Catalysis Science & Technology
·
2018
·Vol. 8
·期 5
·1423-1434
·
IF 5.365
Rui Yu,Rui Liu,Jie Deng,Maofei Ran,Ning Wang,Wei Chu,Zhiwei He,Zheng Du,Chengfa Jiang,Wenjing Sun
Pd nanoparticles (NPs) supported on polyaniline (PANI)-coated carbon nanotubes (CNTs) were synthesized using a low-cost and simple method for application in the Heck reaction. The effects of the PANI/CNT coating weight ratio on the catalytic stability and recyclability of the composite were determined by using a combination of experimental and computational methods. The results show that through coordination of the N-species in PANI with the Pd NPs, the nitrogen-rich PANI@CNT provides a strong support for the Pd NPs. The thickness of the PANI layer is the key in determining the stability of the catalyst. PANI becomes protonated in the presence of CNTs, as electron transfer from the former to the latter creates strong interactions between the two. Thus, PANI becomes more stable in nanocomposites with a higher CNT content, e.g., PANI/CNT = 0.5 : 1. The catalyst with a PANI/CNT ratio of 0.5 : 1 exhibited the best recycling performance, and only a small loss of activity was observed after 10 cycles. However, upon increasing the PANI content (e.g., PANI/CNT = 4 : 1), the PANI units tend to form bulk structures that are less stable than those that wrap around the CNTs. Such a structure is unstable; therefore, the PANI layers can easily deform or break away from the CNT backbones. Hence, these catalysts deactivate during recycling. Thus, our study demonstrates that the assembly of noble-metal NPs on CNTs bearing a thin coaxial PANI coating is a powerful technique to prepare reusable catalysts for the Heck reaction. Coating thickness is also a key factor affecting the efficiency and stability of the catalyst.
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BIOSENSORS & BIOELECTRONICS
·
2025
·
IF 10.5
Yuping Liu,Beibei Zhang,Xueyuan Wu,Fan Wang,Zhiyi Yang,Mengyi Li,Kaixuan Sheng,Yue Yan,Liang Zhu,Hui Jing,Yanmin Wu,Lili Hu,Yanyan Yu,Chenglin Li
Programmed cell death 1 ligand 1 (PD-L1) immunotherapy holds a pivotal role in lung cancer treatment. However, current methods for monitoring PD-L1 expression exhibit several limitations, including hysteresis and the invasive nature of tissue sampling. Circulating tumor cells (CTCs), the important biomarkers in liquid biopsy, are minimally invasive and facilitate continuous monitoring. Consequently, integrating CTC counting with PD-L1 expression analysis offers more comprehensive insights for the development of personalized treatment strategies development and efficacy evaluations. In this study, we presented a facile liquid biopsy assay designed for the dynamic monitoring of PD-L1 expression on CTCs captured from non-small cell lung cancer (NSCLC) patients. This assay was achieved by fabricating two high-performance probes: EpCAM and Vimentin dual-aptamer modified nitrogen-doped carbon quantum dots probe (E/V-apt-N-CQDs) and hairpin PD-L1 aptamer coupled with gold nanoparticles (PD-L1-apt-AuNPs). The E/V-apt-N-CQDs probe effectively captured two types of CTC models (H1299 and A549) exhibiting differential PD-L1 expression. Additionally, reagent-less detection of PD-L1 levels on CTCs was achieved using a portable magnetic electrochemical sensor with excellent specificity and sensitivity, which was capable of measuring PD-L1 concentrations as low as 2 ng/mL. Finally, this assay was applied in 41 NSCLC patients to investigate the correlation between CTC numbers or PD-L1 expression and disease progression and immunotherapy efficacy. The results indicated a significant association between elevated CTC counts or reduced PD-L1 levels and clinical progression. Moreover, this liquid assay successfully monitored dynamic changes in CTCs and PD-L1 expression in NSCLC patients receiving immunotherapy, indicating its potential for clinical application.
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MATERIALS CHEMISTRY AND PHYSICS
·
2024
·
IF 4.3
Qinghao He,Dongmei Yu,Tongtong Ma,Jianfeng Bao,Jianping Wang,Jianbo Zhang,Ji Cheng,Wenxuan Fan,Jinghua Li
In this study, we employ a straightforward one-pot heating method to synthesize coral-like palladium-gold-copper trimetallic alloy nanoparticles (Pd–Au–Cu NPs). These nanoparticles are characterized by a coral-like structure with multiple spines radiating outward. Their unique morphology, substantial specific surface area, and trimetallic composition confer exceptional Fenton catalytic activity and photothermal conversion capabilities. We characterized the materials using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM), transmission electron microscopy (TEM), and UV–visible spectroscopy of organic dyes. The material demonstrates strong photothermal properties and significant Fenton catalytic activity in the near-infrared region, achieving up to 98 % degradation of organic dyes, such as methylene blue (MB). Even after multiple cycles, Pd–Au–Cu NPs retain distinct nanoprotrusions, exhibit good photothermal stability, and maintain sustained Fenton catalytic activity, achieving up to 90 % degradation of MB after five cycles. Compared to previous and existing nanomaterials, our trimetallic nanoparticles with unique structure exhibit superior photothermal conversion efficiency and contribute to environmental protection. This study presents a novel approach for environmentally sustainable treatments.
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Materials Today Bio
·
2026
·
IF 11
Hui Zhang,Xu Zhu,Jingchun Wang,Yibo Huo,Yikai Ma,Shengzhong Rong,Yuting Lu,Yingxue Jin
To address the core issue of low clinical response rates (10%-30%) to α-PD-L1 immune checkpoint blockade therapy, this study targeted the immunosuppressive bottleneck mediated by lactate accumulation in the tumor microenvironment (TME). A targeted drug delivery system (HLC) was constructed using hyaluronic acid (HA) nanomicelles co-loaded with lactate oxidase (LOX) and copper-doped carbon dots (CuCDs). Combined with α-PD-L1, a synergistic antitumor strategy integrating lactate metabolic regulation, cuproptosis, and immune activation was established. HLC achieves targeted accumulation through specific binding between HA and CD44 receptors on tumor cells. It directionally releases LOX and CuCDs in the acidic TME via pH-responsive properties. LOX efficiently clears lactate and elevates pH, blocking the HIF-1α/PD-L1 pathway to reverse immunosuppression. It also generates H 2 O 2 in situ to provide substrates for Cu-mediated Fenton-like reactions, enhancing cuproptosis. In vitro experiments confirm that HLC promotes dendritic cell maturation and drives M2-type macrophage polarization toward the M1 phenotype. In vivo studies using CT26 tumor-bearing mouse models show that HLC combined with 808 nm laser and α-PD-L1 significantly inhibits primary and distant tumor growth. It remodels the antitumor immune microenvironment with favorable biosafety. This study elucidates the synergistic mechanism between lactate metabolic regulation and cuproptosis, establishes an association between lactate level and cuproptosis sensitivity, and provides a novel strategy and experimental basis for combined cancer immunotherapy with important clinical translation value.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Xu Zhang,Chaochen Sun,Ruiling Li,Xin Jin,Yongning Wu,FengFu Fu
Enzyme mimics now play a significant role in biochemistry. Especially, peroxidase mimics have been widely used for developing colorimetric sensors of blood glucose. The peroxidase mimics previously reported could not be recycled for reusing and may generate scattering to cause unwanted optical interference when it was used for fabricating colorimetric sensors. We herein prepared a broad-applicable and reusable magnetic enzyme-loading nanoplatform with enhanced peroxidase-like activity by simultaneously loading Fe3O4 nanoparticles (Fe3O4NPs) and palladium nanoparticles (PdNPs) on graphitic carbon nitride (g-C3N4) nanosheets (Fe3O4NPs/PdNPs/g-C3N4). The prepared Fe3O4NPs/PdNPs/g-C3N4 possesses stable and enhanced peroxidase-like activity and good enzyme-loading capacity and can be used to load various natural enzymes to form highly-efficient and stable double-active nanozyme for fabricating colorimetric sensors for the visual detection of small molecules. Especially, the magnetic feature facilitates the magnetic separation of Fe3O4NPs/PdNPs/g-C3N4 from sample solution, which is in favor of recycling and eliminating the optical interference caused by nanozyme in colorimetric sensors. The prepared Fe3O4NPs/PdNPs/g-C3N4 has been successfully used to load glucose oxidase (GOx) and cholesterol oxidase (Chox) to form magnetic peroxidase-GOx and peroxidase-Chox double-active nanozymes, which can be used to fabricate colorimetric methods for the detection of glucose and cholesterol, respectively, with a visual detection limit of 15 μM and a spectrometry detection limit of 1.0 μM. With the developed glucose and cholesterol detection methods, we have successfully detected glucose and cholesterol in serum with a recovery of 98–104% and a RSD (n = 5) < 5%. With high peroxidase-like activity, good stability, reusable features, and broad applicability of loading enzyme, the developed magnetic Fe3O4NPs/PdNPs/g-C3N4 provided a promising approach for fabricating cost-effective, sensitive, and simple colorimetric sensors for the visual detection of various small molecules.
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RSC Advances
·
2019
·Vol. 9
·期 32
·18098-18105
·
IF 3.049
Lamaocao Ma,Hengchang Ma
In this study, we report the synthesis of π-conjugated network polymers via palladium-catalyzed direct arylation polycondensation of triphenylamine (TPA) and tetraphenylethylene (TPE) with different active substrates. Moreover, six conjugated porous polymers were obtained (named as TPA-TPA-MA, TPA-PB-MA, TPA-TFB-MA, TPA-TPE-MA, TPE-PB-MA, and TPE-TFB-MA). Then, the fluorescence properties in the solid and dispersed states, the corresponding microporous structures, and the Brunauer–Emmett–Teller (BET) surface areas of all polymers were well studied. Among the obtained materials, TPA-PB-MA possessed not only largest BET surface area (686 m2 g−1) and largest pore volume (0.716 cm3 g−1), but also the smallest pore size of 0.823 nm. These properties are very beneficial for the application of TPA-PB-MA in CO2 storage and PA sensing. At 1 bar, TPA-PB-MA demonstrated the significant CO2 uptake of 2.70 and 1.35 mmol g−1 at 273 and 298 K, respectively. Furthermore, TPA-PB-MA was most sensitive and selective towards PA recognition. The KSV constant was measured as 4.0 × 104 M−1.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 27
·13315-13324
·
IF 3.925
Yongyong Shi,Donghai Jiang,Jingyun Zhao,Lang Wu,Chenchen Zhao,Jun Ma,Hongyan Pan,Qian Lin
PdMulti@HCS catalysts with Pd nanoparticles partially embedded in the inner wall of hollow carbon spheres were synthesized by a hard template method. The synthesis process of PdMulti@HCS catalysts and the influence of the pore structure of the hollow carbon shell on the catalytic performance for the direct synthesis of H2O2 from H2 and O2 were systematically researched in this work. When the mass ratio of resorcinol (R) and formaldehyde (F) was R/F = 0.20 g/0.286 g, the mass of CTAB was 2.0 g, and the additional amount of 0.075 M H2PdCl4 solution was 1.0 ml; Pd nanoparticles obtained by in situ reduction using freshly prepared NaBH4 solution with an average size of 6.7 nm showed good dispersion and partial embedding in the inner wall of the hollow carbon shell. The average size of cavity diameter and the hollow carbon shell thickness were 145 nm and 8.03 nm, respectively. More importantly, there were a large number of micropores with a pore size distribution of 1.5 nm in the hollow carbon shell. This special hollow structure ensured the maximum exposure of Pd active sites and the optimal transfer and diffusion ability, which were conducive to improving the catalytic activity and stability of the PdMulti@HCS catalysts.
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ANALYTICAL LETTERS
·
2024
·
IF 1.6
Chunli Fan,Mingying Cao,Qiuju Zheng,Youfa Cheng,Ping Wang,Jinyu Feng
The evaluation of the flow direction of platinum group elements (PGEs) during gold-copper ore mining is challenging due to the uneven distribution and low content. Therefore, it is vital to accurately and simultaneously determine ultra-trace PGEs Pt, Pd, Rh, and Ir in gold mining residue samples. In this study, a method to simultaneously determine ultra-trace Pt, Pd, Rh, and Ir in gold mining residue is reported using Sb–Cu fire assay, microwave digestion, and inductively coupled plasma-mass spectrometry (ICP-MS). The Sb–Cu fire assay was used to enrich Pt, Pd, Rh, and Ir, obtaining Sb–Cu alloy particles that concentrate these elements. An optimal microwave method was employed to digest the Sb–Cu alloy particles. In ICP-MS, the collision reaction interface was used to eliminate the interferences of other elements and improve the accuracy. Moreover, the matrix-matched multi-external standards combined with internal standard calibration were utilized to reduce the error. High concentrations of Au, Ag, and Pb showed no interferences with Pt, Pd, Rh, or Ir determination. The limits of detection for Pt, Pd, Rh, and Ir were 0.018, 0.052, 0.064, 0.035 ng·g−1, respectively, and the relative standard deviation was 5.18, 4.66, 1.55, and 3.17%. Additionally, the determination of Pt, Pd, Rh, and Ir in standard reference materials showed good agreement with the certified values. In summary, a reliable and efficient method is provided to determine various PGEs which is of great significance for gold-copper ore mining.
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HYDROMETALLURGY
·
2023
·
IF 4.7
Haitao Zhou,Kun Huang
In conventional liquid-liquid extraction, Pt(IV) and Pd(II) chloride complex anions PtCl 6 2− and PdCl 4 2− in concentrated hydrochloric acid cannot be separated using simple amine extractants according to the ion association mechanism based on the thermodynamic difference in the interaction of their inner sphere coordinated chloride ions with protonated amine. This study exhibits a novel strategy for enhancing the separation of PtCl 6 2− and PdCl 4 2− anions using thin-layer organic membrane-based laminar flow (TOMLF) extraction by controlling the acidified primary amine N1923 (A-N1923) molecular orientation on the surface of concentrated hydrochloric acid with a laminar shear flow. Experiments revealed that the separation selectivity is primarily determined by the interaction of A-N1923 molecules with the outer sphere-bound water molecules around PtCl 6 2− and PdCl 4 2− anions, and is easily controlled by regulating the A-N1923 molecular orientation on the surface of laminar flow. It is a new phenomenon that has not been previously documented. The evolution of A-N1923 molecular orientation and complexation sites induced by laminar shear flow would result in a controllable spatial geometry recognition, therefore promoting or inhibiting the separation of PtCl 6 2− and PdCl 4 2− anions in concentrated hydrochloric acid. This work is expected to provide new insight into the development of hydration-sphere coordination strategies based upon shear-switch laminar flow for controllable host-guest molecule recognition at a flowing liquid-liquid interface.
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JOURNAL OF BIOMEDICAL MATERIALS RESEARCH PART A
·
2023
·
IF 4.9
Hui Jiang,Yingying Zhou,Dongdong Zheng,Yexiazi Cheng,Dacheng Xiang,Lixin Jiang,Jing Du
Triple negative breast cancer (TNBC) has the worst prognosis of all breast cancers, and it is difficult to progress through traditional chemotherapy. Therefore, the treatment of TNBC urgently requires agents with effective diagnostic and therapeutic capabilities. In this study, we obtained programmed death-ligand 1 (PD-L1) antibody conjugated gold nanoshelled poly(lactic-co-glycolic acid) (PLGA) nanocapsules (NCs) encapsulating doxorubicin (DOX) (DOX@PLGA@Au-PD-L1 NCs). PLGA NCs encapsulating DOX were prepared by a modified single-emulsion oil-in-water (O/W) solvent evaporation method, and gold nanoshells were formed on the surface by gold seed growth method, which were coupled with PD-L1 antibodies by carbodiimide method. The fabricated DOX@PLGA@Au-PD-L1 NCs exhibited promising contrast enhancement in vitro ultrasound imaging. Furthermore, DOX encapsulated in NCs displayed good pH-responsive and photo-triggered drug release properties. After irradiating 200 μg/mL NCs solution with a laser for 10 min, the solution temperature increased by nearly 23°C, indicating that the NCs had good photothermal conversion ability. The targeting experiments confirmed that the NCs had specific target binding ability to TNBC cells overexpressing PD-L1 molecules. Cell experiments exhibited that the agent significantly reduced the survival rate of TNBC cells through photochemotherapy combination therapy. As a multifunctional diagnostic agent, DOX@PLGA@Au-PD-L1 NCs could be used for ultrasound targeted contrast imaging and photochemotherapy combination therapy of TNBC cells, providing a promising idea for early diagnosis and treatment of TNBC.
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