Small
·
2021
·Vol. 17
·期 36
·2102002
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IF 13.281
Hong Li,Xinxin Shu,Peiran Tong,Jihui Zhang,Pengfei An,Zhengxing Lv,He Tian,Jintao Zhang,Haibing Xia
In this work, Fe–Ni alloy nanoclusters (Fe–Ni ANCs) anchored on N, S co-doped carbon aerogel (Fe–Ni ANC@NSCA catalysts) are successfully prepared by the optimal pyrolysis of polyaniline (PANI) aerogels derived from the freeze-drying of PANI hydrogel obtained by the polymerization of aniline monomers in the co-presence of tannic acid (TA), Fe 3+ , and Ni 2+ ions. In addition, the optimal molar ratio of the TA, Fe 3+ , and Ni 2+ ions for synthesis of Fe–Ni ANC@NSCA catalysts are 1:2:5, which can guarantee the formation of carbon aerogel composed of quasi-2D porous carbon sheets and the formation of high-density Fe–Ni ANCs with an ultrasmall size between 2 to 2.8 nm. These Fe–Ni ANCs consisting of N 4 –Fe–O–Ni–N 4 moiety are proposed as a new type of active species for the first time, to the best of the authors’ knowledge. Thanks to their unique features, the Fe–Ni ANC@NSCA catalysts show excellent performance in oxygen reduction reaction with a half-wave potential ( E 1/2 ) of 0.891 V and oxygen evolution reaction (260 mV @ 10 mA cm −2 ) in alkaline media as bifunctional catalysts, which are better than the state-of-the-art commercial Pt/C catalysts and RuO 2 catalysts. Moreover, Zn–air battery assembled with the Fe–Ni ANC@NSCA catalysts also shows a remarkable performance and exceptionally high stability over 500 h at 5 mA cm −2 .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Yihui Wu,Yuan Zhang,Yuxin Wang,Zhen He,Zhengjian Gu,Shuochao You
Ni–Fe–Sn electrocatalyst supported on nickel foam (Ni–Fe–Sn/NF) with high efficiency of hydrogen evolution reaction (HER) has been successfully fabricated through one-step potentiostatic electrodeposition route. The optimized Ni–Fe–Sn/NF displayed an extremely low overpotential of, respectively, 144 and 180 mV at 50 and 100 mA cm −2 for HER in alkaline condition. Moreover, it could retain its superior stability for at least 12 h. The remarkable electrocatalytic activity of our electrocatalyst is ascribed to the high conductivity originated from synergistic effects between Ni, Fe, and Sn during HER process.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Liuyang He,Lixin Lv,Suresh C. Pillai,Hailong Wang,Jianming Xue,Yongfei Ma,Yanli Liu,Yulin Chen,Li Wu,Zulin Zhang,Lie Yang
Iron/copper bimetallic nanoparticles based sludge biochar (Fe/Cu-SBC) was prepared by using a modified co-precipitation route. The Fe/Cu-SBC system prepared was subsequently applied to activate periodate (IO 4 − ) to degrade diclofenac sodium (DCF) by using UV light at room temperature (25 °C). The physicochemical properties of both SBC and Fe/Cu-SBC such as morphology, physical properties, crystal structures and functional groups were examined. The type and number of surface functional groups were found to be increased and the catalytic performance was improved by the modification of Fe/Cu bimetallic nanoparticles. The influence of various parameters to evaluate the catalytic efficiency such as periodate (PI) concentration, dosage of catalysts, UV power, initial pH and coexisting anions were investigated. Under the optimized conditions (pH 6.9, UV-power 60 W, PI concentration of 5 mM and 0.1 g Fe/Cu-SBC), it was observed that 99.7% of DCF was degraded with a pseudo-first-order kinetics reaction constant 9.39 × 10 −2 min −1 . The radical scavenging experiments showed that IO 3 radicals were the predominantly reactive oxidants in the Fe/Cu-SBC/UV system. Therefore, this investigation provides a feasible alternative for the degradation of PPCPs in wastewater.
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ENVIRONMENTAL RESEARCH
·
2020
·
IF 5.715
Yun Bai,Doudou Wu,Wei Wang,Pei Chen,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Herein, the application of organic acids as chelating agent , including citric acid (CA), tartaric acid (TA), oxalic acid (OA) and ethylenediaminetetraacetic acid (EDTA), to enhance the degradation performance of MgO 2 /Fe(III) system was investigated in the terms of chelating agent dosage, Fe(III) dosage, reaction temperature, initial solution pH and inorganic anion. When the molar ratio of MgO 2 /Fe(III)/chelating agent was 1 : 0.7 : 0.3, the degradation efficiencies of Rhodamine B (RhB) increased from 6.7% (without chelating agent) to 42.3%, 98.5%, 48.9% and 25.8% within 30 min for CA, TA, OA, and EDTA, respectively. The promotion effect was mainly attributed to the chelation between chelating agents and Fe(III), rather than the acidification of chelating agents. The pseudo-first-order kinetic model well fitted RhB degradation in MgO 2 /Fe(III)/TA system, and the kinetic rate constant reached up to 0.295 min −1 . Hydroxyl radical was confirmed to be the dominant active species to degrade organics in the MgO 2 /Fe(III)/TA system. Notably, the degradation system could work in a broad pH (3–11) and temperature (5–35 °C) range. Moreover, the MgO 2 /Fe(III)/TA system can also effectively degrade methylene blue , tetracycline and bisphenol A. This work provided a new, efficient and environmentally-friendly Fenton-like system for stubborn contaminant treatment.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Wei Zhang,Wei Liu,Guoliang Li,Wei Du,Jianbo Lu,Jianguo Song,Qixia Yang,Xiangming Li,Huizhong Xu,Xu He,Jun Ma
The para arsanilic acid ( p -ASA) used as feed additive in the poultry and swine industries tends to transform into more toxic inorganic arsenic (As(V) and As(III)), leading to a greater risk to human health and environmental system. In this study, simultaneous adsorption and oxidation of p -ASA was achieved by a synthesized highly efficient nanostructured Fe-Ti-Mn composite oxide (FTMO), with a high specific surface area of 424.7 m 2 /g. The maximum adsorption capacity for p -ASA could be as high as 45.6 mg/g, meanwhile the combined oxidation/photo-oxidation processes led to the formation of intermediate containing hydrazine group, however, without release of toxic inorganic As(III) and As(V). The p -ASA adsorption by FTMO was verified as the chemisorption process with the formation of inner-sphere complexes at the solid/water interface, which was prominently influenced by solution pH, coexisting ions and humic acid, however relatively insensitive to ionic strength. The systematic characterization by FTIR, XPS, EPR and XANES revealed that Fe phase of FTMO played the dominant role for p -ASA adsorption, while Mn and Ti phases were responsible for the oxidation and photo-oxidation of p -ASA, respectively.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Yuanming Deng,Xi Zou,Zairan Liu,Jinzhi Wang,Zhong Wang,Jiaoning Tang
Here we present a simple method to prepare a highly efficient three components nanocomposites via thermal degradation of layered double metal hydroxides (LDHs)@polyvinyl alcohol (PVA) composites. Co 7 Fe 3 /CoFe 2 O 4 @C obtained from this method is applied to activate peroxymonosulfate (PMS) to degrade polluted organics and showed excellent performance. The best removal RhB efficiency of Co 7 Fe 3 /CoFe 2 O 4 @C (Co/Fe = 1:1) is near 100% within 10 min and the lowest ions elution (∼0.05 mg/L) under pH = 7, which is also better than the performance of the precursor Co–Fe LDH. Through further cycling experiments and degradation of p -nitrophenol, the stability and catalytic performance of the catalyst were verified. Finally, free radical scavenging experiments prove ·OH and SO 4 · - radicals participating in the reaction, which are the key factors for degradation. Based on the above, the derivation of the mechanism of Co 7 Fe 3 /CoFe 2 O 4 @C (Co/Fe = 1:1) catalyzing PMS to degrade polluted organics was proposed, and we consider this catalyst has great application prospect.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Zhengfeng Shen,Feifei Li,Jiangrui Lu,Zhidan Wang,Rui Li,Xiaochao Zhang,Changming Zhang,Yawen Wang,Yunfang Wang,Zhiping Lv,Jianxin Liu,Caimei Fan
Photocatalytic nitrogen fixation has been considered to be a safe, green, eco-friendly, and sustainable technology. However, photoinduced activation of inert dinitrogen is an important factor hindering the development of this technology. Herein, in-situ Fe 3+ doped flower-like BiOCl with highly active sites exposure was prepared by a solvent thermal method, which has excellent performance of N 2 photofixation. Compared with virgin BiOCl with no nitrogen fixation activity, Fe-BiOCl reached 30 μmol·L −1 ·h −1 ammonia evolution rate under simulated sunlight without any sacrificial reagent. Characterization results demonstrated that the enhancement of N 2 photofixation capacity was mainly attributed to the in-situ doped Fe 3+ in BiOCl, the doped Fe 3+ not only acts as a reaction center for N 2 activation also as an “electron transfer bridge” trapping and migrating electrons from BiOCl to N 2 molecules. Furthermore, the transformation of crystal facets from virgin BiOCl (0 0 1) to Fe-BiOCl (1 1 0) and (1 0 2) is more conducive for the exposure and accessibility of iron reactive sites. This work developed a potential strategy by in-situ introducing Fe 3+ active sites in BiOCl semiconductor substrate, which establishes a good basis for the application of semiconductor catalysts in nitrogen fixation.
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APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Wanliang Yang,Meng Chen,Jiayuan Zhou,Yingnan Duan,Yinmin An,Mao Liu,Mengkui Tian
Porous carriers play an important role in the catalytic transformation of syngas into higher alcohols, which promises higher sustainability in C1 chemistry. In this work, a series of hierarchical hollow silica spheres (HHSS) supported Cu-Fe bimetal catalysts were successfully prepared through ultrasonic-assisted impregnation for higher alcohols synthesis from syngas. Structural characterization results indicate that the hierarchical hollow structure of HHSS support can be maintained and the Cu-Fe bimetallic nanoparticles are highly dispersed on HHSS surface. The catalytic performances of samples in the test of CO hydrogenation for higher alcohols synthesis were investigated. The results revealed that the conversion rate of CO and the selectivity of C 2+ OH alcohol increased first and then decreased with the decrease of the amount of Cu content in the Cu x Fe y @HHSS catalyst. The highest CO conversion, alcohol selectivity and STY ROH over Cu-Fe@HHSS catalyst are 65.1 %, 46.6 %, and 118.1 gkg −1 h −1 , respectively. It was found that a large number of CuFe 2 O 4 were formed in Cu-Fe@HHSS catalyst and also confirmed that the CuFe 2 O 4 spinel and CuO-CuFe 2 O 4 were converted to Cu-Fe 5 C 2 composite in the spent Cu-Fe@HHSS catalyst, which can enhance the synergy between Cu-Fe bimetals. Furthermore, copper and iron are highly dispersed on HHSS after the reaction, which enhances the structural stability of the catalyst. Based on the development and utilization of low-cost catalysts and the production of clean liquid fuels, HHSS has a great prospect of catalyst support in the energy field.
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ENERGY & FUELS
·
2021
·
IF 3.605
Jianwen Guo,Jiang Wu,Yu Guan,Jianmin Wang,Qizhen Liu,Xu Mao,Xuemei Qi,Ping He,Huaning Wang
A Z-scheme heterojunction polyhedral-shaped BiOIO3/MIL-53(Fe) photocatalyst is prepared by a solvothermal method. The samples are characterized by XRD, XPS, SEM, TEM, FT-IR, UV–vis, PL, and other material characterization analysis methods. The photocatalytic performance of photocatalysts is studied for removal of vapor-phase mercury (Hg0) under visible-light irradiation. The results suggest that the Hg0 removal efficiency of the BiOIO3/MIL-53(Fe) composite is significantly improved compared with that of MIL-53(Fe). When the molar ratio of BiOIO3 and MIL-53(Fe) is 2:1, the BiOIO3/MIL-53(Fe) composite photocatalyst exhibits the best Hg0 removal efficiency, reaching 74.19%. BiOIO3 and MIL-53(Fe) form a Z-scheme heterojunction with a suitable energy band structure, which results in the effective separation of photoinduced electron–hole pairs and delays their recombination. Finally, the photocatalytic oxidation mechanism of Hg0 by the BiOIO3/MIL-53(Fe) composite is proposed, which paves the way for the study of the built-in electric field and electron transport channels between binary photocatalyst materials.
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ULTRASONICS SONOCHEMISTRY
·
2020
·
IF 6.513
Nannan Geng,Wei Chen,Hang Xu,Mingmei Ding,Tao Lin,Qiangshun Wu,Lei Zhang
In this work, as a new strategy, ultrasound/H 2 O 2 /MOF system was firstly applied by environmental-benign Fe-MOFs (MIL-53, MIL-88B and MIL-101) for tetracycline hydrochloride removal. The synthetic Fe-MOFs were characterized by XRD, FTIR, SEM, XPS, N 2 sorption-desorption isotherms and CO-FTIR. MIL-88B demonstrated the best catalytic performance because of its highest amount of Lewis acid sites. Influencing factors, contrast experiment, and corresponding dynamics were carried out to obtain the best experimental conditions and reaction system. Under optimal conditions ([Tetracycline hydrochloride] = 10 mg/L, [MIL-88B] = 0.3 g/L, [H 2 O 2 ] = 44 mM, [ultrasound power] = 60 W, and pH = 5.0), the-first-order kinetic rate constant k was calculated to be 0.226 min −1 , higher than the simple combination of the ultrasound system (0.004) and MIL-88B/H 2 O 2 system (0.163), indicating the importance of synergistic effect between ultrasound and Fenton reaction. EPR test and quenching experiment proved that ·OH is mainly responsible for tetracycline hydrochloride removal. The major reaction path is the adsorption and decomposition of H 2 O 2 by coordinative unsaturated iron sites on Fe-MOF, but it is not the only path. The direct decomposition of H 2 O 2 and the cavitation effect caused by ultrasound also contribute to the generation of OH.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wendong Liu,Lin Chu,Chenghui Zhang,Pengjuan Ni,Yuanyuan Jiang,Bo Wang,Yizhong Lu,Chuanxia Chen
Revealing the relationship between composition and enzyme-like activities is essential for the rational designs of nanozymes and related assays with improved performances. Here, a series of Fe-N co-doped porous carbon (Fe-N-C) nanozymes containing different Fe contents have been successfully prepared by facilely pyrolyzing hemin trapped zeolitic-imidazolate-frameworks (Hemin@ZIF-8). The special doping agent hemin will endow Fe-N-C with exceptionally high peroxidase-mimetic activities due to the hierarchically porous structure, high specific surface area, and high dispersed Fe-N x sites. Notably, the optimal Fe 55 -N-C nanozymes are used to detect bio-enzymes, by taking alkaline phosphatase (ALP) as a model, based on the inhibition of nanozymatic activity by ascorbic acid (AA). A linear activity range of 0.05–20 U/L is obtained with a low detection limit of 0.03 U/L, which is superior to the most published optical ALP assays. This work provides not only a new method for the design of the transition metal-N-C nanozyme with enhanced peroxidase-like activity but also a promising strategy for the detection of ascorbic acid-generating bio-enzymes with the assistance of specific substrates.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Xixi Chen,Shujuan Zhan,Dingsheng Chen,Chun He,Shuanghong Tian,Ya Xiong
Grey Fe doped CeO 2-σ with tunable surface and bulk oxygen vacancies (OVs) were facilely prepared by a hydrothermal method. The light absorption, charge transfer efficiency, and catalytic activity and mechanism closely depended on the OVs. By tailoring the surface and bulk OVs, the catalytic activity of grey ceria was boosted due to the enhanced production of reactive oxygen species (i.e. OH, surface O). Density functional theory calculations show that the OVs, especially the bulk OVs, modulate the electronic structure for narrowing the bandgap and accelerating the charge transfer. Meanwhile, the surface OVs more promote the adsorption of ozone and the bulk OVs more induces the dissociation of ozone into reactive surface O. The calculation results agree well with the experimental observations. This study provides a simple method for engineering the surface and bulk OVs of ceria and gains insight into their roles in photocatalytic ozonation .
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