POLYHEDRON
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2019
·
IF 2.284
Lihong Qian,Yuqing Miao
The nanosheets of Co/Zn phosphate were deposited on nickel foam with the organized flower-like structure through a facile one-pot hydrothermal method. The resulted Co-Zn-P/NiFoam exhibits excellent electrocatalytic performance of oxygen evolution in basic solution and hydrogen evolution in acid solution with low onset potentials, high current responses, low Tafel slopes and good long-term stabilities. The nanosheet organized flower-like structure may contribute to the more active sites for target molecules, the higher efficiency for mass migration and electron transfer. The compact layer of Co/Zn phosphate may play a great role in its electrocatalytic stability for both OER in basic solution and HER in acid solution. This work offers a facile strategy to fabricate inexpensive and efficient electrocatalysts towards water splitting for possible applications in the future.
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ChemCatChem
·
2019
·Vol. 12
·期 2
·584-592
·
IF 4.495
Li-Ping Yang,Jian-Li Mi,Hui-Jie Wang,Jia-Hao Liang,Xue-Jing Yang,Yong-Hai Feng,Peng Zhang,Lu Liu
Graphical ORR and oxidation of alcohol : Bimetallic Cu−Zn co-doped porous N/C catalysts with the presence of different Cu forms show promising activity toward oxygen reduction reaction and oxidation of 1,2-propanediol. The development of non-precious metal catalysts toward oxygen reduction reaction (ORR) is essential for widespread application of fuel cells. Herein, bimetallic Cu−Zn co-doped porous N/C catalysts (Cu−Zn−N/C) with high N content were synthesized via a simple metal-organic framework (MOF)-derived method. The as-prepared Cu−Zn−N/C catalyst presents superior catalytic activity toward ORR with an onset potential of 0.90 V, a half-wave potential of 0.79 V, and a diffusion limiting current density of 5.82 mA cm −2 . It is found that Cu exists in three forms: one exists in Cu particles, and the others exist in Cu single atoms (either in high valence or in zero valence) that embedded in the carbon substrate. The evaporation of Zn atoms during the pyrolysis induces the pore structure of the carbon matrix, making it possible to support for the zero valent Cu atoms. In addition, as an efficient Cu-based catalyst for many applications, we show that the as-prepared catalyst can selectively oxidize 1,2-propanediol to lactic acid with 75.7 % selectivity at 82.8 % conversion.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
·
IF 3.375
Jian Zhang,Liang Wang,Zhiyi Wu,Hai Wang,Chengtao Wang,Shichao Han,Feng-Shou Xiao
We report the synthesis of Zn/ZSM-5 particles coated with a silicalite-1 zeolite shell (core–shell Zn/ZSM-5@silicalite-1) via grinding of the raw silica source materials with TPAOH and Zn/ZSM-5, followed by solvent-free crystallization at 180 °C for 72 h. The product was well characterized by the XRD patterns, N2 sorption isotherms, SEM images, and TEM images. Because of the core–shell structure, the Zn/ZSM-5@silicalite-1 sample exhibits high selectivities for benzene, toluene, and xylenes in the conversion of methanol, compared with those over ZSM-5 and Zn/ZSM-5 samples. The solvent-free synthesis offers an alternative method for preparing core–shell Zn/ZSM-5@silicalite-1 catalysts.
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APPLIED CLAY SCIENCE
·
2019
·
IF 3.89
Zilin Meng,Mi Wu,Shifeng Zhao,Ruisen Jing,Shutao Li,Yifei Shao,Xijuan Liu,Fengzhu Lv,Aiju Liu,Qian Zhang
A new approach to remove anionic dyes from wastewater was developed by forming Fe 3 O 4 @Zn-Al layered double hydroxides (ZnAl-LDH) in self-assembly process and naphthol green B (NG) with three negative charges was selected as target contaminant. In this process, the successful synthesis of compound and removal of contaminant were accomplished simultaneously. NG in wastewater can be totally removed and the removal efficiency reached the theoretical maximum of LDH removal capacity. The charge-limited removal process and the molecular arrangement of NG molecules in the ZnAl-LDH interlayer were analyzed experimentally and through simulation. The Fe 3 O 4 with small size was complete cover the layers of ZnAl-LDH making it easily separate from wastewater.
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CATALYSIS LETTERS
·
2019
·Vol. 149
·期 7
·1800-1812
·
IF 2.372
Yang Yalin,Liu Yanhong,Mao Baodong,Luo Bifu,Zhang Kewei,Wei Wei,Kang Zhenhui,Shi Weidong,Yuan Shouqi
I–III–VI quantum dots (QDs) play an important role in visible-light-driven photocatalysis due to their unique optical properties and widely tunable bandgap. However, these materials suffer from rich defect states and high charge carrier recombination. In this work, a facile mixed-ligand method was developed for the manipulation of the optical and photocatalytic properties of multinary Ag–In–Zn–S QDs by introducing 3-mecaptopropionic acid (MPA) into the l -cysteine (Cys) capped QDs system during synthesis. The effect and mechanism of MPA addition was systematically investigated. With the increase of MPA/Cys, the photoluminescence (PL) quantum yield (QY) of the QDs shows an obvious increase at the first stage (MPA/Cys < 5:5), whereas the particle size and UV–Vis absorption remain almost unchanged. Photocatalytic properties of QDs shows similar trend as PL QY with the increase of MPA/Cys, where the hydrogen production rate was doubled with MPA/Cys = 5:5. With ascorbic acid (AA) as the sacrificial reagent, the MPA/Cys capped QDs gave a hydrogen production rate as high as 6.64 mmol g −1 h −1 , which is comparable to the state-of-the-art results but without any cocatalyst, indicating the fascination of the simple mixed-ligand method. Further mechanism study indicates that the introduced MPA resulted in dramatic increase of the PL lifetime and the reduction of nonradiative decay, which can be ascribed to the strong passivation effect of MPA. The MPA/Cys capped QDs also show compressed charge recombination as indicated in electrochemical impedance spectra, slightly more negative ζ-potential and reduced hydrated particle radius, which may also contribute to the improved charge transfer for photocatalysis. Our method provides a super simple strategy for the defect manipulation of the Ag–In–Zn–S QDs without the sacrifice of charge transfer, which could be a useful guideline for efficient QDs-based visible-active photocatalysts. Graphical Abstract Mixed-ligand-modified Ag–In–Zn–S quantum dots with improved hydrogen production were prepared.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Tingzhen Li,Yinghuan Chen,Zhenghua Tang,Zhen Liu,Changhong Wang
The development of durable and high-efficiency bifunctional electrocatalysts for both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is critical to boost the performance of rechargeable zinc-air batteries (RZABs). Herein, we report a general approach for fabricating FeNi 3 C x -Pd y (x represents the indeterminate amount of carbon, y denotes the initial Pd mass loading percentage) nanorods using bimetallic metal-organic frameworks (MOFs) as sacrificial precursor. Among the series, FeNi 3 C x -Pd-7% demonstrates the best performance as bifunctional oxygen catalyst. It exhibits a high electrocatalytic activity with an unexpectedly low overpotential of 288 mV for OER at 50 mA cm −2 , which is far superior than the state-of-art RuO 2 catalyst, and its performance for ORR also approximates to the benchmark Pt/C catalyst. When incorporated as air-cathode catalyst in a self-assembled RZAB, FeNi 3 C x -Pd-7% exhibits a high power density of 234 mW cm −2 , a large energy density of ∼967 W h kg −1 , as well as a huge specific capacity of 772 mA h g −1 outperforming the noble-metal-based Pt/C + RuO 2 catalyst. Additionally, FeNi 3 C x -Pd-7% enables RZAB to obtain a long cycling life (over 900 cycles) with high efficiency and an overall overpotential of only 720 mV at 10 mA cm −2 , presenting great potential for the commercial applications of RZABs.
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ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Hualin Lin,Daming Chen,Chenbao Lu,Chao Zhang,Feng Qiu,Sheng Han,Xiaodong Zhuang
The development of efficient and low cost electrocatalysts for oxygen reduction reaction (ORR) to replace precious metal-based catalysts is one of the emerging issues for wide applications of fuel cells and metal-air batteries . In order to develop better catalysts for ORR and study the effect of co-doping, in this work, we prepared S/N co-doped porous carbons by using commercially available monomers and the radical polymerization method. Besides, silica sphere hard template was also used to prepare porous carbons with hierarchical porous structure. Sulfur blending and ammonia activation were used to rational control the S/N ratios for the porous carbons. The as-prepared S/N doped porous carbons exhibit high specific areas up to 681 m 2 /g, high N and S contents up to 4.9% and 0.9%, respectively. As electrocatalysts in alkaline media, these porous carbons show high ORR activity with half wave potential up to 0.825 V vs . RHE, electron transfer number of 3.9 and good tolerance to methanol. As air cathode for Zn-air batteries, these porous carbons show peak power density of 10.7 mW cm −2 at 17.4 mA cm −2 . This work indicates that great potential of S/N -doped carbons as high efficient electrocatalysts for ORR and Zn-air batteries.
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JOURNAL OF SOLID STATE CHEMISTRY
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2018
·
IF 2.179
Yong-Qiang Chen,Yuan Tian,Na Li,Sui-Jun Liu
Two isomorphous metal-organic frameworks (MOFs) {[M 2 ( μ 3 -OH)(trz)(sdba)(H 2 O)]·3H 2 O} ∞ (M = Ni for 1 , Zn for 2 , Htrz = 1,2,4-triazole, H 2 sdba = 4,4′-sulfonyldibenzoate) were obtained under the same reaction condition. Both of complexes present a three dimensional 8- c framework with whc1 topology based on M 4 -( μ 3 -OH) units. Moreover, the magnetic properties of 1 and anion sensing of 2 were investigated. The magnetic study show that the domain antiferromagnetic interactions exist in 1 . However, complex 2 can be considered as a promising chemical sensor for detecting PO 4 3¯ by means of fluorescence enhancement among various anions in aqueous solutions.
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高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Yuanxun Chen,Dan Ni,Xiaowei Yang,Congcong Liu,Junlin Yin,Kefeng Cai
A Zn-doped Ni-based metal−organic framework (Ni-MOF) material with honeycomblike hierarchical spherical structure is synthesized by a microwave-assisted method using HCl as the modulator for the first time. By adjusting the amount of the Zn ions doped, an optimal Zn doped Ni-MOF electrode material is obtained, which possesses a superior electrochemical performance: specific capacity of 237.4 mA h g -1 and 122.3 mA h g -1 at 1 A/g and 20 A/g, respectively. This is one of the highest performances reported so far for MOFs. The excellent electrochemical properties are ascribed to the unique crystal structure and special morphology of the Zn-doped Ni-MOF material. This work shows that the microwave-assisted synthesis is a rapid and efficient method for preparation of Ni-MOF supercapacitor electrode material.
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ADVANCED POWDER TECHNOLOGY
·
2019
·
IF 3.25
Kedir Ebrahim Ahmed,Dong-Hau Kuo,Worku Lakew Kebede
Heterojunction construction with low band gap materials is an effective way of utilizing UV light active materials under visible light irradiation. Here, we report the synthesis of Bi 2 (O,S) 3 /Zn(O,S) heterostructure using simple solvothermal method without surfactant. The catalysts were investigated with different characterization techniques. All the composite catalysts showed high light absorption capacity in the whole visible light spectrum. The catalytic activity of the catalysts was evaluated by Cr(VI) reduction. While pure Zn(O,S) catalyst showed no significant Cr(VI) reduction, higher photocatalytic activity than individual components were exhibited after heterojunction construction with Bi 2 (O,S) 3 . 20-BiZnOS catalyst with Bi/Zn molar percentage of 20% showed the best photocatalytic activity among the composites with 99.5% Cr(VI) reduction within 12 min under visible light irradiation. Heterojunction formation between Bi 2 (O,S) 3 and Zn(O,S) nanoparticle, and selective adsorption of Cr(VI) and desorption of Cr(III) on the surface of 20-BiZnOS composite catalyst were ascribed to the enhanced photocatalytic activity of the composite catalyst.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Anquan Zhu,Lulu Qiao,Pengfei Tan,Yongjin Ma,Weixuan Zeng,Rui Dong,Cheng Ma,Jun Pan
It still requires further investigations on the status of iron-based compounds and actual active sites in iron and nitrogen modified carbon based oxygen reduction catalysts (Fe N C), even though Fe-N x groups have been confirmed as a type of dominating active site for most Fe N C systems. Herein, a facile and practical surface engineering process is adopted to transform metallic iron and iron trioxide nanoparticles into Fe 2 N nanocrystals, meanwhile to make their coated graphitic carbon shells interrupted and broken. This sufficiently facilitates the elimination of embedded Fe 2 N with a subsequent acid-etching process, eventually obtaining AA-Fe 2 N@NC sample. Based on various physicochemical characterizations, it is found that the relative concentrations of defective carbon and pyridinic N for AA-Fe 2 N@NC are clearly enhanced, compared to its counterpart (Fe 2 N@NC sample). Electrochemical measurements demonstrate that AA-Fe 2 N@NC instead of Fe 2 N@NC has optimal onset potential (72 mV positive shift), half-wave potential (45 mV positive shift) and limiting current density values (increased by 0.97 mA cm −2 ). When used as an air cathode of rechargeable Zn-air battery, it delivers a high power density of 168.15 mW cm −2 , meanwhile a long-life cycling durability (60 h operation with an increased voltage gap of only 70 mV) is realized at 5 mA cm −2 . Combined with the calculation of TOF values and SCN - inhibition test, we make a conclusion and highlight that, in alkaline electrolyte, carbon defects and pyridinic N for this Fe N C system rather than Fe 2 N compounds or Fe-N x groups actually serve as the dominant active sites to afford a high-performance output of ORR activity.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 23
·20356-20366
·
IF 2.324
Du Yingying,Zhao Lei,Chen Hui,Huang Zhaohui,He Xuan,Fang Wei,Li Weixin,Zhang Fuqing,Wang Guanghui
Heterojunction is considered as very promising material for various applications in photocatalysis. Herein, an efficient heterojunction photocatalyst N/Zn–TiO 2 @NH 2 -MIL-125 was successfully synthesized for photo-degradation organic oxidation by biological-templated method. The electron–hole pairs can be separated in space more efficiently because of heterojunction structure. Systematical analyses of spectroscopy and microscopy measurements revealed that N/Zn–TiO 2 @NH 2 -MIL-125 heterojunction materials exhibited hierarchical porous structure with high surface area of 366.02 m 2 g −1 and outstanding optical properties. Photocatalytic activity was investigated by degradating of rhodamine B (1000 µM) under visible-light irradiation. The N/Zn–TiO 2 @NH 2 -MIL-125 showed enhanced photocatalytic activity for RhB degradation, which is respectively about 1.81 and 1.97 times higher than that of the pristine N/Zn–TiO 2 and NH 2 -MIL-125. Various advanced spectroscopic characterizations were applied including photoluminescence, Mott–Schottky curves and electrochemical impedance spectroscopy. A possible mechanism of enhanced photocatalytic oxidation activity for N/Zn–TiO 2 @NH 2 -MIL-125 composite under visible light irradiation was discussed.
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