MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Yiquan Xie,Xiangju Meng,Shan Gao,Zhongbiao Wu,Feng-Shou Xiao
Catalytic combustion of CH 4 to CO 2 and H 2 O was studied over Pd nanoparticles supported on different siliceous zeolites ( MFI , BEA and CHA ) with γ-Al 2 O 3 as the reference support, and it was found that as supports, zeolites exert remarkable influence on the catalytic performance of methane oxidation , with the Pd catalyst (1 wt% loading) supported by siliceous MFI (ZSM-5-Si) presenting the highest activity. Over the exceptional catalyst, a complete conversion of methane can be achieved at around 380 °C, which is about 120 °C lower than the temperature needed for the Pd nanoparticles supported on γ-Al 2 O 3 (Pd/γ-Al 2 O 3 ), one of the best catalysts for the methane combustion. Physicochemical characterizations including X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM), temperature programmed desorption of methane (CH 4 -TPD) and temperature programmed reduction of methane (CH 4 -TPR) techniques were used to acquire an idea what is behind the discrepancy in the catalytic performances of methane combustion over these Pd-based catalysts. Based on these results, it is proposed that the different methane adsorption and the oxygen migration capability are mainly related to the difference in the catalytic performances of methane combustion over these catalysts. Among these factors, the difference in the methane adsorption is critical for the different catalytic performances, as evidenced by the kinetic measurements.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Shuhua Yang,Gaofeng Chen,Qian Guan,Haiyan Xu,Zhiwei Wang,Bing Liu,Shuliang Yang,Tingzhou Lei,Xianhai Zeng,Lu Lin
Bio-oil is a kind of viable renewable and environmentally sustainable energy, which is obtained from fast pyrolysis of biomass. However, bio-oil is not suitable for direct application due to the high content of oxygen and moisture. The upgrading of bio-oil, especially hydrodeoxygenation of bio-oil is highly demanded but remains a challenge owing to the absence of efficient and stable catalysts. Herein, an amphiphilic Pd/carbon-silica-alumina catalyst could catalytic reactions at the oil/water interface and simultaneously stabilized the oil/water emulsions, which would be highly advantageous in bio-oil upgrading. Significantly, the hydrophilicity and hydrophobicity of the catalyst could be adjusted by changing the input amount of precursor with resols, tetraethyl orthosilicate and aluminum chloride hexahydrate. In the catalytic reaction, phenol was used as a model bio-oil compound, where decalin and water were used to simulate an oil/water mixed bio-oil system. The as prepared amphipathic Pd/MCSA-24 catalyst showed the highest conversion of phenol (98.0%) and highest selectivity for cyclohexane (87.7%) at 200 °C, which presented great potential in further bio-oil upgrading applications.
研究领域:
能源化学
·
催化化学
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DOI
高影响因子
Chemistry-An Asian Journal
·
2017
·Vol. 12
·期 23
·3039-3045
·
IF 4.083
Yan Sun,Tao Wang,Ang Li,Ling Zhang,Qisheng Huo,Zhen-An Qiao
Graphical A simple and straightforward route is reported to knit benzene heterocycles to synthesize a series of hierarchical porous polymers with high surface area and abundant N sites. The N-doped porous polymers can effectively stabilize ultra-small Pd nanoparticles for solvent-free catalysis. Hierarchical porous polymers with more than one pore size distributions can effectively support noble metal catalysts and circumvent the limitation of the diffusion of the reactants, and thus exhibit both excellent catalytic activity and superior diffusive properties. Herein, we report a simple one-step Friedel–Crafts reaction to knit a series of benzene heterocycle monomers, such as indane, indoline, indole and tetrahydronaphthalene to obtain hierarchical porous polymers with high surface areas and/or abundant N sites. These polymers can be directly used to immobilize Pd ions, and stabilize Pd nanoparticles during the thermal reduction process to obtain Pd/polymer catalysts. In particular, indoline- and indole-based polymers with high N content up to 7 wt % exhibit outstanding ability to stabilize uniform ultrasmall Pd nanoparticles. The obtained Pd-polymers exhibit excellent catalytic activity in the solvent-free oxidation of benzyl alcohol with O 2 .
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Mudong Tu,Wenhan Dai,JunFeng Huang,Zhe Zhao,Yantao Wang,Yahan Fang,Lanjuan Yao,Hua Li,Baodui Wang
The efficient utilization of active hydrogen (*H) in electrocatalytic processes remains a critical challenge for achieving high selectivity in nitrate reduction to ammonia (NO 3 − RR), as excessive *H often promotes the competing hydrogen evolution reaction (HER), leading to reduced Faradaic efficiency and ammonia yield. Herein, we address this issue by designing a single-atom Pd-doped Cu/Cu 2 O electrocatalyst (SA Pd–Cu/Cu 2 O) that precisely modulates *H generation and consumption. The SA Pd–Cu/Cu 2 O catalyst achieves an exceptional NH 3 yield rate of 1634.14 μg h −1 mg −1 , a NO 3 − –N conversion of 97.56%, a NH 3 –N selectivity of 98.13%, and a Faradaic efficiency of 92.13% at −0.8 V vs. RHE. In situ spectroscopic studies and density functional theory (DFT) calculations reveal that single-atom Pd sites serve as hydrogenation centers that generate moderate *H, which is efficiently consumed by nitrogen-containing intermediates, thereby suppressing HER. In contrast, nanoparticle Pd doping produces excess *H, favoring HER. This work demonstrates an innovative strategy for balancing *H utilization via atomic-scale metal doping, offering new insights into the design of high-selectivity electrocatalysts for sustainable ammonia synthesis and environmental nitrate remediation.
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Qian Wang,Rubo Fang,Heng Yuan,Xinyi Zhang,Guilong Hu,Qunfeng Zhang
To address the high consumption and cost of noble metal catalysts during the production of hexanitrohexaazaisowurtzitane (HNIW, CL-20), nitrogen-doped titanium dioxide (TN) was synthesized using urea as a nitrogen source. PdO/TN catalysts were then fabricated via a deposition–precipitation route and applied to the continuous hydrogenolysis debenzylation of hexabenzylhexaazaisowurtzitane (HBIW). Characterization by XRD, TEM, Raman, XPS, and H₂-TPR revealed that nitrogen incorporation effectively promoted the generation of surface oxygen vacancies and strengthened metal–support interactions, thereby enhancing catalyst stability. Moreover, the oxygen vacancy concentration could be tuned by adjusting calcination conditions. The PdO/TN-400-2 catalyst, prepared at 400 °C for 2 h, exhibited the highest catalytic activity, with an oxygen vacancy fraction of 19.64%. Further decreasing the calcination severity increased defect density but did not yield additional performance gains. These findings demonstrate that nitrogen doping can regulate surface defect chemistry and metal–support coupling, offering a viable strategy for the design of efficient catalysts for hexabenzylhexaazaisowurtzitane (HBIW) debenzylation.
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产品关联
DOI
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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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2014
·
IF 4.086
Shaojie Li,Daojian Cheng,Xiangguo Qiu,Dapeng Cao
A core-shell Cu@Pd nanowire with enhanced activity and stability for formic acid oxidation (FAO) was prepared by decorating Pd shell on the surface of Cu nanowire. Detailed characterization (XRD, TEM and HAADF-STEM) results confirm that the prepared nanowires are of Cu@Pd core-shell structure with enlarged surface areas. The catalytic activity of Cu@Pd/C (2197.88 mA/mg at 0.257 V) toward FAO is about 4 times higher than that of the commercial Pd/C (547 mA/mg at 0.257 V). The enhanced activity of the catalyst may mainly result from the synergetic effect of Cu and Pd, which was confirmed by density-functional theory (DFT) calculations.
研究领域:
材料科学
·
电化学
·
理论计算
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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
Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
Wei Min,Shen Xiao,Fan Xueqi,Li Jiwei,Bai Jingwen
Immune checkpoint blockade is now recognized as a paradigm-shifting cancer therapeutic strategy, whereas there remains difficulty in accurately predicting immunotherapy efficacy by PD-L1 expression. In addition, radiotherapy for cancer patients faces the problem of insufficient dose of radiotherapy at the tumor site while which have been not tolerated by normal tissues. In this study, we created PD-L1 aptamer-anchored spherical nucleic acids (SNAs) with a shell made of PD-L1 aptamer and indocyanine green (ICG) embedded in a mesoporous hafnium oxide nanoparticle core (Hf@ICG-Apt). Upon low pH irradiation in the tumor sites, the nano-system enabled the release of ICG in the high PD-L1 expression tumor to develop a high tumor-to-background ratio of 7.97 ± 0.76 and enhanced the ICG tumor retention to more than 48 h. Moreover, Hf@ICG-Apt improved radiation therapy (RT) when combined with radiation. Notably, Hf@ICG-Apt showed scarcely any systemic toxicity in vivo. Overall, this research offered a novel approach for applying reliable monitoring of PD-L1 expression and localization and robust RT sensitization against cancer with good biosafety.
研究领域:
癌症治疗
·
纳米技术
·
医学成像
·
放射生物学
·
免疫疗法
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Liangmin Xiong,Shuang Liu,Yong Men,Lin Li,Xiaoda Niu,Kailiang Guo,Junzhe Xu,Wei An,Jinguo Wang,Yu Cong
CO 2 hydrogenation to liquid fuels is significant to reduce CO 2 emissions and replace fossil fuels . Herein, we reported that Fe catalysts promoted by combination of K and Pd showed a three-synergistic catalytic effect to high selectivity of C 5+ hydrocarbons in CO 2 hydrogenation reaction. The catalysts were prepared using an impregnation method and characterized with physical adsorption , XRD , XPS , HRTEM , H 2 -TPR, H 2 -TPD and CO 2 -TPD. The results indicated that K 0.016 Pd 0.12 Fe catalysts showed K-overlapped PdFe-like alloy structure which enhanced H 2 activation behaviors and moderately chemisorption of CO 2 . K addition promoted Fe to activate carbide species while active H originated from H 2 pool generated by PdFe alloy spilled to Fe species surface, consequently boosting not only conversion of CO 2 to 41.8% but also selectivity of C 5+ hydrocarbon to 70.6%. The maximum yield of long-chain C 5+ hydrocarbon reached up to 20.0% under high space velocity 6000 mL g cat −1 h −1 . These results provide a new insight to develop highly selective Fe based catalysts for long-chain hydrocarbons via CO 2 hydrogenation.
研究领域:
化学工程
·
催化反应
·
能源转化
✓ 已验证
DOI
高影响因子
Nanotoxicology
·
2026
·
IF 3.6
Yanting Zhan,Yiyang Wu,Chanting Huang,Siyi Liu,Ke Ma,Li Zheng,Zainen Qin
The high expression of classically activated macrophages (M1) subtypes and the elevated levels of reactive oxygen species (ROS) are specifically observed in osteoarthritis (OA) patients. In this study, we synthesized a Pd@CeO2 nanozyme with a core-shell hetero-nanostructure that enhances enzyme activity through shell-core electron transfer. The goal of this work was to look into the potential of Pd@CeO2 nanozyme in scavenging ROS and regulating macrophages for the treatment of OA. The results demonstrated that the Pd@CeO2 nanozyme displayed multiple enzyme-like antioxidative activities, efficiently eliminating excessive intracellular ROS. This resulted in a significant decrease in the release of pro-inflammatory cytokines, consequently leading to a decline in the presence of M1-type macrophages. Furthermore, the Pd@CeO2 nanozyme showed excellent potential in promoting the shift of macrophages toward the M2 phenotype. Additionally, the factors secreted from the cell supernatant of Pd@CeO2-treated macrophages treated with Pd@CeO2 demonstrated anti-inflammatory properties in the chondrocytes located within inflamed synovial joints. These findings offer valuable insights into the advancement of effective enzyme-mimetic therapies for the treatment of OA.
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DOI
PubMed
高影响因子
ChemistrySelect
·
2026
·Vol. 11
·期 10
·e07382
·
IF 2.3
Tong Zhang,Haiyong Wang,Chenguang Wang,Chen Shen,Qiying Liu
Monohydric alcohols are important platform molecules with diverse applications in organic synthesis, pharmaceuticals, food, and polymer industries. The production of monohydric alcohols via the selective hydrogenolysis of diols holds significant scientific and practical value. However, the precise catalytic control of the cleavage of target C–C and C–O bonds remains an open challenge, which often leads to low yields of the target products. Herein, metal-acid bifunctional catalysts were employed to boost the conversion of diols and improve the production of monohydric alcohols through hydrogenolysis. By regulating key reaction intermediates, a maximum yield of 76.2% for 1-propanol and a total monohydric alcohol yield of 84.9% were achieved within a short reaction time of 1 h. Our investigations demonstrate that the composite system of 5% Pd/C and phosphotungstic acid (HPW) catalyzes the conversion of ethylene glycol (EG) and 1,2-propanediol via a metal-acid synergistic effect, which enables the selective cleavage of C–C and C–O bonds. Ethylene glycol and 1,2-propanediol were thus converted to the monohydric alcohols (ethanol, n-propanol, and isopropanol) through hydrogenolysis and dehydration-hydrogenation processes. Additionally, the reaction order and activation energy barriers for the conversion of diols over the 5% Pd/C catalyst were determined experimentally. This work establishes a preliminary method for the production of monohydric alcohols from the hydrogenolysis of small-molecule diols by 5% Pd/C and HPW catalysts. Given the commercial availability of these catalysts, the developed catalytic system exhibits promising practical application potential and may facilitate the scale-up of this reaction. Graphical A 5% Pd/C–phosphotungstic acid (HPW) composite catalyzes the conversion of ethylene glycol and 1,2-propanediol via metal–acid synergy, enabling selective C–C/C–O cleavage. Hydrogenolysis and dehydration–hydrogenation yield ethanol, n-propanol, and isopropanol. Reaction orders and activation energies were determined, linking mechanistic insights to industrial scale-up for biomass diol upgrading.
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高影响因子
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