ACS Catalysis
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2017
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IF 10.614
Chengtao Wang,Zhiqiang Liu,Liang Wang,Xue Dong,Jian Zhang,Guoxiong Wang,Shichao Han,Xiangju Meng,Anmin Zheng,Feng-Shou Xiao
The metal-catalyzed selective hydrogenation of biomass-derived molecules is in great demand but is challenging due to the complex reaction pathways. Herein, we report a persuasive example for achieving selective hydrogenation of furfural over Pd catalysts by controllable sorption of molecules in zeolite micropores. The key to this success is fixation of Pd nanoparticles inside of silicalite-1 zeolite with controllable wettability (Pd@S-1-OH) by functionalizing silanol groups into the zeolite framework. In the hydrogenation of furfural as a model reaction, the Pd@S-1-OH catalyst with appropriate hydrophilicity exhibits extraordinary selectivity for the formation of furan, giving furan selectivity as high as >99.9% with a complete conversion of furfural, outperforming the conventional Pd nanoparticles supported on zeolite crystals (Pd/S-1) and S-1 zeolite fixed Pd catalysts without an artificially functionalized silanol group (Pd@S-1). The extraordinary performance of Pd@S-1-OH is reasonably attributed to the controllable diffusion of molecules within the hydrophilic zeolite micropores, which favors the adsorption of furfural and a series of byproducts but promotes the desorption of furan. Very importantly, Pd@S-1-OH is stable and gives the furan productivity of ∼583.3 g gPd–1 day–1 in a continuous test.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Huizhen Sun,Xiuhua Chen,Shaoyuan Li,Wenhui Ma,Xiumin Chen,Dandan Wu,Kaixin Fu,Mingjun Xiao,Ming Wen
Developing efficient and selective recovery of Pd(II) adsorbents is crucial for addressing environmental pollution issues. Among them, covalent organic framework (COF) and metal organic framework (MOF) composites due to the multi-site functional groups are expected to exhibit excellent Pd(II) adsorption. However, the design and preparation of COF and MOF composite adsorbents for highly efficient adsorption of heavy metal Pd(II) still face many challenges. Herein, we constructed a series of novel core–shell structure UiO-66-NH 2 @TAP-COF (denoted as M@C) adsorbents (M@C-X, X = 1–5, representing different MOF doses) by Schiff base reaction and applied in the adsorption of Pd(II). The findings indicated that the M@C-3 exhibited ultra-high adsorption performance, reaching a capacity of 2134.1 mg/g, and displayed excellent selectivity, making it the best among similar materials. Experimental data and density functional theory (DFT) calculations revealed that the efficient and selective adsorption of Pd(II) is attributed to coordination interaction and strong electrostatic between Pd(II) and the abundant N and O groups in M@C. This work demonstrates the significant potential of the constructed core–shell M@C composites for the efficient and selective recovery of precious metal Pd(II).
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APPLIED ORGANOMETALLIC CHEMISTRY
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2024
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IF 3.7
Xiaohua Zhao,Xiaoxiao Liu,Xiang Liu,Weiyi Li,Ping Wang
Integration of localized surface plasmon resonance (LSPR) metallic nanocrystals into photocatalysis is an intriguing approach for light-driven organic transformations. However, uncertain direction of hot carriers is a grand challenge, which fails to take full advantage of the LSPR excitation. In this work, core–shell gold@ceria nanosphere–supported segregated palladium species (Au@CeO 2 –Pd) have developed to steer the light absorption capability and charge carrier migration. Under simulated solar light irradiation, the core–shell–satellite Au@CeO 2 –Pd exhibited efficient light harvesting and colossal activity in the Suzuki coupling reaction. The plasmon-induced hot electrons overpassed the Schottky barrier at the Au@CeO 2 interfaces and migrated from Au core to CeO 2 shell accordingly. Subsequently, the photogenerated electrons and hot electrons migrated from Au@CeO 2 core–shells to Pd, which acted as an electron acceptor. Detailed photocatalytic mechanism studies revealed that both photoexcited electrons and holes were the main active species involved in the photocatalytic Suzuki coupling reaction process. In particular, the diphenyl yield over Au@CeO 2 –Pd catalyst was ~1.7 times higher than that of core–shell–satellite Au@SiO 2 –Pd, where a 19-nm-thick SiO 2 shell was introduced to prevent the migration of hot electrons. This distinctly certified that the hot electrons transfer in the core–shell–satellite Au@CeO 2 –Pd under illumination played an important role to drive Suzuki reaction. Overall, this design of core–shell–satellite Au@CeO 2 –Pd plasmonic photocatalyst has the potential in the field of photo-driven organic transformations.
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APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Hehe Qian,Yuetan Su,Shu Yan,Wenjun Fang,Kun Yang,Xiaole Weng
Electrocatalytic hydrodechlorination (EHDC) emerges as a promising technology for remediating chlorinated organic pollutants, garnering considerable attention. However, the long-term performance evolution of EHDC, specifically its size-dependent aspect, remains relatively unexplored. This work aims to address this gap by examining Pd nanocubes with controlled sizes of 7.2 nm for Pd Cube-S, 10.6 nm for Pd Cube-M, and 14.7 nm for Pd Cube-L. The specific activity and electrochemical turnover frequency (TOF) of these Pd cubes increased with particle size, a pattern that is inverse to the trend of mass activity. Although Pd Cube-S initially demonstrated heightened EHDC efficiency, a long-term examination over multiple EHDC cycles revealed that Pd Cube-L exhibited escalating mass activity (from 2.10 to 3.11 min −1 g −1 after 5 cycles) and maintained stability over 180 h of continuous electrolysis. This phenomenon arose from structural reorganization of Pd cubes occurring during the EHDC cycles, leading to an expansion of the electrochemically specific surface area. Such structural reorganization brought about more enhancements in large-sized Pd cubes, whereas Pd Cube-S suffered more from particle agglomeration. Consequently, by fine-tuning the particle size, this work provided valuable insights into the long-term EHDC process, offering practical implications for enhancing the durability of Pd nanocatalysts.
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SENSORS
·
2024
·Vol. 24
·期 7
·2110
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IF 3.4
Yinfeng Shen,Yiping Liu,Chao Fan,Qudong Wang,Ming Li,Zhi Yang,Liming Gao
The mature processes of metal oxide semiconductors (MOS) have attracted considerable interest. However, the low sensitivity of metal oxide semiconductor gas sensors is still challenging, and constrains its practical applications. Bimetallic nanoparticles are of interest owing to their excellent catalytic properties. This excellent feature of bimetallic nanoparticles can solve the problems existing in MOS gas sensors, such as the low response, high operating temperature and slow response time. To enhance acetone sensing performance, we successfully synthesized Au-Pd/ZnO nanorods. In this work, we discovered that Au-Pd nanoparticles modified on ZnO nanorods can remarkably enhance sensor response. The Au-Pd/ZnO gas sensor has long-term stability and an excellent response/recovery process. This excellent sensing performance is attributed to the synergistic catalytic effect of bimetallic AuPd nanoparticles. Moreover, the electronic and chemical sensitization of noble metals also makes a great contribution. This work presents a simple method for preparing Au-Pd/ZnO nanorods and provides a new solution for the detection of acetone based on metal oxide semiconductor.
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高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2012
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IF 4.859
Qiao-Xin Zhang,Li-Bing Yin
Spherical Au–Pd bimetallic nanoparticles , for the first time, have been elucidated to have a high electrochemical performance toward As(III) by square wave anodic stripping voltammetry . A strong Pd tuned effect on electrochemical performance in the detection of As(III) was found. A high sensitivity of 3.9 μA/ppb with a low limit of detection (LOD) of 2.40 × 10 − 2 ppb was obtained for Au 1 Pd 3 bimetallic nanoparticle.
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Regenerative Biomaterials
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2024
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IF 5.6
Chen Zhengrong,Mo Quansheng,Mo Dandan,Pei Xiaomin,Liang Anru,Cai Jinhong,Zhou Bo,Zheng Li,Li Hongmian,Yin Feiying,Zhao Jinmin
Injury caused by excess reactive oxygen species (ROS) may lead to susceptibility to bacterial infection and sustained inflammatory response, which are the major factors impeding diabetic wound healing. By utilizing optimal anti-inflammatory, antioxidant, and antibacterial biomaterials for multifunctional wound dressings is critical in clinical applications. In this study, a novel electrospun PLGA/MoS2@Pd nanofiber membrane was synthesized by encapsulating antioxidant and near-infrared (NIR) responsive MOS2@Pd nanozymes in PLGA nanofibers to form a multifunctional dressing for diabetic wound repair. With excellent biocompatibility and hemostatic ability, this novel PLGA/MoS2@Pd nanofiber membrane can effectively reduce oxidative stress damage and intracellular inflammatory factors expression in fibroblasts by scavenging ROS. Additionally, the PLGA/MoS2@Pd nanofiber membrane exhibited favourable NIR-mediated photothermal antibacterial activity in vitro, with inhibition rates of 97.14% and 97.07% against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli), respectively. In a diabetic rat wound infection model, NIR-assisted PLGA/MoS2@Pd nanofiber membrane effectively inhibited bacterial growth in the wound, reduced infection-induced inflammatory response, and promoted tissue epithelialization and collagen deposition, resulting in a wound healing rate of up to 98.5% on day 14. This study highlighted the construction of a multifunctional nanofiber membrane platform and demonstrated its promising potential as a clinical dressing for diabetic wounds.
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ACS Sensors
·
2024
·
IF 8.2
Chengming Sui,Mingxue Zhang,Yueyue Li,Yilin Wang,Yuanzhen Liu,Ziqi Liu,Jihao Bai,Fengmin Liu,Geyu Lu
Bimetallic nanocrystals (NCs) have obtained significant attention due to their unique advantages of the intrinsic properties of individual metals and synergistic enhancements resulting from the electronic coupling between two constituent metals. In this work, Pd@Pt core–shell NCs were prepared through a facile one-pot solution-phase method, which had excellent dispersion and uniform size. Concurrently, ZnO nanosheets were prepared via a hydrothermal method. To explore their potential in nitrogen dioxide (NO2) gas sensing applications, sensitive materials based on ZnO nanosheets with varying mass percentages of Pd@Pt NCs were generated through an impregnation process. The sensor based on 0.3 wt % Pd@Pt-ZnO exhibited remarkable performance, demonstrating a substantial response (Rg/Ra = 60.3) to 50 ppb of NO2 at a low operating temperature of 80 °C. Notably, this sensor reached an outstanding low detection limit of 300 ppt. The enhancement in gas sensing capabilities can be attributed to the sensitization and synergistic effects imparted by the exceptional catalytic activity of Pd@Pt NCs, which significantly promoted the reaction. This research introduces a novel approach for the utilization of core–shell structured bimetallic nanocrystals as modifiers in metal-oxide-semiconductor (MOS) materials for NO2 detection.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yaping Wang,Jie Liu,Chao Liu,Yongwei Lin,Xuefei Duan,Yongfei Ma,Hua Zhang,Muwen Deng,Qian Wang
The heterogeneity of tumors and complex pathways present significant challenges for effective treatment. In response, we developed a multifunctional platform combining photothermal therapy (PTT) and chemodynamic therapy (CDT), PB@Pd nanoparticles (NPs), to enhance the therapeutic efficacy of colorectal cancer. PB@Pd NPs were synthesized by doping palladium (Pd) on the surface of Prussian blue (PB) nanomaterials, enabling synergistic therapeutic effect. PTT generates localized hyperthermia, which accelerates the Fenton-like reaction and promotes the production of reactive oxygen species (ROS) in the tumor microenvironment. Meanwhile, ROS generated by CDT disrupts the tumor’s antioxidant defence system and increases the thermal sensitivity of cancer cells, thus enhancing the efficacy of PTT. This PTT/CDT synergistic approach overcomes the limitations of monotherapies, such as the limited penetration depth of PTT and the inefficiency of CDT in low H 2 O 2 environments. In vitro cellular experiments demonstrated that PB@Pd NPs significantly improved the therapeutic efficacy through synergistic effects. The nanoplatform also has good biocompatibility and stability, reducing the risk of side effects and drug resistance. By integrating PTT and CDT in vivo colon cancer model, PB@Pd NPs offer a promising strategy for more precise, efficient and less toxic tumor therapy, demonstrating their potential in advanced cancer therapies.
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Molecular Catalysis
·
2024
·
IF 3.9
Chi Ma,Zhiyong Zhong,Quanjun Xiang
The photocatalytic efficiency of bismuth-based metal-organic framework (Bi-MOF) is extremely restricted by the rapid recombination of photogenerated electron-hole pairs, which reduce the number of electrons involved in the photocatalytic reduction reaction. Constructing precise interfacial bond bridges between metal nanoparticles (NPs) and MOFs has emerged as an effective strategy to address the above-mentioned issues, promoting the electrons transfer. Herein, this study improves the sluggish dynamics of photogenerated charge in Bi-MOF by inducing the Pd-O-Bi bond bridges at the interface on a Pd NPs-decorated Bi-MOF (Pd/Bi-MOF) nanosheets. This phenomenon results in an interaction between Pd NPs and the Bi-MOF support. And Pd-O-Bi bond bridges provide the fast electron transfer channels, triggering the directional migration of photogenerated electrons from Pd to Bi node, then enhancing the spatial separation of photogenerated electron-hole pairs, finally facilitating overall photocatalytic CO 2 reduction. The presence of these bond bridges leads to higher enhancement in CO production for Pd/Bi-MOF nanosheets compared to the Bi-MOF nanosheets under visible light irradiation after 4.5 h. This research demonstrates the importance of interfacial bond bridges and provides a reasonable guide to design efficient photocatalyst for reduction of CO 2 to CO.
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Particuology
·
2024
·
IF 4.1
Jingchuan Wang,Junhong Luo,Yong Yao,Jiangfeng Song,Yan Shi
To improve room-temperature hydrogen storage, palladium (Pd) nanoparticles were innovatively decorated by carbon bridge onto the amino-group functioned Zr-terephthalate metal-organic framework (MOF) UiO-66 to reduce the diffusion energy barrier and then improve the hydrogen spillover effect. Powder X-ray diffraction shows broad Pd peak and retained UiO-66-NH 2 integrity after Pd decoration. The hydrogen uptake capacity show that UiO-66-NH 2 -Pd exhibits best hydrogen storage performance than UiO-66-NH 2 and pristine UiO-66. The hydrogen up taken in Pd decorated UiO-66 (UiO-66-NH 2 -1Pd) was close to 4 wt% under 20 MPa at room temperature. Density functional theory (DFT) calculations show that hydrogen adsorption energy of UiO-66-NH 2 -Pd was −0.5897 eV, which was much lower than that of UiO-66-NH 2 (−0.3716 eV) and UiO-66 (−0.2975 eV). Ultimately, Pd decorated NH 2 group functioned UiO-66 enable improve storage capacities through hydrogen spillover under ambient conditions which could satisfy the demand for sustainable energy, especially for the long-term storage energy media.
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ACS Catalysis
·
2025
·
IF 13.1
Zhao Wang,Hao Yuan,Jian Tao,Shu-Lin Liu,Ying Hong,Zhi-Yi Hu,Jian Zhang,Bao-Lian Su
Semihydrogenation plays a key role in industrial hydrorefining of light alkenes, with a market above 400 billion by 2027. The high cost of commercial palladium-based catalysts strongly calls for innovation but with great challenges. Herein, copper nanoparticles decorated with a minimized ppm of Pd are developed through a chemical plating process to integrate the catalytic advantages of copper and palladium for achieving maximized catalysis in the semihydrogenation of a fatal impurity of butadiene in alkene feedstocks. The developed Pd–Cu catalyst (i.e., 114 ppm of Pd in Pd0.0033Cu1/TiO2) exhibits an unprecedented catalytic performance superior to commercial Pd/Al2O3, with 100% butene selectivity above 90% of butadiene conversion over 130 h on stream at 90 °C. Further exploration reveals that the atomically dispersed Pd on Cu nanoparticles, obtained at ultralow ppm levels of Pd loading, induces a hidden but critical H2 trap, which concentrates H2 on the Pd site for further H2 dissociation that offers intermediate hydrogen atoms to the tandem butadiene semihydrogenation over the third layer of Cu atoms neighboring Pd through hydrogen spillover. Moreover, a threshold on Pd density was identified at Pd/Cu surficial atomic ratio of 1/138 (i.e., Pd0.0033Cu1/TiO2) for maximizing butadiene semihydrogenation performance, based on an extreme collaboration between Pd for H2 dissociation and Cu for butadiene hydrogenation. This work provides important guidance for developing noble metal-saving catalysts in industrial applications.
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