Frontiers in Chemistry
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2022
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IF 5.545
Zhao Jinchong,Jiang Jie,Wen Song,Zhang Jing,Zhang Changsheng,Sheng Nan,Liang Wei,Sun Bing,Xu Wei,Yang Zhe,Pan Yuan
A series of alkali metal (Li, Na, and K)-modified Pd catalysts and Pd/Al2O3 were prepared and used to remove oxygen in a propylene flow with hydrogen’s existence. The results showed that the alkali metals could enhance the performance of the Pd catalysts and the effect followed the order of K > Na > Li. X-Ray diffraction (XRD), N2-physisorption, transmission electron microscopy (TEM), hydrogen temperature programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS) were carried out to investigate the alkali metal-modified Pd catalysts and the promotional effect mechanism was explained. The results showed that alkali metal modification increased the electron density of Pd atoms to induce the negatively charged Pd species, which could enhance the adsorption of oxygen while weakening the adsorption of propylene, and then enhance the performance of the modified catalysts for oxygen removal from unsaturated hydrocarbon. The Pd-K/A catalyst performed the best on both oxygen removal and propylene hydrogenation inhibition.
研究领域:
催化化学
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材料科学
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DOI
PubMed
高影响因子
CATALYSIS LETTERS
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2024
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IF 2.3
Zhao Chunzhi,Mao Dongsen,Meng Tao,Guo Qiangsheng,Yu Jun
Owing to the intrinsic nature of the uniformed topologies and ultrasmall Zr 6 nodes of Zr-MOFs, herein, we employed Zr-MOFs (UiO-66 and UiO-67), as opposed to the support of traditional ZrO 2 , to prepare the Pd catalysts for toluene degradation. Compared with the catalysts of Pd/UiO-66 and Pd/ZrO 2 , Pd/UiO-67 catalyst boosted an excellence catalytic performance for toluene degradation, giving the lowest T 90% value of 235 °C with long-term stability. With the assisting of the cavity confinement of Zr-MOFs, Pd nanoparticles are prone to be encapsulated in the 3D frameworks of Zr-MOFs, and the bigger micropores of UiO-67 are more conducive to the formation of larger Pd nanoparticles. The in situ FT-IR results further declared that although the active sites are partly sacrificed due to the larger Pd nanoparticles formed in UiO-67, the stable adsorbed toluene on Pd/UiO-67 boosted the quick degradation of toluene in the reaction interval even without undergoing intermediate processes of benzoate and benzaldehyde. Graphical Abstract UiO-66, UiO-67 and ZrO 2 were employed to prepare the Pd catalysts for toluene degradation, Pd/UiO-67 catalyst boosted an excellence catalytic performance with long-term stability.
研究领域:
催化化学
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环境科学
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材料科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Dongyue Zhao,Zhongnan Gao,Hui Xian,Lingli Xing,Yuexi Yang,Ye Tian,Tong Ding,Zheng Jiang,Jing Zhang,Lirong Zheng,Xingang Li
Herein, we report the function of Pd species in the Pd-added La0.7Sr0.3CoO3 perovskite for removal of NOx (NO+NO2) in the lean-burn NOx traps (LNT) process. The addition of Pd significantly improves the De-NOx activity of the perovskite-based catalysts. The Pd-supported catalyst has an excellent NOx removal efficiency of 90.4%, which is higher than the Pd-doped catalyst (74.4%) and pure La0.7Sr0.3CoO3 (51.6%). Our results show that the addition of Pd species enhances both the NOx desorption behaviors to regenerate the NOx storage sites and NOx reduction ability of the catalysts in the fuel-rich period, which induces the improved NOx trapping performance in the followed lean-burn period. These achievements result in the enhanced De-NOx activity of the Pd-added catalyst in the alternative NOx storage and reduction operations. Compared with the Pd-doped catalyst, the Pd-supported catalyst possesses the higher utilization efficiency of the Pd, thus exhibiting a higher catalytic activity.
研究领域:
化学
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环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF CONTROLLED RELEASE
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2023
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IF 10.8
Tiantian Liu,Zehang Zhou,Mengxing Zhang,Puxin Lang,Jing Li,Zhenmi Liu,Zhirong Zhang,Lin Li,Ling Zhang
The cuproptosis cell death pathway brings fresh opportunities for tumor therapy. However, efficient and targeted cuproptosis induction in tumors is still a challenge. Unfortunately, the well-known cuproptosis initiator, disulfiram and copper complex (DSF/Cu 2+ ), also increases PD-L1 level in tumors, which may diminish the final therapeutic outcome. In this study, DSF/Cu 2+ -loading MXene nanosheets are coated with PD-1 overexpressing T cell membrane to generate CuX-P system. CuX-P could recognize and stick to PD-L1 on tumor cells like a patch, which promotes the endocytosis of both CuX-P and PD-L1 by tumor cells. Following internalization and release of DSF/Cu 2+ in the cytoplasm, PD-L1 expression is upregulated. However, due to the presence of CuX-P in the tumor microenvironment , the then supplemented PD-L1 on tumor surface again binds CuX-P for internalization. This feedback loop keeps blocking and consuming the PD-L1 on tumor surface and promotes the enrichment of CuX-P in tumors to induce cuproptosis. After CuX-P treatment with laser irradiation, strong anti-tumor immune responses are stimulated in a mouse model with triple-negative breast cancer. Thus, this study develops a tumor-targeted biomimetic system that offers simultaneous cuproptosis killing, photothermal therapy (PTT) and immunotherapy in mice.
研究领域:
肿瘤学
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免疫治疗
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纳米技术
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癌症生物学
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
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2021
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IF 13.084
Zhongjie Cai,Meng Huang,Jiajun Dai,Guowu Zhan,Fu-li Sun,Gui-Lin Zhuang,Yiying Wang,Pan Tian,Bin Chen,Shafqat Ullah,Jiale Huang,Qingbiao Li
Methanol synthesis from CO2 hydrogenation with H2 produced from renewable energy has emerged as a promising method for carbon neutrality. The supported Pd/In2O3 catalyst has attracted great attention due to its superior activity and methanol selectivity, but the formation of the In–Pd bimetallic phase upon over-reduction would lead to quick catalyst deactivation. In this work, we elucidate the reduction behavior of Pd/In2O3 catalysts by using TCPP(Pd)@MIL-68(In) as precursors. During catalyst fabrication, metalloporphyrins (viz., TCPP(Pd)) served as both a capping agent for the growth of MIL-68(In) and a shuttle for transporting the Pd2+, which enhanced the dispersion of Pd0 species on In2O3–x during the calcination and reduction treatments and prevented the formation of In–Pd bimetallic phase by over-reduction. With a low Pd loading of 0.53 wt %, the resultant Pd/In2O3 catalyst exhibited a maximum methanol space–time yield of 81.1 gMeOH h–1 gPd–1 with a CO2 conversion of 8.0% and a methanol selectivity of 81% over 50 h on stream (295 °C, 3.0 MPa, 19,200 mL gcat–1 h–1). In contrast, the comparative Pd/In2O3 catalyst prepared by the impregnation of PdCl2 in MIL-68(In) showed poor activity and stability due to the formation of InPd/In2O3–x surface structures. In addition, we found a strong connection between the reduced degree of In2O3 and the catalytic performance of the supported Pd/In2O3 catalysts by integrating catalyst characterization results with density functional theory (DFT) calculations. Interestingly, the surface In/O ratio detected by XPS can reflect information about both metal–support interaction and the amount of oxygen vacancy, which is highly related to the catalytic activity. The DFT calculation also shows that the Pd/In2O3 catalyst has excellent thermodynamic selectivity for the CH3OH product. This work provides an alternative synthetic strategy for Pd/In2O3 nanocatalysts and sheds light on the deactivation mechanism of the supported catalysts.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
MOLECULES
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2024
·Vol. 29
·期 16
·3843
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IF 4.2
Xinbao Li,Kai Sun,Ying Chen,Ye Yuan
As a widely used support, TiO2has often been combined with Pd to form highly sensitive gas-chromic materials. Herein, we prepared a series of Pd/TiO2catalysts with different Pd content (from 0.1 to 5 wt.%) by the impregnation method for their utilization in fast room-temperature CO detection. The detection was simply based on visible color change when the Pd/TiO2was exposed to CO. The sample with 1 wt.% Pd/TiO2presented an excellent CO gasochromic character, associated with a maximum chromatic aberration value of 90 before and after CO exposure. Systematic catalyst characterizations of XPS, FT-IR, CO-TPD, and N2adsorption–desorption and density functional theory calculations for the CO adsorption and charge transfer over the Pd and PdO surfaces were further carried out. It was found that the interaction between CO and the Pd surface was strong, associated with a large adsorption energy of −1.99 eV and charge transfer of 0.196e. The color change was caused by a reduction in Pd2+to metallic Pd0over the Pd/TiO2surface after CO exposure.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
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2024
·Vol. 130
·期 10
·1-12
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IF 2.5
Tang Mingxin,Qin Cong,Sun Xueya,Li Mengwei,Wang Yihui,Cao Jianliang,Wang Yan
Hydrogen (H 2 ) energy, as a clean energy source, has high energy density and durability, while H 2 is flammable and explosive, which requires strict safety technology measures to ensure the safety of high-pressure storage transportation. Therefore, the development of sensitive sensors is needed. In this study, In 2 O 3 microspheres with different Pd loadings were fabricated by hydrothermal method. Compared with the pristine In 2 O 3 gas sensor, the optimal operating temperature of the In 2 O 3 sensor is reduced from 160 ℃ to 80 ℃ after loading Pd. Among the prepared Pd/In 2 O 3 gas sensors, the response value of the 2 at% Pd/In 2 O 3 sensor towards 1000 ppm H 2 is 50.743 at 80 ℃. The response/recovery time is 80 s/235 s. The improved H 2 sensing performance can be ascribed to the chemical and electron sensitization of Pd, and the formation of PdO, PdH x . This study shows that Pd-loaded In 2 O 3 can effectively reduce the optimal operating temperature and enhance the response value for detecting H 2 in the range of 5-5000 ppm. Therefore, this sensor has good application prospects for detecting H 2 at low temperatures.
研究领域:
材料科学
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传感器技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
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IF 6.216
Guofu Huang,Mianmian Wang,Yongyou Hu,Jianhua Cheng,Sihao Lv,Kui Yang
As a typical congener of Polybrominated diphenyl ethers (PBDEs), 2,2′,4,4′-tetrabromodiphenyl ether (BDE47) has attracted more and more attention due to its high biological toxicity and environmental abundance. In this study, a novel polyanionic cellulose stabilized Pd/Fe (PAC-Pd/Fe) nanoparticle was successfully synthesized for BDE47 degradation under ambient condition. Batch experiments showed that BDE47 degradation followed pseudo first-order kinetic model. Pd loading played a crucial role as it affected the formation of activated hydrogen species H ∗ and accelerated electron transfer. At Pd loading of 0.3 wt%, nearly 100% BDE47 was degraded completely within 10 min by 0.4 g L −1 PAC-Pd/Fe nanoparticles. When compared with strong acidic (pH 3) and alkaline (pH 9 and 11) conditions, weak acidic condition (pH 5) was more favorable for BDE47 degradation, with nearly 100% BDE47 was removed within 7.5 min. In the presence of HA inhibited the degradation of BDE47, and the degradation efficiencies within 15 min decreased from 100%, 88.6%, 79.5% to 73.1% as HA concentration increased from 0, 10, 40 to 70 mg L −1 . The degradation of BDE47 by PAC-Pd/Fe nanoparticles was a reductive debromination process, and a stepwise debromination from n-Br to (n-1)-Br BDEs was the dominant reaction, in which the para -Br was more susceptible to remove than ortho -Br. This study suggests PAC-Pd/Fe nanoparticle can be utilized as a promising remediation technology for PBDEs contaminated wastewater.
研究领域:
环境科学
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污染治理
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2024
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IF 2.3
Liu Hang,Liu Sixu,Liang Yaozhen,Sun Yifei,Xiong Haifeng
Palladium (Pd)-based catalysts are widely used for CO 2 hydrogenation reactions due to the capability to activate H 2 , which enhances the overall CO 2 conversion. However, most of the current Pd catalysts reported show high CO 2 conversion only at higher temperature, and the exploration of efficient catalyst enabling low temperature conversion (180–300 °C) is of importance. In this study, a series of Pd-B/ZnAl 2 O 4 catalysts were synthesized via in-situ doping, resulting in the Pd crystal transformation induced from crystal to amorphous. The catalytic hydrogenation activity of the amorphous Pd-B catalyst reaches its zenith at a Pd-B mole ratio of 1:2, accompanied by the superior catalysis stability in CO 2 hydrogenation. Various characterization techniques, including XRD, CO-DRIFTS, H 2 -TPR, XPS and TEM, were used to investigate the properties of the Pd-B/ZnAl 2 O 4 catalyst. The results showed that the Pd-B/ZnAl 2 O 4 catalyst exhibited higher dispersion and better CO 2 conversion efficiency compared to unmodified Pd catalyst. Additionally, the methanol space–time yields are nearly doubled when the B decoration is employed. At 280 °C, CO 2 conversion was improved and methanol selectivity remained at ~ 65%. This study provides valuable insights into the design and optimization of Pd-B based catalysts for CO 2 hydrogenation at low temperatures. Graphical Abstract
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
Advanced Science
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2024
·
IF 14.3
Tianliang Li,Dan Xu,Zhao Ruan,Jie Zhou,Wenbo Sun,Bo Rao,Haibo Xu
Intrinsic immunosuppressive tumor microenvironment (ITM) and insufficient tumor infiltration of T cells severely impede the progress of glioblastoma (GBM) immunotherapy. In this study, it is identify that inhibiting the expression of glucose transporter 1 (GLUT1) can facilitate the prevention of lactate excretion from tumor glycolysis, which significantly alleviates the lactate-driven ITM by reducing immunosuppressive tumor-associated macrophages (TAMs) and regulatory T cells (Tregs). Simultaneously, the findings show that the generated inflammatory cytokine IFN-γ during immune activation aggravates the immune escape by upregulating immune checkpoint programmed death-ligand 1 (PD-L1) in tumor cells and TAMs. Therefore, an injectable thermogel loaded with a GLUT1 inhibitor BAY-876 and a PD-1/PD-L1 blocker BMS-1 (Gel@B-B) for dual-regulation of metabolism and immunity of GBM is developed. Consequently, in situ injection of Gel@B-B significantly delays tumor growth and prolongs the survival of the orthotopic GBM mouse model. By actively exposing tumor antigens to antigen-presenting cells, the GBM vaccine combined with Gel@B-B is found to significantly increase the fraction of effector T cells (Th1/CTLs) in the tumor microenvironment, thereby remarkably mitigating tumor recurrence long-term. This study may provide a promising strategy for GBM immunotherapy.
研究领域:
肿瘤学
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免疫学
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生物医学工程
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药理学
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产品关联
DOI
PubMed
高影响因子
CURRENT CANCER DRUG TARGETS
·
2024
·Vol. 25
·期 3
·294-305
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IF 2.3
Yiping Zheng,Jianfeng Cai,Qiuhong Ji,Luanmei Liu,Kaijun Liao,Lie Dong,Jie Gao,Yinghui Huang
BackgroundLung cancer remains a major global health threat due to its complex microenvironment, particularly the role of neutrophils, which are crucial for tumor development and immune evasion mechanisms. This study aimed to delve into the impact of lung cancer cell-conditioned media on neutrophil functions and their potential implications for lung cancer progression.MethodsEmploying in vitro experimental models, this study has analyzed the effects of lung cancer cell-conditioned media on neutrophil IL-8 and IFN-γ secretion, apoptosis, PD-L1 expression, and T-cell proliferation by using techniques, such as ELISA, flow cytometry, immunofluorescence, and CFSE proliferation assay. The roles of IL-8/PD-L1 in regulating neutrophil functions were further explored using inhibitors for IL-8 and PD-L1.ResultsLung cancer cell lines were found to secrete higher levels of IL-8 compared to normal lung epithelial cells. The conditioned media from lung cancer cells significantly reduced apoptosis in neutrophils, increased PD-L1 expression, and suppressed T-cell proliferation and IFN-γ secretion. These effects were partially reversed in the presence of IL-8 inhibitors in Tumor Tissue Culture Supernatants (TTCS), while being further enhanced by IL-8. Both apoptosis and PD-L1 expression in neutrophils demonstrated dose-dependency to TTCS. Additionally, CFSE proliferation assay results further confirmed the inhibitory effect of lung cancer cell-conditioned media on T-cell proliferation.ConclusionThis study has revealed lung cancer cell-conditioned media to modulate neutrophil functions through regulating factors, such as IL-8, thereby affecting immune regulation and tumor progression in the lung cancer microenvironment.
研究领域:
肿瘤学
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免疫学
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细胞生物学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yihao Zhao,Bingzhu Wang,Qimin Fang,Songyang Wu,Yuan Ma,Changxiang Xie,Haiwang Wang
To achieve efficient photocatalytic degradation of multi-component wastewater, the solvothermal method was employed to synthesize g-C 3 N 4 /BiOBr, leading to a homogeneous encapsulation of lamellar g-C 3 N 4 around the flower-like spherical BiOBr structure. In this work, the control of the temperature and the composition ratio during the solvothermal process was used to achieve the modulation of the g-C 3 N 4 /BiOBr microscopic morphology and enhance the photocatalytic activity, and the mechanism of the evolution of its microstructure and photocatalytic activity was elucidated. Moreover, the electron transport bridge between heterojunctions was constructed by introducing metal Pd, which further reduced the probability of photogenerated electron-hole complexation, leading to a higher photocatalytic performance. The elimination rates of RhB, Cr(VI), and TCH of g-C 3 N 4 /Pd/BiOBr under the irradiation of visible light were 99.74 %, 89.20 %, and 44.62 %, respectively, which achieved efficient elimination of a wide range of pollutants. Besides, the carrier transport mechanism in g-C 3 N 4 /Pd/BiOBr heterojunction was proven to Z scheme, which mainly induced the complexation of e - in the conduction band of BiOBr and h + in the valence band of g-C 3 N 4 , which provided higher energy for oxidation and reductive degradation. This work provides an important reference for the research focusing on photocatalyst design and sewage treatment.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）