ENERGY & FUELS
·
2025
·
IF 5.3
Qiulin Ye,Dongdong Wang,Jiabao Lv,Minghui Tang,Angjian Wu,Yaqi Peng,Shengyong Lu
The electrocatalytic CO2 conversion offers a sustainable pathway for generating ecofriendly chemicals and fuels while simultaneously enabling the storage of intermittent renewable energy. Herein, CuPd bimetallic catalysts were specifically designed through displacement reaction, with a magnetron sputtering Cu film as a substrate. The optimized CuPd catalyst achieved an ethylene Faradaic efficiency (FE) of 51.07% and a C2+ FE of 82.18% at a 200 mA/cm2 current density. In situ Raman spectroscopy indicates that the CuPd electrode exhibited a high local surface pH during the CO2 reduction reaction, which was favorable for C–C coupling. The observation of the *OCCOH intermediate by in situ FTIR, combined with density functional theory calculations, confirms that the CuPd surface promotes C–C coupling instead of direct hydrogenation. This mechanistic insight explains why the addition of Pd enhances the selectivity for C2+ products.
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高影响因子
Nanomaterials
·
2025
·Vol. 16
·期 1
·
IF 4.3
Yu Zhang,Ying Xin,Lizheng Tang,Shihao Cui,Hongling Duan,Qingshan Zhao
The selective hydrogenation of phenol to cyclohexanone is a pivotal reaction for producing nylon precursors. Conventional Pd/C catalysts, however, suffer from weak metal–support interactions, leading to size heterogeneity and agglomeration of Pd nanoparticles, which degrades their activity and stability. Herein, we report a facile argon plasma treatment to engineer rich defects on an activated carbon (AC) support, resulting in a highly dispersed and stable catalyst (denoted as PL-Pd@ACAr). Characterization results indicate that the abundant carbon defects in PL-Pd@ACArenhance the anchoring of Pd precursors, ensure the uniform dispersion of Pd nanoparticles, and effectively modulate their electronic structure. Consequently, the plasma-enabled PL-Pd@ACArcatalyst achieves 99.9% phenol conversion with 97% selectivity to cyclohexanone at a mild temperature of 70 °C and maintains exceptional stability over six consecutive cycles. This work provides a robust and efficient strategy for the surface engineering of carbon supports to design high-performance hydrogenation catalysts.
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DOI
PubMed
高影响因子
BMC MICROBIOLOGY
·
2024
·Vol. 24
·期 1
·1-15
·
IF 4
Wang Benlin,Qiu Yifeng,Xie Ming,Huang Pengcheng,Yu Yao,Sun Qi,Shangguan Wentai,Li Weijia,Zhu Zhangrui,Xue Jingwen,Feng Zhengyuan,Zhu Yuexuan,Yang Qishen,Wu Peng
Objective Bladder cancer(BCa) was a disease that seriously affects patients’ quality of life and prognosis. To address this issue, many researches suggested that the gut microbiota modulated tumor response to treatment; however, this had not been well-characterized in bladder cancer. In this study, our objective was to determine whether the diversity and composition of the gut microbiota or the density of specific bacterial genera influence the prognosis of patients with bladder cancer. Methods We collected fecal samples from a total of 50 bladder cancer patients and 22 matched non-cancer individuals for 16S rDNA sequencing to investigate the distribution of Parabacteroides in these two groups. Further we conducted follow-up with cancer patients to access the impact of different genera of microorganisms on patients survival. We conducted a Fecal Microbiota Transplantation (FMT) and mono-colonization experiment with Parabacteroides distasonis to explore its potential enhancement of the efficacy of anti-PD-1 immunotherapy in MB49 tumor-bearing mice. Immunohistochemistry, transcriptomics and molecular experiment analyses were employed to uncover the underlying mechanisms. Results The 16S rDNA showed that abundance of the genus Parabacteroides was elevated in the non-cancer control group compared to bladder cancer group. The results of tumor growth curves showed that a combination therapy of P. distasonis and ICIs treatment significantly delayed tumor growth and increased the intratumoral densities of both CD4 + T and CD8 + T cells. The results of transcriptome analysis demonstrated that the pathways associated with antitumoral immune response were remarkably upregulated in the P. distasonis gavage group. Conclusion P. distasonis delivery combined with α-PD-1 mAb could be a new strategy to enhance the effect of anti-PD-1 immunotherapy. This effect might be achieved by activating immune and antitumor related pathways.
研究领域:
肿瘤学
·
微生物学
·
免疫学
·
分子生物学
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高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Li Jia-Kai,Li Xiang-Yu,Xu Zhong-Ning,Sun Jing,Lin Shu-Juan,Qin Qiu-Pei,Liu Bin-Wen,Wang Ming-Sheng,Guo Guo-Cong
Reduction of nitric acid reaction (2NO + HNO 3 + 3CH 3 OH → 3CH 3 ONO + 2H 2 O) can convert by-product nitric acid into raw material methyl nitrite in the coal to ethylene glycol (CTEG) technology. This not only realizes the efficient recycling of nitrogen resources but also plays a crucial role in mitigating environmental pollution. Despite being a promising catalyst, the Pd/C catalyst face challenges due to its high metal loading, substantial loss rate, and consequent issues of poor stability, presenting obstacles in meeting industrial requirements. To address this issue, a defect strategy has been employed to develop a low-loaded 0.3% Pd/NC catalyst with robust metal-support interaction, resulting in a significant enhancement of catalyst stability. Remarkably, even after undergoing five cycles, the catalyst maintains a high nitric acid conversion rate of 90%. This improved performance can be attributed to the strong metal-support interaction driven by electron transfer from the nitrogen-doped carbon (NC) substrate to the Pd nanoparticles evident in the Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma (ICP) results. This interaction effectively suppresses the leaching of the active Pd nanoparticles, leading to significantly enhanced stability and a noticeable reduction in the loss rate. Raman spectrum and electron paramagnetic resonance (EPR) results can further reveal that the increase in the defect density lead to the strong metal-support interaction after nitrogen doping (pyridinic-N-dominated). These findings highlight the significant potential of the Pd/NC catalyst and its applicability in expediting the industrialization process of catalyst. Graphical Abstract
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高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2024
·
IF 3.3
Zhikang Chen,Jiahao Liu,Weiying Ou,Terumasa Kato,Zhe Wang,Yong Chen,Yan Liu,Keiji Maruoka
A series of novel axially chiral pyridylidene amine (PYE) ligands has been developed, and their catalytic capability has been demonstrated in various highly efficient and enantioselective Pd-catalyzed asymmetric allylic substitutions. A density-functional theory (DFT) study explains the preferential enantiocontrol in the key transition states of the axially chiral PYE ligand-promoted Pd-catalyzed allylic alkylation.
研究领域:
有机化学
·
催化化学
·
理论化学
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PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Ping Li,Ziwei Zhang,Zhihua Zhuang,Jinhan Guo,Zhongying Fang,Shemsu Ligani Fereja,Wei Chen
Metal oxide semiconductors (MOS) with different nanostructures have been widely used as gas sensing materials due to the tunable interface structures and properties. However, further improvement of the sensing sensitivity and selectivity is still challenging in this area. Constructing appropriate heterogeneous interface structures and oxygen vacancies is one of the important strategies to tune the sensing properties of MOS. In the present study, interfacial heterostructures in PdxW18O49 nanowires (PdxW18O49 NWs) were fabricated and manipulated by doping different Pd contents through a simple hydrothermal process. Relevant characterization proved that the structure and composition of the one-dimensional (1D) nanomaterial can be effectively changed by Pd doping. It was found that the oxygen vacancy concentration increases first with the increase of Pd content, and when the Pd content increases to 7.18% (Pd7.18%W18O49 NWs), the oxygen vacancy content reaches the maximum (52.5%). If the Pd content continues to increase, the oxygen vacancy ratio decreases. The gas sensing investigations illustrated that the PdxW18O49 NWs exhibited enhanced sensing properties than pure W18O49 NWs toward acetone. Among the as-prepared catalysts, the Pd7.18%W18O49 NWs showed the best sensing response and the fastest response-recovery speeds (5 and 10 s, respectively) at a working temperature of 175 °C. In addition, this 1D nanostructure with fabricated heterostructures also delivers a good sensing selectivity and a wide detection range from 100 ppb to 300 ppm, with maintaining excellent performance in the presence of high concentrations of ethanol and carbon dioxide. The excellent gas sensing behavior could be attributed to the generated oxygen vacancies and the heterostructures upon Pd doping. This study offers a novel strategy for the design of high-performance gas sensors for ppb-level acetone sensing.
研究领域:
材料科学
·
化学工程
·
传感器技术
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高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xueyan Sun,Shaofeng Li,Jinzhe Cao,Yuchao Wang,Wenbo Yang,Lijing Zhang,Yijin Liu,Jieshan Qiu,Shengyang Tao
Suzuki cross-coupling reactions catalyzed by palladium are authoritative protocols in fine-chemical synthesis. Mass transfer and catalyst activity are both significant factors affecting the reaction efficiency in heterogeneous reactions. Although the holistic catalysts hold great promise in heterogeneous reactions due to the enhanced mass transport and convenient recycling, the unsatisfied catalytic activity has impeded further large-scale applications. In addition, another pronounced barrier is the product separation in the intricate system. Here, the catalytic production and separation of biphenyl (purity of 99.7%) were achieved by integrating the Suzuki cross-coupling reactions and the crystallization separation for the first time. A hierarchical-structured impeller with Pd nanoparticles (NPs) loaded on the Ni(OH)2 nanosheets was prepared to catalyze the Suzuki reactions for bromobenzene, which exhibits a high turnover frequency (TOF) value of 25,976 h–1 and a yield of 99.5%. The X-ray absorption fine structure (XAFS) analysis has unveiled that the electron transfer between the Pd NPs and Ni(OH)2 accounts for the greatly enhanced catalytic activity. The findings inspire new insights toward rational engineering of highly efficient holistic catalysts for Suzuki reaction, and the innovative integrated technology offers an avenue for the separation and collection of products.
研究领域:
化学工程
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材料科学
·
催化技术
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DOI
高影响因子
CATALYSIS LETTERS
·
2010
·Vol. 139
·期 1
·56-60
·
IF 2.021
Zhang Junli,Chen Xiaorong,Hu Tongjie,Zhang Yuan,Xu Kunling,Yu Yanpeng,Huang Jun
Abstract A highly improved Pd-catalyzed cyanation of aryl chlorides to corresponding benzonitriles was demonstrated in aqueous media. Moreover, Pd-catalyzed cyanation of aryl tosylates and benzenesulfonates with K 4 [Fe(CN) 6 ] was developed under the similar conditions, which extended application scope of the cyanation. Graphical Abstract
研究领域:
有机化学
·
绿色化学
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高影响因子
ACS Omega
·
2021
·
IF 3.512
Lin-Xi Wan,Yong-Qi Zhen,Zhen-Xiang He,Yang Zhang,Lan Zhang,Xiaohuan Li,Feng Gao,Xian-Li Zhou
A new series of N-aryltacrine derivatives were designed and synthesized as cholinesterase inhibitors by the late-stage modification of tacrine, using the palladium-catalyzed Buchwald–Hartwig cross-coupling reaction. In vitro inhibition assay against acetylcholinesterase (AChE) and butyrylcholinesterase (BuChE) demonstrated that most of the synthesized compounds had potent AChE inhibitory activity with negative inhibition of BuChE. Among them, N-(4-(trifluoromethyl)phenyl)-tacrine (3g) and N-(4-methoxypyridin-2-yl)-tacrine (3o) showed the most potent activity against AChE (IC50 values of 1.77 and 1.48 μM, respectively). The anti-AChE activity of 3g and 3o was 3.5 times more than that of tacrine (IC50 value of 5.16 μM). Compound 3o also displayed anti-BuChE activity with an IC50 value of 19.00 μM. Cell-based assays against HepG2 and SH-SY5Y cell lines revealed that 3o had significantly lower hepatotoxicity compared to tacrine, with additional neuroprotective activity against H2O2-induced damage in SH-SY5Y cells. The advantages including synthetic accessibility, high potency, low toxicity, and adjunctive neuroprotective activity make compound 3o a new promising multifunctional candidate for the treatment of Alzheimer’s disease.
研究领域:
药物化学
·
药理学
·
神经科学
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DOI
PubMed
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2017
·Vol. 314
·期 1
·59-67
·
IF 1.282
Liu Zhanxiang,Dong Yang,Liao Jiali,Li Xingliang,Yang Jijun,Yang Yuanyou,Luo Shunzhong,Liu Ning
A novel extractant, 5-octyloxymethyl-7-bromo-8-quinolinol (HBrO 8 Q), was employed to extract Pd(II) from low-acidity aqueous solution. The extraction behaviors indicated that HBrO 8 Q had high extraction efficiency and selectivity for Pd(II) under the experimental conditions, and the stoichiometry of Pd(II) with HBrO 8 Q was found to be 1:1 by means of mole ratio method and Job’s method. The thermodynamic study indicated that the extraction process was endothermic and spontaneous. Additionally, complete back extraction of palladium could be achieved by using acidic thiourea solution.
研究领域:
化学
·
环境科学
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DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Shuzhen Lv,Kangyao Zhang,Ling Zhu,Dianping Tang,Reinhard Niessner,Dietmar Knopp
With the introduction of gas-based contactless electrochemical biosensors lies the prospects of separating the sensing interface from the bioassembly platform, enhancing stability, and exploring signal transduction mechanism, all intimately linking to development of immunoassay. Herein, we report on a H2-based electrochemical biosensor whose signals derived from the chemical signal transduction between a H2 and Pd nanowires@ZIF-67 (ZIF: Zeolitic Imidazolate Frameworks) bilayered sensing interface for immunoassay. Dendritic Pt nanoparticles (DPNs) conjugated on the detection antibody were introduced on the interface of a magnetic microsphere according to an immune sandwich assembly between the antigen and antibody. H2 as a bridge originates from DPNs catalyzing NH3BH3 and links biological signals to electrical signals by reacting with Pd nanowires. Nevertheless, the response of Pd nanowires being extremely effected by O2 in air due to the competitive adsorption on the surface of Pd nanostructures as well as the reaction between chemisorbed O (Pd–O) and adsorbed dihydrogen lead to a decrease in H absorption into PdHx and poor sensing responses under low target concentration. Porous ZIF-67 (window aperture 0.331 nm) as a molecular sieve self-assembling on the surface of the Pd nanowires film could easily permeate H2 (kinetic diameter of 0.289 nm), while interferential O2 (kinetic diameter of 0.346 nm) has difficultly passing through the ZIF-67 layer to contact Pd nanowires and achieves a response of a lower concentration target as well as faster response rate. Under optimal conditions, H2-based electrochemical biosensors exhibit great response toward target alpha-fetoprotein (AFP) within a dynamic working range of 0.1–50 ng mL–1 at a detection limit of 0.04 ng mL–1. Our strategy provides a reusable sensing interface, high specificity, and acceptable accuracy for the immunoassay. In addition, it also expands a promising platform for application as a molecular sieve in electrochemical biosensors.
研究领域:
生物传感器
·
纳米技术
·
分析化学
·
材料科学
·
生物医学工程
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DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 13
·4398-4405
·
IF 6.119
Liangcai Zhang,Xinyu Liu,Hengwei Wang,Lina Cao,Chenxi Huang,Shang Li,Xiaohui Zhang,Qiaoqiao Guan,Xiang Shao,Junling Lu
Strong metal–support interaction (SMSI) has long been studied in catalytic reactions. Proper utilization of the SMSI effect might not only improve the stability of the catalysts, but also the activity and selectivity. In this work, using the atomic layer deposition (ALD) technique, we synthesized a series of Pd/ZnO catalysts with Pd particle sizes ranging from 1.6 to 7.9 nm. Upon H2 reduction at elevated temperatures, these Pd/ZnO catalysts display a size-dependent SMSI effect wherein the larger-size Pd particles are more prone to be encapsulated by ZnO compared to the smaller ones. In the reaction of CO2 hydrogenation, we show that such size-dependent SMSI, together with the size-related CO binding strength on Pd particles, provides a higher activity and methanol selectivity to the Pd particles larger than ~2.5 nm.
研究领域:
催化化学
·
材料科学
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高影响因子
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