Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 36
·18755-18766
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IF 11.301
Yingzhang Shi,Huan Wang,Zhiwen Wang,Taikang Wu,Yujie Song,Binbin Guo,Ling Wu
Optimizing the structure of semiconductor materials and introducing functional metal clusters have emerged as an effective strategy to improve the photocatalytic performances of catalysts through the synergistic effect between metals and supports. In this work, Pt nanocluster decorated hierarchical Sb2WO6 microspheres which are assembled from ultra-thin nanosheets with only 3.3 nm thickness (Pt/SWO-NS) jointly achieve an efficient photocatalytic reduction of nitrobenzene to aniline and show 10 times higher activity than Pt decorated bulk Sb2WO6 (Pt/SWO-bulk). More importantly, the respective roles of SWO-NS and Pt nanoclusters are deeply studied. SWO-NS with a unique 2D structure, abundant unsaturated surface sites and good visible light response would be favorable for stabilizing Pt nanoclusters, adsorbing and activating more nitrobenzene molecules and providing abundant photo-generated electrons. Meanwhile, Pt nanoclusters serve as electron enrichment centers to decompose HCOONH4 to produce rich ·CO2− and active H for reducing the activated nitrobenzene molecules. In addition, on combining coordination chemistry, a possible synergistic mechanism for hierarchical Sb2WO6 microspheres and Pt nanoclusters is proposed to elucidate the efficient reduction of nitrobenzene to aniline. We believe that this work would provide an effective strategy to optimize catalytic performance by the design of applicable nanocomposites with synergistic effects.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Jianguo Yu,Dan Wei,Zhe Zheng,Wenjie Yu,Honghui Shen,Yuning Qu,Shuya Wen,Young-Uk Kwon,Yongnan Zhao
x%Pt-Naf-CV (Pt-Nafion-Cyclic Voltammetry) catalysts with homogeneously distributed platinum nanoparticles and ultra-low Pt loading are successfully synthesized by using a facile potential cycling approach. The as-synthesized 0.8%Pt-Naf-CV catalyst exhibits an enhanced electrocatalytic activity for hydrogen evolution reaction (HER) in 0.5 M H 2 SO 4 solution, which obtains a low overpotential of 34 mV at 10 mA cm −2 . The linear sweep voltammetry (LSV) curve of 0.8%Pt-Naf-CV catalyst is almost consistent with that of commercial Pt/C. However, the 0.8%Pt-Naf-CV catalyst displays a more excellent stability and durability in comparison with commercial Pt/C. Besides, the Pt loading of Pt/C (Pt–10 wt%) is about 10 times that of 0.8%Pt-Naf-CV catalyst. The improved electrocatalytic performances are derived from the synergistic effects of Pt and Nafion. The Nafion plays a significant role as a dispersant , carrier and structure directing agent on the morphology and size of the Pt catalyst. This result contributes a promising method to enhance the catalytic activity and reduce the amount of Pt.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2019
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IF 3.218
Yang Tan,Yan Zhang,Xiuxiu Wang,Lingxing Zeng,Fenqiang Luo,Aihua Liu
Multi-walled carbon nanotubes (CNTs) modified with amorphous nickel coating was reported as a novel support for platinum (Pt) for methanol oxidation reaction (MOR). First, an amorphous nickel coating on pristine CNTs (Ni/CNTs) via a simplified electroless deposition method without sensitization and activation is easily developed. Then, Pt nanoparticles (10 wt%) supported on Ni/CNTs (Pt/Ni/CNTs) were fabricated using a microwave-assisted reduction method. The as-prepared Pt/Ni/CNTs electrocatalyst exhibited higher electrocatalytic activity towards MOR in acidic solution, supported by the fact that its methanol oxidation current density was about 0.38 fold higher than that value of Pt/CNTs. Additionally, the proposed Pt electrocatalyst showed a little better electrocatalytic activity than the Pt/C catalyst containing Pt up to about 20%. Moreover, the Pt/Ni/CNTs also exhibited the best stability during the process of MOR. The improved activity and durability of Pt/Ni/CNTs electrocatalyst can be attributed to a more uniform distribution of Pt nanoparticles as well as the synergistic effect between Pt and amorphous nickel coating. Therefore, the as-prepared Pt/Ni/CNTs electrocatalyst is active and stable, which may be applied to the direct methanol fuel cells with high performance.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 34
·16043-16049
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IF 3.3
Hongbo Yu,Fei Zhang,Shuibo Wang,Yang Cong,Shiwei Wang,Lin Zhu
Hydrodeoxygenation of lignin-derived phenolic compounds to produce alkanes is a promising method used for mitigating fossil energy consumption, but they often require high temperature and high pressure, resulting in their poor catalytic stability and durability. In this study, we encapsulated ∼3.9 nm active metal Rh nanoparticles (NPs) into ∼40 nm hollow mesoporous aluminosilicate nanospheres (HMANs) to synthesize M@Alx–mSiO2 nanoreactors with adjustable Al contents for guaiacol hydrodeoxygenation. The optimized Rh@Al2.0–mSiO2 catalyst displayed significantly enhanced guaiacol activity and cyclohexane selectivity relative to the Rh@mSiO2 catalyst under mild reaction conditions. According to the characterization results, the high hydrodeoxygenation activity of Rh@Al2.0–mSiO2 could be attributable to the synergistic effect between the metallic Rh and Lewis and Brønsted acid sites, and the introduction of Al species greatly facilitated the adsorption of 2-methylcyclohexanol, thereby enhancing cyclohexane selectivity. The confinement effect of Rh NPs inside the hollow cavities effectively prevents the leaching and aggregation of Rh NPs, thereby improving their catalytic durability and stability.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Minghao Bao,Junhong Chen,Bozhong Pi,Qizhen Zhang,Zhongbo Han,Hongbiao Huo,Chunpei Yu,Wenchao Zhang
A green electrocatalytic system for co-production of SATz energetic material and H 2 . • Clean electrons replace hazardous chemical oxidants for SATz synthesis with SATz yield of 75.2%. • CoSe 2 @MoSe 2 @Pt/NF achieves 30 mV@10 mA·cm −2 and 192 mV@10 mA·cm −2 overpotential for HER. • Coupling system achieves low cell voltage of 1.44 V at 10 mA·cm −2 . Replacing the kinetically sluggish oxygen evolution reaction (OER) with thermodynamically more favorable electrochemical oxidation reactions represents an effective strategy to enhance energy efficiency and economic viability in water electrolysis. Herein, we designed a CoSe 2 @MoSe 2 @Pt/NF heterostructured catalytic electrode and construct an integrated electrocatalytic coupling system that enables the co-production of azo-bridged nitrogen-rich energetic material (sodium 5,5′-azotetrazolate, SATz) at the anode and clean hydrogen energy at the cathode. Mechanistic studies reveal that hydroxyl radicals generated via water electrolysis initiate the oxidative coupling of 5-aminotetrazole, achieving a SATz yield of 75.2% under optimized conditions. The CoSe 2 @MoSe 2 @Pt/NF cathode exhibits exceptional HER catalytic activity with a low overpotential of 192 mV at 100 mA·cm −2 and a Tafel slope of 50.2 mV·dec −1 , along with remarkable stability. Notably, the assembled coupling system requires a substantially reduced cell voltage of only 1.44 V to achieve 10 mA·cm −2 , significantly lower than that of conventional overall water splitting (>1.71 V). This work presents a sustainable and energy-efficient strategy for the simultaneous production of green energetic materials and clean hydrogen fuel, opening new avenues for advanced electrocatalytic coupling systems. Download: Download high-res image (166KB) Download: Download full-size image
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Weili Qiao,Baoshan He,Jun Yang,Wenjie Ren,Renyong Zhao,Yurong Zhang,Chunqi Bai,Zhiguang Suo,Yiwei Xu,Min Wei,Huali Jin
Lateral flow immunoassay (LFIA) has been employed extensively for the rapid, accurate, and portable detection of foodborne toxins. Here, the platinum gold nanoflower core-shell (Pt@AuNF) nanozyme with excellent optical properties, good catalytic ability and controllable reaction conditions were prepared to effectively improve the performance of lateral flow immunoassay (LFIA) strips. The Pt@AuNF nanozyme and horseradish peroxidase (HRP) combined with monoclonal antibody were used as signal probes based on the dual enzymes catalytic signal amplification strategy to detect Zearalenone sensitively. Dual enzymes catalyze the decomposition of hydrogen peroxide into hydroxyl radicals, and under the influence of hydroxyl radicals, colorless 3,3′,5,5′ -tetramethylbenzidine (TMB) is oxidized to blue ox-TMB, which is superimposed on the strips for signal amplification to broaden the detection range. The limit of detection (LOD) of the Pt@AuNF-HRP labeled LFIA strips after signal amplification was 0.052 ng/mL, and the detection range was 0.052–7.21 ng/mL. Compared with the Pt@AuNF labeled strips, while reducing the probes amount by half to achieve antibody conservation, the detection range was expanded by 5-fold based on achieving improved sensitivity. The study provided a meaningful reference for expanding the detection range based on immunoassay.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ran Hao,Gangwan Zhang,Jiahe Zhang,Leyong Zeng
The weak catalytic activity of nanocatalysts and the insufficient endogenous hydrogen peroxide (H 2 O 2 ) in tumor microenvironment (TME) seriously restricted the efficacy of catalytic therapy, and the non-degradability of inorganic nanocarriers was also unfavorable for their clinical applications. Herein, by depositing gold nanoparticles (AuNPs) and platinum nanoparticles (PtNPs) with ultrasmall size and modifying photosensitizer (IR808), a biocompatible bovine serum albumin (BSA) nanoplatform (BSA@Au/Pt-IR808) with triple-amplification of enzyme activity was constructed to enhance photodynamic therapy (PDT) and catalytic therapy. Ultrasmall AuNPs possessed glucose oxidase (GOx)-like activity, by which the self-supplying H 2 O 2 accelerated the dual-enzyme activity of peroxidase (POD) and catalase (CAT) of ultrasmall PtNPs, promoting the generation of hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ). Compared with BSA-IR808 and BSA@Pt, the yields of 1 O 2 and ·OH of BSA@Au/Pt-IR808 increased by 38.2% and 18.6%. Under the combination action of photothermal therapy (PTT)/PDT/catalytic therapy of BSA@Au/Pt-IR808, the cell viability significantly reduced to 12.8%, and the tumors were completely eliminated, demonstrating the enhanced PDT and catalytic therapy against breast cancer.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Lei Wang,Yonggang Sun,Yulong Ma,Min Xu,Juan Zhang,Yingbo Zhu,Jie Ding,Li Zhu,Jing Ma,Wenxin Ji,Liqiong Wang,Yuanyuan Li
Dual activation of molecular and lattice oxygen is an important step in the catalytic oxidation of volatile organic compounds. Herein, CeO 2 was derived from MOF as an electron donor support to develop a co-catalyst with Pt-Pd alloy nanoparticles (Pt-Pd/CeO 2 ). The Prepared Pt-Pd/CeO 2 exhibits excellent catalytic activity towards toluene oxidation, showing a turnover frequency (TOF 0.26 s −1 ) higher than those of Pt/CeO 2 (0.05 s −1 ) and Pd/CeO 2 (0.02 s −1 ). Several in situ experimental techniques and density functional theory calculations have revealed that the introduction of Pd valence electrons can intensify the electronic metal-support interactions (EMSIs) effects of Pt-Pd/CeO 2 catalysts, which can weaken the Ce-O bond, thereby promoting the production and circulation of lattice oxygen and oxygen vacancies, and modulating the d -band centre to enhance the adsorption and activation of reactants. This study presents a comprehensive investigation of toluene oxidation on alloy-supported catalysts, providing practical guidance for designing reliable catalysts suitable for industrial applications.
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RSC Advances
·
2015
·Vol. 6
·期 1
·730-739
·
IF 3.84
Qianli Wang,Yiwei Zhang,Yuming Zhou,Zewu Zhang,Jinjuan Xue,Yuanmei Xu,Chao Zhang,Xiaoli Sheng,Naishu Kui
Ordered mesoporous ceria (meso-CeO2) was fabricated by nanocasting employing Ia3d mesoporous silica KIT-6 as the template. For comparison, ceria nanoparticles (nano-CeO2) with non-ordered mesoporous were also synthesized via a sol–gel method. Polyamidoamine (PAMAM) dendrimers were used as stabilizing agents to prepare a dispersed Pt nanoparticle colloidal solution. Afterward, the obtained well-dispersed Pt nanoparticles were immobilized on meso-CeO2 and nano-CeO2, respectively. The prepared samples were characterized through several techniques, such as X-ray diffraction (XRD), nitrogen adsorption–desorption isotherms, transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and energy dispersion X-ray analysis (EDX) with mapping. The results revealed that the as-prepared meso-CeO2 has high crystallinity, a relatively small crystalline size, a well-ordered mesoporous structure and high surface area of 115.3 m2 g−1. In addition, the Pt/meso-CeO2 catalyst showed relatively uniform distribution of Pt nanoparticles with small sizes (∼4 nm). The catalytic performances of the as-synthesized catalysts were evaluated relying on the reduction of 4-nitrophenol monitored by UV-vis spectra. It was found that Pt/meso-CeO2 exhibited better catalytic activity compared with Pt/nano-CeO2. Besides, Pt/meso-CeO2 possessed good reusability and maintained a conversion of no less than 90% even after five cycles.
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ACS ES&T Engineering
·
2023
·
IF 7.1
Haifang Mao,Mengli Xu,Shuangjun Li,Yuqing Ren,Yun Zhao,Jun Yu,Qizhong Zhang,Wenshu Zhao,Gui Zhang,Lan Yan,Zhenmin Xu,Zhenfeng Bian
The activation of surface lattice oxygen is crucial for designing highly efficient photocatalysts for volatile organic compound (VOC) purification. Herein, the Pt/TiO2–x catalyst with abundant oxygen vacancies was successfully prepared via the pyrolysis of the Pt-modified Ti metal–organic framework (MOF) under an air atmosphere. Detailed experimental results and density functional theory calculations revealed that the introduction of oxygen vacancies modulated the electronic configuration of the Pt site and enhanced the charge transfer from Ti to Pt, which created an electronic metal–support Pt–Ti interaction interface (EMSI). The established Pt–Ti interface is favorable for the activation of the surface lattice oxygen adjacent to the Pt site [identified by H2 temperature-programmed reduction (TPR), electron paramagnetic resonance (EPR), and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS)] and subsequently facilitates toluene oxidation via a direct ring opening process. This study offers a promising strategy for the design of high-performance photocatalysts for VOC oxidation.
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Molecular Catalysis
·
2023
·
IF 4.6
Yanlin Xu,Zhuoyi Liu,Bin Liu,Bin Dong,Yuan Pan,Yanpeng Li,Yichuan Li,Hailing Guo,Yongming Chai,Chenguang Liu
Transformation of lignin-derived feedstocks into valuable hydrocarbons is of significant importance but still challenging. This work investigates the hydrodeoxygenation (HDO) of lignin compound guaiacol on Pt-based catalysts with improved surface hydrophobicity and metal dispersion for the first time. The efficiency of guaiacol hydrodeoxygenation into hydrocarbons over Nb 2 O 5 -modified Pt-based catalyst reaches 51 %, nearly doubling that over unmodified Pt/γ-Al 2 O 3 catalyst (25 %). On the one hand, Nb 2 O 5 causes the decrease of hydroxyl groups on catalyst, leading to the enhanced hydrophobicity of catalysts, which increases the reaction rate of guaiacol into hydrocarbons on unit of Pt metal sites. On the other hand, Nb 2 O 5 strengthens the metal-support interaction, which minimizes the size of Pt nanoparticles, providing more exposed metal sites, thus leading to a higher hydrocarbons yield on catalyst. However, excess introduction of Nb 2 O 5 leads to partial coverage of Pt metal sites, resulting in decreased yield of hydrocarbons. Furthermore, the routes of guaiacol HDO reaction over modified Pt-based catalysts are investigated. This work further illustrates the influence of catalyst surface properties on the HDO process of lignin compound, and thereby provides a promising approach for adjustment of catalyst surface properties in order to promote water-liberated reactions.
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Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2023
·
IF 3.6
Kezhong Wu,Feifei Nie,Xi Qi,Yingshan Wu,Hui Zhao,Mingxing Wu
Vanadium-based nitrides have been applied as Pt-free counter electrodes (CEs) electro-catalysts for dye-sensitized solar cells (DSSCs) due to inexpensive cost and easy doping and modification. Herein, polyoxovanadate (NH 4 ) 2 V 6 O 16 assisted by melamine to prepare VN@C composites by five different synthesis routes, including solvothermal, sol–gel, hydrothermal, ball milling, and chemical mixing method. And then, five VN@C composites were assembled as CEs in the encapsulated DSSCs, and yielded power conversion efficiencies of 4.47, 5.04, 5.35, 5.49 and 6.11% for regenerate traditional I 3 − /I − shuttles by the photocurrent-photovoltage ( J - V ) test, respectively. The catalytic performances of VN@C composites CEs were assessed by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and Tafel polarization experiments, and the significant effects of different synthetic routes were confirmed. The results revealed that VN@C composite CEs prepared by chemical mixing method had higher catalytic performance in DSSCs, which is due to the improvement of conductivity and the high concentration of active sites.
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