Materials Today Bio
·
2025
·
IF 10.2
Wenjin Zhong,Pengcheng Wang,Jintian Wang,Yuejia Zhu,Liquan Chen,Yilong Qian,Xiang Huang,Kai Ye
Background The immune checkpoint inhibitor (ICI) PD-1α can effectively treat Lynch syndrome (LS)-associated colorectal cancer (CRC) (LS-CRC). In some cases, LS-CRC is not sensitive to ICIs. Dendritic cell (DC)-based hybrid membrane nanoparticles have great potential to upgrade the efficacy of ICIs, which can theoretically be applied to enhance the efficacy of ICIs in treating LS-CRC. Methods MnO 2 nanomaterials with si-CTLA4 were absorbed by coating mature DCs loaded with PD-1α and liposome hybrid membranes. The morphology and physicochemical properties of DCsLipo@MnO 2 @si-CTLA4@PD-1α were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), dynamic light scattering (DLS), fluorescence resonance energy transfer (FRET), and Fourier transform infrared spectroscopy (FTIR). The activation of DCs and T cells was assessed by utilizing the detection of cell surface markers by flow cytometry. The mRNA levels of CTLA4 in T cells were measured using the qPCR method. The biosafety of DCsLipo@MnO 2 @si-CTLA4@PD-1α was proved by hemolysis test in vitro , CCK-8 assay, and live/dead cell staining. In vitro T-cell uptake experiments proved that the nanomedicine can be effectively absorbed by T cells. Cell proliferation, apoptosis, and ELISA experiments demonstrated that nanomedicine facilitated T-cell proliferation, cytokine secretion, and cancer cytotoxicity. Finally, the anti-cancer effect and immune activation ability of the nanomedicine against LS-CRC were verified by a mouse allograft model. Results The nanomedicine DCsLipo@MnO 2 @si-CTLA4@PD-1α created in this research exhibited good stability and uniform vesicle morphology. In vitro hemolysis test, CCK-8 assay, and live/dead staining experiments indicated that DCsLipo@MnO 2 @si-CTLA4@PD-1α had great biosafety. The nanoparticle loaded with si-CTLA4 effectively reduced the mRNA expression of CTLA4 in T cells. Meanwhile, the results of T cell flow analysis, cell proliferation, cytotoxicity, apoptosis, and ELISA experiments manifested that DCsLipo@MnO 2 @si-CTLA4@PD-1α effectively reinforced the proliferation and activation of T cells, and enhanced the cytotoxicity of T cells to cancer cells. The validation experiments based on the mouse allograft tumor model manifested that DCsLipo@MnO 2 @si-CTLA4@PD-1α boosted the infiltration of T cells into tumor tissues and suppressed the development of LS-CRC. Conclusion DCsLipo@MnO 2 @si-CTLA4@PD-1α can facilitate T cell activation and synergistically enhance the efficacy of ICIs, exhibiting a great inhibitory effect on LS-CRC.
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DOI
PubMed
高影响因子
VACUUM
·
2025
·
IF 3.9
Xiaohua Wang,Yanwei Li,Xinhui Jin,Guang Sun,Jianliang Cao,Yan Wang
The pressing need for health and environmental protection has sparked significant interest among researchers in exploring gas sensors made from metal oxide semiconductors (MOSs). Herein, a co-modification approach involving palladium (Pd) and palladium oxide (PdO) is introduced to enhance the sensing properties of indium oxide (In 2 O 3 ) to hydrogen sulfide (H 2 S). Pd and PdO co-modified In 2 O 3 hierarchical porous nanocubes (Pd/PdO-In 2 O 3 HPNCs) were synthesized using a facile hydrothermal method. With the theoretical doping amount of 2 mol%, the synergistic effect of metal Pd and PdO-In 2 O 3 heterojunction made Pd/PdO-In 2 O 3 show excellent sensing performance to H 2 S compared to In 2 O 3 . Specifically, the material features a lower operating temperature (280 vs 300 °C), higher sensitivity (95.06 vs 28.59 to 20 ppm H 2 S; 2.28 vs 1.17–100 ppb H 2 S), and better selectivity (7.41 vs 2.32 times to triethylamine), while also demonstrating satisfactory reproducibility and stability. The synergistic sensitization mechanism of noble metal catalysis and heterojunction in Pd/PdO–In 2 O 3 HPNCs, along with their underlying mechanism, was discussed. Integrating noble metal modification with heterojunctions adds complexity to the structure and composition of the material. The synergistic effects of these two sensitization strategies on the H 2 S sensitization mechanism need further in-depth investigation.
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高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Jin Zhao,Tianjun Hu,Jinjin Wang,Ying Wang,Junming Zhang,Baoliang Lv,Wanqing Zhang,Jianfeng Jia
Reactive metal-support interaction (RMSI) is an effective means of inducing surface strain and charge transfer in catalysts, which further enhances electrochemical activity and modulates reaction pathways. Nevertheless, the precise synthesis of nanomaterials with tunable strain and unique morphology remains a challenge. In this work, we have synthesized Pd nanoparticles decorated Pd 2+ - doped Co 3 O 4 nanosheets (Pd 7.4% /Co 3 O 4 ) by a NaBH 4 reduction method, which exhibit excellent performance for ethanol oxidation reaction (EOR) and oxygen reduction reaction (ORR). The introduction of the Pd into the Co 3 O 4 by the means of elemental doping and nanoparticle decoration, and the resulting lattice strain and electron redistribution are responsible for the improved performance. Meanwhile, Pd 7.4% /Co 3 O 4 has a relatively low d-band center that reduces the adsorption energy of reaction intermediates to improve reaction selectivity and eliminate EOR toxic intermediates, ultimately promoting reaction kinetics. This work demonstrates a simple and effective strategy to manipulate lattice strain and electronic coupling and provides a novel and advanced way for the development of low-cost and high-quality direct ethanol fuel cells (DEFCs) catalysts.
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高影响因子
Chem
·
2021
·
IF 22.804
Peng Zhou,Qinghua Zhang,Yuguang Chao,Liang Wang,Yiju Li,Hui Chen,Lin Gu,Shaojun Guo
Photocatalytic co-production of high value-added multicarbon compounds and hydrogen from renewable bioethanol is an environmental and long-term approach to industrial activities and remains a great challenge because of the difficulty in bioethanol dehydrogenation. Guided by first-principle simulation, we first synthesized a partially reduced Pd–P 3 single atom (PdPSA) on CdS nanorods with an unoccupied hybrid state of Pd 4d and P 3p via both metal-support interaction effect and Pd–P coordination effect. This unique electronic structure of PdPSA is totally different from highly reduced S-coordinated Pd single atoms or nanoparticles and allows PdPSA-CdS to exhibit a visible-light photocatalytic activity of 35.1 mmol g −1 h −1 for the co-production of high-value-added 1,1-diethoxyethane and H 2 with a selectivity of 100%. Mechanism studies revealed that the unoccupied hybrid states of Pd 4d and P 3p in PdPSA not only greatly promoted the dehydrogenation of ethanol but also promised PdPSA with a high H 2 -production activity.
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Haoyang Fu,Ruizhao Wang,Qianyu Xu,Minwang Laipan,Chenliu Tang,Weixian Zhang,Lan Ling
Typical antineoplastic agent doxorubicin (DOX) contamination is a major environmental concern and its efficient purification remains a daunting challenge so far. This work explored the potential of Fe/Pd-doped graphite carbon nitride (g-C 3 N 4 @Fe/Pd) for DOX removal from water, involving the removal performance, mechanism, and pathway. Structural characterization of g-C 3 N 4 @Fe/Pd showed that the metallic Pd clusters are decorated on the surface of uniformly distributed iron nanoparticles (~ 28 nm) on g-C 3 N 4 . The existence of g-C 3 N 4 effectively relieved the agglomeration and overgrowth of iron nanoparticles, the strong coupling effect among the Fe, Pd and N demonstrates the excellent DOX removal performance (k = 0.115 min −1 ) with versatility under different initial concentrations (30–150 mg/L) and material dosages (0.1–0.4 g/L). Three possible degradation pathways of DOX were proposed, where catalytic saccharide moiety elimination is the primary pathway. Importantly, intermediates exhibit lower toxicity and the final degradation product is efficiently adsorbed by g-C 3 N 4 @Fe/Pd.
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高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Yongyong Shi,Donghai Jiang,Liming Zhou,Jingyun Zhao,Jun Ma,Qian Lin,Hongyan Pan
A well-defined structural morphology can significantly construct a special catalytic micro-reaction environment to enhance the catalytic performance of Pd catalyst in the direct synthesis of hydrogen peroxide from hydrogen and oxygen (DSHP). In this study, SiO 2 was used as a rigid template, PdCl 2 as the Pd precursor, and dopamine hydrochloride (DA) as the carbon and nitrogen source to synthesize a nest-shaped hollow-encapsulated Pd catalyst named Pd Multi @ONHCS. This catalyst was successfully constructed via high-temperature pyrolysis of poly dimethyl diallyl ammonium chloride (PDDA), which generated a blasting effect crucial for this formation. Characterization analysis, catalytic performance evaluation experiment, and molecular dynamics simulation were conducted to explore the structure-performance relationship of Pd Multi @ONHCS catalyst in DSHP. Both experimental and simulation results consistently showed that the nest-shaped hollow structure of Pd Multi @ONHCS catalyst created a distinctive catalytic microreactor environment with a spatial mass transfer constraint, which was not only conducive to adsorption and enrichment of H 2 and O 2 at Pd active sites to produce H 2 O 2 . In addition, the generated H 2 O 2 can be desorbed from Pd active sites in time and rapidly diffused into the reaction solution, effectively inhibiting the dissociation of species containing O O bonds on the Pd surface, resulting in severe hydrogenation and decomposition side reactions, and improving H 2 O 2 productivity and selectivity.
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DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2020
·
IF 7.539
Xingxing Zhang,Yunkang Xia,Chaochao Wang,Jiajia Li,Peng Wu,Liping Ma,Yuguang Wang,Yao Wang,Fanghua Da,Wenru Liu,Lezhong Xu
This study investigated the activity of partial denitrification (PD) biomass/key enzymes, functional gene expressions in response to 0 ~ 50 mg/L hydroxylamine (NH 2 OH) addition. Results indicated that NH 2 OH contributed to nitrite (NO 2 − -N) production, facilitating the maximum increase of nitrate (NO 3 − -N) to NO 2 − -N transformation ratio to 80.47 ± 2.82%, leading to 2.56-fold NO 2 − -N higher than those of control. The observed transient inhibitory effect on NO 3 − -N reduction process was attributed by high-level NH 2 OH (35 ~ 50 mg/L). Enzymatic assays revealed the enhanced activity of both NO 3 − -N and NO 2 − -N reductase while the former showed obvious superiority which led to high NO 2 − -N accumulation. These results were further confirmed by the corresponding functional genes ( nar G, nap A, nir S and nir K). Besides, negative influence of NH 2 OH addition was limited to PD aggregates, due to the increasing secretion of extracellular polymeric substances (EPS) as well as proteins/polysaccharides ratios in tightly-bound structure of EPS.
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PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2018
·Vol. 28
·期 51
·1803815
·
IF 13.325
Lingyu Zhang,Shengnan Li,Xiangjun Chen,Tingting Wang,Lu Li,Zhongmin Su,Chungang Wang
The development of novel Janus nanostructure with desired compositions and functionalities is essential for various applications, especially as drug delivery system to deliver multiple payloads with total different solubility. Here, a unidentified flying object (UFO)-like cyclodextrin–palladium nanosheet/zeolitic imidazolate framework-8 Janus nanoparticle (CD–PdNS/ZIF-8 JNP) prepared via a selective coating of polyacrylic acid (PAA) on one of the flat surfaces of 2D PdNS followed by further formation of ZIF-8 on a PAA template, and alternative modification of CDs on exposed PdNS surface is reported. The CD-PdNS and PAA-ZIF-8 parts are designed to load hydrophobic10-hydroxycamptothecin (HCPT) and hydrophilic doxorubicin (Dox) independently for synergistic chemotherapy (combination index = 0.65). Because of the broad near-infrared (NIR) absorption band of PdNSs, the photothermal effect of UFO-like CD-PdNS/ZIF-8 JNPs in NIR-II biowindow is studied. The in vitro and in vivo results show that the dual-drug loaded JNPs under a laser-irradiation group present highest cancer therapeutic efficiency. The good performance is due to the synergistic chemotherapy and photothermal therapy in NIR-II biowindow. This work significantly broadens the application prospects of metal–metal organic framework JNPs by rationally designing their compositions and discovering related physiochemical properties.
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高影响因子
Scientific Reports
·
2015
·Vol. 5
·期 1
·1-9
·
IF 5.578
Wang Liyuan,Feng Feng,Ma Zhanfang
Electrochemical redox-active species play crucial role in electrochemically multiplexed immunoassays. A one-pot method for synthesizing four kinds of new electrochemical redox-active species was reported using HAuCl 4 and Na 2 PdCl 4 as dual oxidating agents and aniline derivatives as monomers. The synthesized polyaniline derivative-Au/Pd composites, namely poly(N-methyl-o-benzenediamine)-Au/Pd, poly(N-phenyl-o-phenylenediamine)-Au/Pd, poly(N-phenyl-p-phenylenediamine)-Au/Pd and poly(3,3’,5,5’-tetramethylbenzidine)-Au/Pd, exhibited electrochemical redox activity at −0.65 V, −0.3 V, 0.12 V and 0.5 V, respectively. Meanwhile, these composites showed high H 2 O 2 electrocatalytic activity because of the presence of Au/Pd. The as-prepared composites were used as electrochemical immunoprobes in simultaneous detection of four tumor biomarkers (carcinoembryonic antigen (CEA), carbohydrate antigen 19-9 (CA199), carbohydrate antigen 72-4 (CA724) and alpha fetoprotein (AFP)). This immunoassay shed light on potential applications in simultaneous gastric cancer (related biomarkers: CEA, CA199, CA724) and liver cancer diagnosis (related biomarkers: CEA, CA199, AFP). The present strategy to the synthesize redox species could be easily extended to other polymers such as polypyrrole derivatives and polythiophene derivatives. This would be of great significance in the electrochemical detection of more analytes.
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PubMed
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 9
·2889-2900
·
IF 9.48
Song Li,Long Yan,Qiying Liu,Jianguo Liu,Qiyu Liu,Wei Fan,Xuelai Zhao,Xinghua Zhang,Chenguang Wang,Longlong Ma,Qi Zhang
One-pot hydrodeoxygenation (HDO) of biomass furan derivatives into long-chain alkanes remains unclear owing to the complicated reactions at high temperatures. Here, Pd/C combined with phosphotungstic acid (HPW), a strong Brønsted solid acid promoter, was developed to produce decane under mild conditions through the one-pot HDO of δ-furfurylidenelevulinic acid (FDLA). A 93.16% sum yield of alkanes including 89.53% yield of decane was obtained under 3 MPa H2 at 170 °C for 4 h. The ring-opening and HDO of furans are accomplished at preheating stage, which enable to clarify the complicated reaction pathway. In addition, experimental validations and catalytic characterizations confirm that the synergistic effect of active acid–metal sites plays a critical role in the generation of alkanes via the formation and hydrogenolysis of lactone intermediates to aldehyde/alcohol. This work provides guidance for the one-pot HDO of biomass furan derivatives via the combination of metal catalyst and strong Brønsted solid acid under mild conditions.
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高影响因子
COMPOSITES COMMUNICATIONS
·
2019
·
IF 0
Jinglu Chen,Mingtao Qiao,Wenyan Wang,Qiuyu Zhang
It is well known that palladium-catalyzed cross-coupling Suzuki reaction is very important way to build organic compound carbon skeleton. However, when some reactants such as chlorobenzene are used as substrates which has low reactivity, only moderately low yields were obtained using such kind of mobilized catalyst, Insufficient loading on the normal carrier, the problem of easy aggregation of palladium and large particle size of Pd were considered as reasons of it. A novel magnetic mesoporous Fe 3 O 4 @Void@mSiO 2 nanochains with yolk-shell structure have been first developed to solve the problems via magnetic-field induced distillation-precipitation polymerization together with a facile sol-gel method and the final calcination . Interestingly, we found that some pleated layers grown on the surface of Fe 3 O 4 @void@mSiO 2 nanochains during the hydrolysis of 3-aminopropyltriethoxysilane (KH-550) and special microstructures endow them with excellent porosity which are helpful for increasing the loading capacity of Pd nanoparticles . Owing to high aspect ratio and superparamagnetism , the magnetic nanochains can rotate in the water or organic solution and be separated and recycled easily with the drive of alternating magnetic field. In this catalysis system, the orderly mesoporous opening structure of the hollow mesoporous nanochains could effectively facilitate the transfer of reactant molecules, and the existence of the internal cavities would effectively prolong the action time of the Pd nanoparticles for the Suzuki reaction. The reaction yields of coupling reaction between bromobenzene/chlorobenzene and phenylboronic acid catalyzed by the nanochains can reach nearly 100% respectively. and the reaction yields can still maintain 92.93% and 60.86% after 7 cycles, respectively.
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DOI
Catalysts
·
2019
·Vol. 9
·期 2
·114
·
IF 3.444
Ke Yu,Yan Lin,Jinchen Fan,Qiaoxia Li,Penghui Shi,Qunjie Xu,Yulin Min
Ethanol oxidation reaction (EOR) is an important electrode reaction in ethanol fuel cells. However, there are many problems with commercial ethanol oxidation electrocatalysts today, such as poor durability, poor anti-CO poisoning ability, and low selectivity for C–C bond cleavage. Therefore, it is very meaningful to develop a high-performance EOR catalyst. Herein, we designed ternary N, S, and P-doped hollow carbon spheres (C–N,P,S) from polyphosphazene (PCCP) as Pd supports for EOR. Using SiO2spheres as the templates, the PCCP was first coated on the surfaces of SiO2spheres by in situ polymerization. Through high-temperature pyrolysis and hydrofluoric acid-etching, the hollow PCCP has a large surface area and porous structure. After loading Pd nanoparticles (NPs), the Pd/C–N, P, S catalysts with Pd NPs decorated on the surfaces of C–N, P, S can achieve a high mass peak current density of 1686 mA mgPd−1, which was 2.8 times greater than that of Pd/C. Meanwhile, the Pd/C–N, P, S catalyst also shows a better stability than that of Pd/C after a durability test of 3600s.
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高影响因子
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