FUEL
·
2020
·
IF 5.578
Liguang Dou,Mingkai Fu,Yuan Gao,Lei Wang,Cunji Yan,Tianzeng Ma,Qiangqiang Zhang,Xin Li
Direct hydrogenation of CO 2 to synthetic natural gas at a lower temperature remains a big challenge especially in the presence of H 2 S impurity. This contribution describes the synthesis, structure, morphology and doping effect of a series of robust catalysts for CO 2 methanation under resistive heating, based on Ni-layered double hydroxides (LDH) grown on porous and electrically conductive nickel foam (NF) derived structured catalysts. As a result, LaNi/NF showed the highest CO 2 conversion (55%) and CH 4 formation rate (631.5 mmol·g −1 ·h −1 ) at lower temperature of 250 °C and FeNi/NF gave the optimal conversion at 350 °C (75%, 860.9 mmol·g −1 ·h −1 ), which was superior to the most of recently reported Ni-based supported catalysts. We found that the CH 4 selectivity of the H 2 S (50 ppm) poisoned catalysts was significantly decreased and CO was verified as the main by-product. In this case, LaNi/NF and FeNi/NF still retained much higher conversion rate at 300 °C, 29.8% for LaNi/NF and 27% for FeNi/NF, than the almost deactivated unmodified Ni/NF with maximum 5% CO 2 conversion. The extraordinary activities can be explained as that the dopants can greatly strengthen the metal-support interaction and further enhance the reducibility of active metallic Ni, as XRD, HRTEM, TPR and XPS indicated. Besides of this, DFT calculations demonstrated that the existence of La can greatly promote CO 2 adsorption by lowering the adsorption barrier from 0.55 eV of pure Ni to 0.12 eV, and further inhibit the gaseous H 2 S from chemisorbing on the catalyst surface owning to the relatively unstable Ni-S bond.
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高影响因子
Nano Research
·
2020
·Vol. 13
·期 12
·3206-3211
·
IF 8.183
Zhang Meng,Hu Zheng,Gu Lin,Zhang Qinghua,Zhang Linghui,Song Qian,Zhou Wei,Hu Shi
A series of carbon-based binary single-atom catalysts of Fe and Ni coordinated by nitrogen are fabricated using a glucose-chelating method. Depending on the Ni/Fe content, they exhibit a wide-range of controllable CO/H 2 ratio from 0.14 to 10.86, which is meaningful to specific chemical processes. The durability of the catalyst is evaluated over an 8-hour period with no significant degradation of activity. The variation of the faradaic efficiency with Ni/Fe content is justified by density-functional-theory based calculation of the reaction barrier in both hydrogen evolution and CO 2 reduction reactions.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Jawad Ali,Ajmal Shahzad,Jia Wang,Jerosha Ifthikar,Wenli Lei,Gebremedhin G. Aregay,Zhulei Chen,Zhuqi Chen
The slow transformation of Fe 3+ back to Fe 2+ restrict the practical application of Fe-based catalytic treatment of organic pollutants . Herein, we report a new findings of MgAl-MoS 4 to accelerate the redox cycle of Fe 3+ /Fe 2+ in Fe 3+ /PMS system. Based on the degradation of 4-chlorophenol (4-CP) profile, the rate constant of Fe 3+ /MgAl-MoS 4 /PMS system was 40 to 42 folds higher than MgAl-CO 3 /PMS, MgAl-MoS 4 /PMS and Fe 3+ /PMS respectively. Moreover, Fe 3+ /MgAl-MoS 4 /PMS system was superior both in the degradation efficiency of pollutants as well as in the stoichiometric efficiency of oxidants from the recently reported Fe 3+ /WS 2 /PMS, Fe 3+ /MoS 2 /PMS or other well-known nano-catalysts systems. This co-catalytic effect of MgAl-MoS 4 on the studied redox metals falls in the order of Fe 3+ > V 5+ > Cu 2+ > Mn 2+ ~Ag + . Furthermore, the Fe 3+ /PMS/MgAl-MoS 4 system shows smooth degradation over a wide pH (3.0–7.0) and complete stabilities in the recycled studies. Additionally, the presence of excessive amounts of inorganic anions or organic matters also did not influence the degradation profile. In mechanism studies, both the unsaturated S 2− and Mo 4+ of MgAl-MoS 4 were disclosed to fuel electron continuously during the reduction of Fe 3+ ions, and thus accelerate the rate limiting step (Fe 3+ /Fe 2+ ). Additionally, the layered structure, memory effect and suitable surface charge of LDH material also concentrates the reactants molecules and hence, the boosted effect of MgAl-MoS 4 was associated with the better adsorption of Fe 3+ ions, the faster PMS decomposition, and the acceleration of Fe 3+ /Fe 2+ redox cycle. This work indicates a breakthrough in the field of classical homogenous Fe/PMS system, offers the very first report on the role of Mo 6+ and S 2− to modulate the redox behaviour of homogenous Fe ions in persulfate based advanced oxidation processes .
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Quanli Hu,Bin Yue,Hongyang Shao,Fan Yang,Jinghui Wang,Yin Wang,Jinghai Liu
Lanthanum-based LaMO 3 (M = Fe, Co, Ni) perovskite nanofibers were effectively fabricated by electrospinning approach coupled with calcination process. The crystallinity, microstructures, morphologies, elemental compositions, and chemical bonding states of LaMO 3 perovskites were investigated in detail. The electrochemical properties of LaMO 3 perovskite nanofibers as supercapacitor electrodes and lithium-ion battery anodes were elucidated. The specific capacitances of LaFeO 3 , LaCoO 3 , and LaNiO 3 nanofibers were 183.6, 95.8 and 116.3 F g −1 at the current density of 1 A g −1 , respectively. The supercapacitive properties of LaMO 3 NFs had originated from the redox reactions of M 3+ /M 2+ . As lithium-ion battery anodes, LaMO 3 (M = Fe, Co, Ni) nanofibers exhibited the specific discharge capacities of 331, 646, and 92 mAh g −1 after 200 cycles, respectively. This research endowed the potential and competent candidates of the perovskite type lanthanum-based nanofibers for supercapacitor electrodes and lithium-ion battery anodes.
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高影响因子
TALANTA
·
2018
·
IF 4.244
Qiumeng Chen,Chunhong Liang,Xiaodan Zhang,Yuming Huang
The N-doped porous carbon (NC) has been regarded as one of the promising support materials for nanoparticles (NPs) catalyst due to its inherent virtues such as porosity, large surface areas, and heteroatom incorporation. In this work, Fe/NC-800 hybrid was facilely prepared by uniform dispersion of in situ formed FeNPs onto NC-800 from carbonization of ZIF-8 at 800 °C for the first time. The optimized Fe/NC-800 catalyst was characterized by TEM , XPS and XRD. Compared with sole FeNPs and NC-800, the Fe/NC-800 catalyst exhibited an enhanced oxidase-like activity that could oxidize the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to the heavy blue without extra oxidants such as H 2 O 2 . The possible reason for the enhanced oxidase-like activity of the Fe/NC-800 was discussed on the basis of the experiments of radical scavengers , indicating the importance of superoxide (O 2 •- ) and singlet ( 1 O 2 ) in colorimetric reaction between TMB and Fe/NC-800 hybrid. Furthermore, the oxidase-like activity of Fe/NC-800 was significantly inhibited by dopamine (DA), leading to blue color fading. On this basis, a sensitive and selective colorimetric sensor was fabricated for the quantitative analysis of DA with a linear range of 0.01–40 μM and a low detection limit of 10 nM. The proposed colorimetric method was successfully applied to determine DA in human serum and injection samples, suggesting a promising application in biological analysis.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Zhen Zhong,Min Li,Jinghao Fu,Yuexin Wang,Yaseen Muhammad,Sihan Li,Jiaxing Wang,Zhongxing Zhao,Zhenxia Zhao
Cu 2 O/MIL(Fe/Cu) composite was fabricated via an in-situ Cu-bridging strategy to enhance interfacial synergistic effect of photo-Fenton catalysis for thiacloprid (TCL) degradation. Characterization results showed that: (1) Cu 2 O was proved to grow on the surface of MIL(Fe/Cu) in Cu 2 O/MIL(Fe/Cu) composite and display a high BET surface area of 1553 m 2 /g; (2) Cu 2 O/MIL(Fe/Cu) reduced band gap from 2.5 to 1.3 eV and extended absorption from UV to visible region; (3) Cu-bridge was proved to promote the intimate interface between Cu 2 O and MIL(Fe/Cu), which accelerated charge transferred and shortened the binding gap and the reaction pathway from photo-induced electrons to Fenton-generated radicals. As a result, this boosted the redox reaction of Fe 2+ /Fe 3+ and promoted the reversible degree of this catalytic redox ability of MIL(Fe). Catalytic performance exhibited that (1) Cu 2 O/MIL(Fe/Cu) showed a fast kinetics (2–40 times faster than the state-of-the-art catalysts) and ultra-high mineralization (82.3% within 80 min) for TCL degradation; (2) Cu 2 O/MIL(Fe/Cu) showed a promising cycling stability due to improved charge transfer ability that could protect Cu 2 O from photo-corrosion during photo-Fenton reaction; (3) The catalytic performance of Cu 2 O/MIL(Fe/Cu) was characterized and seven photocatalytic intermediates were identified by both HPLC/MS and Surface Enhanced Raman Spectroscopy. The cyanoimino group in TCL was proved for the first time to be attacked primarily. Moreover, among all the detected intermediates, thiazolidin-2-amine (P6) was found to be the most stable intermediate to be degraded, and it can directly influence the TOC determination during photodegradation process.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yuexin Wang,Zhen Zhong,Yaseen Muhammad,Hui He,Zhongxing Zhao,Shuangxi Nie,Zhenxia Zhao
Engineering of monodentate ligands induced defects was proposed to modify NH 2 -MIL-88B(Fe) in order to promote its synergetic photo-Fenton catalytic degradation performance for acetamiprid (ACTM) as model neonicotinoid insecticides. Three monodentate ligands with different coordination groups (benzoic acid, pyrrole and pyrrole-2-carboxylic acid) were applied to in-situ induce ligand vacancies on NH 2 -MIL-88B(Fe). Effect of defect coordination mode on its photo-Fenton catalytic performance was investigated through the ACTM degradation reaction. Ligand defects on NH 2 -MIL-88B(Fe) would generate three merits: (1) it can modulate surface properties to enhance adsorption affinity towards ACTM; (2) it can introduce large amount of monodentate ligands and ligand vacancies in MOFs to promote light absorption and electron-hole separation capacity for photo-catalysis; (3) it can increase the amount of Fe Lewis acid sites to improve redox capacity of Fe 2+ /Fe 3+ for Fenton-catalysis. In this work, Pyrrole-2-carboxylic acid (Pac) was proved to introduce more monodentate ligands in MOFs and generate more ligand vacancies as well. As a result, ACTM can be easily captured by defective NH 2 -MIL-88B(Fe) and degraded by in-situ triggered oxidative reaction through the synergistic “photo-Fenton catalysis”. Performance measurements showed that Pac-MIL88(Fe) achieved 7.3 times higher adsorption rate and 5.5 times higher catalytic rate for ACTM than that of pristine MIL88(Fe). Moreover, total organic carbon (TOC) conversion reached 97.0% within only 90 min using Pac-MIL88(Fe) as photo-Fenton catalyst, showing 1.7 times higher than pristine MIL88(Fe). Thus, the in-situ fabrication of ligand defect-containing MIL88(Fe) can be foreseen of potential for designing new MOFs for wider practical applications.
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高影响因子
Journal of Nanomaterials
·
2020
·
IF 1.98
Yan Li,Yuhui Weng,Shikong Lu,Meihua Xue,Bixia Yao,Wen Weng,Tao Zheng
In this paper, N, Fe-codoped carbon dots (N, Fe-CDs) were synthesized from β-cyclodextrin, ethylenediamine, and ferric chloride for the first time using a convenient one-step hydrothermal method. The obtained N, Fe-CDs were characterized by various methods including transmission electron microscopy, X-ray photoelectron spectroscopy, and Fourier-transform infrared spectroscopy. The N, Fe-CDs exhibited better catalytic activity than horseradish peroxidase (HRP) and caused an evident color change for 3,3,5,5-tetramethylbenzidine in the presence of H2O2. Kinetic experiments show that the apparent Km value for the N, Fe-CDs with TMB (0.40 mM) or H2O2 (0.35 mM) as the substrate was lower than that of HRP (0.43 and 3.70 mM), suggesting that the N, Fe-CDs have a much higher affinity for TMB and H2O2 than HRP. The Km/Vmax value for the N, Fe-CDs ( for H2O2) is significantly lower than that for HRP (), suggesting that the N, Fe-CDs have a stronger catalytic efficiency for H2O2 than HRP. Furthermore, a highly efficient and sensitive colorimetric detection method for glucose was developed using the N, Fe-CDs as mimic peroxidase to detect the hydrogen peroxide generated by the oxidation of glucose by glucose oxidase. The limit of detection for H2O2 and glucose was found to be 0.52 and 3.0 μM, respectively. The obtained N, Fe-codoped carbon dots, which possess simulated peroxidase activity, can potentially be used in the field of biotechnology.
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
·
IF 3.807
Jianpeng Li,Xianfeng Li,Hongyan Chen,Dingshu Xiao,Jiajia Li,Dekang Xu
In this paper, we present a facile and one-step way for synthesizing Fe, N dual doped highly porous graphitic biomass carbon (FeNC) by using K 2 FeO 4 to fulfill the activated process and catalytic graphitization of straws. The FeNC demonstrates hierarchically porous structure with large surface area of 1034 m 2 g −1 , Fe, N dual doping with certain amount of Fe-N x , and graphitic structure. With these favorable features, the electrocatalytic activity for oxygen reduction reaction (ORR) reveals that the FeNC exhibits positively onset potential with highly comparable limiting current density when comparing with the sample using conventional KOH activated agent. In additional, the assembled Zn-air battery using FeNC as air-cathode catalyst delivers a maximal power density of 128.4 mW cm −2 . Considering the abundance of straws on the earth and the low-cost and green prepared process, the present FeNC materials are highly promising in application in ORR catalysts for Zn-air battery and other energy-related fields.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 27
·期 27
·34503-34512
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IF 3.056
Huang Kai,Bian Hao,Zhang Meng,Zhan Cong,Li Can,Zhang Wei,Cui Changzheng,Lu Qiang,Lin Kuangfei,Zhao Jianhua
The iron and nickel bimetallic nanoparticles supported by the block copolymer polystyrene- block -poly (acrylic acid) (PS-b-PAA-nZVI-Ni) were synthesized successfully and were applied to assess the degradation of 1,1,1-trichloroethane (1,1,1-TCA) in water. An optimal dose of Ni loading was 2 wt%, while an optimal mass ratio of PS-b-PAA to Ni/Fe, i.e., 0.5:1, at which the dechlorination efficiency was a maximum. The size of PS-b-PAA-nZVI-Ni nanoparticles (average size ~ 50 nm) was three times smaller than that of nZVI-Ni due to the prevention of agglomeration of the resultant zerovalent iron nanoparticles by PS-b-PAA. In the applying aspect, the pseudo-first-order rate constant ( K obs ) of 1,1,1-TCA removal by PS-b-PAA-nZVI-Ni was 0.0142 min −1 within 240 min, which was approximately five times higher than nZVI. Meanwhile, PS-b-PAA-supported nZVI-Ni nanoparticles penetrated much deeper in quartz sand columns than nZVI-Ni nanoparticles, indicating PS-b-PAA had significant influence on nZVI transport. The findings from this study suggested that PS-b-PAA-nZVI-Ni, with its high reactivity, selective screening for 1,1,1-TCA, could be one significant potential for use as remedial agent to treat chlorinated solvents in water.
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PubMed
高影响因子
CARBON
·
2020
·
IF 8.821
Shuqi Hu,Wenpeng Ni,Daihui Yang,Chao Ma,Jiaheng Zhang,Junfei Duan,Yang Gao,Shiguo Zhang
Atomically dispersed Fe–N–C catalysts with additional Fe-containing nanoparticles including metal, carbides or oxides have shown great potentials towards oxygen reduction reaction (ORR) catalysis. However, the formation of these synergistically active nanoparticles and the effect of the porous carbon structures remain unclear. In this work, a novel single-atom-involved electrochemical catalyst, i.e. , Fe 3 O 4 nanoparticles encapsulated in atomically dispersed Fe–N–C (Fe 3 O 4 @FeNC) was reported. The optimized Fe 3 O 4 @FeNC exhibits excellent ORR activity with a half-wave potential of 0.890 V and a Tafel slope of 58.8 mV dec −1 , comparable with recently reported ORR catalysts and superior to these of commercial Pt/C. More importantly, the porous architectures not only affect the mass transfer and active sites, but casts huge influence on the nucleation of Fe 3 O 4 nanoparticles, the graphitization degree of the carbon support, the chemical environments of the elements, and the ORR catalytic pathways. Density functional theory calculations show stronger O 2 adsorption on Fe–N–C when supported on Fe 3 O 4 moieties, which may increase the reactant concentration for ORR and promote the overall activity. These findings will provide important references for the future understanding and design of single-atom-involved catalysts with enhanced electrochemical properties .
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高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 150
·期 8
·2437-2445
·
IF 2.482
Yang Zhi,Luo Mingsheng,Liu Qinglong,Shi Buchang
A potassium- and copper-modified iron-based catalyst (K–Cu–Fe/SiO 2 ) was synthesized by the co-precipitated method. The general structural properties of the catalyst were characterized with various techniques, including SEM, XRD, H 2 -TPR, N 2 adsorption–desorption and Raman spectroscopy. The results reveal that the fresh catalyst is mainly composed of α-Fe 2 O 3 phase with rod-shaped morphology formed by nanoparticles. The effect of activation process on the Fischer–Tropsch synthesis catalytic performance was then investigated. It shows that activation process has an important influence on the reactive stability. The in situ XRD and in situ Raman spectroscopy were used to study the structural changes of the Fe-based catalyst during reduction and reaction processes. The Fe 2 C iron carbide as the main active phase was observed after reduction process. Graphic Abstract
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高影响因子
危险品化学品经营许可证（带存储）