CHEMISTRY-A EUROPEAN JOURNAL
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2022
·Vol. 29
·期 16
·e202203142
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IF 5.02
Jingwen Luo,Anqi Huang,Yao-Yue Yang,Xing-Yu Ma,Quan-Liang Chen,Junxian Chen,Yajuan Wu
Graphical Put to good use : A Pd-doped Co (Pd/Co) catalyst with high Pd atom utilization efficiency was designed and prepared for hydrogenation of nitroarenes. Its catalytic activity was much better than commercial Pd powder (>150 times) in nitrobenzene hydrogenation reaction. This work might provide a simple and low-cost methodology to design and synthesize highly efficient catalysts. Enhancing catalytic performance as well as reducing catalyst cost are the eternal pursuit for the catalysis community. Herein, a simple and effective palladium-doped cobalt (Pd / Co) catalyst with high Pd atom utilization efficiency was synthesized via galvanic replacement reaction for the selective hydrogenation of nitrobenzene with H 2 at room temperature, delivering >99 % yield of aniline with up to 158 times higher catalytic activity than commercial palladium powder. Detailed characterizations and DFT calculations revealed that Co−Pd interaction leads to a decrease in electron density of Pd and the distance between Pd atoms that results in the enhanced catalytic performance. Further experiments indicated that the Pd / Co catalyst serves as a highly efficient, selective, and recyclable catalyst for a range of nitroarene substrates. This work might provide a green and sustainable methodology to design and synthesize highly active catalysts with high utilization efficiency of the noble metals in fundamental and applied research.
研究领域:
催化化学
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材料科学
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理论计算化学
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DOI
PubMed
高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 46
·465404
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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.
研究领域:
材料科学
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能源科学
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催化化学
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DOI
PubMed
高影响因子
Scientific Reports
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2025
·Vol. 15
·期 1
·1-14
·
IF 3.9
Sun Jinzhou,Chen Qianqian,Zhuang Chumeng,Li Xiaohong,Yu Li,Jin Weifeng
Develop a novel coupled PK-PD model and apply it to quantitatively evaluate the synergistic effects of Hydroxysafflor Yellow A (HSYA) combined with Calycosin (CA) in the treatment of ischemic stroke. A total of 6 rats were modelled for middle cerebral artery occlusion (MCAO). Plasma was collected from the submandibular venous plexus of rats after the administration of HSYA and CA, and was detected and analyzed by LC-MS method. The plasma expression levels of Caspase-9, IL-1β and SOD in rats were also determined by ELISA kit. Meanwhile, a coupled PK-PD model was proposed, incorporating interaction terms between drugs and coupling of pharmacodynamic effects, to quantitatively reveal their interactions. Moreover, a numerical solution technique based on optimization methods was proposed, enabling the model to be effectively applied to experimental data. Based on the coupled PK model, HSYA and CA significantly increased each other’s metabolic rates. The model also showed that CA had a larger apparent volume of distribution and clearance in rats, while HSYA had a shorter mean retention time and elimination half-life. The coupled PK-PD model indicated a synergistic effect between HSYA and CA on all three pharmacodynamic markers, with HSYA contributing more significantly. Despite individual variability among the six rats, the parameter interpretations remained consistent. The proposed coupled PK-PD model and its numerical solution algorithm successfully revealed the synergistic effects of HSYA and CA in the treatment of ischemic stroke. This model lays the foundation for future models with more complex interactions and effects.
研究领域:
药理学
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生物医学工程
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神经科学
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DOI
PubMed
高影响因子
Journal of Environmental Sciences
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2023
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IF 6.9
Xingyu Liu,Jingkun Chen,Bowen Han,Renna Li,Le Shi,Zhongbiao Wu,Xiaole Weng
Zeolites are a promising support for Pd catalysts in lean methane (CH 4 ) combustion. Herein, three types of zeolites (H-MOR, H-ZSM-5 and H-Y) were selected to estimate their structural effects and deactivation mechanisms in CH 4 combustion. We show that variations in zeolite structure and surface acidity led to distinct changes in Pd states. Pd/H-MOR with external high-dispersing Pd nanoparticles exhibited the best apparent activity, with activation energy ( E a ) at 73 kJ/mol, while Pd/H-ZSM-5 displayed the highest turnover frequency (TOF) at 19.6 × 10 −3 s −1 , presumably owing to its large particles with more step sites providing active sites in one particle for CH 4 activation. Pd/H-Y with dispersed PdO within pore channels and/or Pd 2+ ions on ion-exchange sites yielded the lowest apparent activity and TOF. Furthermore, Pd/H-MOR and Pd/H-ZSM-5 were both stable under a dry condition, but introducing 3 vol.% H 2 O caused the CH 4 conversion rate on Pd/H-MOR drop from 100% to 63% and that on Pd/H-ZSM-5 decreased remarkably from 82% to 36%. The former was shown to originate from zeolite structural dealumination, and the latter principally owed to Pd aggregation and the loss of active PdO.
研究领域:
催化
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化学工程
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环境科学
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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
Yanyun Hao,Hui Li,Xiaoyan Ge,Yang Liu,Jialin Yin,Xia Li,Yutong Liu,Hongfei Chen,Lingling Huang,Jing Zou,Shiying Zhang,Hao Wu,Zhiyue Zhang
Immunotherapy has fundamentally altered cancer treatment; however, its effectiveness is clinically hampered by insufficient intratumoral T lymphocyte infiltration and failed T lymphocyte priming. Additionally, inducing cancer-specific immune responses while sparing normal cells remains challenging. Herein, we developed a redox-activatable polymeric nanoswitch (c-N@IM/JQ) that remained ‘off’ status in circulation but rapidly switched ‘on' after entering the tumor. Toll-like receptor (TLR) 7/8 agonist (imidazoquinoline, IMQ) and bromodomain and extraterminal inhibitor (JQ1) are locked in c-N@IM/JQ with a redox-cleavable linker (switch off). Upon systemic administration , c-N@IM/JQ with c-RGD peptide modification preferentially accumulated at tumor sites and responded to the high glutathione levels to release native IMQ for fully mobilizing T lymphocyte army, and JQ1 for removing the programmed death ligand (PD-L)-1 protection on tumor cells (switch on). These strengthened T lymphocyte armies are easily accessible to these de-protected tumor cells, revitalizing the immune response against tumors.
研究领域:
癌症免疫疗法
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纳米技术
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药学
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分子生物学
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DOI
PubMed
高影响因子
Catalysts
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2021
·Vol. 11
·期 5
·543
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IF 4.146
Zechen Liang,Mingkai Zhang,Sai Zhang,Yongquan Qu
Selective hydrogenation of halonitrobenzenes into haloanilines represents a green process to replace the environmentally unfriendly non-catalytic chemical reduction process in industry. However, this transformation often suffers from serious dehalogenation due to the easy break of carbon-halogen bonds on metal surfaces. Modulations of the electronic structure of the supported Pd nanoparticles on Lewis-basic layered double hydroxides have been demonstrated to promote catalytic activity and selectivity for hydrogenation of halonitrobenzenes into haloanilines. Mechanism studies suggest that Pd with the enhanced electron density not only improves the capability for hydrogen activation, but also generates the partially negative-charged hydrogen species to suppress the electrophilic attack on the carbon-halogen bond and avoid the dehalogenation.Keywords:Pd nanoparticles;hydrogenation;halonitrobenzenes;haloanilines
研究领域:
化学
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催化材料科学
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2024
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IF 6.5
Yiming Chen,Chuan Wang,Yi Liu,Qianwen Zhang,Ling Zhou,Yi Zhang
The selectivity and stability of catalysts for methanol synthesis from CO 2 still remain to be enhanced. In this work, we synthesized a series of Pd/ZrO 2 catalysts inversely loaded with various metal oxide promoters (ZnO, In 2 O 3 , and CeO 2 ), those would partially cover Pd metal surface and form some new metal-promoter interface, to explore the nature in the performance of CO 2 hydrogenation to methanol. The catalyst synthesized by this approach could limit the growth of Pd particles during the reduction and form new metal–metal oxide interfaces with different functions of CO 2 hydrogenation, improving the reaction performance of Pd-ZrO 2 catalysts. As a result, the ZnO-Pd/ZrO 2 catalyst exhibited the highest CO 2 conversion (12.0 %), methanol selectivity (95.6 %), and STY of methanol (472 g MeOH kg cat -1 h −1 ), with excellent stability. The results of HRTEM, H 2 -TPR, XPS, and XAFS showed that the ZnO-Pd/ZrO 2 catalyst had the typical Pd-ZnO interface with Pd 2+ species after the H 2 reduction, which could enhance the adsorption and activation of CO 2 . In addition, the in situ DRIFTS and NAP-XPS results implied that the Pd-ZnO interface significantly improved the formation of formate (HCOO*) and methoxy (H 3 CO*) species, which were considered to be the key intermediates of methanol generation, and thus greatly enhanced the selectivity of methanol.
研究领域:
催化
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化学工程
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材料科学
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环境化学
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Pei An,Wang Peng,Zhang Shiyi,Zhang Qinghua,Jiang Xiaoyi,Chen Zhaoxi,Zhou Weiwei,Qin Qizhen,Liu Renfeng,Du Ruian,Li Zhengjian,Qiu Yongcai,Yan Keyou,Gu Lin,Ye Jinyu,Waterhouse Geoffrey I. N.,Huang Wei-Hsiang,Chen Chi-Liang,Zhao Yun,Chen Guangxu
Challenges in direct catalytic oxidation of biomass-derived aldehyde and alcohol into acid with high activity and selectivity hinder the widespread biomass application. Herein, we demonstrate that a Pd/Ni(OH) 2 catalyst with abundant Ni 2+ -O-Pd interfaces allows electrooxidation of 5-hydroxymethylfurfural to 2, 5-furandicarboxylic acid with a selectivity near 100 % and 2, 5-furandicarboxylic acid yield of 97.3% at 0.6 volts (versus a reversible hydrogen electrode) in 1 M KOH electrolyte under ambient conditions. The rate-determining step of the intermediate oxidation of 5-hydroxymethyl-2-furancarboxylic acid is promoted by the increased OH species and low C–H activation energy barrier at Ni 2+ -O-Pd interfaces. Further, the Ni 2+ -O-Pd interfaces prevent the agglomeration of Pd nanoparticles during the reaction, greatly improving the stability of the catalyst. In this work, Pd/Ni(OH) 2 catalyst can achieve 100% 5-hydroxymethylfurfural conversion and >90% 2, 5-furandicarboxylic acid selectivity in a flow-cell and work stably over 200 h under a fixed cell voltage of 0.85 V.
研究领域:
电化学
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催化
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材料科学
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可持续化学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
DePing Chen,ZhenYi Shao,LiRong Yang,Ying Chen,Yanghong Wei,Zhihua Hu,Liyang Cai,Yifan Zhang,Xun He
The design of efficient electrocatalysts for ethanol oxidation is essential for commercializing direct ethanol fuel cells (DEFCs). In this strategy, a mesoporous carbon microsphere (MC) was first synthesized by inverting the micro-emulsion technique. The MC@Au/Pd catalyst with a particular core-shell structure was obtained by utilizing mesoporous carbon as a core to load the Au/Pd layer. The novelty of the MC@Au/Pd catalyst with specialized core-shell structures lies not only in the high specific surface area inherited from the carbon core but also in the strong electronic interactions caused by the lattice mismatch between the core (Au) and shell (Pd) atoms. Particularly, electrochemical measures demonstrated that the Au/Pd catalyst exhibits superior catalytic activity toward the ethanol oxidation reaction (EOR) compared with commercial Pd/C catalysts. This is mainly due to the high specific surface area and mesoporous pore size inherited from the core carbon microspheres. In addition, the mesoporous carbon core and Au/Pd shell in the well-organized core-shell catalyst (MC@Au/Pd) influence the catalytic activity for ethanol oxidation by adjusting the electronic structure of Pd.
研究领域:
材料科学
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能源化学
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产品关联
DOI
高影响因子
Advanced Science
·
2025
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IF 14.1
Xinyi Lu,Pingping Jin,Qianyun Tang,Min Zhou,Hanjie Xu,Chen Su,Lei Wang,Feng Xu,Min Zhao,Yongxiang Yin,Jinqiu Zhang,Zhen Jia,Xinrui Peng,Jie Zhou,Lu Wang,Yan Chen,Min Wang,Min Yang,Daozhen Chen,Yu Chen
Cervical cancer (CC) is a major health threat to women, with immunotherapies targeting the programmed death receptor 1/programmed death ligand 1(PD-1/PD-L1) axis showing promise but encountering resistance in a significant patient population. This resistance has driven a critical quest to uncover the underlying mechanisms. This study uncovers a novel metabolic axis involving the nicotinamide adenine dinucleotide (NAD + ) salvage pathway enzyme nicotinamide phosphoribosyltransferase (NAMPT) and the deacetylase Sirtuin 1 (SIRT1), which regulates PD-L1 expression and nuclear localization in CC. This axis may be a key factor contributing to the resistance observed in immunotherapy. This study reveals that PD-L1 overexpression in cancers is regulated by both transcriptional and post-transcriptional processes. Acetyl-proteomic analysis pinpoints SIRT1 as a central regulator in the deacetylation of histone H3 at lysines 27, which may influence PD-L1 subcellular distribution. This finding reveals the epigenetic control of immune checkpoint proteins by metabolic pathways, offering a new perspective on the regulation of PD-L1. The identification of the NAMPT/SIRT1 metabolic axis as a critical factor suggests that targeting this axis may enhance therapeutic responses.
研究领域:
肿瘤学
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分子生物学
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免疫学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF PHOTOENERGY
·
2020
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IF 1.88
Jing Yan,Xiaojuan Li,Bo Jin,Min Zeng,Rufang Peng
A series of TiO2, TiO2/Pd, and TiO2/PdO hollow sphere photocatalysts was successfully prepared via a combination of hydrothermal, sol-immobilization, and calcination methods. The structure and optical properties of the as-prepared samples were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, Brunauer-Emmett-Telleranalysis, Barrett-Joyner-Halenda measurement, and UV-Vis diffuse reflectance spectroscopy. The photocatalysis efficiencies of all samples were evaluated through the photocatalytic degradation of rhodamine B under visible light irradiation. Results indicated that TiO2/PdO demonstrated a higher photocatalytic activity (the photocatalytic degradation efficiency could reach up to 100% within 40 min) than the other samples and could maintain a stable photocatalytic degradation efficiency for at least four cycles. Finally, after using different scavengers, superoxide and hydroxyl radicals were identified as the primary active species for the effectiveness of the TiO2/PdO photocatalyst.
研究领域:
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
ACTA PHYSICO-CHIMICA SINICA
·
2025
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IF 13.5
Lele Feng,Xueying Bai,Jifeng Pang,Hongchen Cao,Xiaoyan Liu,Wenhao Luo,Xiaofeng Yang,Pengfei Wu,Mingyuan Zheng
Ethanol dehydrogenation is a vital elementary step in ethanol upgrading, for which Cu-based alloy catalysts are the most promising candidates. Nevertheless, elucidating the underlying reasons for the synergistic effect between alloying components and host metals remains challenging due to the intrinsic structural complexity and dynamic evolution of alloy catalysts under operational conditions. Herein, single-atom Pd modified Cu-MFI catalysts with well-defined structures were designed for ethanol dehydrogenation to acetaldehyde and hydrogen. Comprehensive characterizations using aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM), X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations revealed that Pd atoms are isolated by surrounding Cu atoms with a coordination number of 9–10, forming −0.36 e charged single-atom sites and being uniformly dispersed on the surface of Cu catalysts. The newly generated Pd δ − and Cu δ + sites synergistically reduced the activation energy barrier for C–H bond cleavage in ethanol. These sites simultaneously enhanced hydrogen adsorption and H–H bond coupling, leading to improved ethanol conversion and acetaldehyde productivity over Pt/Cu-MFI catalysts.
研究领域:
催化化学
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材料科学
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表面科学
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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）