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
·
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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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yakai Chen,Xinya Feng,Xiaohan Yu,Xingliang Xu,Jing Xu
Catalytic transfer hydrogenation of nitro compounds to amines under mild conditions offers an alternative strategy to traditional hydrogenation processes involving pressurized molecular hydrogen, which necessitate the rational design and integration of multifunctional catalyst. Herein, a ternary composite catalyst (Pd/CeO 2 -C 3 N 4 ) was designed and synthesized for the transfer hydrogenation of nitro compounds to corresponding amines compounds using formic acid as hydrogen donor. The Pd/CeO 2 -C 3 N 4 catalyst shows remarkably high performance for the catalytic transfer hydrogenation of nitrobenzene (NB) to aniline (BA), achieving > 98 % conversion and exceedingly high selectivity (>99 %). The catalyst exhibits a high turnover frequency (TOF) of up to 2868 h - , significantly surpassing both the reference catalyst (Pd/C 3 N 4 and Pd/CeO 2 ) and the conventional Pd/C catalyst. The multi-functional Pd/CeO 2 -C 3 N 4 catalyst features enhanced electron transfer properties,well-exposed Pd active sites, and abundant acid-base sites, enabling effective enhancement of formic acid dehydrogenation and nitro group activation. Moreover, Pd/CeO 2 -C 3 N 4 demonstrates excellent recyclability and a broad substrate scope for the catalytic transfer hydrogenation of various nitro compounds. The rational design of Pd/CeO 2 -C 3 N 4 will broaden the application range of Pd-based catalysts and provide a sustainable and effective approach for the catalytic transfer hydrogenation of other industrially relevant organic compounds.
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DOI
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
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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
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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
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纳米技术
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分析化学
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材料科学
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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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DOI
高影响因子
CARBON
·
2022
·
IF 11.307
Lizhen Hu,Teng Wang,Qianqian Nie,Jiayou Liu,Yunpei Cui,Kefei Zhang,Zhongchao Tan,Hesheng Yu
Efficient, stable, and selective photocatalytic conversion of nitric oxide (NO) into nitrogen dioxide (NO 2 ) is highly desirable but remains a big challenge. We prepare single atom catalyst (SAC) by anchoring single Pd atoms onto graphitic carbon nitride (CNPd) via chemical impregnation followed by calcination . The prepared CNPd SAC is confirmed by aberration-correction high-angle-annular-dark field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy. The synthesized SAC outperforms its competitors reported earlier for photocatalytic removal of NO under visible light and simulated sunlight irradiation in terms of selectivity and stability. The SAC maintains a NO removal efficiency of 83% and an instantaneous selectivity for NO 2 of 92.8% over 117.6 h under simulated sunlight with the inlet NO concentration of 12 ppm. This duration is about 23.5 times the longest duration tested for other catalysts in the literature. The experimental results and density functional theory (DFT) calculations reveal that single Pd atom promotes the photocatalytic degradation of NO. Moreover, the DFT calculations prove that the nitrate ions that accumulate on the surface of the SAC can react with NO to produce NO 2 . This reaction enhances the selectivity for NO 2 and stability of the SAC.
研究领域:
环境科学
·
材料科学
·
化学
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DOI
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
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DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 20
·6732-6741
·
IF 6.119
Yafeng Chen,Guimin Jiang,Xiangzhi Cui,Zuotai Zhang,Xinmei Hou
Eliminating indoor formaldehyde (HCHO) pollution at room temperature is highly needed to improve the environment while saving energy. Herein, Pd/CeO2 catalysts with different morphologies of the CeO2 support were employed to investigate their performance for HCHO oxidation. The Pd/CeO2 nanocube (Pd/CeO2-C) catalyst exhibited excellent catalytic activity compared to commercial CeO2 and CeO2 nanorods. HCHO can be completely converted into CO2 and H2O over the Pd/CeO2-C (0.64 wt% Pd) catalyst at a weight hourly space velocity of 36 000 mL g−1 h−1 at room temperature. Multiple characterization results confirmed that the strong interfacial interaction between Pd and the CeO2-C support guarantees a high percentage of metallic Pd on the CeO2-C surface and its high dispersion, which is crucial for the oxidation of formaldehyde at low temperature. The in situ diffuse reflectance infrared Fourier transform results indicated that CO, formate and dioxymethylene species are the main intermediates over the Pd/CeO2-C catalyst, and the active O species is responsible for their decomposition and oxidation. This work may promote the practical application of high performance Pd-based catalysts for indoor HCHO purification and related catalytic processes.
研究领域:
环境科学
·
催化化学
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DOI
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
Molecular Catalysis
·
2024
·
IF 3.9
Yu Chen,Ming-Yu Qi,Zi-Rong Tang
Integrating selective organic transformation and hydrogen (H 2 ) evolution in one photoredox reaction system is one of the most sustainable and promising approaches to efficiently produce solar fuels and chemicals by simultaneously utilizing photogenerated electrons and holes. Herein, through the cation-exchange engineering method, the nanoleaf-like Pd/CdS composites are gingerly fabricated for visible-light-driven receptor-free dehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to 3,4-dihydroisoquinoline (DHIQ) and H 2 under ambient conditions. The optimized electronic structure endows Pd/CdS with a narrow band gap and suitable energy band positions, thus facilitating the light harvesting as well as the separation and transfer of photoexcited charge carriers. Consequently, the Pd/CdS exhibits significantly improved photoredox activity compared to bare CdS . In-situ Fourier-transform infrared spectroscopy and electron paramagnetic resonance spectroscopy track the progression of reaction intermediates during such a dual-functional photoredox-catalyzed system, revealing that the carbon-centered radical is the key reaction intermediate in this reaction process. It is anticipated that this work would guide the rational utilization of CdS-based materials to enable simultaneous photochemical coupling of organic transformation and H 2 evolution.
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