RSC Advances
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2015
·Vol. 5
·期 14
·10352-10357
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IF 3.84
Zhen Sun,Qingshan Zhao,Guanghui Zhang,Yang Li,Guoliang Zhang,Fengbao Zhang,Xiaobin Fan
Au–Pd bimetallic nanoparticles (NPs) with core–shell structures have been successfully anchored on chemical exfoliated MoS2 (Au–Pd/MoS2) through a facile co-reduction method at room temperature. The Au–Pd/MoS2 hybrids were characterized by X-ray diffraction (XRD), scanning electronic microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), energy dispersive X-ray spectroscopy (EDX) and X-ray photoelectron spectroscopy (XPS). The pristine MoS2 nanosheets exhibit some peroxidase-like activity for the oxidation of 3,3,5,5-tetramethylbenzidine (TMB), and their catalytic activity is significantly enhanced by the deposition of Au–Pd NPs. A systematic study revealed that Au–Pd NPs with a mass ratio of 1 : 2 on MoS2 (Au1.0Pd2.0/MoS2) showed the highest catalytic activity compared with other counterparts. This excellent performance of the Au1.0Pd2.0/MoS2 hybrids should be ascribed to not only the intrinsic catalytic activity of MoS2, but also the complicated metal–metal and metal–support interactions.
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ELECTROCHIMICA ACTA
·
2014
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IF 4.086
Jing-Jing Lv,Jie-Ning Zheng,Li-Li Chen,Meng Lin,Ai-Jun Wang,Jian-Rong Chen,Jiu-Ju Feng
In this work, a one-pot solvothermal method was developed for large-scaled synthesis of well-defined bimetallic alloyed Pt-Pd nanocubes uniformly supported on reduced graphene oxide nanosheets (Pt-Pd nanocubes/RGOs). Herein, poly(vinylpyrrolidone) (PVP) and KI were employed as a capping agent and a structure-directing additive, respectively, and N , N -dimethylformamide (DMF) is used as a solvent and a reducing agent. The as-prepared Pt-Pd nanocubes/RGOs exhibited the enlarged electrochemically active surface area, enhanced electrocatalytic activity, and improved stability for ethanol oxidation reaction (EOR) and oxygen reduction reaction (ORR), compared with commercial Pt-C (10 wt %).
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 6
·2619-2628
·
IF 8.867
Yuzhen Zhu,Zaixiang Xu,Wenya Jiang,Shuxian Zhong,Leihong Zhao,Song Bai
The utilization of a metal cocatalyst is a promising route to improve the solar-to-chemical conversion efficiency of semiconductor-based photocatalysts. The efficiency of the improvement is greatly dependent on the architectural structure of the metal cocatalysts, especially the catalytically active sites on the surface of the cocatalysts. In this article, Pd nanosheets with different sizes have been hybridized with TiO2 nanosheets to disclose how the edge of Pd cocatalysts influences the photocatalytic performance of TiO2–Pd hybrid structures in the reduction of CO2 to fuels. It was found that the highest photocatalytic activity was realized by small Pd nanosheets with the highest edge density on the TiO2 nanosheets. The reason is that the edges of the nanosheets act as the highly active sites for the CO2 reduction reaction. To further verify the edge-dependent photocatalytic performance, Pd nanorings were also deposited on the TiO2 nanosheets, which further improve the photocatalytic activity as compared with original nanosheets resulting from the additional edge sites exposed on the side of the hollow interior in the rings. This work underlines the importance in the edge engineering on the surface of cocatalysts in realizing high-performance photocatalytic applications.
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CHEMOSPHERE
·
2024
·
IF 8.1
Juan Qiao,Zhenyu Zhao,Zhengwei Zhou,Deli Wu
Palladized iron (Pd/Fe) represents one of the most common modification strategies for nanoscale zero-valent iron (nZVI). Most studies prepared Pd/Fe by reducing iron salts and depositing Pd species on the surface of pre-synthesized nZVI, which can be called the two-step method. In this study, we proposed a one-step method to obtain Pd/Fe by the concurrent formation of Fe 0 and Pd 0 and investigated the effects of these two methods on 4-chlorophenol (4-CP) removal, with carboxymethylcellulose (CMC) coated as a surface modifier. Results indicated that the one-step method, not only streamlined the synthesis process, but also Pd/Fe-CMC one-step , synthesized by it, exhibited a higher 4-CP removal rate (97.9%) compared to the two-step method material Pd/Fe-CMC two-step (82.4%). Electrochemical analyses revealed that the enhanced activity of Pd/Fe-CMC one-step was attributed to its higher electron transfer efficiency and more available reactive species, active adsorbed hydrogen species (H ads *). Detection of intermediate products demonstrated that, under the influence of Pd/Fe-CMC one-step , the main route of 4-CP was through hydrodechlorination (HDC) to form phenol and H* was the main active specie, supported by EPR tests, quenching experiments and product analysis. Additionally, the effects of initial 4-CP concentration, initial pH, O 2 concentration, anions such as Cl − , SO 4 2− , HCO 3 − , and humic acid (HA) were also investigated. In conclusion, the results of this study suggest that Pd/Fe-CMC one-step , synthesized through the one-step method, is a convenient and efficient nZVI-modifying material suitable for the HDC of chlorinated organic compounds.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Junxin Guo,Zhenyu Wang,Tongtong Gao,Zhao Wang
Binary Pd/In 2 O 3 and Pt/In 2 O 3 catalysts exhibit technological potential in CO 2 methanol synthesis. However, the key to achieving high productivity lies in resolving the unfavorable Pd-In alloy and Pt nanoparticles formation during the reaction. In this study, we present the surface restructuring of Pd-Pt/In 2 O 3 catalysts under CO 2 hydrogenation conditions. Detailed quasi-operando characterization and theory calculation reveal stable reconstruction driven by Pt with Pd. The bimetallic Pd-Pt inhibits the formation of both Pd-In alloy and Pt nanoparticles. Moreover, this restructuring process generates more oxygen vacancies during the reaction. These oxygen vacancies promote electron transfer from the indium oxide surface to the Pd-Pt clusters. Consequently, a shift occurs from interface-induced CO 2 adsorption to cluster-induced adsorption. Thereby, the STY of methanol on Pd-Pt/In 2 O 3 at 300 °C increased by approximately 20 % compared to that on Pd/In 2 O 3 along. The findings highlight the crucial role of component-induced restructuring and oxygen vacancies in influencing the change of adsorption sites.
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JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 46
·21265-21276
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IF 3.5
Zhang Kewen,Fan Benwei,Wang Shidong,Zhang Hongwei,Liu Qunhong,Bao Xiaojun,Yuan Pei
Heterogeneous hydrogenation is an effective way to improve the performance of unsaturated polymers, but the preparation of supported catalysts with high metal dispersion and stability remains challenging. Herein, we synthesize a SiO 2 -based support wrapping with carbon nitride on the surface (CN x @SiO 2 ) via the thermal polycondensation of melamine, on which Pd nanoclusters with highly exposed active sites are formed and stably anchored via the strong interaction between N and Pd. The thermal temperature affects the properties of CN x , which further modulates the electronic and structural state of Pd nanoclusters. The Pd/CN x @SiO 2 -500 catalyst, prepared at 500 °C with an optimal CN x structure ( g -C 3 N 4 ) and high nitrogen content, features highly dispersed and electron-rich Pd nanoclusters (1.3 nm). This catalyst exhibits a hydrogenation activity of 98.0% for nitrile rubber, with a selectivity of 100% for C=C bonds. This work provides a facile method to prepare Pd catalysts with high activity and stability, paving the way for the upgrading of unsaturated polymers via hydrogenation. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Kefa Sheng,Hongyu Xia,Jianping Ge
Selective hydrogenation of nitroaromatics is a crucial industrial reaction, but there are still challenges in developing nanocatalysts with stable active centers, yet easily recyclable characteristics. Here, a magnetically separable Pd/Fe 3 O 4 @SiO 2 nanocatalyst was prepared through the seeding growth of silica on the Fe 3 O 4 nanocrystal cluster (NC) followed by in situ reduction of Pd nanoparticles (NPs) on the amino group modified Fe 3 O 4 @SiO 2 nannotube (NT). The nanocatalyst showed good activity and stability in the hydrogenation of a series of nitroaromatics as the Pd NPs were highly dispersed on the nanotubes. Meanwhile, it could be easily separated from the reaction solution and well-redispersed in the solvent for the next-round reaction due to the superparamagnetic property of the Fe 3 O 4 NC and the good dispersibility of silica in many organic solvents. The magnetically separable nanocatalyst combined the high activity of the nanocatalyst and the convenient separation of a traditional heterogeneous catalyst, which effectively promote the practical application of nanomaterials in catalysis.
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CHEMISTRY-A EUROPEAN JOURNAL
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2024
·
IF 3.9
Bo Zhao,Yao Yao,Kexin Huang,Jiaxin Li,Minjie Chen,Chao Liu,Hongjian Xu,Xinyu Zhao,Ganggang Chang
The selective hydrogenation of furfural (FFA) to furfuryl alcohol (FA) is regarded as attractive transformation to achieve the sustainable synthesis of value-added chemicals from biomass resources. However, the conventional supported catalysts are significantly restricted by their narrow pore size, ununiform dispersion and easy leaching or aggregation of catalytic sites. Herein, we designed hollow UiO-66-NH2 as the support to encapsulate Pd nanoparticles (Pd@H-UiO-66-NH2) to achieve the highly active and selective conversion of FFA to FA. Benefiting from the void-confinement effect and substrate enrichment of hollow structure, as well as the surface wrinkles, the as-prepared catalyst Pd@H-UiO-66-NH2 exhibited 96.8 % conversion of FFA with satisfactory selectivity reaching up to 92.4 % at 80 °C, 0.5 MPa H2 in isopropanol solvent within 6 h. More importantly, as-prepared Pd@H-UiO-66-NH2 catalyst exhibited excellent long-term stability, as well as good universality toward a series of hydrogenation of unsaturated hydrocarbons.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Lijun Yue,Wanjun Zhao,Jinfang Li,Ruifang Wu,Yongzhao Wang,Hongxi Zhang,Yongxiang Zhao
The impact of Indium (In) doping upon the catalytic performance of Pd-Cu/Al 2 O 3 for carbon monoxide preferential oxidation (CO-PROX) in hydrogen (H 2 ) rich atmosphere at low temperature has been studied. A series of catalysts with extremely low palladium (Pd) loading (0.06 wt%) are synthesized by the facile co-impregnation method. When the In/copper (Cu) atomic ratio equals 0.25, Pd-Cu-In 0.25 /Al 2 O 3 can keep 40% CO conversion and 100% carbon dioxide (CO 2 ) selectivity at least 120 min at 30 °C, which is significantly superior to the catalytic performance of Pd-Cu/Al 2 O 3 . The elaborate characterization findings reveal that the added In species to Pd-Cu/Al 2 O 3 causes Indium oxide (In 2 O 3 ) to generate, which produces the interaction of In 2 O 3 with Pd-Cu/Al 2 O 3 , further promoting the dispersion of copper chloride hydroxide (Cu 2 Cl(OH) 3 ). Moreover, the modification of In facilitates the re-oxidation of Pd 0 to Pd + through reducing the formation of palladium hydride (PdH x ) during the CO-PROX reaction. Meanwhile, the addition of In leads to the decrease of Cu + electron cloud density, making it easier to be oxidized to Cu 2+ . Collectively, the easy re-oxidation of Pd 0 and Cu + is favorable to fulfill the Wacker cycle between Pd and Cu species, thus improving the catalytic performance for CO-PROX.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Hualei Wang,Cong Xi,Huiming Yin,Yi Ding
Conventional strategies for developing highly efficient electrocatalysts involve enhancing thermodynamics to minimize overpotential and improving kinetics to maximize reaction current. However, current research on Pd-based catalysts for formic acid oxidation reaction (FAOR) mainly focuses on accelerating its kinetics to increase the peak current. This study proposes a catalyst design that can simultaneously improve the kinetics and thermodynamics of FAOR. Specifically, the home-made catalyst (NPG-Pt 1 -Pd 1 ) is obtained by sequentially depositing monolayer Pt and Pd shells on the surface of nanoporous gold (NPG) substrate. Compared with commercial Pd/C, this electrocatalyst exhibits a noticeable negative shift in onset potential (∼100 mV) and a significantly improved peak current (∼6 times). Experimental data and theoretical calculations demonstrate that NPG-Pt 1 -Pd 1 exhibits a comparatively suitable adsorption energy for small molecules, not only reducing the overpotential but also accelerating the reaction rate of FAOR. Moreover, when applied in direct formic acid fuel cells (DFAFC), the NPG-Pt 1 -Pd 1 anode with an exceptionally low Pd loading of 8.5 μg cm −2 , achieves a remarkable power density of 141 mW cm −2 . The power efficiency of Pd is 230 times that of Pd/C (1 mg cm −2 , 73 mW cm −2 ). Therefore, this work provides a new methodology for developing efficient Pd-based FAOR electrocatalysts .
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yuxuan Wei,Zuxiao Chen,Chuyu Huang,Hong Cheng,Xiaofeng Jiang,Shiying Li
Spatiotemporal downregulation of immune checkpoint provides a promising strategy to activate anti-tumor immunity. In this work, a breast cancer targeted photodynamic degrader (designated as EIpro) is constructed to activate immunotherapy through EGFR degradation mediated PD-L1 downregulation. To be specific, we develop a chimeric peptide, comprising the photosensitizer Protoporphyrin IX (PpIX) and EGFR targeting peptide (QRHKPRE), to encapsulate an EGFR inhibitor afatinib (AFA) forming nanomicelle, namely EIpro. EIpro has a favorable stability and uniform nanosize distribution, preferring to accumulate in EGFR overexpressed breast cancer cells to amplify the chemotherapeutic effect and photodynamic elimination behavior. More interestingly, photodynamic therapy (PDT) produced reactive oxygen species (ROS) is able to damage breast cancer cells and induce immunogenic cell death (ICD) to release tumor associated antigens (TAAs), thereby degrading the nearby EGFR to downregulate PD-L1 and activate anti-tumor immunity. Beneficially, the multi-synergistic effects of EIpro show a robust therapeutic efficacy against primary and metastatic breast cancer with negligible systemic toxicity. This work provides a spatiotemporal strategy for protein degradation, which might inspire the development of sophisticated nanomedicine for effective tumor treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Kai Guo,Hui Liu,Mengmeng Zhang,Nengyi Ni,Mengyao Mu,Ke Ren,Jiahui Chen,Qing Fan,Xueli Xu,Xiao Sun,Ximing Wang
Low-dose radiotherapy can lead to upregulation of PD-L1 expression in tumor cells, limiting the effectiveness of radio-immunotherapy. Currently, anti-PD-L1 drugs only disrupt the interaction of the PD-1/PD-L1 axis on the cell surface, without considering the immune regulatory ability of intracellular PD-L1. Additionally, antibody-bound PD-L1 can lead to internalization and recycling, allowing tumor cells to regain immune suppression. In this study, a novel PD-L1-affibody (Z PD-L1 )-grafted gadolinium-palladium nanoplatform incorporated with glucose oxidase (GOx) (GPGP) was fabricated to improve tumor-targeted magnetic resonance imaging (MRI) and synergistic radio-immunotherapy. GPGP with catalase- and peroxidase-like activity could catalyze the generation of oxygen to relieve tumor hypoxia and the generation of •OH to boost ferroptosis, respectively. GOx could enhance the nanoplatform’s dual nanozyme activity in a cascade, further sensitizing radiotherapy and intensifying subsequent immunogenic cell death. Crucially, GPGP induced AMPK phosphorylation and downregulated CMTM6, inhibiting intracellular PD-L1 production and blocking its transport to the cell membrane, thereby overcoming low-dose radiotherapy-induced PD-L1 upregulation. Systemic delivery of GPGP also demonstrated notable MRI contrast enhancement, providing precise imaging guidance for determining the optimal timing for radiotherapy. Therefore, GPGP has shown great potential in achieving effective MRI and collaborative tumor radio-immunotherapy.
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