APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiahang Qiu,Zhen Xin,Mu Zhang,Xudong Sun
Due to the multiple scattering of microwaves and the existence of electron aggregation polarization at heterogeneous interfaces, the design of hollow or anisotropic microstructures has always been one of the research focuses of microwave absorption materials (MAMs). In this work, an effective strategy has been proposed reasonably to manufacture yolk-shell pompon-like Fe@void@CeO 2 @Ni nanospheres via hydrogen reduction and multiple solvothermal procedures. The results show that the metallic iron core with a diameter of 300 nm and the outer CeO 2 layer with a thickness of 70 nm compound to form a yolk-shell structure, and the metallic nickel nanosheets with a length of about 100 nm are evenly embedded in the CeO 2 layer to form a pompon-like structure. These unique microstructures provide heterogeneous interfacial polarization, three-dimensional conductive networks, and multiple electromagnetic scattering which bring excellent dielectric loss to the composites. Combined with the inherent strong magnetic loss of magnetic metals, as-prepared composites exhibit excellent microwave absorption properties. The minimal RL value reaches −48.9 dB and the efficient absorption bandwidth reaches 14 GHz with the thickness ranges from 2.5 to 7 mm. Hence, this unique microstructural design scheme has great prospects in the field of MAMs.
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Catalysis Science & Technology
·
2022
·Vol. 13
·期 2
·468-478
·
IF 6.177
Xinyu Lu,Xiaoli Gu
The chemical demand for alkyl phenols (mainly extracted from fossil-derived resources) has been increasingly growing, which has accelerated global energy shortages. Due to the inherent aromaticity of lignin, its effective conversion into alkyl phenols is central to its adoption as a sustainable precursor to produce biochemicals. In this study, catalytic transfer hydrogenation (CTH) of alkali lignin was carried out in a mixed medium (isopropanol/formic acid) at 240 °C for 8 h over a series of bimetallic Ni based catalysts. The acidity and reducibility of the as-prepared catalysts are enhanced via WO3 introduction (to form a WO3–Al2O3 mixed support) and a bimetallic synergistic effect, respectively, leading to improved catalytic activity and selectivity towards alkyl phenols. Different kinds of phenolic compounds (e.g., those with substitutions of methoxyl, alkyl, alkenyl, carbonyl, carboxyl, or hydroxyl groups) were generated over these bimetallic Ni based catalysts with various combinations of Ni + Fe/Zn/Co/Mo/Cu, which was due to their own catalytic promotion of certain reactions (e.g., hydrogenation, deoxygenation, and/or hydrogenolysis). Reaction mechanisms of lignin depolymerization were proposed according to the distribution of phenolic compounds. This work provides a comprehensive investigation on yielding alkyl phenols from lignin CTH over a series of inexpensive bimetallic Ni based catalysts (Ni/(Fe/Zn/Co/Mo/Cu)–WO3/Al2O3), and undertook a catalytic evaluation of the bimetallic synergistic effects on improving the chemical selectivity towards alky phenols, which is beneficial for lignin valorization.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Katam Srinivas,Fei Ma,Yanfang Liu,Ziheng Zhang,Yu Wu,Yuanfu Chen
It is crucial but challenging to promote sluggish kinetics of oxygen evolution reaction (OER) for water splitting via finely tuning the hierarchical nanoarchitecture and electronic structure of the catalyst. To address such issues, herein we present iron-doped Ni3Se4/NiSe2 heterostructure-embedded metal–organic framework-derived mesoporous tubes (Ni-MOF-Fe-Se-400) realized by an interfacial engineering strategy. Due to the hierarchical nanoarchitecture of conductive two-dimensional nanosheet-constructed MOF-derived mesoporous tubes, coupled with fine tuning of the electronic structure via Fe-doping and interactions between Ni3Se4/NiSe2 heterostructures, the Ni-MOF-Fe-Se-400 catalyst delivers superior OER activity: it requires only a low overpotential of 242 mV to achieve 10 mA cm–2 (Ej=10), surpassing the benchmark RuO2 (Ej=10 = 286 mV) and displays exceptional durability in the chronoamperometric i–t test with a small current decay (6.2%) after 72 h. Furthermore, the water splitting system comprises a Ni-MOF-Fe-Se-400 anode and a Pt/C cathode requires a low cell voltage of 1.576 V to achieve Ej=10 with an excellent Faradic efficiency (∼100%), outperforming the RuO2–Pt/C combination. This work presents a novel interfacial engineering strategy to finely adjust the morphology and electronic structure of the non-noble metal-based OER catalyst via a facile fabrication method.
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高影响因子
Biomass Conversion and Biorefinery
·
2022
·
IF 4.05
Gao De,Han Feng,Waterhouse Geoffrey I. N.,Li Yan,Zhang Lili
A series of FeTPP-N/C-X catalysts were successfully prepared by adsorption of Fe tetraphenylporphine (FeTPP) onto a porous nitrogen-doped carbon (N/C) support using an ultrasonication method. The FeTPP-N/C catalysts were then used for the preparation of 5-hydroxymethyl-2-furan acid (HMFCA) by catalytic oxidation of 5-hydroxymethylfurfural (HMF) at 80 °C. The effects of reaction temperature, NaOH dosage, reaction time, and oxygen pressure on HMF conversion and HMFCA yield were systematically investigated. Under optimized testing conditions, a FeTPP-N/C-1 catalyst prepared using equal masses of FeTPP and N/C delivered a HMF conversion in water of 92.4%, with a selectivity to HMFCA of 97.2% over 6 h at an oxygen pressure of 1.0 MPa. Further, the catalyst showed good stability in five consecutive HMF oxidation tests. Based on the catalytic tests, and detailed catalyst characterization studies before and after reaction, a probable reaction mechanism was proposed for the selective oxidation of HMF to HMFCA by the FeTPP-N/C catalysts. Graphical Abstract
A series of FeTPP-N/C
catalysts were successfully prepared by the adsorption of iron
tetraphenylporphine (FeTPP) onto a porous nitrogen-doped carbon (N/C) support
using an ultrasonication method. The FeTPP-N/C catalysts were then used for the
catalytic aerobic oxidation of HMF to HMFCA. Under the optimized reaction conditions (temperature
80 °C, reaction time 6 h, O 2 pressure 1 MPa), a high HMF conversion
of 92.4% and a remarkable HMFCA selectivity of 97.2% were obtained, suggesting
that the developed noble-metal free catalyst has excellent promise for the
synthesis of valuable HMFCA from HMF.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Chengyuan Duan,Yi Feng,Yuming Xie,Meili Ding,Jianfeng Yao
A facile one-step synthetic strategy is proposed here to realize simultaneous amine-functionalized and Fe-doping modification of ZIF-8, aiming to optimize the Lewis acidic and basic properties of ZIF-8 for enhanced CO 2 adsorption and subsequent cycloaddition reaction of CO 2 and epichlorohydrin under solvent-free and relatively mild conditions (0.1 MPa and 80 °C). The obtained Fe-ZIF-8-NH 2 exhibits an improved CO 2 adsorption capacity of 63 mmol/g as compared to that of 18 mmol/g for pristine ZIF-8 and delivers a high catalytic CO 2 cycloaddition efficiency with the yield of target product of 92%, much higher than that of Fe-ZIF-8 (80%), ZIF-8-NH 2 (62%) and pristine ZIF-8 (40%). The improved performance can be attributed to the introduction of abundant –NH 2 groups and Fe-doping that enrich the Lewis acidity and basicity. Moreover, the obtained Fe-ZIF-8-NH 2 also exhibits high chemical stability and satisfactory recycling ability, which makes the obtained sample a promising catalyst for CO 2 capture and utilization.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Weiwei Li,Wenlan Ji,Murat Yılmaz,Tian C. Zhang,Shaojun Yuan
Arsenic is a toxic carcinogen, and arsenic pollution in groundwater is one of the most serious environmental problems in the world. Thus, it is an urgent problem to efficient removal of arsenic from groundwater. In this work, a novel MWCNTs/MIL-53(Fe) nanocomposite was successfully synthesized to improve the water stability of MIL-53(Fe) by incorporation of carboxylated multi-walled carbon nanotubes (MWCNTs) using a one-pot hydrothermal method, and was then used to efficiently adsorb As(V) ions from groundwater. Adsorption experimental results demonstrated an ultrafast adsorption rate of As(V) on the MWCNTs/MIL-53(Fe) nanocomposites in solution pH values of 3 to 10, and the adsorption equilibrium could be reached in circa 20 min with an adsorption capacity of 27.24 mg·g −1 in a low As(V) concentration of 10 mg·L −1 . The adsorption kinetics of As(V) on the MWCNTs/MIL-53(Fe) was found in line with the pseudo-second-order (PSO) kinetic model, and was simultaneously controlled by both internal diffusion and liquid film diffusion. The adsorption isotherm data conformed to the Redlich-Peterson isotherm model, indicating both physical and chemical adsorption occurred at heterogeneous interfaces. Moreover, the postulated adsorption mechanism of As(V) on MWCNTs/MIL-53(Fe) nanocomposites was ascribed to hydrogen-bond interaction, electrostatic attraction and chemical complexation. Therefore, the as-prepared MWCNTs/MIL-53(Fe) nanocomposites not only exhibit superior water stability and outstanding adsorption performance in removing arsenic-contaminated groundwater, but also offer a novel insight for rational preparation of water-stable MOF-based composites.
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ChemCatChem
·
2022
·Vol. 15
·期 1
·e202201234
·
IF 5.497
Lu Lin,Guikai Zhang,Liqun Kang,Tao Yu,Yang Su,Guang Zeng,Shengqi Chu,Wenhao Luo
Graphical Methane oxidation : Highly dispersed mononuclear Fe species encapsulated by ZIF-8 (Fe-ZIF-8) afford an optimal turnover rate of ∼45 mol C1 mol Fe −1 h −1 and a formic acid selectivity of ∼97 % in the direct methane oxidation at 323 K. The direct catalytic oxidation of methane into C1 oxygenates is a promising approach for methane valorization. However, the difficulties in CH 4 activation and inhibition of over-oxidation hinder the development of efficient catalysts for this transformation. Herein, highly dispersed Fe species confined by ZIF-8 are developed for the direct transformation of methane into value-added C1 oxygenates with H 2 O 2 as oxidant at 323 K. The as-obtained Fe-ZIF-8 can afford an optimal turnover rate (TOR) of ∼45 mol C1 mol Fe −1 h −1 . Note that the selectivity to HCOOH is ∼97 %, outstanding among the reported Fe-based heterogeneous catalysts. Combined analysis of X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, ultraviolet-visible diffuse reflectance spectroscopy and 57 Fe Mössbauer spectroscopy suggests that the catalytically active sites in Fe-ZIF-8 are mononuclear six-coordinated Fe 3+ species. The confinement of mononuclear Fe species within a porous metal-organic framework material can provide an exquisite, enzyme-like performance for highly selective oxidation of methane towards formic acid under mild conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xueying Cheng,Renquan Guan,Yunning Chen,Yudan Qian,Qingkun Shang,Yingnan Sun
In this study, the adsorption and photocatalytic degradation of oxytetracycline (OTC) were systematically investigated using different metal-doped anatase-phase mesoporous TiO 2 nanocatalysts (M−TiO 2 , M = Fe, Co, Ni, Cr). The results showed that doping with different metals had a significant effect on the ability of TiO 2 to adsorb and degrade OTC . Comparing the photoelectric properties of four photocatalysts (Fe-TiO 2 , Co-TiO 2 , Ni-TiO 2 and Cr-TiO 2 ), it was observed that the mutual synergy between the separation ability of the photogenerated carriers and the adsorption ability of pollutants was the fundamental reason for the excellent photocatalytic performance of Fe-TiO 2 . The relative intensities of the high-resolution mass spectrometry (HRMS) peaks were used to track and analyse the degradation products of pollutants at different adsorption or light-irradiation times during the photocatalytic process. The ability of the pollutants to undergo dark-state adsorption significantly influenced their degradation paths and products. The possible mechanism of the photocatalytic decomposition of pollutants using Fe-TiO 2 along different paths was proposed according to the Fukui function calculation and MS results. To the best of our knowledge, this is the first time that quantitative HRMS results have been used to assess the degradation pathways of pollutants.
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Catalysts
·
2022
·Vol. 12
·期 5
·534
·
IF 4.501
Zhaohui Teng,Shan Huang,Na Li,Qulan Zhou
Rice husk ash (RHA) has potential as a supporter of catalysts. In this research, we studied the activity and SO2tolerance of RHA-based Fe-Cu oxide in the reduction of NO by CO. Characterization methods were employed to study the properties of the catalysts and their SO2tolerance. Activity and SO2resistance were also tested at different temperatures. We recommend two catalysts with SO2resistance ability: Fe0.67Cu0.33/RHA (the highest catalytic activity) and Fe0.8Cu0.2/RHA. The NO removal rate hardly changed with the addition of SO2and was kept at about 100%. However, the CO conversion rate decreased with increasing SO2at the lower reaction temperatures, which may be due to the formation of sulfites. Fortunately, the deactivation was reversible and can be reduced with an increase in the reaction temperature. The results of our research may help promote the application of CO-SCR.Keywords:rice husk ash;Fe-Cu catalysts;NO reduction;SO2resistance;CO-SCR
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zongtang Liu,Haini Yang,Mian Wang,Yufeng Sun,Zhenghao Fei,Shujuan Chen,Rui Luo,Lin Hu,Chenggang Gu
Effective removal of polybrominated diphenyl ethers (PBDEs) from the environment is essential for the ecosystem and human health. Reductive debromination of PBDEs by nanoscale zerovalent iron (nZVI) has become an important technology. However, the agglomeration and low persistence catalytic activity of nZVI particles have become urgent problems to be improved. Herein, we report the first application of a new organo-attapulgite (OA) supported Fe/Pd nanoparticles (OA-Fe/Pd) composite for decabromodiphenyl ether (BDE209) removal. BDE209 was efficiently removed using OA-Fe/Pd with a reaction rate that was 9.97 times greater than that of the nZVI due to the synergetic effect of support material OA and Pd loading. OA could prevent nZVI particles from agglomeration and adsorb BDE209 molecules to its surface. Pd could supply atomic hydrogen and also prevent the oxidation of nZVI particles. The degradation of BDE209 by OA-Fe/Pd was affected by many factors and followed pseudo first-order kinetics. The degradation of BDE209 by OA-Fe/Pd underwent a stepwise debromination manner with the H-transfer dominant mechanism. BDE209 (25 mg∙L -1 ) could be degraded to penta-BDEs to diphenyl ether (DE) by 3.0 g∙L -1 OA-Fe/Pd within 240 min under neutral condition. This study provides some inspiration for improving the removal efficiency of PBDEs with nZVI-based materials.
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Small
·
2022
·Vol. 18
·期 9
·2104941
·
IF 15.153
Lixue Yang,Haoqi Yang,Shengyan Yin,Xiuyan Wang,Mingwei Xu,Guolong Lu,Zhenning Liu,Hang Sun
The Fenton-like reaction has great potential in water treatment. Herein, an efficient and reusable catalytic system is developed based on atomically dispersed Fe catalyst by anchoring Fe atoms on nitrogen-doped porous carbon (Fe SA/NPCs). The catalyst of Fe SA/NPCs exhibits enhanced performance in activating peroxymonosulfate (PMS) for organic pollutant degradation and bacterial inactivation. The Fe SA/NPCs + PMS system demonstrates a high turnover frequency of 39.31 min −1 in Rhodamine B (RhB) degradation as well as a strong bactericidal activity that can completely sterilize an Escherichia coli culture within 5 min. Meanwhile, the degradation activity of RhB by Fe SA/NPCs is improved up to 28 to 371-fold in comparison with the controls. Complete degradation of RhB can be achieved in 30 s by the Fe SA/NPCs + PMS system, demonstrating an efficiency much higher than most traditional Fenton-like processes. Experiments with different radical scavengers and density functional theory calculations have revealed that singlet oxygen ( 1 O 2 ) generated on the N-coordinated single Fe atom (Fe-N 4 ) sites is the key reactive species for the effective and rapid pollutant degradation and bacterial inactivation. This work innovatively affords a promising single-Fe-atom catalyst/PMS system for applying Fenton-like reactions in water treatment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Di Li,Zengyong Li,Ren Zou,Ge Shi,Yiming Huang,Wu Yang,Wang Yang,Chuanfu Liu,Xinwen Peng
Developing efficient bifunctional electrocatalyst for overall water splitting and conversion of biomass into value-added products at large current density is essential but challenging. Herein, a hierarchical Fe-doped Ni 2 P nanosheets hybridized with C on Ni foam (Fe-Ni 2 P@C/NF) was developed as a robust bifunctional catalyst with excellent catalytic activity for hydrogen evolution reaction (HER) with overpotentials of 75 and 313 mV at 10 and 1000 mA cm −2 , respectively, and as well as for OER with a lower overpotential of 269 mV at 400 mA cm −2 . Particularly, the integrated double-electrode electrolyzer for simultaneous HER and biomass-derived monosaccharide oxidation reaction (MOR) using Fe-Ni 2 P@C/NF only requires a low voltage of 1.55 V to drive a current density of 100 mA cm −2 . Meanwhile, the value-added lactic acid is obtained at the anode. This strategy of coupling biomass oxidation to promote H 2 production can significantly reduce energy consumption and obtain additional high value-added products.
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