Journal of the Taiwan Institute of Chemical Engineers
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2017
·
IF 4.217
Fu He,Yong Ji,Yang Wang,Yun Zhang
Nanoscale zerovalent iron (nZVI) loaded magnetic hollow mesoporous bimetallic Fenton-like catalyst, Fe 0 @C@MnFe 2 O 4 , was prepared by a one-pot solvothermal method. Carbon shell of polydopamine (PDA) was formed through self-oxidation of dopamine by adding MnFe 2 O 4 hollow spheres into dopamine solutions. Then Fe 2+ ions were adsorbed on the surface of PDA@MnFe 2 O 4 to obtain active nZVI in-situ through subsequent calcinations. Thus, the mesoporous carbon shell of Fe 0 @C@MnFe 2 O 4 had a great contribution to high adsorption capacity for concentrating TBBPA around the catalyst. The high concentration of TBBPA outside would further facilitate the transportation to the inside of the hollow catalyst to achieve a high catalytic efficiency. Fe 0 @C@MnFe 2 O 4 , as an integrated adsorbent-catalyst, was used to remove Tetrabromobisphenol A (TBBPA) in aqueous solution with the presence of H 2 O 2 and NH 2 OH. Over 90% of TBBPA can be removed within 120 min. According to the result of ESI–MS, β -scission and debromination were involved in the degradation of TBBPA. The reused catalyst could be easily separated by using an external magnetic field in seconds. After ten cycles, the catalyst was still of good activity. The excellent removal efficiency of TBBPA might be attributed to the synergistic effect from high adsorption capacity and efficient Fenton-like catalytic reaction of Fe 0 @C@MnFe 2 O 4 .
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Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 20
·7924-7929
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IF 8.262
Syed Comail Abbas,Kui Ding,Qin Liu,Yiyin Huang,Yakun Bu,Jing Wu,Jiangquan Lv,Muhammad Arsalan Ghausi,Yaobing Wang
The development of efficient oxygen reduction reaction (ORR) electrocatalysts composed of low cost and earth abundant elements is imperative for several energy systems. It has been reported that metal-free co-doped materials play a key role in the oxygen reduction reactions. However, a Si/F co-doped material has never been considered as an electrocatalyst for the ORR. Herein, we report a Si–C–F decorated three-dimensional porous carbon material by a facile pyrolysis of a mixture of D-glucose, ammonium fluoride and SiO2 nanoparticles in an argon atmosphere. It shows an excellent electrocatalytic performance with an onset potential of E = 0.24 V and a limiting current density of I = 4.5 mA cm−2 which is better than that of traditional electrocatalysts under neutral conditions. This outstanding electrocatalytic performance is due to the synergistic effect of silicon and fluorine which causes a change in the charge distribution and energetic characteristics of the Si–C–F decorated porous carbon material. For the practical application, a microbial fuel cell equipped with this electrocatalyst as the cathode reveals a high maximum power output and open circuit voltage (1026 mW m−2 and 780 mV), which are higher than those of commercial 20% Pt/C catalysts (913 mW m−2 and 750 mV).
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RSC Advances
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2017
·Vol. 7
·期 82
·51831-51837
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IF 3.108
Yunrui Zhang,Haihong Niu,Xiangjie Zhang,Junxiu Pan,Yang Dong,Haijun Wang,Yongjun Gao
A kind of magnetic N-containing carbon material was synthesized by a simple method using sustainable N-acetyl-D-glucosamine (NAG) and iron nitrate as the raw materials. In C–H oxidation reactions such as the epoxidation of stilbene and styrene, and the oxidation of ethylbenzene, the carbon catalyst exhibited excellent catalytic activity and selectivity for the target products. The superparamagnetic properties at room temperature facilitated catalyst recycling and reusability when it was used as a catalyst. The relationship between the catalytic results and the N 1s XPS analysis indicated that the graphitic N species located in the carbon skeleton was the key accelerating factor which promoted the catalytic C–H oxidation. Density functional theory (DFT) calculations further indicated that the iron species were not an essential factor but they acted as promoters for the catalytic performance of the catalyst. This study will expand the application of biomass-based heteroatom-containing compounds.
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
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2017
·Vol. 85
·期 1
·140-148
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IF 1.575
Guo Xingzhong,Yin Pengan,Wang Zichen,Yang Hui
Abstract Porous MoS 2 /C nanocomposites have been successfully via a sol–gel route with ammonium molybdatetetrahydrate ((NH 4 ) 6 Mo 7 O 24 ·4H 2 O) as molybdenum source, glucose as carbon source and tetramethyloxysilane (TMOS) as gelation accelerator, subsequently followed by high-temperature sulfuration and further NaOH etching to remove silica template derived from TMOS. The as-prepared MoS 2 /C nanocomposites were characterized by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), Fourier transform infrared spectroscopy (FT-IR), and nitrogen adsorption–desorption, and the effect of molybdenum precursor mass on the synthesis of product was also investigated. The Mo and TMOS mass ratio obviously affects the gelation time, phase composition and morphology of the resultant product, and an appropriate Mo and TMOS mass ratio allows the formation of lamellar structure as well as perfect MoS 2 phase. The as-prepared MoS 2 /C nanocomposite with Mo and TMOS mass ratio of 7:3 exhibits a BET surface area of 31 m 2 g −1 and a mesopore size of 20 nm, and demonstrates good electrochemical performances with 400 mA h g −1 specific reversible capacity after 60 cycles owing to the pore structure and synergistic effect between MoS 2 and amorphous carbon. Graphical abstract
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ChemCatChem
·
2016
·Vol. 8
·期 21
·3317-3322
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IF 4.724
Ziyu Liu,Dan Wu,Shu Ren,Xinqing Chen,Minghuang Qiu,Xian Wu,Chengguang Yang,Gaofeng Zeng,Yuhan Sun
Graphical Gasoline from methanol : ZSM-5 crystals with controllable c -axis length were successfully synthesized through a one-pot solvent-free route, with urea as an additive. Catalytic tests for the methanol to gasoline (MTG) conversion showed that the prepared c -axis oriented hierarchical ZSM-5, which allow fast mass transfer, exhibited both 100 % methanol conversion and far longer lifetime (900 h) than those of ZSM-5 with conventional morphology (350 h). ZSM-5 crystals with controllable c -axis length were successfully synthesized through a one-pot solvent-free route, with urea as an additive. X-ray diffraction patterns (XRD) show that the prepared samples exhibit high crystallinity. N 2 adsorption–desorption isotherms and mercury intrusion porosimetry (MIP) analysis together with TEM observations indicate that micro-, meso-, and macropores exist in the obtained samples. Catalytic tests for the methanol to gasoline (MTG) conversion showed that the prepared c -axis oriented hierarchical ZSM-5, which allow fast mass transfer, exhibited both 100 % methanol conversion and far longer lifetime (900 h) than those of ZSM-5 with conventional morphology (350 h) in the MTG reaction. The enhanced MTG performance by the c -axis oriented zeolite under one-pot solvent-free synthesis is of great importance as it is easily scaled-up for industrial applications.
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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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高影响因子
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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APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Baolin Yan,Juan Zhou,Xiaoyu Liang,Kainan Song,Xintai Su
The production of H 2 by photocatalytic water splitting has become a promising approach for clean, economical, and renewable evolution of H 2 by using solar energy. In spite of tremendous efforts, the present challenge for materials scientists is to build a highly active photocatalytic system with high efficiency and low cost. Here we report a facile method for the preparation of TiO 2 /C nano-flakes, which was used as an efficient visible-light photocatalyst for H 2 evolution. This composite material was prepared by using a phase-transfer strategy combined with salt-template calcination treatment. The results showed that anatase TiO 2 nanoparticles with the diameter of ∼10 nm were uniformly dispersed on the carbon nano-flakes. In addition, the samples prepared at 600 °C (denoted as T600) endowed a larger surface area of 196 m 2 g −1 and higher light absorption, resulting in enhanced photocatalytic activity. Further, the T600 product reached a high H 2 production rate of 57.2 μmol h −1 under visible-light irradiation. This unusual photocatalytic activity arose from the positive synergetic effect between the TiO 2 and carbon in this hybrid catalyst. This work highlights the potential of TiO 2 /C nano-flakes in the field of photocatalytic H 2 evolution under visible-light irradiation.
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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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CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 23
·期 66
·16898-16905
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IF 5.317
Jing Zeng,Yang Yang,Shaobo Lai,Jianxing Huang,Yiyong Zhang,Jing Wang,Jinbao Zhao
Graphical Cathode for magnesium-ion batteries : An electrochemically desodiated phase NaV 2 (PO 4 ) 3 /C has been developed as a high-voltage cathode material (ca. 2.5 V vs. Mg 2+ /Mg) for rechargeable magnesium batteries, offering good cycle performance. The electrochemical reaction involves an intercalation mechanism and shows good reversibility. The lack of suitable high-voltage cathode materials has hindered the development of rechargeable magnesium batteries (RMBs). Here, mesoporous Na 3 V 2 (PO 4 ) 3 /C (NVP/C) spheres have been synthesized through a facile spray-drying–annealing method, and their electrochemically desodiated phase NaV 2 (PO 4 ) 3 /C (ED-NVP/C) has been investigated as an intercalation host for Mg 2+ ions. The obtained ED-NVP/C exhibits an average discharge voltage of around 2.5 V (vs. Mg 2+ /Mg), higher than those of most previously reported cathode materials. In addition, it can deliver an initial discharge capacity of 88.8 mA h g −1 at 20 mA g −1 , with good cycling stability. Ex situ X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results demonstrate that the electrochemical reaction is based on an intercalation mechanism and shows good reversibility. Galvanostatic intermittent titration technique (GITT) data have revealed that the intercalation process involves a two-phase transition. The reported ED-NVP/C cathode material with high working voltage offers promising potential for application in RMBs.
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高影响因子
CATALYSIS COMMUNICATIONS
·
2017
·
IF 3.33
Junyi Liu,Hua Huang,Xianxiang Liu,Jiafu Xiao,Sheng Zhong,Xichun She,Zaihui Fu,Steven Robert Kirk,Dulin Yin
A series of Fe 2 O 3 doped SBA-15 materials were prepared via an equivalent-volume impregnation method. The resultant Fe 2 O 3 -containing SBA-15 materials showed good performance in phenol methylation . Under the same conditions, the mesoporous catalyst with 5 wt.% Fe 2 O 3 showed the superior catalytic activity to that of pristine α -Fe 2 O 3 even at lower reaction temperature (320 °C vs. 350 °C). The elevated catalytic activity observed for the mesoporous catalyst could be due to high level dispersion of Fe 2 O 3 species in the mesoporous framework. Furthermore, the mesoporous catalyst possessed long lifetimes, which could be used continuously for 2000 h without significant loss of activity.
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MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 7
·2089-2095
·
IF 4.58
Dong YongPing,Peng Ying,Wang Jiao,Wang ChengMing
Carbon dots (C-dots) display strong cathodic electrogenerated chemiluminescence (ECL) in neutral aqueous solution in the presence of potassium persulfate. ECL intensities strongly depend on the method of synthesis of C-dots. The reactions between the electrochemically reduced intermediates of C-dots and potassium persulfate generate a strong ECL signal. Spectral and electrochemical studies revealed that cytochrome c reacts with potassium persulfate before its electrochemical reduction to generate the strong oxidant radical SO 4
•- which reacts with C-dots to give an enhanced ECL signal. This finding was exploited to design a sensitive ECL assay for cytochrome c. The effects of the amount of C-dots, the pH value, and the persulfate concentration were optimized. Under the optimal conditions, the ECL signals (generated at −1.4 V) increase linearly with the concentration of cytochrome c in the range from 1.0 nM to 10 μM, with a detection limit of 0.2 nM. The modified electrode exhibits high sensitivity and good selectivity.
Carbon dots display strong cathodic electrogenerated chemiluminescence (ECL) in neutral condition with potassium persulfate as coreactant. Cytochrome c strongly enhances the ECL signal, and can be sensitively detected by exploiting this effect.
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