APPLIED SURFACE SCIENCE
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2020
·
IF 6.182
Xiaoxue Zhao,Jingru Guan,Jinze Li,Xin Li,Huiqin Wang,Pengwei Huo,Yongsheng Yan
The conversion of CO 2 into high value-added carbon-based compounds through photocatalytic reduction technology is considered as one of the more promising strategies to solve the greenhouse effect. And construction of heterojunction photocatalysts can promote the separation of photoelectron-hole pairs, so as to achieve higher activity of photocatalytic CO 2 reduction. Hence, Pt@CeO 2 /3DCN heterojunction are prepared by calcination method and photoreduction technology. The photocatalytic results revealed that Pt@CeO 2 /3DCN show better photocatalytic activity for reducing CO 2 into CO and CH 4 , compared with 3DCN. Especially, Pt@45CeO 2 /3DCN shows the maximum photocatalytic activity of 4.69 and 3.03 μmol·h −1 ·g −1 for CO and CH 4 under UV light irradiation, respectively, and the reduction activity did not decrease significantly after five cycles. The enhanced photoreduction of CO 2 performance can be ascribed to the synergistic effects of the oxygen vacancies in CeO 2 for CO 2 activation and heterojunction for electron separation. Besides, Pt nanoparticles (NPs) on CeO 2 /3DCN can further promote the transfer of electrons, resulting in higher photocatalytic activity.
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Catalysts
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2020
·Vol. 10
·期 11
·1304
·
IF 3.52
Qiang Yuan,Jifeng Pang,Wenguang Yu,Mingyuan Zheng
A high-performance Pt catalyst supported on SBA-15 was developed for furfural decarbonylation. Compared to Pt catalysts loaded on microporous DeAl-Hbeta zeolite and hierarchical micro-mesoporous MFI nanosheet (NS) materials, the 1%Pt/SBA-15 catalyst afforded notably higher activity, furan selectivity and stability owing to the negligible acid sites and proper mesopores on the SBA-15 support. Among a set of 1%Pt/SBA-15 catalysts bearing Pt nanoparticles (NPs) with sizes of 2.4–4.3 nm, the catalyst with 3.7 nm Pt NPs afforded the highest furan selectivity. Over the optimal catalyst, 88.6% furan selectivity and ca. 90% furfural conversion were obtained at 573 K and a high weight hourly space velocity (WHSV) of 16.5 h−1. Moreover, the reaction temperatures at 440–573 K and the ratios of H2to furfural at 0.79–9.44 did not affect the reaction selectivity notably, showing that the reaction over 1%Pt/SBA-15 can be conducted over a wide range of conditions. The catalyst was stable under the harsh reaction conditions and lasted for 90 h without significant deactivation, demonstrating the superior property of SBA-15 as a catalyst support for furfural decarbonylation.Keywords:decarbonylation;furfural;furan;platinum;SBA-15
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RSC Advances
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2021
·Vol. 11
·期 5
·2848-2853
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IF 3.361
Xiaoliang Ren,Shufang Wang,Xiaoshu Ding,Dongsheng Zhang,Yanji Wang
In the chemical industry, reactors are typically designed and filled with supported catalyst particles. However, the intrinsic problems associated with the internal/external diffusion effect and catalyst separation/loss in these traditional reactors can be very challenging to mitigate. To address these issues, herein, an active metal sintered membrane reactor anchored with Pt atoms was successfully developed, and applied into continuous, liquid-phase, hydrogenation processes. The catalyzing reactions transpired on the active sites that were fastened onto the surface of the reactor's microchannels. As a result, the mass transfer at the gas–liquid–solid three-phase was greatly enhanced, and an incredibly high reaction efficiency was obtained. The novel, active reactor demonstrated a superior catalytic performance and stability to nitrobenzene (NB) hydrogenation at 120 °C and 0.5 MPa H2, which enabled an aniline (ANI) yield of 19.28 molANI h−1 L−1. This work opens a new window for the design of high-performance gas–liquid–solid reactor toward multiphase catalytic reactions.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xuteng Zhao,Dejun Xu,Yinan Wang,Zuwei Zheng,Ke Li,Yiran Zhang,Reggie Zhan,He Lin
A novel catalytic system for benzene oxidation at low temperature is constructed by combining electric field with Pt-Ce-Zr nano-catalyst. The 1 wt% Pt/Ce 0.75 Zr 0.25 O 2 catalyst assisted by electric field shows the best catalytic performance with 90% benzene conversion at 96.5 °C and excellent water resistance. The effect of electric field on catalysts and catalytic process is comprehensively investigated. The results of XRD, TEM, XPS and H 2 -TPR reveal that the electric field show negligible influence on the crystal structure and surface morphology of the catalyst, but it can lead to more oxygen vacancies. Therefore, more adsorbed oxygen with higher activity will be produced on the catalyst surface. The redox performance is improved due to the fact that valence distribution of Pt is changed in forms of more active sites composed of high valence oxides (PtO) generated in electric field. In situ DRIFTS is used to investigate the oxidation process of benzene and the results prove that electric field could accelerate the production and consumption of intermediate products, and produce new intermediate products such as carboxylic acid species, indicating that the introduction of electric field may open up a new rapid reaction path and promote the activation of benzene at low temperature.
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高影响因子
ENERGY & FUELS
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2021
·
IF 3.605
Meiqiu Hu,Xiaolong Liu,Hong Yuan,Jingye Ma
An in situ encapsulation process was used to prepare ordered worm-like mesoporous Pt@SAPO-11 catalysts with different Pt loadings. Transmission electron microscopy images showed that Pt nanoparticles encapsulated within the SAPO-11 support mesopores were uniformly distributed and highly dispersed and had a narrow particle size distribution of 2–7 nm. Scanning electron microscopy indicated that increasing the Pt loading from 0.6 to 1.6 wt % did not significantly change the crystalline morphology of the catalyst, although the crystallinity decreased slightly. The specific surface area and average pore diameter of the Pt@SAPO-11 were in the ranges of 72–116 m2/g and 8.1–9.5 nm, respectively, which are determined by the Brunauer–Emmett–Teller method and Barrett–Joyner–Halenda method, respectively. The NH3 thermal-programmed desorption established that increasing the Pt loading gradually decreased the total NH3 desorption and that a loading of 1.2 wt % produced the highest concentration of medium-strong acid sites (6.2 cm3/g STP). X-ray photoelectron spectroscopy and H2 temperature-programmed reduction showed that a Pt loading of 1.2 wt % gave the strongest interaction between Pt nanoparticles and the SAPO-11 support. The Pt@SAPO-11 catalysts were used for the preparation of C8–C17 alkanes by decarboxylation of oleic acid. Employing a reaction temperature of 340 °C, a CO2 atmosphere, a Pt loading on the catalyst of 1.2 wt %, and a reaction time of 4 h, 100% oleic acid conversion was obtained together with an 80% yield of C8–C17 alkanes.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Bin Wang,Laifei Xiong,Hanjing Hao,Hairui Cai,Pengfei Gao,Fuzhu Liu,Xiaojing Yu,Chao Wu,Shengchun Yang
In this work, we prepared the PtNi alloy nanoparticles on Al 2 O 3 (Al 2 O 3 –PtNi) via a simple wet-grinding method followed by a thermal reduction process. The as-prepared Al 2 O 3 –PtNi displayed a higher TOF of 426.84 mol H2 (mol Pt ·min) −1 toward the dehydrogenation of AB (ammonia borane) than Al 2 O 3 –Pt and Al 2 O 3 –Ni. Based on the theoretical calculations, an “electric-dipole” effect generated by the neighboring Pt–Ni atoms was found to facilitate the catalytic dehydrogenation process of ammonia borane (AB). The external electric field produced by the Pt–Ni dipole can elongate the B–H bond and increase the negative charges of H atoms on the BH 3 group, which helps to activate the B–H bond in the AB molecule, and thus enhances the kinetic process of catalysis.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Chaohui Liu,Junyuan Xia,Jincui Gu,Wenqin Wang,Qingquan Liu,Luke Yan,Tao Chen
A surge of effort has been devoted to establishing super-wetting membranes with versatility for oily waste water purification. However, persistent challenge remains the lower separation flux. Moreover, the majorities of catalysts are only adsorbed on the surface and easily fall off after multiple cyclic separations. In this work, an effective strategy has been taken to construct a composite membrane consisting of polyacrylic acid functionalized carbon nanotubes (CNTs-PAA) and MIL101(Fe)@platinum nanoparticles (MIL101(Fe)@Pt NPs). The obtained CNTs-PAA/MIL101(Fe)@Pt composite membrane can achieve degradation of dye molecules and at the same time effective separation of oil-in-water emulsions. The separation throughput of this composite membrane can reach up to 11000 L m −2 h -1 bar -1 , which has exceeded most of the previous reported multifunctional separation membranes. Furthermore, this composite membrane has presented stable mechanical property and excellent anti-corrosion ability. This work gives comprehensive consideration to excellent separation performance, versatility and stability, which could have potential applications in practical oily wastewater treatment.
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高影响因子
Nanomaterials
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2020
·Vol. 10
·期 6
·1015
·
IF 4.324
Qin Cheng,Yong Yang,Yusi Peng,Meng Liu
Noble metal nanoenzymes such as Pt, Au, Pd, etc. exhibit magnificent activity. However, due to the scarce reserves and expensive prices of precious metals, it is essential to investigate their enzyme-like activity and explore the possibility of their reuse. In this work, the oxidase-like activity and reusability of several Pt nanoparticles with different morphologies were detected. We compared the Pt nanoparticles (NPs) with a size of about 30 nm self-assembled by 5 nm Pt nanoparticles and Pt nanoparticles (Pt-0 HCl) with a diameter of about 5 nm, and found that their Michaelis−Menten constants (Km) were close and their initial performance similar, but the Pt NPs had better reusability. This was probably attributed to the stacked structure of Pt NPs, which was conducive to the substance transport and sufficient contact. At the same time, it was found that the size, dispersion, and organic substances adsorbed on the surface of Pt nanoparticles would have a significant impact on their reusability. A colorimetric detection method was designed using the oxidase-like activity of Pt NPs to detect ascorbic acid in triplicate. The limits of detection were 131 ± 15, 144 ± 14, and 152 ± 9 nM, with little difference. This research not only showed that the morphology of the catalyst could be changed and its catalytic performance could be controlled by a simple liquid phase synthesis method, but also that it had great significance for the reuse of Pt nanoenzymes in the field of bioanalysis.Keywords:Pt nanoparticles;oxidase-like activity;reusability;colorimetric method;ascorbic acid
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高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 15
·5059-5066
·
IF 9.48
Kaihang Sun,Ning Rui,Zhitao Zhang,Zeyu Sun,Qingfeng Ge,Chang-Jun Liu
Supported Pt catalysts have been extensively investigated for CO2 hydrogenation with methane and CO as the principal products. In this work, a Pt/In2O3 catalyst prepared with decomposition precipitation was tested for CO2 hydrogenation to methanol. The Pt/In2O3 catalyst exhibited a highly improved activity towards CO2 hydrogenation, with methanol selectivity of ca. 100% at temperatures below 225 °C, 74% at 275 °C and 54% at 300 °C, respectively, compared to the pure In2O3 catalyst. This represents the highest methanol selectivity reported on Pt catalysts for CO2 hydrogenation. The stability of the Pt/In2O3 catalyst at elevated temperatures has also been higher than that of the pure In2O3 catalyst, indicated by the methanol formation rate decreasing only to 95% of the initial rate after 5 h in the reaction stream and remaining largely constant thereafter. In contrast, the pure In2O3 catalyst loses 20% of the initial methanol formation rate after 9 h in the reaction stream. The characterization of the catalysts confirms that the Pt nanoparticles are well dispersed on In2O3 with a particle size below 3 nm. The strong metal–support interaction (SMSI) between Pt and In2O3 improves the stability of the catalyst and prevents the over-reduction of In2O3. The synergy between the supported Pt nanoparticles and In2O3 balances the hydrogen activation and the density of the surface oxygen vacancies in In2O3, resulting in the high activity for CO2 hydrogenation and enhanced stability of the Pt/In2O3 catalyst.
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Journal of Energy Chemistry
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2020
·
IF 7.216
Juan Bai,Nan Jia,Pujun Jin,Pei Chen,Jia-Xing Jiang,Jing-Hui Zeng,Yu Chen
Recently, the surface chemical functionalization and morphology control of precious metal nanostructures have been recognized as two efficient strategies for improving their electroactivity and/or selectivity. In this work, 1, 10-phenanthroline monohydrate (PM) functionalized Pt nanodendrites (Pt-NDs) on carbon cloth (CC) (denoted as PM@Pt-NDs/CC) and polyethylenimine (PEI) functionalized Pt-NDs on CC (denoted as PEI@Pt-NDs/CC) are successfully achieved by immersing Pt-NDs/CC into PM and PEI aqueous solutions, respectively. PEI functionalization of Pt-NDs/CC improves its electroactivity for hydrogen evolution reaction (HER) due to local proton enrichment whereas PM functionalization of Pt-NDs/CC improves its electroactivity for formic acid oxidation reaction (FAOR) by facilitating dehydrogenation pathway. With such high activity, a two-electrode electrolyzer is assembled using PM@Pt-NDs/CC as the anodic electrocatalyst and PEI@Pt-NDs/CC as the cathodic electrocatalyst for electrochemical reforming of formic acid, which only requires 0.45 V voltage to achieve the current density of 10 mA cm −1 for high-purity hydrogen production, much lower than conventional water electrolysis (1.59 V). The work presents an example of interfacial engineering enhancing electrocatalytic activity and indicates that electrochemical reforming of formic acid is an energy-saving electrochemical method for high-purity hydrogen production.
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ChemCatChem
·
2019
·Vol. 12
·期 2
·642-648
·
IF 4.495
Gang Yuan,Chan Wu,Guorong Zeng,Xiaopo Niu,Guoqiang Shen,Li Wang,Xiangwen Zhang,Rafael Luque,Qingfa Wang
Graphical Harvest from inexhaustible nature : Intermittent renewable electricity can be stored in chemical bonds by atomic economy production of fuels and chemicals from the aqueous solution of biomass over efficient and stable nanoscale electrodes. Electrochemical valorization of non-food biomass-derived carboxylates into fuels is promising for the conversion, storage, and distribution of renewable electricity. Herein, we demonstrate that biofuels, hydrogen, and bicarbonate can be simultaneously produced in an electrochemical cell by one-step electrolysis of free fatty acids under ambient conditions on 3D self-supported ultralow Pt loading (2 wt %) electrode. The three valuable products can naturally separate from each other during the electrolysis in the alkaline aqueous solution. The experimental suggests that Pt(100) and Pt(110) are favorable for the production of non-Kolbe and Kolbe hydrocarbons, respectively. DFT calculation further clarifies the adsorption and stabilization of the reaction intermediates on Pt(100) and Pt(110).
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Chunjie Li,Songliang Liu,Shuli Yin,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
The porous Pt-based nanomaterials are highly desired for their superb methanol oxidation reaction (MOR) activity. In this work, an effective method was proposed to synthesize Pd@mesoporous PtAu cage-bell structured nanomaterials (Pd@mPtAu CBs). In the synthetic process, Pd@SiO 2 nanoparticles and F127 were used as template and structure directing agent , respectively. The obtained Pd@mPtAu CBs are evenly distributed in size with highly porous surface and interconnected micro-structure. Significantly, the prepared Pd@mPtAu CBs exhibit outstanding catalytic activity and stability toward MOR, which is confirmed as a promising electrocatalyst of direct methanol fuel cells. Furthermore, the proposed method is also suitable for the preparation of other Pt-based nanomaterials with cage-bell architecture, such as Pd@mPt CBs.
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