ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Liu Mengyu,Feng Wenji,Wu Yunshuo,Wang Haiqiang,Wu Zhongbiao
Methane valorization is important for climate change mitigation and sustainable carbon utilization, but conventional nonoxidative coupling of methane (NOCM) suffers from the high activation barrier of CH 4 , limited product selectivity, and rapid coking-induced deactivation. Herein, we develop a spark discharge−dielectric barrier discharge (DBD) coupled plasma-catalytic system for the selective conversion of high-concentration methane to ethylene. Spark discharge first activates CH 4 and preferentially converts it to C 2 H 2 , while a downstream catalyst bed, maintained at 100−130 ° C by residual discharge heat, enables acetylene semihydrogenation to C 2 H 4 . A coupled DBD unit is further introduced for in situ carbon removal and catalyst regeneration. Among the tested catalysts, impregnation−reduction-derived 0.1Pd-5Cu/γ-Al 2 O 3 -R with atomically dispersed Pd exhibited the best performance, achieving 72.38% CH 4 conversion, 72.19% C 2 H 4 selectivity, 92.48% acetylene-based C 2 H 4 selectivity, and a C 2 H 4 space-time yield of 69.97 mmol·g· −1 ·h −1 at 36.2 kJ·L −1 . With DBD-assisted regeneration, efficient NOCM operation was maintained for 630 min. Mechanistic analyses associate the enhanced ethylene selectivity with highly dispersed Pd sites and their electronic modulation by predominantly low-valent Cu species, which suppress overhydrogenation and facilitate ethylene desorption.
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高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qinglin Wang,Zhuojun Wei,Jin Li,Danyang Feng,An Feng,Hui Zhang
Water-soluble captopril-capped atomically precise Pd nanoclusters (Pd17Capt8 NCs: 1.3 ± 0.5 nm) produced by a simple chemical reduction were supported on preprepared hybrid Co3Al-layered double hydroxide/reduced graphene oxide (Co3Al-LDH/rGO) by a pH-adjusted electrostatic adsorption strategy followed by proper calcinations, giving a series of novel catalysts x-PdNCs/CoAl(O)/rGO-T (x (Pd loading) = 0.09, 0.17, 0.43 wt % (ICP), T = 230, 250, 280, 300, 320 °C). The characterization results show that the as-obtained catalysts possess the hierarchical nanosheet array morphology. Pd NCs with a size of ∼1.3 to 1.8 nm are highly distributed at the edge sites of the CoAl(O) nanosheets. All of the x-PdNCs/CoAl(O)/rGO-T catalysts show superior catalytic efficiency for the conversion of 4-nitrophenol to 4-aminophenol, particularly 0.17-PdNCs/CoAl(O)/rGO-300 possesses the highest performance with a turnover frequency (TOF) of 30 042 h–1, which is the highest among the reported Pd-based catalysts so far. The superior activity of 0.17-PdNCs/CoAl(O)/rGO-300 can be owing to ultrafine Pd NCs with a clean surface, the strongest PdNCs–Co2+-OH(LDH)–rGO three-phase synergy, and the much improved adsorption of the substrate via π–π stacking upon nanosheet array morphology. Meanwhile, 0.17-PdNCs/CoAl(O)/rGO-300 exhibits excellent catalytic activities for various nitroarenes and anionic azo dyes as well as good reusability with the complete reduction of 4-nitrophenol (4-NP) within 90 s after 10 successive runs. The present work provides not only a simple and convenient strategy for the synthesis of clean, efficient, and environmentally friendly supported metal nanocluster catalysts but also a new idea for the efficient catalytic degradation of environmental pollutants.
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DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 124
·102210-102218
·
IF 3.84
Wanchun Guo,Jiao Jiao,Kesong Tian,Yongfu Tang,Yin Jia,Ruifei Li,Zhaopeng Xu,Haiyan Wang
A soft template-assisted simultaneous redox strategy has been developed to fabricate Fe3O4@polypyrrole/Pd (Fe3O4@PPy/Pd) nanocomposites with a single Fe3O4 core and multiple PPy satellites, into each of which multiple tiny Pd nanocrystals are uniformly confined. The dispersion of Pd nanocrystals into PPy satellites and the Pd loading of the nanocatalyst could be finely tuned by tailoring the polarity of the reaction medium and by changing the molar ratio of pyrrole monomer to Pd precursor, respectively. The Pd-based catalyst shows high activity, robust stability and magnetic recyclability for the reduction of nitroaromatic compounds. Superior activity could be attributed to the short transport route toward the active Pd nanocrystals within the small PPy satellite for the outer substitutes. Meanwhile, high stability could be ascribed to the confinement of Pd nanocrystals uniformly into PPy satellites against aggregation and even loss of active sites during catalytic transformations.
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高影响因子
International Journal of Nanomedicine
·
2024
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IF 6.6
Haishui Sun,Xiao Wang,Zhaoyang Guo,Zhenrong Hu,Yuanchen Yin,Shuhan Duan,Wenwen Jia,Wei Lu,Jingzhou Hu
Introduction Traditional surgical resection, radiotherapy, and chemotherapy have been the treatment options for patients with head and neck squamous cell carcinoma (HNSCC) over the past few decades. Nevertheless, the five-year survival rate for patients has remained essentially unchanged, and research into treatments has been relatively stagnant. The combined application of photothermal therapy (PTT) and immunotherapy for treating HNSCC has considerable potential.Methods Live-dead cell staining and CCK-8 assays proved that Fe3O4 nanoparticles are biocompatible in vitro. In vitro, cellular experiments utilized flow cytometry and immunofluorescence staining to verify the effect of Fe3O4 nanoparticles on the polarisation of tumor-associated macrophages. In vivo, animal experiments were conducted to assess the inhibitory effect of Fe3O4 nanoparticles on tumor proliferation under the photothermal effect in conjunction with BMS-1. Tumour tissue sections were stained to observe the effects of apoptosis and the inhibition of tumor cell proliferation. The histological damage to animal organs was analyzed by hematoxylin and eosin (H&E) staining.Results The stable photothermal properties of Fe3O4 nanoparticles were validated by in vitro cellular and in vivo animal experiments. Fe3O4 photothermal action not only directly triggered immunogenic cell death (ICD) and enhanced the immunogenicity of the tumor microenvironment but also regulated the expression of tumor-associated macrophages (TAMs), up-regulating CD86 and down-regulating CD206 to inhibit tumor growth. The PD-1/PD-L1 inhibitor promoted tumor suppression, and reduced tumor recurrence and metastasis. In vivo studies demonstrated that the photothermal action exhibited a synergistic effect when combined with immunotherapy, resulting in significant suppression of primary tumors and an extension of survival.Conclusion In this study, we applied Fe3O4 photothermolysis in a biomedical context, combining photothermolysis with immunotherapy, exploring a novel pathway for treating HNSCC and providing a new strategy for effectively treating HNSCC.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jian Wu,Zhiqiang Chen,Haojie Shang,Yonghua Tong,Wen Deng,Yu He,Xiaozhuo Ba,Zichen Zhong,Yongke Bai,Tao Ye,Xiaoqi Yang,Kehua Jiang,Yijing Liu,Kun Tang
Limited lymphocyte infiltration and insufficient tumor immunogenicity remain major challenges for effective immunotherapy in bladder cancer, particularly in immunologically “cold” tumors with a highly suppressive immune microenvironment. Effective activation of the innate immune system is critical for initiating a robust adaptive anti-tumor immune response, primarily mediated by dendritic cells (DCs). Here, we designed genetically engineered hybrid membrane-coated nanoparticles (HM-MPS NPs) with excellent photothermal stability, tumor-targeting capability, and biocompatibility. HM-MPS NPs demonstrated significant tumor-suppressive effects in multiple preclinical models, including murine subcutaneous, orthotopic, and distant bladder tumor models. By combining photothermal therapy (PTT), a STING agonist (SR717), and antigen presentation, HM-MPS NPs achieve triple activation of DCs, leading to enhanced T-cell activation and a remodeled immune microenvironment. Furthermore, HM-MPS NPs synergize effectively with anti-PD-1 therapy, amplifying immunogenic cell death (ICD) and overcoming immune suppression within the tumor microenvironment. This strategy significantly boosts tumor immunogenicity and enhances anti-tumor immune responses, offering a promising approach for bladder cancer treatment.
研究领域:
肿瘤学
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免疫学
·
纳米医学
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高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Xinjun He,Mengqiao Gao,Fukun Li,Zhiyang Tang,Jie Qu,Jinxing Long,Qiang Zeng,Xuehui Li
Catalytic hydrogenolysis of lignin has attracted steady attentions in regard of producing high-value aromatic chemicals from the renewable resource and achieving the “carbon neutrality” goal. However, current techniques for lignin hydrogenolysis are highly challengeable due to the necessity of pure H2 and relatively low yields in monomers. In this work, a novel and efficient approach has been proposed for the conversion of lignin to monophenols under readily available and cost-effective syngas. The results demonstrated that CO has the dramatic promotion on the bagasse lignin hydrogenolysis over commercialized Pd/C at 230 °C for 4 h, the yield of monophenols reaches 357.2 mg/g at 3.0 MPa syngas (CO/H2=2/1), which is approximately 1.7 times of that under pure H2. As evidenced by quantitative 31P NMR analysis, the promoting effects of CO on lignin depolymerization are positively correlated with the content of side-chain hydroxyl groups in lignin. Further investigations on lignin model conversion reveal that CO suppresses the dehydroxylation at Cα-OH, with concomitant enhancement of Cβ-O bond cleavage (increasing from 10% in H₂ to 64% in syngas). This inhibitory effect on side-chain hydroxyls elimination directly correlates with the 1.7-fold increase of monophenol yields observed during catalytic depolymerization. Therefore, this work provides a new insight in lignin depolymerization using industrial catalyst of Pd/C and the cost-effective syngas.
研究领域:
化学工程
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可再生能源
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催化
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生物质转化
·
绿色化学
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高影响因子
JOURNAL OF CHEMICAL RESEARCH
·
2011
·
IF 0.55
Yong-Rui Pi,Jun Tan,Hui Liu,Jie Chen,Zhu-You Qun,Yan-Bo Zeng,Lei Li
Catalytic cracking reaction of 1,2-dimethyl-1,1,2,2-tetrachlorodisilane with a halobenzene (PhCl, PhBr) to prepare methylphenyldichlorosilane has been investigated. Pd(PPh3)4 exhibited the best catalytic activity among the catalysts used. The activity of chlorobenzene was significantly lower than that of bromobenzene. With the latter and toluene as solvent, in the presence of 0.3 mol % Pd(PPh3)4, the conversion of disilane was 100% with a selectivity to MePhSiCl2 of 97.1%.
研究领域:
有机化学
·
催化化学
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DOI
高影响因子
HYDROMETALLURGY
·
2023
·
IF 4.7
Shaoping Feng,Kun Huang
Dialkylsulfide is considered as the most promising extractant for separating Pd(II) and Pt(IV) in industrial processes. However, the slow kinetics for Pd(II) extraction limits its extensive application. The development of new extractants with faster kinetics, high extraction efficiency, and exceptional Pd(II) separation selectivity has been a persisting goal over the past few decades. In this study, a new functionalized extractant, 1-methyl-2-(nonylthio)-1H-imidazole (MNI) containing both N and S atoms, was synthesized and employed to separate Pd(II) from mixed hydrochloric acid solutions with different initial Pd(II)/Pt(IV) concentration ratios. Experimental results revealed that MNI not only has a high selectivity for Pd(II) over Pt(IV) but also has faster kinetics for Pd(II) extraction than diisopentylsulfide (S201) under similar extraction conditions. In contrast to traditional dialkylsulfide extractants, MNI coordinates with Pd(II) ions via the N(5) atom in its imidazole ring to form Pd(MNI) 2 Cl 2 complexes, instead of using the S atom as with dialkylsulfide. The extraction mechanism involving the coordination between Pd(II) and MNI was demonstrated using the slope analysis method and ultraviolet (UV), Fourier-transform infrared (FT-IR), 1 H NMR, and 13 C NMR spectroscopic methods. The fast extraction kinetics between MNI and Pd(II) was possibly attributed to the high charge density of the N(5) atom in the imidazole ring, whereas the outstanding separation selectivity for Pd(II) was due to the strong affinity of the N(5) atom. The facile synthesis, high saturation capacity, excellent Pd(II) selectivity, and remarkable reusability endow MNI with potential applications in Pd(II) recovery from leach solutions of waste automotive catalysts and other secondary resources.
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高影响因子
JOURNAL OF ORAL PATHOLOGY & MEDICINE
·
2021
·Vol. 51
·期 1
·74-85
·
IF 4.253
Jing-Ya Yang,Fang Wang,Gang Zhou
Background Oral lichen planus (OLP) is a T-cell-mediated chronic inflammatory disease with uncertain aetiology. Mucosal-associated invariant T (MAIT) cells and γδT cells are unconventional, innate-like T cells with immunoregulatory capacity. This study aimed to investigate the potential effects of MAIT and γδT cells on the pathogenesis of OLP. Methods Circulating MAIT cells and γδT cells were identified using flow cytometry. Surface proteins including CD4, CD8, CD69, CD103, CD49d, programmed death-1 (PD-1) and its ligand PD-L1 were assessed. Cytokines containing interleukin (IL)-4, IL-17, interferon (IFN)-γ, granzyme B and tumour necrosis factor (TNF)-α released by MAIT and γδT cells were measured following PMA and ionomycin stimulation. Results Circulating MAIT and γδT cells were deficient in OLP. The percentage of CD4 + , CD69 + , CD103 + and PD-1 + MAIT cells was increased in OLP, while that of CD8 + and CD49d + MAIT cells was decreased. The percentage of CD103 + , PD-1 + and PD-L1 + γδT cells was upregulated in OLP. Both the MAIT and γδT cells in OLP produced less IL-4 than controls. The granzyme B-producing MAIT cells were increased, while γδT cells secreting granzyme B and TNF-α were reduced in OLP. IL-17 and IFN-γ in OLP MAIT and γδT cells were not significantly different from that in controls. The frequency of OLP MAIT cells and the MAIT/γδT rate were positively associated with the disease severity. Conclusion The deficient MAIT and γδT cells expressing functional proteins and releasing cytokines may play an immunoregulatory role in the pathogenesis of OLP.
研究领域:
免疫学
·
炎症
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口腔疾病
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细胞生物学
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DOI
PubMed
高影响因子
Applied Sciences-Basel
·
2019
·Vol. 9
·期 9
·1792
·
IF 2.217
Anqiu Liu,Xiaochen Wang,Daming Gao,Le Wang,Junjie Cheng,An Wang,Zehui Zhang
Chemoselective hydrogenation of aldehydes with heterogeneous catalysts under mild conditions is of great importance but remains a major challenge. Herein, an efficient strategy was developed for low temperature chemoselective hydrogenation of aldehydes with broad substrate scope over a magnetic material supported palladium catalyst (γ-Fe2O3@HAP-Pd). Aldehydes bearing various reducible functional groups readily underwent hydrogenation to give the corresponding primary alcohols with moderate to excellent yield at room temperature in aqueous solutions. The Hammett equation revealed that the hydrogenation of aromatic aldehydes proceeded via an anionic intermediate. Additionally, when the temperature increased to 70 °C, toluene was obtained by the deoxygenation of benzaldehyde in excellent yield. Furthermore, the γ-Fe2O3@HAP-Pd could be recycled up to six times without loss of activity and metal leaching.Keywords:selective hydrogenation;aldehydes;Pd catalysts;mild conditions
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2018
·
IF 4.841
Chanjuan Liao,Xixi Liu,Yongshen Ren,Daoxin Gong,Zehui Zhang
A sustainable method was developed for the upgrade of biomass derived vanillin (a typical model compound of lignin) into the potential liquid biofuels over a layered double hydroxide supported Pd catalyst (abbreviated as CoAl–LDH/Pd). The CoAl–LDH/Pd catalyst showed high catalytic activity towards the hydrodeoxygenation of vanillin into 2-methoxy-4-methylphenol (MMP) under mild conditions in aqueous media. High MMP yield up to 86% was produced at 120 °C after 4 h. Kinetic studies revealed that the rate-determining step for the hydrodeoxygenation of vanillin was the hydrogenolysis of vanillyl alcohol. More importantly, the CoAl–LDH/Pd catalyst was highly stable without the loss of activity.
研究领域:
催化化学
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生物质能
·
绿色化学
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 46
·20367-20374
·
IF 3.288
Dan Zhang,Bowei Wang,Lijuan Yan,Ruixiao Gao,Lu Liu,Ziyi Xia,Xilong Yan,Yang Li,Ligong Chen
Synthesis of an easily separable and efficient catalyst is of great significance for selective hydrogenation of unsaturated functional groups. In this work, novel magnetic flower-like carbonaceous Pd catalysts are constructed for the selective reduction of the CC bond. According to the characterization results, a flower-like architecture is observed in the catalysts containing both Fe3O4 and Pd NPs, which is constructed by the secondary self-assembly in the preparation process due to the interaction between Pd and magnetic nitrogen-doped graphene (Fe3O4-NG). More flower-like structures are formed by increasing the Pd loading amount, further enhancing the specific surface area of the catalyst. The specific surface area of Pd-FONG-3 is the highest (521.17 m2 g−1). Combining the results of characterization and experiments, it is found that the catalytic activity is positively related to the flower-like architecture and the interaction between Pd NPs (6.0 nm) and Fe3O4 NPs (6.7 nm). Fe3O4 is not only beneficial to the magnetic recovery of the catalyst, but also acts as a cocatalyst, which can significantly improve the reactant conversion. Moreover, N species play an important role in protecting the CO bond, resulting in the selective hydrogenation of the CC group. Herein, Pd-FONG-3 exhibits excellent activity in the selective hydrogenation of cinnamaldehyde (CAL) with 99.5% conversion and 96.5% hydrocinnamaldehyde (HCAL) selectivity, and its catalytic performance is much better than that of the commercial 5% Pd/C catalyst (100% conversion and 69.1% HCAL selectivity). This work provides a new strategy to construct highly active catalysts with magnetic recovery properties for selective hydrogenation of CC bonds, and Pd-FONG-3 shows tremendous application foreground.
研究领域:
催化化学
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材料科学
·
纳米技术
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高影响因子
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