PHARMACOLOGICAL RESEARCH
·
2022
·
IF 10.334
Qing Li,Meng-Sheng Deng,Ren-Tao Wang,Hao Luo,Yuan-Yuan Luo,Dong-Dong Zhang,Kui-Jun Chen,Xiao-Fu Cao,Guang-Ming Yang,Tie-Mei Zhao,Bo Xu,Cheng-Xiong Xu,Jian-Min Wang
Idiopathic pulmonary fibrosis (IPF) is a progressive disease with high mortality and limited therapeutic options. The immune checkpoint PD1/PD-L1 axis is related to the pathogenesis of pulmonary fibrosis, and upregulated expression levels of PD-L1 have been demonstrated in IPF patients. However, the mechanism of PD-L1 in pulmonary fibrosis is not fully understood. Here, we demonstrated upregulated expression of PD-L1 in fibrotic lung tissues and sera of IPF patients. Bleomycin (BLM) treatment induced PD-L1 upregulation, EMT (Epithelial-Mesenchymal Transition) and fibrosis-like morphology changes in human pulmonary alveolar epithelial cells (HPAEpiCs). Silencing PD-L1 attenuated BLM-induced EMT and fibrosis-like morphology changes in HPAEpiCs. In addition, we identified that PD-L1 directly binds to vimentin and inhibits vimentin ubiquitination, thereby increasing vimentin levels in HPAEpiCs. Silencing of vimentin inhibited BLM- and PD-L1-induced fibrosis in HPAEpiCs. The correlation between PD-L1 and EMT or vimentin expression was further confirmed in clinical samples and animal models. Finally, we used BLM- and paraquat-induced pulmonary fibrosis animal models to confirm the anti-pulmonary fibrosis effects of PD-L1 silencing. Taken together, our findings suggest that upregulated PD-L1 stimulates EMT of alveolar epithelial cells by increasing vimentin levels by inhibiting vimentin ubiquitination, thereby contributing to pulmonary fibrosis.
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高影响因子
Small Methods
·
2022
·Vol. 7
·期 1
·2201225
·
IF 15.367
Zemeng Dong,Qiyan Sun,Guang-Rui Xu,Zexing Wu,Yanyan Li,Jianping Lai,Guangjiu Li,Lei Wang
The electrocatalytic nitrogen reduction reaction (NRR) is emerging as a great promise for ambient and sustainable NH 3 production while it still suffers from the high adsorption energy of N 2 , the difficulty of *NN protonation, and inevitable hydrogen evolution, leading to a great challenge for efficient NRR. Herein, we synthesized a series of amorphous trimetal Pd-based (PdCoM (M = Cu, Ag, Fe, Mo)) nanosheets (NSs) with an ultrathin 2D structure, which shows high efficiency and robust electrocatalytic nitrogen fixation. Among them, amorphous PdCoCu NSs exhibit excellent NRR activity at low overpotentials with an NH 3 yield of 60.68 µg h −1 mg cat −1 and a corresponding Faraday efficiency of 42.93% at −0.05 V versus reversible hydrogen electrode as well as outstanding stability with only 5% decrease after a long test period of 40 h at room temperature. The superior NRR activity and robust stability should be attributed to the large specific surface area, abundant active sites as well as structural engineering and electronic effect that boosts up the Pd 4d band center, which further efficiently restrains the hydrogen evolution. This work offers an opportunity for more energy conversion devices through the novel strategy for designing active and stable catalysts.
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FUEL
·
2022
·
IF 8.035
Hua Yan,Xiaowei Liu,Junhong Zhou,Dawei Li,Xiaoye Yang,Yiming Gu,Hongjiu Su,Shudong Wang
The development of anthraquinone (AQ) hydrogenation catalysts with high activity and selectivity remains a challenge, but it is critical in industrial applications from both economic and environmental perspectives. In this work, an amine-modified catalyst, i.e., Pd/A/SiO 2 , was designed and synthesized via grafting 3-aminopropyltrimethoxysilane (APTMS) onto silica support and then loading Pd via the Shiff-base reaction. Multiple techniques were used to thoroughly characterize and analyze the catalysts' structural and electronic properties, such as transmission electron microscopy (TEM), H 2 temperature-programmed reduction (H 2 -TPR), and X-ray photoelectron spectroscopy (XPS), etc. The Pd particle size (3.86 nm) in Pd/A/SiO 2 was found to be very close to the reported optimal value, which balances well between the number of active sites and the required size for AQ adsorption; also, the residual carbon species from APTMS improves the hydrophobic properties of the support, which benefits AQ adsorption and anthrahydroquinone (AQH 2 ) desorption; and furthermore, the electron transferred from N to Pd increases the electron density of the latter, favoring the activation of the C O bond in AQ. These factors combine to give a very superior performance of Pd/A/SiO 2 for AQ hydrogenation, including a hydrogenation efficiency as high as 15.7 g/L with an intriguing selectivity of 96.1 %, and a good reusability merit within a six-run test, all of which are among the best results reported so far. This work, we believe, provides food for thought in the development of a highly efficient catalyst for AQ hydrogenation.
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NANOTECHNOLOGY
·
2023
·Vol. 34
·期 46
·465404
·
IF 3.5
Penghui Bai,Kai Lei,Juan Xie,Hu Wang,Xiaolan Kang,Xia Wang
This paper investigates the impact of Pd/Ni modification on the photocatalytic hydrogen production performance of SrTiO3 (STO). STO catalysts were synthesized using a hydrothermal method, and Pd/Ni modification was applied on the surface of STO through chemical deposition. Experimental results demonstrate that the hydrogen evolution rate of Pd/Ni-modified STO (Pd/Ni-STO) reaches 2232.14 μmol g−1 h−1. X-ray absorption fine structure spectroscopy analysis reveals substitutional doping of Ni with Ti and coordination of Pd with surface O. X-ray photoelectron spectroscopy analysis indicates the introduction of oxygen vacancies due to Pd/Ni doping. Density functional theory calculations suggest that Ni doping activates neighboring Ti atoms, leading to the formation of bimetallic catalytic sites composed of oxygen vacancies and Ti atoms, greatly enhancing the photocatalytic hydrogen evolution performance. This study not only provides an effective catalyst for photocatalytic applications but also offers insights into the underlying mechanism, which may stimulate the development of metal-doped catalytic materials and have implications for a range of other applications.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2022
·Vol. 23
·期 22
·14072
·
IF 6.208
Shiyue Chen,Yujun Yang,Mingjun Zhang,Xiaohong Ma,Xiaoxiao He,Teng Wang,Xi Hu,Xiang Mao
Dye degradation is a key reaction in organic decomposition production through electron donor transferring. Palladium (Pd) is the best-known element for synthesis Pd-based catalyst, the surface status determines the scope of relative applications. Here we first prepare Pd-Cu alloy nanoparticles (NPs) by co-reduction of Cu(acac)2(acac = acetylacetonate) and Pd(C5HF6O2)2in the presence of sodium borohydride (NaBH4) and glutathione (GSH). The obtained Pd-Cu is about ~10 nm with super-hydrophilicity in aqueous mediums. The structural analysis clearly demonstrated the uniform distribution of Pd and Cu element. The colloidal solution keeps stability even during 30 days. Bimetallic Pd-Cu NPs shows biocompatibility in form of cell lines (IMEF, HACAT, and 239 T) exposed to colloidal solution (50 µg mL−1) for 2 days. It shows the catalytic multi-performance for dye degradation such as methyl orange (MO), rhodamine B (RhB), and methylene blue (MB), respectively. The as-synthesized nanoparticles showed one of the best multiple catalytic activities in the industrially important (electro)-catalytic reduction of 4-nitrophenol (4-NP) to corresponding amines with noticeable reduced reaction time and increased rate constant without the use of any large area support. In addition, it exhibits peroxidase-like activity in the 3, 3′, 5, 5′-Tetramethylbenzidine (TMB) color test and exhibit obvious difference with previous individual metal materials. By treated with high intensity focused ultrasound filed (HIFU), Pd-Cu NPs might be recrystallized and decreased the diameters than before. The enhancement in catalytic performance is observed obviously. This work expedites rational design and synthesis of the high-hierarchy alloy catalyst for biological and environment-friendly agents.Keywords:Pd-Cu NPs;hydrophilic;biocompatibility;catalytic agent;dye degradation
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Xuan Tang,Ming Wang,Bingjing Tang,Yunkun Zhao,Wangcheng Zhan,Yanglong Guo,Li Wang,Sheng Dai,Yun Guo
Realizing the potential benefits of nanoscale metal catalysts requires highly dispersed active sites and control of their local environment. Herein, we develop a catalyst synthesis route for manipulating the local environment of highly dispersed metal-active sites via the targeted deposition of Pd near highly dispersed ZrOx on ZSM-5 zeolite using electrostatic interactions. The formed heteroatom Pd-ZrOx in zeolite catalysts is characterized by scanning transmission electron microscopy (STEM), in situ infrared spectroscopy, temperature-programmed desorption (TPD) of O2, and temperature-programmed surface reaction (TPSR) of CH4. The combination of diverse characterization results demonstrates the heteroatom Pd-ZrOx species rendering a higher dispersion and lower oxygen coordination of Pd species, appropriately tuning the strength of Pd–O bonds, and providing abundant active oxygen species to accelerate the dissociation of CH4. Therefore, the catalytic performance of Pd species is effectively enhanced with the lowest temperature of 90% CH4 conversion decreasing from 390 °C (without ZrOx) to 340 °C. Our work provides a strategy of engineering to anchor highly dispersed noble metal species and regulate the local environment to tune catalytic properties.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2021
·Vol. 22
·期 24
·13314
·
IF 5.924
Feng Guo,Junfeng Ke,Zhengdong Fu,Wenzhao Han,Liping Wang
Cell penetrating peptides (CPPs) are peptides that can directly adapt to cell membranes and then permeate into cells. CPPs are usually covalently linked to the surface of nanocarriers to endow their permeability to the whole system. However, hybrids with lipids or polymers make the metabolism much more sophisticated and even more difficult to determine. In this study, we present a continuous sequence of 18 amino acids (FFAARTMIWY(d-P)GAWYKRI). It forms nanospheres around 170 nm, which increase slightly after loading with siRNA and DOX. Notably, it can be internalized by cancer cells mainly through electronic interactions and PD-L1-mediated endocytosis. Compared with poly-l-lysine and polyethyleneimine, it has a much higher efficiency (about four times) of gene transduction while lowering toxicity. In the treatment of cancer, it causes apoptosis (21%) and inhibits the expression of SURVIVIN protein in vitro. In vivo, it shows good biocompatibility as there are no changes in mice’s body weight. When administering peptide-siRNA-DOX, tumor growth is inhibited the most (about three times). These results above prove the sequence to be a good candidate for gene therapy and drug delivery.Keywords:peptide;self-assembly;gene therapy;PD-L1
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Haiping Li,Xue Wang,Yanan Liu,Yufei He,Junting Feng,Dianqing Li
The catalytic upgrading of phenolic derivatives is vital for the efficient utilization of biomass resources. Herein, we construct a reductive layered double oxide material (CoAlCe-LDO) with the Ce–Co interface and abundant oxygen vacancy (VO) via heat-treating layered double hydroxide (LDH) precursors. The support spontaneous in situ redox method is employed to prepare the supported catalyst using CoAlCe-LDO as a support and reductant. Interestingly, highly dispersed Pd nanoparticles prefer to distribute at the contact edge of the Ce–Co interface. Pd2+ is successfully reduced to Pd0 by the reductive Co/Ce sites. Due to the redox reaction between the support and Pd species, a strong metal–support interaction is introduced. The Pd/CoAlCe-LDO catalyst shows high activity for phenol hydrogenation under mild conditions and a low molar ratio of Pd to phenol. The kinetic study suggests that the highly dispersed Pd sites could preferably activate H2 molecules, thereby boosting the rapid phenol hydrogenation.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Xiaoting Deng,Min Lao,Haikun Zhou,Jingwen Huang,Shihui Li,Yili Liang,Shaofeng Yin,Zhiyong Xie
The development of efficient catalysts for proton exchange membrane fuel cells (PEMFCs) is crucial for their commercial viability. This study introduces a method for synthesizing Pd nanoparticles on carbon supports as electrocatalysts using microbial synthesis, specifically employing the bacterium Shewanella oneidensis MR-1. The so-produced catalysts exhibit enhanced catalytic activity and stability for the oxygen reduction reaction (ORR). The microbial synthesis approach offers advantages, such as high purity, cost-effectiveness, and environmental friendliness. Additionally, the use of sodium alginate (SA) hydrogel in the synthesis process further improves the catalyst’s performance due to its metal chelating properties. The resulting Pd/C electrocatalysts, especially those synthesized with a composite matrix of SA and CaCO3, demonstrate superior ORR performances outperforming that of commercial Pd/C catalysts. It was found that the composite substrate affected the palladium recovery rate, whose increasing palladium absorption, refined particle size, improved graphitization degree, and increasing pyridinic-N of the resultant catalyst synergistically enhanced the availability of active centers that eventually contributed to the superior ORR performances. This research paves the way for the development of high-performance and cost-effective catalysts for PEMFCs.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2023
·
IF 3.9
Xuejiao Wang,Guangguang Pi,Jianye Yang,Kai Wu,Yanshuo Li,Wei Fang
Developing a highly active and stable electrode with a controllable size is greatly demanded to satisfy the large-scale application of electrochemical hydrogen production via water splitting. To overcome this challenge, a novel binder-free membrane electrode comprising Pd anchored on ZIF-62 glass supported on a porous TiC substrate has been developed to catalyze the hydrogen evolution reaction (HER) in both acidic and alkaline conditions. The optimal Pd@ZIF-62/TiC membrane electrode only requires a stable overpotential of ∼90 mV to reach a current density of 30 mA cm −2 within 20 h of operation. The outstanding HER performance of such electrode can be ascribed to its unique porous membrane structure, which accelerates the mass transfer kinetics of electrolyte ions and in situ generated hydrogen bubbles. As the Pd decorated molten ZIF-62 glass penetrated heavily into the TiC support pores, a very strong adhesion between Pd@ZIF-62 electrocatalytic layer and TiC substrate could be formed, which lowers the interfacial resistance between the catalyst and its substrate as well as promotes the charge transfer kinetics of HER electrode.
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Molecular Catalysis
·
2021
·
IF 5.062
Yue Zhang,Zhiyong Pan,Nan Wang,Li Wang
Silica SBA-15 without removal of template P123 was calcined in an inert atmosphere and the carbon-modified SBA-15 thus obtained was used as the support of Pd catalyst for the hydrogenation of 2-ethylanthraquinone (EAQ). The effects of extraction times of P123 in SBA-15 with water prior to inert calcination and calcination temperature on the structure and catalytic performance of Pd catalyst were studied. The results of elemental analysis, X-ray diffraction, X-ray photoelectron spectroscopy, inductively coupled plasma, Fourier transform infrared spectroscopy, Raman spectra, water contact angle measurement, N 2 adsorption-desorption, transmission electron microscopy and energy dispersive X-ray mapping showed that carbon content of catalysts varied in the range of 3.4 % and 1.1 % with increasing extraction times from 0 to 6 due to the decrease in the residual amount of P123 in uncalcined SBA-15. With rising calcination temperature, the occurrence state of carbon in catalysts was converted from amorphism into graphite. The Pd catalyst supported on SBA-15 extracted for 3 times and calcined at 650 °C had 2.0 % carbon, and exhibited the highest activity (0.37 molH 2 ·gPd −1 ·min −1 ) and selectivity (98.9 %). This is due to the presence of appropriate amount of carbon, which provided a relatively high hydrophobicity without significantly reducing the specific surface area and pore size of SBA-15 support. The high hydrophobicity benefits the adsorption of EAQ from the working solution to the surface of catalyst.
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高影响因子
CRYSTENGCOMM
·
2021
·Vol. 23
·期 15
·2897-2904
·
IF 3.545
Beixi An,Yibing Luo,Jinglong Bai,Yanrong Wang,Xu Cheng,Jianpeng Li,Qiao Wang,Yifan Yang,Erqing Xie
In this study, we used a hydrothermal method to prepare WO3 nanospheres doped with a bimetal of Pd and Ni and used them in hydrogen sensing. The results show that the bimetal-doped WO3 nanospheres have a higher response, faster response/recovery time, and better selectivity than single metal-doped WO3. Moreover, they still have a high response to hydrogen at a low concentration. With 5 ppb of hydrogen, the sensor's response can reach 1.5, which is 1.5 times greater than that of pure WO3. Furthermore, the bimetal-doped WO3 has a shorter response time (14 s) and recovery time (8 s). This superior performance of the Pd/Ni-doped WO3 to hydrogen is most probably because of the strong adsorption of hydrogen, which results from the synergistic effect of two metals.
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