum IL-17A concentration in asthmatic children.
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Materials Chemistry Frontiers
·
2022
·Vol. 6
·期 17
·2511-2523
·
IF 8.683
Yudi Feng,Qiangsheng Sun,Jia Guo,Changchun Wang
High-performance polymers in possession of excellent thermal stabilities and mechanical strength have been explored for many years in high-tech fields. However, a big challenge still remains for balance of the processability and performance. Herein, to address this problem, a new design was attempted to conduct the manufacturing process on amorphous micromolecular precursors, rather than traditional crystals, oligomers or polymers. Firstly, a series of crosslinkable precursors were synthesized from commercial aromatic diamines by simple one-step amidation reaction. These molecular materials showed different glass-forming abilities, which were obviously associated with their molecular structures (size, flexibility and symmetry). Owing to the disordered molecular arrangement, amorphous precursors obtained excellent fluidity when the temperature exceeded the glass transition temperatures (Tg, 52–88 °C), allowing for facile processing at low temperatures. The considerable temperature difference between the Tg and reaction temperature (∼200 °C) led to wide processing windows, at which the viscosities could be adjusted by temperature or shear rate within a wide range from 105 to 100 Pa s (|η*|), showing their broad applicability in diverse traditional processing operations for polymers. All the cured resin films prepared by direct molding and subsequent curing exhibited high thermal decomposition temperatures (Td,5% > 428 °C), high Tg (>234 °C) and robust mechanical strength (storage moduli >1.8 GPa). By taking the advantages of amorphous molecular precursors and BCB crosslinking, the outstanding processability and high performance were well-integrated.
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Reaction Chemistry & Engineering
·
2022
·Vol. 7
·期 11
·2313-2321
·
IF 5.2
Hong-Qing Fu,Haifang Mao,Chaoyang Wang,Kun Yin,Miaomiao Jin,Zhenbiao Dong,Yun Zhao,Jibo Liu
Aimed at greenhouse gas CO2 high value-added utilization, a N,N′-(propane-1,3-diyl)dipicolinamide (PPPA) supported Al(III) metal–organic polydentate chelate complex (Al-PPPA) was designed and used to efficiently catalyze CO2 to cyclic carbonates. The substrate conversion and product selectivity were more than 95% and 98%, respectively, at 120 °C and 2 MPa CO2 without the presence of a co-catalyst. After 5 times of recycling, the substrate conversion was no less than 88%, which indicated the excellent thermal stability and reusability of the catalyst. Simultaneously, the catalyst showed a widely universal range of substrates including olefin chains, phenyl chains, internal epoxides and fluorine-containing epoxides. Furthermore, the plausible mechanism of the CO2 cycloaddition reaction was explored by employing in situ IR technology. The ring opening of PO, CO2 activation and the formation of the final products were examined visually. This work supplies a new route for the theoretical and experimental exploration of new catalyst design and process understanding for efficient greenhouse gas reuse.
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Molecular Catalysis
·
2023
·
IF 4.6
Yangyang Sun,Zhuzhu Tang,Tingze Pan,Ke Zhang,Liuzhu Wang,Xingye Zhai,Yiran Jia,Tianqi Yuan,Yujia Qian,Hualei Wang,Dongzhi Wei,Shengli Yang
Catalytic promiscuity makes nitrilase-mediated unnatural reactivity a promising pathway in the production of primary amides . However, during the functional switch of nitrilase, a trade-off between the newly developed hydration activity and relative activity hinders the application of nitrilase in the production of amides. Our previous study showed that the mutant F193N (Mut0) of nitrilase NIT6803 from Synechocystis sp. PCC6803 improved the hydration activity as the amide ratio increased to 73.4%, whereas the relative activity was only 50.1% of that of the wild-type (WT). In this study, we succeeded in alleviating the trade-off of Mut0 through an evolutionary combination of the key identified sites 101, 192, and 201. Inside the active pocket, the co-evolution of residue Q192 was identified by hotspot prediction to correlate with N193, and Q192H exhibited an improved amide ratio of 76.9% with a relative activity of up to 72%. Outside the active pocket, the flexible loop surface residue G101 and homodimer “A” interface residue I201 were identified using sequence alignment-based mutations. Further evolutionary combination of the three key sites yielded the best triple mutant G101K/Q192H/I201M, which had the highest amide ratio of 98.5% and considerably recovered relative activity of 82.6% while retaining only 1.5% of the carboxylic acid ratio. The transition-state analogue sheds light on the basis of the almost identical switch of the reaction pathways, and our results expand the toolbox of nitrilase-catalysed promiscuity for amide formation.
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Molecular Catalysis
·
2023
·
IF 4.6
Wen Liu,Qian Su,Zhenyang Xu,Mengqian Fu,Heming Zhang,Weiguo Cheng
Non-halogen ionic liquids are considered efficient catalyst for CO 2 conversion into cyclic carbonates. In this work, six carboxylic acid ionic liquids with different types and sizes of cations are designed and synthesized to systematically investigate the catalytic contribution of the non-halogen cation and anion for CO 2 conversion into cyclic carbonate. The result shows that the anion could improve the catalytic activity by improve the basicity of ionic liquids, and the cation that has a weak interaction with anion is more conducive for the reactivity. Further, the reaction mechanism is deeply studied by using the optimized [P 4444 ][IsoNic]: two reaction intermediates are captured by In-situ infrared, combined with DFT calculation, the anion directly inducing ring-opening mechanism is proposed. This work provides an in-depth understanding of catalytic contribution of non-halogen ionic liquids used in cycloaddition reaction.
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