CRYSTENGCOMM
·
2017
·Vol. 19
·期 34
·4964-4971
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IF 3.474
Qi Zhao,Qin Wang,Yiguo Su,Keke Huang,Guangran Xu,Yingjun Li,Jiayin Liu,Baocang Liu,Jun Zhang
Driven by the need of high catalytic performance and low cost Pt-based catalysts for methanol oxidation (MOR) and oxygen reduction (ORR) reactions, we developed a highly active nitrogen species-decorated Pt–Ni–N catalyst with tunable architectures and facets toward high catalytic activity. The synthetic procedure was conducted by Ni2+-assisted morphology and facet transformation from nanoflowers (NFs) (111) to nanoparticles (NPs) (220) and simultaneous optimization of both hierarchical structure and active surface sites. It is found that the adsorption of nitrogen species plays critical roles in determining both facet control of the Pt–Ni–N hierarchical structure and energetic activation of the catalytic reaction. Decoration of surface nitrogen species can effectually improve the relative content and electronic density of Pt0, leading to formation of a hierarchical structure and significantly improved catalytic activity toward both MOR and ORR compared with Pt–Ni and Pt–N, as well as the commercial Pt/C catalysts, indicating a new strategy to obtain highly efficient catalysts. Moreover, the results demonstrate that the catalytic enhancement is mainly due to the synergistic electronic effects among Pt, Ni, and N species.
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ANALYTICA CHIMICA ACTA
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2016
·
IF 4.712
Na Xu,Hong-Wei Li,Yuqing Wu
A novel one-step hydrothermal synthesis of highly fluorescent platinum nanoclusters protected by polyethylenimine (Pt-NCs@PEI) is described. The products are characterized well by UV–vis absorption, fluorescence spectra , X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) imaging. The Pt-NCs@PEI possess high quantum yield at 28%, which is the relatively high one among the reported Pt-NCs; especially, the synthesis is in one-step and the reaction time is much shorter (<1 h) than the related methods. In addition, the Pt-NCs@PEI have large Stocks-shift (∼150 nm), high tolerability to the extreme pH and high ionic strengths , and excellent photo-stability under UV–vis irradiation, lay the foundation for the practical bio-applications. Finally, the obtained Pt-NCs@PEI are used to determine trace amount of metronidazole (MTZ) in buffer solution in showing a linear response over a concentration range of 0.25–300 μM and a low detection limit of 0.1 μM. Furthermore, the related investigation on response mechanism will be helpful to design and synthesize new metal nanoclusters as fluorescent probe to detect the trace amount of harmful medicine residuum as nitroimidazoles in human body.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2016
·
IF 3.205
Lin Chen,Hao Hua,Qi Yang,Muhammad Sufyan Javed,Chenguo Hu,Cuiling Zhang
TiO 2 microflowers assembled by nanosheets are prepared by a one-step solvothermal process. The anatase-TiO 2 (B) dual-phase coexistence or anatase single phase is obtained under different annealing temperatures. Pt nanoparticles supported on the anatase-TiO 2 (B) microflowers are first applied to alcohol electrooxidation . The electrocatalytic performances of Pt/anatase-TiO 2 (B), Pt/anatase and Pt/carbon-black (Pt/C) on graphite substrates are systematically investigated. The Pt/anatase-TiO 2 (B) catalyst exhibits superior electrocatalytic activity and stability compared with that of Pt/anatase and Pt/C catalysts for methanol and ethanol in acidic and alkaline media , which is attributed to the large specific surface area, the porous channels to reduce the liquid sealing effect, the enhanced electronic conductivity by dual-phase coexistence and quick electron transfer from anatase phase to TiO 2 (B).
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2017
·
IF 3.582
Lirong Huang,Yanping Hou,Zebin Yu,Zhenbo Peng,Li Wang,Jun Huang,Boge Zhang,Lun Qian,Leidan Wu,Zongchen Li
The electrode with high catalytic activity , low hydrogen overpotential and low cost is desired for hydrogen evolution reaction (HER) via electrocatalytic water splitting. In this study, Pt/Fe-Ni foam (Pt/Fe-NF) electrode was synthesized via cathodic electrodeposition followed by impregnation deposition. Physical and electrochemical properties of Pt/Fe-NF, NF and Pt/NF electrodes were characterized by various techniques. The Pt/Fe-NF electrode exhibited better electrochemical activity for HER under alkaline condition than those of Pt/NF and NF electrodes, owing to the introduction of zero valences Pt and Fe onto the NF, and synergetic effect resulted from the formation of Fe-Ni alloy. Furthermore, Pt/Fe-NF electrode showed extremely high double-layer capacitance (69.1 mFcm −2 ), suggesting high active sites for the Pt/Fe-NF. Tafel slope of Pt/Fe-NF was 59.9 mV dec −1 , indicating that the Volmer-Heyrovsky HER mechanism was the rate-limiting step. The Pt/Fe-NF electrode with great electrocatalytic activity is a promising electro-catalyst for industrial hydrogen production from alkaline electrolyte .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2017
·
IF 3.582
Cunbiao Song,Guitai Wu,Beilei Sun,Yao Xiong,Sheng Zhu,Yongming Hu,Haoshuang Gu,Yu Wang,Wanping Chen
Pt–WO 3 porous composite ceramics have been prepared from Pt and WO 3 nanoparticles through pressing and sintering. These ceramics exhibit extraordinary room-temperature sensing capabilities, including high sensitivities, fast response and recovery speeds, and good stability, for low concentrations of hydrogen (at and below 1000 ppm) in air; while for high concentrations of hydrogen (above 2000 ppm) in air, the recoveries in air are only partial in given amounts of time. We propose that for low concentrations of hydrogen, the response results from the reaction of hydrogen with chemisorbed oxygen on WO 3 ; while for high concentrations of hydrogen, hydrogen chemisorption on WO 3 will occur after all chemisorbed oxygen on WO 3 is reacted. The relatively high stability of chemisorbed hydrogen on WO 3 is responsible for the observed partial recoveries. Our results show that Pt–WO 3 composite ceramics are highly competitive for sensing low concentrations of hydrogen in air at room temperature among various metal oxide semiconductor bulk materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Bao-Xia Dong,Hui Tian,Yi-Chen Wu,Fan-Yan Bu,Wen-Long Liu,Yun-Lei Teng,Guo-Wang Diao
Liquid ammonia electrolysis is conducted out at ambient temperature using different ammonium salt electrolytes with and without the reference electrode. It is determined that electrolytes containing NH 4 + increase the current density and reduce the solution resistance. Moreover, ammonium salts of NH 4 Br, NH 4 NO 3 and NH 4 Cl preserve >80% current efficiency and a 0.6–0.8 mL min −1 average rate of H 2 generation during chronopotentiometry tests at 120 mA cm −2 for 3 h. A minimum electrolysis voltage ( E min ) of ca . 1.2 V is required for the NH 4 Cl electrolyte when using Pt-foil as the anode and cathode . To decrease the overpotential of the anode reaction, five types of electrocatalysts were prepared and characterized: Pt-black, Rh, Pt–Ir, Rh–Pt and Ph–Pt–Ir alloys. Trimetallic Rh–Pt–Ir and bimetallic Pt–Ir, Rh–Pt (1:1) alloy electrodes exhibit a combined benefit of better activity and minimized deactivation. The ternary Rh–Pt–Ir alloy anode shows the best electrocatalytic activity with the lowest E min of ca . 0.47 V and highest current density of 46.9 mA cm −2 at 2.0 V. In comparison with the Pt-foil anode, the E min is reduced by two-thirds, and the current density is increased two-fold.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2016
·
IF 2.822
Fen-Ying Kong,Yu Luo,Jin-Wei Zhang,Jing-Yi Wang,Wei-Wei Li,Wei Wang
In this work, we successfully prepared well-defined bimetallic alloyed Pt-Pd nanocubes (NCs) supported on reduced graphene oxide nanosheets (rGO-Pt-Pd NCs). Pt-Pd NCs were uniformly dispersed on rGO by hydrothermal treatment of preformed Pt-Pd NCs and GO in alkaline media. The detailed morphology, crystal structure and composition were well characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Furthermore, with the special structure of Pt-Pd NCs and the synergetic effects of Pt, Pd and rGO, the rGO-Pt-Pd NCs modified electrode exhibited excellent electrocatalytic performance in the sensing of chloramphenicol (CAP). The linear covered the range of 0.2–30 μM and the detection limit reached 0.1 μM (S/N = 3). The modified electrode also displayed good stability, high reproducibility and satisfactory selectivity.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2016
·Vol. 21
·期 2
·391-401
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IF 2.327
Peng Meiling,Xu Wei,Cui Weihao,Wang Tao,Wang Sheng
This study reports the synthesis of octahedral Pd-Pt bimetallic alloy nanocrystals through a facile, one-pot, templateless, and seedless hydrothermal method in the presence of glucose and hexadecyl trimethyl ammonium bromide. The morphologies, compositions, and structures of the Pd-Pt nanocrystals were fully characterized by various physical techniques, thereby demonstrating their highly alloying octahedral nanostructures. The formation or growth mechanism of the Pd-Pt bimetallic alloy nanocrystals was explored and is discussed here based on the experimental observations. In addition, the synthesized Pd-Pt nanocrystals were applied to the methanol oxidation reaction (MOR) in alkaline media, which proved that the as-prepared catalysts exhibit enhanced electrocatalytic activity for MOR. Pd 1 Pt 3 exhibited the best stability and durability, and its mass activity was 3.4 and 5.2 times greater than those of Pt black and Pd black catalysts, respectively. The facile synthetic process and excellent catalytic performance of the as-prepared catalysts demonstrate that they have the potential to be used in direct methanol fuel cell techniques.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2016
·Vol. 24
·期 1
·676-684
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IF 2.76
Tu Baosheng,Shi Nian,Sun Wei,Cao Limei,Yang Ji
In this paper, Pt supports on carbon black powder (Vulcan XC-72) were synthesized via a hydrothermal method for selective catalytic reduction (SCR) of NO with H 2 in the presence of 2 vol% O 2 over a wide temperature of 20–300 °C. The results showed that the 3 and 5 wt% Pt/C catalysts resulted in high NO conversion (>90 %) over a temperature range of 120 to 300 °C, and the maximum NO conversion of 98.6 % was achieved over 5 wt% Pt/C at 120 °C. Meanwhile, the influence of SO 2 and H 2 O on the catalyst performance of 3 wt% Pt/C was investigated. The catalysts exhibited good SO 2 poisoning resistance when the SO 2 concentration was lower than 260 ppm. Moreover, a positive effect on NO conversion was detected with the addition of 3 and 5 vol% H 2 O in the feed gas stream.
TEM image and good NO conversion performance of the Pt/C catalysts
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2016
·Vol. 2017
·期 1
·172-178
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IF 2.686
Gui-lin Zhuang,Jia-qi Bai,Xiang Zhou,Yi-fen Gao,Hong-liang Huang,Hai-quan Cui,Xing Zhong,Chong-Li Zhong,Jian-guo Wang
Graphical The effects of metal–organic framework (MOF) supports on catalytic activity were uncovered for highly dispersed Pt nanoparticles (NPs) loaded in UiO-67. Investigations of the effects of the support on catalytic properties are important for heterogeneous systems. Herein, we report the preparation of highly dispersed Pt nanoparticles (NPs) in three isomorphous UiO-67-type metal–organic frameworks (MOFs), namely, pristine UiO-67, N-UiO-67, and NH 2 -UiO-67. Structural measurements revealed that the sizes of the Pt NPs were 4.5 nm for Pt/UiO-67 and 2.5 nm for N-UiO-67 and NH 2 -UiO-67. The dominant influences on the sizes of the Pt NPs are the functional groups of the support and the pore size of the MOF. Furthermore, CO catalytic oxidations were performed as a model reaction. Interestingly, the catalytic performance sequence is 5 % Pt/N-UiO-67 > 5 % Pt/UiO-67 > 5 % Pt/NH 2 -UiO-67. A combination of experimental measurement and DFT calculation revealed that the catalytic properties depend on not only the size of the Pt NPs but also the nature of the support.
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Catalysts
·
2016
·Vol. 6
·期 10
·150
·
IF 2.964
Gaixiu Yang,Yongming Sun,Pengmei Lv,Feng Zhen,Xinyue Cao,Xiaojie Chen,Zhongming Wang,Zhenhong Yuan,Xiaoying Kong
Carbon-supported Pt–Ru alloys with a Pt/Ru ratio of 1:1 were prepared by NaBH4reduction at room temperature. X-ray diffraction (XRD) measurements indicate that the as-prepared Pt–Ru nanoparticles had a face-centered cubic (fcc) structure. X-ray photoelectron spectroscopy (XPS) analyses demonstrate that alloying with Ru can decrease the 4f electron density of Pt, which results in a positive binding energy shift of 0.2 eV for the Pt 4f peaks. The catalytic properties of the synthesized Pt–Ru alloy catalysts were compared with those of commercial Pt/C catalysts by linear sweep voltammetry (LSV). The results show that the mass activity of the oxygen reduction reaction (ORR) is enhanced by 2.3 times as much mass activity of Pt relative to the commercial Pt/C catalyst. Single-chambered microbial fuel cell tests also confirm that the Pt–Ru alloys as cathode catalysts have better performance than that of commercial Pt/C catalysts.Keywords:Pt–Ru nanoparticles;oxygen reduction reaction;electrocatalyst;microbial fuel cell
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Nano Research
·
2017
·Vol. 10
·期 5
·1749-1755
·
IF 7.354
Jiang Binbin,Yang Lulu,Liao Fan,Sheng Minqi,Zhao Haozhe,Lin Haiping,Shao Mingwang
Hydrogen evolution by electrocatalysis is an attractive method of supplying clean energy. However, it is challenging to find cheap and efficient alternatives to rare and expensive platinum based catalysts. Pt provides the best hydrogen evolution performance, because it optimally balances the free energies of adsorption and desorption. Appropriate control of these quantities is essential for producing an efficient electrocatalyst. We demonstrate, based on first principles calculations, a stepwise designed Rh-Au-Si ternary catalyst, in which adsorption (the Volmer reaction) and desorption (the Heyrovsky reaction) take place on Rh and Si surfaces, respectively. The intermediate Au surface plays a vital role by promoting hydrogen diffusion from the Rh to the Si surface. Theoretical predictions have been explored extensively and verified by experimental observations. The optimized catalyst (Rh-Au-SiNW-2) has a composition of 2.2:28.5:69.3 (Rh:Au:Si mass ratio) and exhibits a Tafel slope of 24.0 mV·dec –1 . Its electrocatalytic activity surpasses that of a commercial 40 wt.% Pt/C catalyst at overpotentials above 0.19 V by exhibiting a current density of greater than 108 mA·cm –2 . At 0.3 V overpotential, the turnover frequency of Rh-Au-SiNW-2 is 10.8 times greater than that of 40 wt.% Pt/C. These properties may open new directions in the stepwise design of highly efficient catalysts for the hydrogen evolution reaction (HER).
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