NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 46
·20367-20374
·
IF 3.288
Dan Zhang,Bowei Wang,Lijuan Yan,Ruixiao Gao,Lu Liu,Ziyi Xia,Xilong Yan,Yang Li,Ligong Chen
Synthesis of an easily separable and efficient catalyst is of great significance for selective hydrogenation of unsaturated functional groups. In this work, novel magnetic flower-like carbonaceous Pd catalysts are constructed for the selective reduction of the CC bond. According to the characterization results, a flower-like architecture is observed in the catalysts containing both Fe3O4 and Pd NPs, which is constructed by the secondary self-assembly in the preparation process due to the interaction between Pd and magnetic nitrogen-doped graphene (Fe3O4-NG). More flower-like structures are formed by increasing the Pd loading amount, further enhancing the specific surface area of the catalyst. The specific surface area of Pd-FONG-3 is the highest (521.17 m2 g−1). Combining the results of characterization and experiments, it is found that the catalytic activity is positively related to the flower-like architecture and the interaction between Pd NPs (6.0 nm) and Fe3O4 NPs (6.7 nm). Fe3O4 is not only beneficial to the magnetic recovery of the catalyst, but also acts as a cocatalyst, which can significantly improve the reactant conversion. Moreover, N species play an important role in protecting the CO bond, resulting in the selective hydrogenation of the CC group. Herein, Pd-FONG-3 exhibits excellent activity in the selective hydrogenation of cinnamaldehyde (CAL) with 99.5% conversion and 96.5% hydrocinnamaldehyde (HCAL) selectivity, and its catalytic performance is much better than that of the commercial 5% Pd/C catalyst (100% conversion and 69.1% HCAL selectivity). This work provides a new strategy to construct highly active catalysts with magnetic recovery properties for selective hydrogenation of CC bonds, and Pd-FONG-3 shows tremendous application foreground.
研究领域:
催化化学
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材料科学
·
纳米技术
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高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 12
·4485-4489
·
IF 8.262
Wei Hong,Peiyan Bi,Changshuai Shang,Jin Wang,Erkang Wang
A simple one-pot synthesis of multi-walled carbon nanotube supported Pd nanocubes is described in this work. Pd nanocubes were in situ grown on carbon nanotubes. The Pd nanocubes show a single-crystal nanostructure and an average diameter of about 9.6 nm. The use of KBr is essential for the formation of Pd nanocubes; without KBr, only irregular Pd nanoparticles can be generated. The structural properties and electronic states of the prepared Pd nanocubes were studied by transmission electron microscopy and X-ray photoelectron spectroscopy, respectively. The developed nanomaterials present enhanced electrocatalytic activity which is 1.3 times and 1.75 times higher than that of their counterpart multi-walled carbon nanotube supported Pd nanoparticles and a commercial Pd/C reagent, respectively, for formic acid electrooxidation.
研究领域:
材料科学
·
电化学
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高影响因子
Catalysis Science & Technology
·
2013
·Vol. 3
·期 10
·2620-2626
·
IF 3.753
Chunhui Chen,Ensheng Zhan,Na Ta,Yong Li,Wenjie Shen
Pd nanocubes of 6–19 nm in size were synthesized using a seeded growth method and examined for enantioselective hydrogenation of α,β-unsaturated carboxylic acids. It was found that the Pd nanocubes had two types of active sites on the planes and at the edges, respectively. Small nanocubes having a higher edge/plane ratio were more active in enantioselective hydrogenation of α,β-unsaturated carboxylic acids, but afforded a lower enantioselectivity because their sharp edges could not offer stable adsorption of the chiral modifier and the reaction intermediates. In contrast, large nanocubes with a higher fraction of flat planes provided a higher enantioselectivity but a much lower activity.
研究领域:
化学
·
纳米材料科学
·
催化反应
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高影响因子
International Journal of Electrochemical Science
·
2023
·Vol. 10
·期 9
·7783-7793
·
IF 1.5
Fen Wang,Xian Jing Yang,Qi Guo Chen,Mei Chao,Chun An
Pd/Ag/Cu electrode was successfully prepared on Ag dendrites with Cu substrate (Ag/Cu) by galvanic replacement reactions, and was characterized by scanning electron microscopy, X-ray diffraction and transmission electron microscopy. The electroreductive dechlorination reaction of 2,3-dichlorophenol on Pd/Ag/Cu electrode was investigated by cyclic voltammetry and in situ FTIR techniques. Compared with Pd/Cu, Ag/Cu and Cu electrodes, Pd/Ag/Cu electrode exhibited the highest electrocatalytic activity for electroreductive reaction of 2,3-dichlorophenol. C-Cl bond was broken by reaction of adsorbed 2,3-dichlorophenolate with (H) ads Pd on Pd/Ag/Cu electrode surface. The main intermediate was 2-chlorophenolate, and the final product was phenolate.
研究领域:
环境化学
·
电催化
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材料科学
·
分析化学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2021
·
IF 3.171
Chunhua Zhang,Zhengyan Qu,Hong Jiang,Rizhi Chen,Weihong Xing
Phenol hydrogenation is a green route to prepare cyclohexanone, an intermediate for the production of nylon 66 and nylon 6. The development of high-performance catalysts still keeps a great challenge. Herein, the activated carbon (AC) was modified with an acidic material Nb 2 O 5 to adjust the microstructure and surface properties of AC, and the influences of the calcination temperature and Nb 2 O 5 content on the catalytic performance of the Pd/AC-Nb 2 O 5 catalysts for the phenol hydrogenation to cyclohexanone were investigated. The Nb 2 O 5 with proper content can be highly uniformly distributed on the AC surface, enhancing the acidity of the Pd/AC-Nb 2 O 5 catalysts with comparable specific surface area and Pd dispersion, thereby improving the catalytic activity. The hybrid Pd/AC-10Nb 2 O 5 -500 catalyst exhibits the synergistic effect between the Pd nanoparticles and AC-10Nb 2 O 5 , which enhances the catalytic activity for the hydrogenation of phenol. Furthermore, the as-prepared Pd/AC-10Nb 2 O 5 -500 catalyst shows good reusability during 7 reaction cycles.
研究领域:
化学工程
·
催化材料
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Jiayu Jin,Shuozhen Hu,Xinsheng Zhang,Shigang Sun
Palladium is a promising formic acid electro-oxidation (FAO) catalyst due to its higher initial activity than platinum. However, suffering from the adsorption of hydrogen and CO-like species, the activity and stability of Pd are still unsatisfied. Herein, palladium nanoparticles deposited on carbon supported molybdenum trioxide (Pd–MoO 3 /C) is prepared with MoO 3 as the promoter for FAO. X-ray photoelectron spectroscopy analysis proves the close contact between Pd and MoO 3 , which generates the hydrogen spillover effect and forms the Pd–Mo structure. The hydrogen spillover effect enhances the desorption of hydrogen from Pd and facilitates the FAO activity. Both the spillover effect and Pd–Mo structure contribute to the removal of CO ad and facilitate the durability and anti-CO poisoning ability of the catalyst. With the optimized ratio of MoO 3 to carbon black, the Pd–MoO 3 /C-20 catalyst owns the best specific activity of 5.86 mA cm −2 , which is 1.86 times of Pd/C.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Ying Wang,Wanying Xiong,Yiyan Xu,Nan Yang,Huige Zheng,Qian Zhao,Xiaojing Liang,Huishuang Yin,Yunyan Zhang,Wenhu Zhou,Liangsheng Fan
Acid-responsive aPD-L1@CaP/A23187 enhances PD-L1 checkpoint blockade. • CaP nanoparticles encapsulate aPD-L1 and release it selectively in acidic TME. • Ca²⁺ from CaP synergizes with A23187 to boost Ca²⁺ influx and immune signaling. • The formulation elevates intracellular Ca²⁺, promotes DC maturation, and M1 polarization. • In vivo, it increases tumor accumulation, inhibits growth, reverses TME, and induces immune memory. Immune checkpoint inhibitors (ICIs) targeting the PD-1/PD-L1 axis have revolutionized cancer therapy, but their efficacy is restricted by the highly immunosuppressive tumor microenvironment and is often accompanied by systemic toxicities.To overcome these limitations, we developed a novel acid-responsive nanoplatform, aPD-L1@CaP/A23187, integrating anti–PD-L1 antibodies (aPD-L1) with calcium phosphate (CaP) nanoparticles and the Ca 2+ ionophore A23187. CaP nanoparticles encapsulated aPD-L1 with high efficiency and stability, enabling tumor-specific release under acidic conditions while minimizing systemic distribution. Simultaneously, Ca 2+ released from CaP synergized with A23187 to promote transmembrane Ca 2+ influx, thereby activating downstream Ca 2+ signaling pathways in immune cells. In vitro, this formulation increased intracellular Ca 2+ levels, induced dendritic cell maturation, and polarized macrophages toward the pro-inflammatory M1 phenotype. In vivo, aPD-L1@CaP/A23187 achieved ∼7.4-fold higher tumor enrichment than free antibody, exhibited potent tumor suppression in TC-1 tumor–bearing mice. Mechanistic studies revealed enhanced dendritic cell activation, robust CD8 + T cell infiltration and granzyme B secretion, reduced Treg proportions, and M1 macrophage polarization, collectively reversing the immunosuppressive tumor microenvironment. Importantly, treatment also induced durable effector memory T cell responses in a distant tumor model, providing protection against tumor recurrence and metastasis. These findings highlight the Ca 2+ -assisted nanoplatform offers a broadly applicable strategy for next-generation cancer immunotherapy.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Faisal Irshad,Dan Zhang,Hamzah A.S.M. Yaseen,Xianming Zhu,Muhammad Chawla,Shengping Wang,Yongli Shen,Xinbin Ma
Pd/H-MOR exhibits superior catalytic activity and stability for CO 2 hydrogenation to formateover other Pd/Zeolites and M/H-MOR. • Brønsted acid sites at Pd-H-MOR interface polarize CO 2 , while highly dispersed Pd nanoparticles dissociate H 2 barrierlessly. • Low Si/Al ratio optimizes metal-support synergy and reducing apparent activation energy to HCOOH. • Bicarbonate identified as the key reaction intermediates by in-situ DRIFTS and DFT study. Catalytic hydrogenation is a promising route for CO 2 conversion, yet the highly efficient formation of formic acid remains challenging. Herein, Pd nanoparticles dispersed on mordenite (Pd/H-MOR) are reported as an efficient and stable catalyst for CO 2 hydrogenation to produce formates. Under optimized conditions, Pd/H-MOR achieved an intrinsic turnover number of 1828 and a turnover frequency of 914 h −1 at 120 °C, surpassing all the other prepared catalysts with different metal active sites and zeolite supports. The high activity arises from the co-effect of Pd and the H-MOR support: Pd sites dissociate H 2 into active hydrogen, while Brønsted acid sites enhance CO 2 adsorption via polarization and stabilize bicarbonate intermediates, which subsequently convert to formates. Density functional theory (DFT) results revealed that Pd/H-MOR lowers the activation barriers for both H 2 dissociation and CO 2 activation at the Pd-MOR interface and combined with in-situ DRIFTS, identifying surface bicarbonates as the key reactive intermediates en-route to formate formation. Comparatively, kinetic studies of Pd/H-MOR revealed a reduced apparent activation energy of 15.81 ± 0.79 kJmol −1 , reflecting strong metal-support interactions, while the observed R = k ∙ P CO 2 0.56 ∙ P H 2 0.62 reaction orders indicate that the reaction rate is weakly dependent of H 2 and CO 2 pressures but strongly dependent on the nature of the metal and the zeolite support. This work highlights metal dispersion and support acidity as key factors for CO 2 hydrogenation. Download: Download high-res image (224KB) Download: Download full-size image
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高影响因子
ACS Applied Nano Materials
·
2026
·Vol. 9
·期 30
·14592-14602
·
IF 5.8
Mu Yueru,Lian Rui,Zhang Jingjing
Silver ions (Ag + ) pose significant ecological
and health
risks due to their toxicity and potential for bioaccumulation. While
conventional detection methods such as ICP-MS and AAS offer high sensitivity,
they are often hindered by complex operations, high costs, and limited
suitability for on-site analysis. To address this, we developed a
highly active and selective colorimetric sensor for Ag + based on a DNA-encoded Pd/DNA/CeO 2 nanozyme. Cerium oxide
nanorods (CeO 2 ) serve as an effective support for the directional
immobilization of single-stranded DNA through phosphate-Ce 4+ coordination and electrostatic interactions. The DNA template guides
the uniform in situ growth of palladium nanoparticles (Pd NPs), forming
a well-dispersed and highly exposed catalytic interface. The resulting
Pd/DNA/CeO 2 nanozyme exhibits enhanced peroxidase-like
activity, catalyzing the oxidation of 3,3 ′ ,5,5 ′ -tetramethylbenzidine
(TMB) in the presence of H 2 O 2 . Ag + ions are specifically reduced on the Pd surface to form a metallic
Ag layer, which effectively blocks the active sites and quenches the
catalytic activity, enabling a “switch-off” detection
mode. The optimized sensor shows a wide linear response to Ag + from 50 to 400 nM with a detection limit of 22.7 nM. It also
demonstrates excellent selectivity against common interfering ions
and good applicability in real water samples. This DNA-encoded nanozyme
design provides a robust and facile platform for the on-site monitoring
of trace Ag + in environmental systems.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Jian Zhang,Jieqiong Zhao,Caifeng Qi,Zhe An,Yanru Zhu,Xin Shu,Hongyan Song,Jing He
Oxidative carbonylation of ethanol to diethyl carbonate (DEC), an essential electrolyte for lithium-ion battery, has attracted broad interest from both academia and industry in recent years. But high selective formation of DEC is a great challenge due to the difficulty in efficient activation of CO at the same time as the site-specific activation of O—H bond in ethanol. Herein, we propose a Pd-Cu x O synergetic catalysis toward oxidative carbonylation of ethanol, where the synergy between Pd and Cu x O promotes CO activation and carbonylation, thus increasing the selectivity to the site-specific activation of O-H bond in ethanol. A nitrogen-doped carbon nanotubes supported Pd-Cu x O (Pd-Cu x O/NCNTs) has been designed via galvanic displacement of Pd on Cu x O to form the strong interactions between Pd and Cu x O, affording a selectivity of 94.7 % to DEC and a space-time yield (STY) of up to 5966 mg∙g –1 ∙h –1 , which is an order of magnitude higher than that reported in the literatures. This work offers novel insights for the design of highly efficient catalysts and advances the industrial development for the oxidative carbonylation of ethanol.
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高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Weijie Jia,Haifeng Wang,Chen Xue,Yaying Li,Qi Xiao
Selective hydrogenation of phenylacetylene is a crucial industrial reaction, yet developing catalysts with both high selectivity and activity remains challenging. Conventional hydrogenation catalysts often exhibit unevenly dispersed active metals, leading to agglomeration and reduced catalytic performance. Herein, with the aid of the ice-templating (ICT) strategy, we present TiO2-supported Pd nanocluster photocatalysts with ultralow Pd loading (0.1 wt %). The optimized Pd/TiO2–ICT catalyst achieves exceptional catalytic performance under ambient conditions (room temperature and atmospheric pressure) with methanol solvent and light irradiation, delivering 99% phenylacetylene conversion alongside 98% styrene selectivity. Advanced characterization reveals the catalyst’s superior structural features, including ultrasmall Pd clusters (1.2 nm diameter) and reduced Pd–Pd coordination number (6.3), which are significantly better than conventional counterparts. Systematic investigations establish a clear positive correlation between catalytic efficiency and critical structural parameters: smaller cluster dimensions and lower metal coordination numbers at equivalent Pd loadings. Mechanistic studies through comprehensive characterization elucidate that the photogenerated hydrogen radicals (•H) from methanol splitting directly drive the selective hydrogenation process. This study offers insights into both the application and structure–activity relationship of the ICT-based catalysts.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Lu Wang,Shanshan He,Xuedong Zhang,Guoshuai Liu
The atomic-local environment of catalytic sites plays a pivotal role in breaking robust C−Cl bonds during electrochemical dechlorination of organic chlorides (OCs). Herein, we propose a novel strategy to tailor the microstructure of carbon nanotubes (CNTs) via ball-milling, which induces controlled cleavage at crossing points to generate abundant tip structures. These high-curvature tips serve as preferential anchoring sites for Pd nanoparticles (Pd/BCNTs), enabling precise modulation of the local atomic environment. The optimized Pd/BCNTs electrocatalyst achieves exceptional performance, degrading 98.1 % of chloramphenicol (CAP) within 40 min and achieving ∼97.8 % dechlorination efficiency at −1.2 V vs. SCE, with a Faradaic efficiency for Cl − (FE Cl ) of 6.16 %. In contrast, conventional Pd/CNTs only removed 73.3 % of CAP with a lower FE Cl (3.32 %) and dechlorination rate (60.7 %). Mechanistic studies reveal that the tip-enhanced microenvironment boosts direct electron transfer (DET contribution: 60.30 % vs. 37.6 % for Pd/CNTs) and amplifies atomic hydrogen (H*) generation, as evidenced by a hydrogen adsorption charge (Q H ) of 75.40 mC that is 2.1 times higher than that of Pd/CNTs (35.91 mC). Finite element analysis (FEA) simulations confirm that the sharp tips concentrate electric fields and current density, accelerating water dissociation and interfacial electron transfer. This work advances the rational design of cost-effective electrocatalysts by leveraging microstructure engineering to synergize direct and indirect dechlorination pathways, offering a promising route for eliminating persistent organic pollutants.
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高影响因子
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