MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Yanshu Luo,Bingqiong Tan,Xianghui Liang,Shuangfeng Wang,Xuenong Gao,Zhengguo Zhang,Yutang Fang
Metal organic frameworks (MOFs) MIL-100(Fe) is considered to be a promising porous adsorbent for dehumidification due to its good hydrophilicity and hydrothermal stability. However, the powdery MIL-100(Fe) prepared by the conventional hydrothermal method is not suitable for industrial rotary desiccant dehumidifier. In order to produce a high-performance rotor core component, a new dry gel conversion in situ synthesis strategy for glass-fiber MIL-100(Fe) monolithic adsorbent was proposed in this paper. The effects of the reaction sol concentration on the crystalline phase, morphology, pore structure , adsorption/desorption performance and the cycling stability of the monolith were discussed in detail. The results showed that MIL-100(Fe) crystals which evenly dispersed in the surface and voids of glass fiber, could be conveniently synthesized in the reaction sols with molar ratios of 1Fe (III)/0.67BTC/xH 2 O (x = 93–185). Among them, the MIL-100(Fe) monolith obtained at x = 93 exhibited a high loading (85.7%), large BET specific surface area (1441 m 2 /g), S-shaped water vapor adsorption isotherm and high saturated adsorption ratio (0.496 g/g) at 298 K and 60% RH , low desorption activation energy (48.28 kJ/mol) as well as a reliable cycling stability. Favorable adsorption/desorption performance of MIL-100(Fe) monolith and convenient dry gel preparation process provide a guidance for the manufacture of high-performance dehumidification rotary wheel.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2020
·Vol. 31
·期 6
·4822-4835
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IF 2.22
Zhou Nan,Tan Junjie,Li Xi,Wang Lu,Jin Chenglong,Chen Ming,Yu Zhengsong,Liang Yani,Qiu Zhidong,Li Wenlong,Dong Yulin,Xie Zhizhong,Lin Yawei,Qu Deyu,Zhang Chaocan
A series of Bi 5 O 7 I/MIL-53(Fe) (BOI/MIL- w ) composites were successfully prepared by a facile in-situ solvothermal approach. The matched energy bands enabled Bi 5 O 7 I and MIL-53(Fe) to form a Z-scheme heterojunction which resulted in an efficient separation of the photo-induced electron–hole pairs. The photocatalytic activity of BOI/MIL- w was evaluated by the degradation of Rhodamine B (RhB) in water under the visible light irradiation. Compared with Bi 5 O 7 I, photocatalytic performances of BOI/MIL- w notably boosted. When the content of added MIL-53(Fe) was 3 wt%, BOI/MIL-3 presented the highest activity with a degradation efficiency of 99.7% only after 60 min of irradiation. The reaction rate constant k could reach 0.0992 min −1 which was nearly 12.6 times as high as that of Bi 5 O 7 I. Moreover, BOI/MIL- w had a good stability and reusability, which could ensure its practical application. Trapping experiments confirmed that h + and ·O 2 − were the dominant active species during the photocatalytic process, and further demonstrated the formation of the Z-scheme heterojunction facilitated the photocatalytic performance of BOI/MIL- w .
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CHEMOSPHERE
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2020
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IF 5.778
Yongjie Wan,Jinquan Wan,Joe R. Zhao,Yan Wang,Ting Luo,Shou Yang,Yaxin Liu
A novel catalyst (Fe-MOFs-MW) was facilely synthesized under microwave-assisted with NaOH as modulator for activating peroxydisulfate (PDS). The accelerated nucleation process was confirmed by Johnson-Mehl-Avrami (JMA) model. There were abundant reactive sites on prepared Fe-MOFs-MW while maintaining high Space-Time-Yield value up to 2300 kg/m 3 ·d. Degradation performance of Fe-MOFs-MW as PDS catalyst on sulfamethoxazole (SMX) removal was evaluated. Results indicated that Fe-MOFs-MW with more Fe element anchored (10%) exhibited excellent catalytic capacity for PDS. Besides, the fantastic stability and reusability were confirmed through recycle experiment. After recycled for 4 times, the removal efficiency of SMX and TOC was 88% and 31.3% compared to 98% and 38% without recycling, respectively. An accurate prediction model on the degradation effect with water matrices coexisted was established by response surface methodology (RSM) method. Moreover, SO 4 ·- , O 2 ·- and ·OH were confirmed as the main reactive species through chemical quenching and EPR tests. The mechanism of Fe-MOFs-MW/PDS process mainly based on electron circulation theory was proposed. As the robust PDS catalyst, facile prepared Fe-MOFs-MW was promising in the treatment of emerging pollutants.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Qiong Wu,Yining Liu,Haochuan Jing,Hongbin Yu,Ying Lu,Mingxin Huo,Hongliang Huo
Special enhanced synergistic effect of ultra-small γ-Fe 2 O 3 and graphene oxide (GO) on MIL-53 (Fe) was achieved for boosting photocatalysis. Compared to traditional methods of surface coverage, the incorporation of γ-Fe 2 O 3 (average size 2–3 nm) inside MOFs particles not only increased the light absorption of catalyst, but also formed numerous micro-heterojunctions with MOFs units and thus effectively facilitated the separation of photogenerated carriers. By supplying attachment sites for MOFs crystal, the functionalized GO reduced the size of MOFs particles to 100–200 nm, meanwhile improved their dispersibility. The active sites and quantum yield of photocatalytic reaction were also intensified benefiting from the large surface area and high electronic conductivity of GO. Therefore, the novel γ-Fe 2 O 3 -MIL-53(Fe)-GO composite exhibited the highest photocatalytic activity towards norfloxacin, with a removal rate of 92.8% in 90 min. The kinetic constant was 4.49-fold higher than that using pure MIL-53 (Fe), and 1.43-time greater than that in the system of MIL-53 (Fe) and hydrogen peroxide, which usually acted as efficient electron acceptors to increase the quantum yield and final photocatalytic performance of MOFs. Based on the identified intermediates, three NOR degradation pathways including the cleavage of piperazine ring, defluorination and decarboxylation, as well as the conversion of quinolones group were proposed. Photocatalytic mechanism investigation revealed the holes and hydroxyl radicals came from the reaction of electrons with oxygen played the important role in γ-Fe 2 O 3 -MIL-53(Fe)-GO photocatalysis. Moreover, the utilization of magnetic nanoparticles improved the recovery and recyclability of ternary catalyst.
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Journal of Environmental Chemical Engineering
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2020
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IF 4.3
Lilan Huang,Leitao Zhang,Deyuan Li,Qingping Xin,Rui Jiao,Xiaoyang Hou,Yuzhong Zhang,Hong Li
Delicate design of hierarchical and porous nanoarchitectures has become a highly effective strategy to develop novel bimetallic catalyst with improved stability and catalytic performance. Herein, a core-shell hierarchical 4A zeolite/Fe@Cu Fenton-like catalyst with 4A zeolite/Fe as core components and two-dimensional Cu hydroxide nanosheets assemblies as shell structure was fabricated through a simple and scalable approach and used for phenol degradation. The results indicated that 4A zeolite/Fe@Cu bimetallic catalyst had higher catalytic activity and utilization efficiency of H 2 O 2 than that of 4A zeolite/Fe and 4A zeolite@Cu monometallic catalysts at near neutral pH. In the presence of H 2 O 2 , the 4A zeolite/Fe@Cu bimetallic catalyst could remove 95.3 % phenol after 4 h at pH 5, which was much higher than that of monometallic catalyst under the same condition. The enhanced activity of 4A zeolite/Fe@Cu was ascribed to the synergistic effect between the 4A zeolite/Fe (core) and two-dimensional Cu hydroxide nanosheets (shell). More importantly, the copper hydroxide nanosheets with open network structure on the surface of 4A zeolite/Fe@Cu improved the stability of the Fe(III) at acidic conditions, and avoided reduced catalytic efficiency of Fe(III) caused by embedding effect. This strategy provided guidance to the design of high-performance bimetallic Fenton-like catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Kun Wu,Meng Wang,Angzhen Li,Zixuan Zhao,Ting Liu,Xiaodan Hao,Shengjiong Yang,Pengkang Jin
Mn-oxide-containing adsorbents have shown outstanding performances for the removal of As(III) through an “oxidation-adsorption” process. In this study, a new adsorbent of Fe-Mn-Cu ternary oxide (FMCTO) was fabricated to improve the redox reaction rate and to enhance the recovery of oxidative ability. FMCTO exhibited a stronger ability for As(III) removal than most of other adsorbents, because it has better oxidative capability for As(III) oxidation. The state of dynamic equilibrium for As(III) removal by FMCTO could be basically achieved within 3 h, and the As removal efficiency reached 98.9% at time = 24 h. The Langmuir As adsorption capacity of FMCTO was determined to be 204.8 mg/g. The As(III) removal efficiency of FMCTO was further boosted by 7% through oxygen gas aeration and decreased by 19% with nitrogen gas in the ambient during the first 3 h, indicating the positive effect of oxygen on As(III) oxidation. EPR and UV spectra methods were used to confirm the generation of superoxide radical (O 2 − ) and the enhanced production of Mn(III) soluble species on FMCTO surfaces, thus achieving a better As(III) oxidation performance. The XPS analysis results showed that the electron transfer from Cu(I) to Mn(IV) could improve the stability of Mn(III) within FMCTO. Meanwhile, Mn(II) ions could be oxidized to Mn(III) by O 2 − . Hence, the formation of a redox cycle between Mn(II) and Mn(III) along with the production of O 2 − plays a vital role in the upgraded As(III) removal mechanisms. This study provides new insights into the promotion of the capability of Mn-containing adsorbents for achieving the improved removal of As from As(III)-contaminated water.
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CHEMOSPHERE
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2020
·
IF 5.778
Haopeng Luo,Xin Zhou,Xiaojie Guo,Zhiyong Fang,Quanyuan Chen,Juan Zhou
The greatest constraint in the advanced oxidation processes involved Fe(II)/PMS was the low utilization of Fe(II) and PMS. In the present study, the co-catalytic effect of WS 2 on the Fe(II)/PMS system for the degradation of organics was investigated. In the presence of WS 2 , Fe(III) was reduced to Fe(II) during the reaction and resulted in improved decomposition of PMS as well as the degradation of 4-chloriphenol (4-CP). The decomposition rate of PMS and degradation efficiency of 4-CP were 10% and 25% in the Fe(II)/PMS process, while the efficiencies respectively increased to 99% and 100% in the WS 2 assisted Fe(II)/PMS system. The degradation of 4-CP was completed via the free radical pathway and SO 4 • - played a more important role than other active species. Low concentration of inorganic ions such as Cl − and HCO 3 − exhibited irrelevant effect while humic acid showed significant suppression on the WS 2 /Fe(II)/PMS system. Additionally, characterization and recycle results implied that WS 2 maintained a good stability during the co-catalytic processes.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Shan Yuan,Lili Cui,Xingquan He,Wei Zhang,Tewodros Asefa
Developing highly active, stable and sustainable electrocatalysts for overall water splitting is of great importance to generate renewable H 2 for fuel cells. Herein, we report the synthesis of electrocatalytically active, nickel foam-supported, spherical core-shell Fe-poly(tetraphenylporphyrin)/Ni-poly(tetraphenylporphyrin) microparticles (FeTPP@NiTPP/NF). We also show that FeTPP@NiTPP/NF exhibits efficient bifunctional electrocatalytic properties toward both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER). Electrochemical tests in KOH solution (1 M) reveal that FeTPP@NiTPP/NF electrocatalyzes the OER with 100 mA cm −2 at an overpotential of 302 mV and the HER with 10 mA cm −2 at an overpotential of 170 mV. Notably also, its catalytic performance for OER is better than that of RuO 2 , the benchmark OER catalyst. Although its catalytic activity for HER is slightly lower than that of Pt/C (the benchmark HER electrocatalyst), it shows greater stability than the latter during the reaction. The material also exhibits electrocatalytic activity for overall water splitting reaction at a current density of 10 mA cm −2 with a cell voltage of 1.58 V, along with a good recovery property. Additionally, the work demonstrates a new synthetic strategy to an efficient, noble metal-free-coordinated covalent organic framework (COF)-based, bifunctional electrocatalyst for water splitting.
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Energy Technology
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2020
·Vol. 8
·期 9
·2000205
·
IF 3.404
Qiang Liu,Jiaming Wang,Kang An,Siran Zhang,Guilong Liu,Yuan Liu
In view of the dual active sites mechanism of direct ethanol synthesis and the excellent catalytic performance of bimetallic catalysts, a series of Ni–Fe alloy catalysts with different Ni/Fe molar ratios derived from layered double hydroxides (LDHs) precursors are synthesized. During the calcination and reduction process of LDHs precursors, the Ni–Fe alloy is obtained, and attributed to all the elements being evenly dispersed at the atomic level in the LDHs precursors; meanwhile, a strong interaction between Ni–Fe alloy and MgAl 2 O 4 support exists. As a result, Ni–Fe alloy nanoparticles are highly dispersed on the MgAl 2 O 4 surface. The high CO adsorption ability on the Ni–Fe alloy and synergism catalysis between Ni and Fe result in excellent catalytic activity and high selectivity to ethanol on the bimetallic Ni–Fe alloy. In addition, the strong antisintering ability and stable alloy structure bring about a good catalytic stability. This research proposes a new catalytic system for direct ethanol synthesis from syngas.
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APPLIED CLAY SCIENCE
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2020
·
IF 4.605
Yaowu Cao,Qinghai Guo,Mengsi Liang,Weihao Sun
Antimony enrichment in aquatic environments is of great concern to international community. High-temperature geothermal waters usually contain excessive Sb, which are apt to contaminate the groundwaters or surface waters used as drinking waters in and around a hydrothermal area. However, Sb removal from geothermal water is rarely documented and the effect of high temperature on Sb removal has not received much attention. In this study, batch sorption experiments were conducted to investigate Sb removal from water by a hydroxyl-intercalated, mechanochemically synthesized Mg-Fe-LDH (i.e. Mg-Fe-OH-LDH) capable of avoiding secondary pollutions commonly related to other Mg-Fe-LDH intercalated by undesirable anions, such as Cl − and NO 3 − . The sorption capacities of Mg-Fe-OH-LDH for Sb(III) and Sb(V) were up to 48.7 and 30.0 mg/g, respectively. Notably, Mg-Fe-OH-LDH performed even better in removing aqueous Sb(V) at higher temperatures, superior to sorption of Sb by iron oxides that is generally exothermic and tends to be inhibited by increasing reaction temperature. The removal of Sb(V) existing as Sb(OH) 6 − by Mg-Fe-OH-LDH was attributable to its exchange with interlayer hydroxyl, and therefore could be impaired to some degree by coexisting anions with stronger electronegativity or smaller ionic radii . In contrast, anion exchange didn't contribute so much to Sb(III) sorption, because the main Sb(III) species at pH < 10 is neutral Sb(OH) 3 . XPS analyses confirmed that inner-sphere complexation between sorbed Sb(III) and Fe on Mg-Fe-OH-LDH layers was formed, which was hardly affected by competitive anions. Mg-Fe-OH-LDH is promising to be practically applied in removing both Sb(III) and Sb(V) from contaminated natural waters, wastewaters, or geothermal waters potentially acting as a pollution source .
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MATERIALS CHEMISTRY AND PHYSICS
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2020
·
IF 3.408
Yu Chen,Jin Guo,Minyi Lu,Bo Liang
A novel Ni–Fe nanosheets catalyst supported on α-Al 2 O 3 foam ceramic was synthesized by a hydrothermal method and used to obtain multi-walled carbon nanotubes (MWNTs) via the propane partial oxidation . Catalytic performance tests were carried out at 600 °C and atmospheric pressure using a fixed-bed reactor. The synthesized catalysts and carbon materials were analyzed using various characterization methods. According to the field emission scanning electron microscope (FESEM) results, the catalyst morphology was a 3D grid structure consisting of nanosheets 800 nm length and 80 nm width. Additionally, the quantity and quality of the carbon nanotubes were greatly influenced by different oxygen-to-propane molar ratios, defined as the equivalence ratio ϕ (ϕ = 1.5, 1.78, 2). Transmission electron microscope (TEM) images showed that carbon nanotubes over all catalysts were MWNTs. In addition, the thermogravimetric analysis and Raman data showed that a high yield of MWNTs was obtained at ϕ = 1.78, but the accumulated MWNTs at ϕ = 1.5 exhibited a higher degree of graphitization (I D /I G = 0.89) compared with the other two equivalence ratios.
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CLAYS AND CLAY MINERALS
·
2019
·Vol. 67
·期 4
·325-333
·
IF 1.835
Guo Yu-Hua,Pan Guo-Xiang,Xu Min-Hong,Wu Tao,Wang Yong-Ya
Adsorption desulfurization is a potential new method for deep desulfurization of fuel oil. The development of adsorbents with high adsorption capacity and selectivity is the core of deep adsorption desulfurization. The adsorption behavior of thiophene in MCM-41 mesoporous materials modified by various metal ions was studied in order to understand the adsorption desulfurization process of molecular sieves. The Fe-, Co-, and Zn-modified MCM-41 materials were prepared using a one-step in situ hydrothermal synthesis method. The modified MCM-41 molecular sieves maintained the mesoporous structure, and the metal ions had specific dispersion on the surface of the molecular sieves. Adsorption of thiophene on the surfaces of molecular sieves had both physical and chemical characteristics. The adsorption desulfurization performance of the modified molecular sieve was superior to that of the pure silica molecular sieve. In the simulated gasoline with sulfur content of 220 μg/g, when the amount of adsorbent used was 100 mg, the adsorptive desulfurization performance tended to be in equilibrium, and the optimum adsorption temperature was 30°C. Fe-MCM-41 and MCM-41 molecular sieves reached adsorption equilibrium after ~60 min, but the desulfurization rate of Co-MCM-41 and Zn-MCM-41 still increased slightly. The kinetic simulation results indicated that the pseudo-second-order kinetics adsorption model described well the adsorption process of thiophene on molecular sieves. The molecular sieve Fe-MCM-41 had the best desulfurization performance with an equilibrium adsorption capacity of 14.02 mg/g and the desulfurization rate was ~90%.
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