Small
·
2021
·Vol. 17
·期 52
·2105643
·
IF 13.281
Bo Liu,Linjuan Zhang,Yuanyuan Luo,Lei Gao,Guotao Duan
The supported metal catalysts on scaffolds usually reveal multiple active sites, resulting in the occurrence of side reaction and being detrimental to the achievement of highly consistent catalysis. Single atom catalysts (SACs), possessed with highly consistent single active sites, have great potentials for overcoming such issues. Herein, the authors used SACs to modulate kinetic process of gas sensitive reaction. The supported Pd SACs, established by a metal organic frameworks-templated approach, promoted greatly the detection capacity to hydrogen sulfide (H 2 S) gas with a very high sensitivity and selectivity. Density functional theory calculations show that the supported Pd SACs not only increased the number of electrons transferring from H 2 S molecules to Pd SACs, but strengthened surface affinity to H 2 S. Moreover, the H S bonds of H 2 S molecules absorbed on Pd atomic sites are more likely to be dehydrogenated directly into sulfur species. Significantly, quasi in situ XPS analysis confirmed the presence of sulfur species during H 2 S detection process, which may be a major cause for such detection signal. Based on these results, a suitable sensing principle for H 2 S gas driven by Pd SACs was put forward. This work will enrich catalytic electronics in chemiresistive gas sensing.
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高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Xiangquan Qin,Yiping Jiang,Jie Chen,Fuquan Yao,Longyi Jin,Zhiqi Cong
Selective hydroxylation of C( sp 3 )–H bonds is a long-standing challenge in the organic synthesis field. We herein report an artificial P450 peroxygenase system facilitated by ω-pyridyl fatty acyl amino acids that can hydroxylate broad-spectrum alkanes, including linear and cyclic alkanes and benzylic and allylic alkane chains. Compared with the previously reported dual-functional small molecule (DFSM) with imidazole as a catalytic group (Im-DFSM), pyridyl DFSM (Pyd-DFSM) produced substantially higher total turnover numbers (TTNs) for the hydroxylation of medium-chain alkanes and cycloalkanes (C6–C8), e.g., 12.0-fold and 17.1-fold increased TTNs of P450 mutant F87A/T268V for heptane and cycloheptane , respectively. In addition, Pyd-DFSM altered the enantioselectivity of benzylic hydroxylation, e.g., it almost inverted the configuration observed in the benzylic hydroxylation of ethylbenzene and tetralin . More importantly, Pyd-DFSM showed excellent regioselectivity for allylic hydroxylation over epoxidation of terminal alkenes and cycloalkenes , e.g., up to 94% allylic hydroxylation of 1-hexene was observed. This work significantly enhances the catalytic toolbox of the DFSM-facilitated P450 peroxygenase system; it not only substantially expands the chemical space of P450 enzymes, but also provides an alternative solution for the selective hydroxylation of C( sp 3 )–H bonds.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Guilin Zhou,Xiaodong Zhang,Xin-Long Ni
A water-soluble terpyridine-based cationic fluorescent probe ( SP - TPy ) was synthesized, which emerged with pH-dependent amphiphilicity, resulting in self-assembly and disassembly in aqueous media with the aggregation-induced emission (AIE) property. In neutral water (pH 7.4), a moderate sensing response to Hg 2+ ions was given by the self-assembly of SP - TPy . However, in acidic aqueous media, the monomer of SP - TPy not only appeared to be highly selective and sensitive for Hg 2+ ions, but also displayed highly efficient removal of Hg 2+ ions from solution by rapid precipitation, which was attributed to the coordination-triggered reassembly of SP - TPy . The removal efficiency of SP-TPy f or Hg 2+ was found to be over 99%. Further study indicated that the precipitates were composed of various polyhedral porous frameworks, a property that was further used to adsorb H 2 S gas to form HgS complexes with higher uptake capacities. In addition, SP - TPy can be efficiently regenerated and recycled using a simple treatment with acidic water after adsorption of the H 2 S gas.
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JOURNAL OF ORGANIC CHEMISTRY
·
2018
·
IF 4.805
Chao Zhang,Yugang Song,Zhihui Sang,Lingpeng Zhan,Yu Rao
A strategy combining O- and N-containing directing groups has been developed for the synthesis of 2,2′-biaryl via Pd-mediated C–H bond activation and oxidative coupling. This new transformation may proceed through a mechanism involving Pd(II) and Pd(IV) intermediates. We found the use of PTSA and HFIP to be critical for the reaction and suggest that these reagents could serve as efficient ligands for this C–C bond formation. This methodology provides broad functional group tolerance, excellent reactivity, and high yields.
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MATERIALS & DESIGN
·
2025
·
IF 7.9
Yuannong Qu,Ji Zou,Weimin Wang,Wei Ji,Zhengyi Fu
The h-BN/ZrO 2 composites for preparing ceramic side sealing plate were obtained with spark plasma sintering (SPS) at 1700 °C for 10 min in the study. By varying AlN content from 0 to 20 wt%, we systematically explored its influence on sintering behavior, microstructure evolution, mechanical performance, and corrosion mechanism at1600 °C. Results show that the rapid heating and uniaxial pressure during SPS and the in-situ reactions between AlN and ZrO 2 promoted the densification of composites. The main reaction products were ZrN, which acted as an effective oxygen scavenger, consuming dissolved oxygen ([O]) and converting into ZrO 2 . These newly formed ZrO 2 particles filled residual porosity within the matrix and nucleated around pre-existing ZrO 2 grains, progressively coalescing into continuous Zr-rich barrier layer.Thereby preventing molten steel from further penetrating into the matrix. The corrosion depth of the composite with 5 wt% AlN content in molten steel at 1600 °C after 2 h was only 69 μm. Meanwhile, it showed a thermal conductivity of 25 W m −1 K −1 and a coefficient of thermal expansion of 3.7 × 10 -6 K −1 , demonstrating excellent thermal shock resistance. The composites are expected to be used to manufacture side sealing plates for the novel continuous casting of thin strip.
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MOLECULAR PHARMACEUTICS
·
2025
·
IF 4.5
Hao Zhang,Dan Xie,Meng Chen,Qiangqiang Yin,Guangyue Shi,Jialong He,Xiaoyang Yu,Qian Lu,Zhengji Wang,Jing Dong,Liguo Hao
Chemotherapy is a widely used cancer treatment modality, while the complex tumor microenvironment (TME) significantly impedes drug delivery and deep tissue penetration. An MR molecular imaging drug-loaded nanomotor has been developed to achieve deep tumor tissue penetration and imaging-guided drug delivery, enabling combined photothermal and chemotherapeutic treatment of pancreatic cancer. A Janus-type nanomotor (Au@H-MP NMs) was fabricated via magnetron sputtering for application in photothermal therapy. Doxorubicin (DOX) was loaded onto one hemisphere of the nanomotor, achieving combined photothermal and chemotherapeutic treatment. Additionally, the nanomotor exhibits dual responsiveness to pH and glutathione (GSH), facilitating the controlled release of DOX within deep tumor tissues. Studies confirmed the nanomotors excellent biosafety, strong photothermal conversion capability, and effective induction of apoptosis. Tumor tissue penetration was validated through in vitro migration and infiltration assays, while in vivo experiments demonstrated significant tumor suppression and enhanced drug accumulation. Moreover, MR imaging technology enables real-time monitoring of nanomotor dynamics. These findings suggest that the synthesized Janus-type MR molecular imaging nanomotor offers a promising strategy for multimodal treatment of pancreatic cancer with significant clinical potential.
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高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2025
·
IF 3.6
Jingru Zou,Lingmeng Xie,Wen Qin,Xingang Xie,Xing Huo
The Groebke–Blackburn–Bienaymé (GBB) reaction provides efficient access to imidazole-fused heterocycles, yet it is inevitably endowed with an isocyanide-derived secondary amino group in products. Herein, we report a Pd(II)-catalyzed sp2 C–H carbonylative amidation strategy using Co2(CO)8 as a safe CO surrogate. Leveraging the native aryl amino group as a directing motif, this protocol enables direct conversion of GBB adducts into pharmaceutically relevant imidazo[1,2-a]pyridine-fused δ-lactams with up to 86% yield. The method demonstrates exceptional functional group tolerance and eliminates prefunctionalization requirements, offering a streamlined approach to access complex nitrogen-rich architectures.
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高影响因子
DRUG DEVELOPMENT RESEARCH
·
2021
·Vol. 82
·期 7
·969-979
·
IF 4.36
Ruixian Xing,Xuewen Liu,Buxian Tian,Yan Cheng,Longguang Li
Parkinson's disease (PD) is a disabling neurodegenerative disease mainly caused by degeneration of mesencephalic dopaminergic neurons in the substantia nigra pars compacta (SNpc). The neuroprotective role of Na + /H + exchangers isoform-1 (NHE1) inactivation in cerebral ischemic damage has been elucidated. The current study aimed to investigate the impacts of NHE1 in PD. In this study, 6-hydroxydopamine (6-OHDA)-induced PD rat models were established to attempt to illuminate the role and underlying mechanisms of NHE1 in SNpc neurons of PD. Meanwhile, nerve growth factor-stimulated PC12 cells followed by 6-OHDA treatment was used to mimic PD in vitro. Results showed that the protein levels of NHE1 were significantly increased in the SNpc neurons of rats and differentiated PC12 cells after 6-OHDA treatment. Inactivation of NHE1 with chemical inhibitor HOE642 suppressed SNpc neuronal loss and NHE1 expression in PD rats. The overlays of tyrosine hydroxylase and NHE1 displayed that NHE1 expression was not colocalized but closely associated with TH. Besides, treatment with HOE642 relieved the dyskinesia, mitochondrial dysfunction, and neuronal apoptosis. Further in vitro evidence confirmed that inhibition of NHE1 by genetic-knockdown prevented mitochondrial dysfunction and apoptosis. Our study represents the first experimental evidence of a potential role for NHE1 in the pathogenesis of PD.
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高影响因子
Journal of Biomedical Nanotechnology
·
2022
·Vol. 18
·期 11
·2484-2497
·
IF 3.641
Li Guiyin,Chen Min,Li Haimei,Li Xinhao,Yao Xiaoqing,Li Liuxun
Golgi protein 73 (GP73) is a novel biomarker for the detection of hepatocellular carcinoma. We prepare a colorimetric aptasensor for GP73 detection based on the catalytic performance of the H-rGO-Mn3O4 nanozyme. The H-rGO-Mn3O4 nanozyme serves
as a peroxidase mimetic which can enhance the reaction with the substrate (3, 3,’ 5, 5′-tetramethylbenzidine, TMB) and H2O2. The peroxidase-like activity of H-rGO-Mn3O4 features a 1.78-fold higher binding affinity value (Km
)
for TMB compared with that of horseradish peroxidase. The H-rGO-Mn3O4 nanozyme not only exhibits admirable peroxidase-like activities due to the synergistic effect of Mn3O4 NPs, rGO and hemin, but also has a large specific surface area to endow the
GP73 aptamer with specific recognition capabilities. A sandwich colorimetric aptasensor is formed to realize the visual detection of GP73 through catalyzing the H2O2-mediated oxidation peroxidase substrate TMB to oxidized TMB accompanied by a color change from colorless
to blue. Under optimal conditions, the logarithm of the GP73 concentration (0.05–50.0 ng/mL) shows a good linear relationship with the absorbance. The calibration equation is Y =−0.0383 lgC+0.4835, with R2 of 0.9964, and the lowest limit of detection is 36.94
pg/mL. Additionally, the content of GP73 in human serum samples is directly detected, and the relative standard deviation is 0.49–4.91%. Compared with the enzyme-linked immunosorbent assay method, the relative error is 0.23–3.61%. All in all, colorimetric aptasensor is demonstrated
to exhibit excellent specificity, stability, and reproducibility.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Wei Bi,Yanjie Hu,Wenge Li,Hao Jiang,Chunzhong Li
In this work, a nanoreactor combining layers of facile traditional two-dimensional (2D) material, hexagonal boron nitride (h-BN, which often called the white graphene) with Pt/Al2O3 catalyst was designed to exhibit higher stability, activity, and selectivity in automobile exhaust treatment. Characterization revealed that h-BN does coat on the surface of platinum and forms a distinct Pt@h-BN/Al2O3 core–shell nanostructure. This as-prepared catalyst possesses good thermal stability and selectivity, because of the excellent high-temperature tolerance and the multidefected structure of the h-BN shell; that is, small molecules such as CO and O2 can easily intercalate into the nanoreactor, while large molecules such as propylene are blocked out. Meanwhile, the intercalated reactants can achieve the conversion of CO to CO2 faster (ΔT100 = 20 °C) with the confinement effect. The study indicates that constructing a nanoscale confined environment with two-dimensional (2D) coating can enhance the performance of the catalyst in multiple aspects and simultaneously provide a good example for designing nanostructured catalysts with multifaceted improvement.
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FOOD CHEMISTRY
·
2026
·
IF 10.4
Yipeng Zhang,Shijia Wu,Yisheng Chen
A portable biosensor for the peanut allergen Ara h 1 was developed by integrating a polydopamine-functionalized pipette tip, CRISPR/Cas12a signal amplification, and a personal glucose meter. Ara h 1 binding induced partial displacement of a cDNA activator, which activated Cas12a trans-cleavage and released glucose oxidase from GOx–DNA conjugates. The released enzyme catalyzed glucose oxidation, producing a quantitative decrease in glucose concentration. Under optimized conditions, the assay showed a linear range of 50–1000 ng/mL and a solution-based limit of detection of 22.19 ng/mL. Post-extraction matrix-spike tests in commercial peanut-biscuit and peanut-beverage extracts yielded recoveries of 101.58–104.68% with relative standard deviations below 3.44%. These results demonstrate the analytical feasibility and preliminary matrix compatibility of the platform, although validation using pre-extraction fortified, incurred, and naturally contaminated foods is still required.
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Journal of Materials Research and Technology-JMR&T
·
2026
·
IF 7.3
Lihao Yang,Pengpeng Yu,Binglong Jiao,Qingwen Yang,Shuqi Ding,Pingping Jia,Yaokun Pan
To address the inherent microporosity and inadequate long-term corrosion protection capacity of plasma electrolytic oxidation (PEO) ceramic coatings deposited on 6063 aluminum alloy substrates, a hierarchical Ce-doped PEO/h-BN/diamondlike carbon (DLC) composite coating architecture was fabricated via combined hydrothermal pore sealing and plasma enhanced chemical vapor deposition (PECVD) post treatment routes. The microstructure, chemical composition, and corrosion behavior of the coatings were systematically characterized using scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, Fourier-transform infrared spectroscopy (FT-IR), potentiodynamic polarization, and electrochemical impedance spectroscopy (EIS). The results demonstrated that hydrothermal treatment effectively introduced h-BN nanosheets into discharge channels and the micropores of the Ce-doped PEO coating. XPS, Raman, and FT-IR analyses confirmed the successful incorporation of h-BN while preserving its characteristic layered structure. Subsequently, a continuous DLC film containing typical sp 2 /sp 3 hybridized carbon bonds was successfully deposited by PECVD. Among all tested processing parameter combinations, the composite coating modified with 1 g L −1 h-BN hydrothermal sealing followed by 60 min PECVD deposition delivered optimal comprehensive anticorrosion performance, featured by a minimum corrosion current density of 1.76 × 10 −9 A cm −2 and the highest impedance response in 3.5 wt% NaCl solution. The significantly improved anticorrosion performance originates from the dual synergistic barrier effect derived from h-BN nanosheet pore plugging and the dense DLC outer capping layer. Specifically, h-BN nanosheets effectively reduced pore connectivity and prolonged the diffusion path of corrosive species, whereas the dense DLC overlayer served as additional physical barrier that suppressed electrolyte penetration and interfacial charge transfer. This study provides valuable experimental guidance and theoretical support for the design of graded ceramic-carbon composite protective coatings for aluminum alloys serving in high chloride marine environments.
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