Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 15
·7171-7176
·
IF 11.301
Xue Zhao,Ziqiong Yang,Wenjing Wang,Yuxin Li,Xiaohai Zhou,Haibo Zhang
Hydrogen is considered as the most promising sustainable and economical energy source that can be used on a large scale as an alternative to fossil fuels, but its production requires additional catalysts. As an outstanding catalyst in the hydrogen evolution reaction, increasing the surface atomic ratio of Pt clusters can further improve its catalytic performance for the hydrogen evolution reaction. Here, using metal boron organic polymers (MBOPs) as bifunctional precursors (both reducing and self-supporting properties), a new approach to rapid large-scale preparation of supported Pt-based catalysts (Pt/MBOPs) with hydrogen evolution activity and stability is presented. First, the Pt nanoparticles in Pt/MBOPs with high dispersion and small particle size showed excellent catalytic performance in the electrochemical hydrogen evolution reaction (E-HER), with an overpotential as low as 22.8 mV (at 10 mA cm−2) and a Tafel slope of only 56 mV dec−1. In addition, Pt/MBOPs also show extraordinary performance in the decomposition of ammonia borane (a hydrogen storage chemical), and the TOF from ammonia borane to H2 is as high as 1654.9 molH2 molPt−1 min−1. It is worth noting that Pt/MBOPs show outstanding stability in electrochemical water splitting to hydrogen and ammonia borane hydrolysis, and are an efficient catalyst in industrial production or the immediate hydrogen production field.
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高影响因子
MATERIALS SCIENCE FORUM
·
2020
·
IF 0
Ming Hong Luo,Yin Ai,Ke Jian Xia
The multilayer composite films consisting of poly (diallyldimethylammonium chloride) functionalized graphene (PDDA-rGO) and phosphomolybdic acid functionalized graphene (PMo12-rGO) were prepared by layer-by-layer self-assembly method. The {PDDA-rGO/PMo12-rGO}n multilayer composite films were used as a support for electro-deposition of Pt particles in situ. Cyclic voltammetry (CV), X-ray photoelectron spectroscopy and scanning electron microscopy were employed for examining the composition, structure, and morphology of the catalyst. Results revealed that the Pt/{PDDA-rGO/PMo12-rGO}n catalyst is successfully prepared and that the multilayer composite films support improves the dispersion of the Pt particles. CV and chronoamperometry were employed to evaluate the electrocatalytic performance for methanol oxidation. Results revealed that the electrocatalytic activity and stability of the Pt/{PDDA-rGO/PMo12-rGO}3 catalyst for methanol oxidation are considerably improved in comparison with that of the Pt/GCE catalyst. The current density for the oxidation of methanol increased from 0.66 mA/cm2 to 1.21 mA/cm2. In addition, the ratio of the forward current density to the backward current density (If/Ib) was 1.92 for Pt/{PDDA-rGO/PMo12-rGO}3 catalyst, corresponding to 1.3 times that of the Pt/GCE catalyst. This result indicated that the multilayer composite films remarkably enhanced the electrocatalytic activity regarding methanol oxidation.
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Guang Gao,Zelun Zhao,Jia Wang,Yongjie Xi,Peng Sun,Fuwei Li
ABSTRACT Engineering the surface microenvironment by tuning the binary interactions between a supported metal with a secondary metal oxide (MO x ) or support has been a common method for improving the catalytic performance of supported metal catalysts. However, few studies have investigated the ternary interactions among the metal, MO x , and support. Here, we report for the first time the formation of metal-MO x -support interaction (MMSI) in reducible TiO 2 -supported PtReO x catalysts, affording 87% yield and 100% ee in the tandem hydrogenation of an aqueous chiral cyclohexane-1,2-dicarboxylic acid into the corresponding diol; the catalytic activity is eight times higher than that obtained with non-reducible support counterparts in the same reaction via traditional batch synthesis with multiple steps and unfriendly reagents. Detailed experimental and computational studies suggest that the TiO 2 crystalline phase-dependent density of the oxygen vacancies induces different Pt-ReO x -TiO 2 interactions, which dominate the electron transfer therein and tune the adsorption strength of the carbonyl moiety of the substrate/intermediate, thus promoting the hydrogenation activity and selectivity. In addition, the strong MMSI endows the optimal rutile TiO 2 supported PtReO x catalyst with an outstanding lifetime of 400 h in a fixed-bed reactor under acidic aqueous conditions and ensures efficient applications in the selective hydrogenation of aliphatic dicarboxylic acids and functional carboxylic acids. This work provides a promising strategy for the development of efficient and stable supported catalysts for the selective hydrogenation of diverse C–O and C=O bonds.
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高影响因子
JOURNAL OF POWER SOURCES
·
2013
·
IF 4.675
Yingqiang Huang,Yingju Liu,Zhuohong Yang,Jinliang Jia,Xin Li,Yan Luo,Yueping Fang
A novel yolk/shell Fe 3 O 4 –polydopamine–graphene–Pt (Fe 3 O 4 @PDA/RGO/Pt) nanocomposite is synthesized using polydopamine as a moderate modifier for graphene as well as a coupling agent for the assembly of Pt nanoparticles . The morphology and structure of the as-prepared catalysts are characterized by transmission electron microscopy , X-ray photoelectron spectroscopy, X-ray diffraction and Fourier transform infrared spectroscopy. The detailed formation mechanism of such yolk/shell nanocomposite is discussed. Subsequently, its catalytic activity towards the methanol oxidation is evaluated by cyclic voltammetry , chronoamperometry , electrochemical impedance spectra and CO-stripping voltammetry. Results show that such york/shell Fe 3 O 4 @PDA/RGO/Pt exhibits higher electrochemical activity and stability to methanol oxidation than Pt/graphene, which is not only attributed to the synergetic cocatalytic effect at the heterojunction interfaces between the Pt nanoparticles and the support, but also due to the high immobilization of Pt nanoparticles by the functional groups of polydopamine. In addition, the separation ability of Pt nanoparticles from the nanocomposite by Fe 3 O 4 can decrease the CO poison from free Pt nanoparticles. Therefore, this unique yolk/shell nanocomposite may be suitable for the production of catalysts with low-cost and high activity.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Lingya Yi,Yang Yu,Yuzhou Tao,Weihua Hu
Pt-based intermetallic nanoparticles demonstrate impressive oxygen reduction reaction (ORR) activity and durability due to their atomically ordered nature but their synthesis remains a tremendous challenge. Herein we report Pt–Co intermetallic nanoparticles anchored on nitrogen-rich graphene (NG) nanosheets for efficient ORR electrocatalysis in acidic media. The rich nitrogen atoms, doped via low-temperature plasma treatment on graphene efficiently inhibit the sintering of the nanoparticles during high temperature annealing via strong metal-support interaction and enhance the anchoring stability. Meanwhile, the electronic interaction between NG and Pt–Co intermetallic nanoparticles negatively shifts the d-band center of Pt to enhance their intrinsic ORR activity. As-prepared PtCo/NG-900 with low Pt loading of 3.4 μg cm −2 exhibits high mass activity of 1.28 A mg −1 at 0.8 V vs. RHE, and enhanced durability with only 1.9 mV decay in half-wave potential (E 1/2 ) after 2000 potential cycles.
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产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Xiang Tan,Peng Luo,Liya Cao
Hydrodeoxygenation (HDO) is pivotal for upgrading lignin-derived streams into drop-in aviation fuels. Efficient aryl C–O bond cleavage with complete deoxygenation typically requires harsh conditions. Here we report electron-rich Pt nanocatalysts that convert lignin-derived model compounds and lignin oil to jet-range cycloalkanes under notably mild conditions (100 °C, 10 % H 2 /Ar at 0.5 MPa). Alkyl cyclohexanes are obtained in 95.2 % yield from a representative model substrate and 90.5 % from lignin oil. Time-resolved profiling and cascade-kinetics analysis indicate that aryl C–O bond scission is the rate‑determining step. Differential charge density and reaction free‑energy analyses support that increasing electron density on Pt promotes H* activation and lowers the free‑energy change (ΔG) for C–O cleavage, consistent with the enhanced activity. The catalysts exhibit broad substrate scope and reusability. This work provides a practical low-temperature route and an electronic-structure design principle for energy-efficient upgrading of lignin-derived oils to jet-range cycloalkanes.
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产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2021
·Vol. 15
·期 6
·1514-1523
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IF 4.204
Qu Huaxin,Deng Jie,Wang Bei,Ouyang Lezi,Tang Yong,Yu Kai,Lou Lan-Lan,Liu Shuangxi
A base-free catalytic system for the aerobic oxidation of 5-hydroxymethyl-2-furfural was exploited by using Pt nanoparticles immobilized onto a thermoresponsive poly(acrylamide- co -acrylonitrile)- b -poly( N -vinylimidazole) block copolymer, with an upper critical solution temperature of about 45 °C. The Pt nanocatalysts were well-dispersed and highly active for the base-free oxidation of 5-hydroxymethyl-2-furfural by molecular oxygen in water, affording high yields of 2,5-furandicarboxylic acid (up to >99.9%). The imidazole groups in the block copolymer were conducive to the improvement of catalytic performance. Moreover, the catalysts could be easily separated and recovered based on their thermosensitivity by cooling the reaction system below the upper critical solution temperature. Good stability and reusability were observed over these copolymer-immobilized catalysts with no obvious decrease in catalytic activity in the five consecutive cycles.
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Mengmeng Shao,Haodeng Chen,Shiji Hao,Haikun Liu,Yongyong Cao,Yanfei Zhao,Jutao Jin,Haifeng Dang,Yue Meng,Yanping Huo,Lifeng Cui
Cocatalyst loading is an efficient strategy to accelerate the hydrogen evolution reaction, which is the final crucial process to complete photocatalytic hydrogen production and realize solar-to-hydrogen conversion. Herein, we report that N-doped vanadium carbide (NVC) is combined with Pt to form a multifunctional cocatalyst capable of enhancing carrier separation, activating H 2 O, and accelerating H 2 evolution. Our designed Pt/NVC/C 3 N 4 displays much higher photocatalytic activity than g-C 3 N 4 loaded with Pt or NVC. The photocatalytic H 2 evolution rate of Pt/NVC/C 3 N 4 reaches 40 μmol/h, which is three times and one hundred times higher than that of Pt/C 3 N 4 and NVC/C 3 N 4 , respectively. The significantly enhanced photocatalytic activity of Pt/NVC/C 3 N 4 is attributed to the partial synergy between Pt and NVC, where NVC promotes carrier separation and activates H 2 O, and Pt is responsible for boosting proton reduction. Our work demonstrates that hybrid cocatalysts exhibit superior performance compared to traditional single-component cocatalysts, providing guidance for exploring highly active cocatalysts for photocatalysis.
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高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 151
·期 1
·124-137
·
IF 2.482
Xi Zhiwen,Jia Wenzhi,Zhu Zhirong
Abstract Two series of WO 3 –ZrO 2 and WO 3 –ZrO 2 –TiO 2 composite oxides were prepared via an Evaporation Induced Self Assembly (EISA) method and applied for the hydrogenolysis of glycerol after loading with Pt. Several techniques like XRD, BET, Raman spectroscopy, NH 3 -TPD, Py-IR, TEM and XPS were adopted to characterize the physicochemical properties of the as-synthesized catalysts. The structure and catalytic activities of these catalysts were significantly affected by the calcination temperature of the composite oxides. The introduction of TiO 2 into Pt/WO 3 –ZrO 2 could inhibit the drastic decrease in catalytic performance due to the formation of inactive crystalline WO 3 under high calcination temperature of 800 ℃. A maximum activity was obtained on the Pt/WO 3 –ZrO 2 –TiO 2 catalyst when the calcination temperature was 600 ℃, which gave 73.8% glycerol conversion and 25.4% 1,3-propanediol yield. While the Pt/WO 3 –ZrO 2 catalyst only exhibited 53.4% glycerol conversion and 20.2% 1,3-propanediol yield. The enhanced activity of Pt/WO 3 –ZrO 2 –TiO 2 was ascribed to the improved acidity originating from (i) higher acidic properties of WO x species when linked to Ti with larger electronegativity other than Zr and (ii) new acid centers caused by heteroatoms linkage as the combination of ZrO 2 and TiO 2 . The effects of Pt loading amount and reaction temperatures were also investigated. Graphic Abstract
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高影响因子
JOURNAL OF NANOPARTICLE RESEARCH
·
2018
·Vol. 20
·期 11
·1-8
·
IF 2.127
Sui Ning,Wang Ke,Bai Qiang,Wang Lina,Wang Tao,Xiao Hailian,Liu Manhong,Colvin Vicki L.,Zhang Qingbo,Yu William W.
Dendritic Pt–Cu nanoparticles were synthesized by a facile one-step method with the help of surfactant Brij58 at room temperature, and we also studied the effects of different Pt–Cu ratios on the morphology and size of nanoparticles. In addition, we further tuned the morphology of the Pt–Cu nanostructures by introducing bromide ions, eventually leading to the appearance of some tripod-like structures. Compared with dendritic Pt–Cu and commercial Pt black, these tripod-like Pt–Cu nanostructures exhibited higher electrocatalytic activity and CO tolerance for catalyzing methanol oxidation.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Shuo Wang,Sheng Wang,Xupeng Zong,Shudong Wang,Xiaoli Dong
Insights into the CO oxidation and sulfur tolerance over supported Pt catalysts were carried out. The nominal 1 wt% Pt was loaded onto Al 2 O 3 , TiO 2 , SiO 2 , and SnO 2 by the incipient wetness impregnation method. Results showed that the presence of H 2 O would promote the catalytic oxidation of CO, and Pt/TiO 2 and Pt/SnO 2 catalysts showed superior catalytic activity. In combination with a series of characterizations, it was concluded that excellent catalytic activity was dependent on higher dispersion and strong metal support interaction (SMSI) whether water is present or not. In the coexistence of H 2 O and SO 2 , the sulfation of the support will lead to the deactivation of the catalyst. Sulfur resistance can be improved over TiO 2 with low sulfate decomposition temperature. While for Pt/SnO 2 catalyst, its superior sulfur-tolerance was strongly associated with its special core-shell structure. It provides guidelines for the development of catalysts with excellent CO catalytic activity and sulfur tolerance.
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高影响因子
Catalysis Science & Technology
·
2019
·Vol. 10
·期 5
·1248-1255
·
IF 5.726
Lei Wang,Yang Wang,Chang-Wu Zhang,Jing Wen,Xuefei Weng,Lei Shi
Minimizing the use of platinum while maximizing its catalytic activity is attractive but challenging in the development of industrially important platinum catalysts. Herein, using a hexagonal boron nitride (h-BN) nanosheet-supported Pt/Cu cluster catalyst, we report the promotion of the platinum utilization efficiency and catalytic performance for the dehydrogenation of propane. Specifically, as little as 100 ppm platinum exhibits high propane conversion (∼15%) and propylene selectivity (>99%) at a relatively low reaction temperature (520 °C); the formation rate of propylene reaches 7.3 mol molPt−1 s−1, which is about 10 times higher than the best value for the reported Pt/Cu single-atom alloy catalyst. The structural analysis reveals that the abundant fault edges of the h-BN nanosheets and strong bonding of copper with the edge B–O defects maintain the unique geometry of the Pt/Cu cluster, together with the metallic platinum ensemble stabilizing on the top layer of the copper cluster, leading to remarkable improvement in catalytic efficiency. This prominent promotion in catalytic efficiency is also exemplified using other supports including Al2O3, SBA-15 and SiC as counterparts.
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高影响因子
危险品化学品经营许可证（带存储）