Fundamental Research
·
2023
·
IF 6.2
Qian Hu,Taoyu Yang,Shanli Wang,Licong Xu,Minghua Wu,Deyou Yu,Kaixing Fu,Jinming Luo
Peracetic acid (PAA) has recently been considered a promising oxidant candidate for heterogeneous Fenton-like reactions; however, the main generation and contribution of organic radicals (R-O•) with unsatisfactory oxidation potential compromises wastewater decontamination efficiency. In this study, we demonstrate the rational design and synthesis of ultrafine FeO x nanocluster-anchored carbonaceous nanosheets (UFe-CN) for altering the PAA activation pathway from R-O• to •OH dominant process via in situ framework collapse carbonization of MIL-53(Fe). The constructed UFe-CN/PAA system effectively accelerated refractory micropollutant ( e.g. , p-nitrophenol (4-NP)) decomposition by the enhanced •OH formation (up to 65.24 μmol L − 1 ) under a wide pH range (3.0–9.0), outperforming the benchmark iron-based catalyst counterparts by 4.2–10.8 times. This outstanding Fenton-like catalytic activity of UFe-CN is primarily attributed to the significant improvement in electron mitigation, ca. 49 times higher than that of its MIL-53(Fe) counterpart, for interface catalysis reactions triggered by iron species cycling. Furthermore, to facilitate adaptive engineering, the organic pollutant removal efficiency could be easily tuned by varying several key treatment factors, including the initial pH, PAA concentration, and UFe-CN dosage. More importantly, the excellent practicality of UFe-CN/PAA was demonstrated by systematically evaluating the impact of the water matrix, catalyst regeneration capability, and wastewater treatment efficiency. Overall, this study provides a significant understanding of •OH-dominated PAA activation and an effective catalyst development paradigm to facilitate the practical application of PAA-based Fenton-like oxidation.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Qichao Lu,Jie Li,Chen Liang,Lei Liu,Jinxiang Dong
Under the dual pressures of oil depletion and low-carbon transition, Fischer-Tropsch synthesis (FTS) technology offers a viable option for producing high value-added lower (C 2 -C 4 ) hydrocarbons from non-oil sources. However, conventional Fe-based catalysts often suffer from deactivation due to carbon deposition and sintering. Here, we report a unique Fe-ZSM-5 catalyst synthesized by doping Fe into ZSM-5, which demonstrates excellent FTS catalytic performance. During high-temperature template removal, Fe species migrated from the zeolite framework to form highly dispersed FeO x clusters (∼2 nm). Upon treatment by syngas, these FeO x clusters aggregate to form uniformly small-sized Fe 5 C 2 @C core-shell particles distributed on ZSM-5 support. The confinement effect of the inter-crystalline structure effectively prevents the sintering of Fe 5 C 2 . The smaller Fe 5 C 2 particles exhibit controlled CO dissociation, reducing the concentration of activated carbon species (C*), and the carbon shells (∼6.5 nm) limit the departure of C*, effectively suppressing carbon deposition. This unique structure enables stable catalytic activity for over 100 hours with maintained product selectivity. The Fe-ZSM-5 catalyst achieved a C 2 -C 4 hydrocarbons selectivity of 54.52 %, nearing the 56 % theoretical limit of the Anderson-Schulz-Flory (ASF) distribution. Additionally, the hydrophobic carbon shell prevents excessive oxidation of Fe 5 C 2 , reducing CO 2 selectivity by ∼56 % compared to conventional Fe/ZSM-5 catalysts, significantly enhancing atomic utilization efficiency and aligning with the principles of green development.
研究领域:
化学工程
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材料科学
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能源催化
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DOI
高影响因子
Applied Sciences-Basel
·
2022
·Vol. 12
·期 8
·3769
·
IF 2.838
Wei Ma,Dong Ye,Haining Wang
Herein, a series of Co-Fe mixed oxide modified ZSM-5 adsorbents were synthesized using the ultrasonic-assisted impregnation method for the capture of elemental mercury. In comparison with other samples, Co4Fe1-ZSM-5 produced a relatively better performance, with the removal efficiency of around 96.6% Hg0and the adsorption capacity of around 901.63 ug/mg Hg0achieved at 120 °C. The interaction between CoOxand FeOximproved the reducibility of oxygen species, thus promoting the oxidation of Hg0. Among a variety of other gas components, O2and NO exerted a positive effect on Hg0, which improved its removal to a certain extent. By contrast, SO2caused an adverse effect on the capture of Hg0, which could be reversed to some degree by the introduction of 5% O2. After five cycles, the mercury removal efficiency of Co4Fe1-ZSM-5 remained above 90%, suggesting excellent recyclability. Finally, XPS analysis was conducted to reveal that Mars–Maessen mechanisms are dominant in the process of mercury adsorption.Keywords:Hg0adsorption;ZSM-5;cobalt oxide;iron oxide;regeneration
研究领域:
环境科学
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化学工程
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DOI
高影响因子
IONICS
·
2022
·Vol. 29
·期 1
·419-427
·
IF 2.961
Zhao Jiang,Zhang Da,Wang Shumeng,Wang Zhitong,Xu Rongqing
Laser direct writing of polyimide (PI) film to induce porous graphene as a flexible electrode facilitates the development of efficient, low-cost, and large-scale preparation of flexible planar micro-supercapacitors (MSCs). Nevertheless, current flexible MSCs based on laser-induced graphene (LIG) face bottlenecks such as poor LIG electrode wettability, inhomogeneous doping of heterogeneous components, and limited electrochemical performance. In view of this, a simple and effective process for in situ fabrication of flexible FeO x nanoparticles embedded N-doped LIG (FeO x @NLIG) electrode is developed by laser direct writing in this study. The as-assembled in-plane FeO x @NLIG MSCs exhibit an excellent areal specific capacitance of 13.82 mF cm −2 , a remarkable energy density of 1.228 mW h cm −2 at a high power density of 0.024 mW cm −2 , good flexibility, and conspicuous cycling stability. Besides, these high-performance in-plane FeO x @NLIG MSCs as a vital micro-energy storage component can be easily miniaturized, modularized, and integrated to suit customized needs of wearable electronics due to great advantages in terms of identicality and stability of the as-fabricated FeO x @NLIG. Graphical abstract
研究领域:
材料科学
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能源存储技术
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Liam John France,Wan Li,Yanke Zhang,Wentao Mu,Zhihang Chen,Junjun Shi,Qiang Zeng,Xuehui Li
A series of Fe-Zr mixed-metal oxides were prepared and examined for the simultaneous reduction of NO and SO 2 with CO. The catalyst containing 40 mol% exhibited near-complete conversion of both pollutants at a minimum temperature of 350 °C and a GHSV of 90,000 h −1 . The addition of Fe 3+ to ZrO 2 decreased the crystallinity of the latter phase and significantly enhanced surface area. Concentrations of 30 mol% or greater produced segregated FeO x phases, which affected catalytic performance in distinctly different ways: supported Fe 3+ (30 mol%) possessed similar activity to doped Fe 3+ ; α-Fe 2 O 3 (50 mol%) inhibited activity due to its’ lower reducibility; an amorphous phase (40 mol%) promoted iron-weighted areal activity. A complete identification of the ambiguous component was not successfully established, but the obtained properties revealed that it exhibited weaker interaction with the support and had a size greater than that of oligomeric-Fe 2 O 3 yet smaller than 3 nm.
研究领域:
催化
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环境科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Mengmeng Xi,Yang Cheng,Fanhui Meng,Xuefang Yao,Muhammad Asif Nawaz,Maria Saif,Zhong Li,Tomas Ramirez Reina
Fe-based catalysts show great promise in advancing the application of high-temperature Fischer-Tropsch synthesis (HT-FTS) for producing value-added chemicals and liquid fuels; however, maintaining high catalytic activity and stability at elevated temperatures remains a significant challenge. Here, a novel approach was employed to prepare carbon sphere (CS)-supported Fe catalysts, where isolated Fe particles are efficiently embedded within a carbon matrix to enhance both catalytic activity and stability. The resulting 3D scaffold structure catalyst featuring ultrafine FeO x nanoparticles (NPs) dispersed within nitrogen-doped carbon frameworks was synthesized from Fe-chitosan/CS composites using a chelate-assisted impregnation method paired with unidirectional freeze treatment. The coordination between chitosan chains and Fe(Ⅲ) has yielded a homogeneous Fe-chitosan composite, with the embedded FeO x NPs within the nitrogen-doped carbon (NC) matrix serving as pivotal barriers against sintering, thus enhancing stability. The synergistic effect of adding K promoter and the resulting 3D scaffold structure in Fe-K@NC/CS catalyst has further fine-tuned catalytic activity, ensuring high stability in HT-FTS. The current strategy of fabricating N-doped 3D scaffold structures of hybrid carbonaceous material achieved unprecedented results, with the CO conversion reached 62.7 % and C 2 -C 4 = olefin selectivity of 29.0 % at 340 °C, 20 bar and space velocity of 48000 mL g cat –1 h −1 .
研究领域:
材料科学
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催化化学
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能源化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Zhipeng Tian,Weijie Zhang,Tao Liu,Jianping Liu,Chenguang Wang,Libin Lei,Mingzheng Liao,Chao Wang,Ying Chen
Hydrogen production by catalytic aqueous phase reforming (APR) of biomass-derived oxygenates is a promising route to produce hydrogen in a renewable way. As the typical APR catalyst, Pt/Al 2 O 3 is confronted with high methanation activity that consumes H 2 and produces undesired CH 4 during the treatment of methanol solution. In contrast, WGS reaction is the main pathway to boost H 2 generation during APR process. In this work, a series of PtFe/Al 2 O 3 catalyst with different Fe contents were prepared, characterized and tested for the methanol APR reaction. XRD , TEM, XPS and H 2 -TPR technologies were applied to study the change of physicochemical properties with the addition of iron. The restriction on methanation and promotion on WGS reaction were proved as well. With the increase of Fe content, the interaction between Pt and FeO x species have both positive and negative effects on APR reactivity while the CH 4 selectivity descending continuously from 9.25% to as low as 0.60%. Besides, the effects of reduction temperatures (250–350 °C) of Pt0.5Fe/Al 2 O 3 catalyst on APR performances were also investigated. An “Oxygen dynamic transfer cycle” between H 2 O/CO∗ and FeO x species with oxygen vacancies is proposed and verified. This indirect WGS reaction through lattice oxygen on FeO x species that boosting WGS reactivity helps improving H 2 selectivity in the gas products of methanol APR.
研究领域:
催化化学
·
可再生能源
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
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IF 4.65
Fu Yang,Liuzhu Zhou,Shuying Gao,Xuyu Wang,Jin Chen,Aihua Yuan,Edison Huixiang Ang
Combining different active states of metal species together in special configuration might trigger interesting synergetic effect for catalytic process. As a proof-of-concept, the present study has developed an ingenious approach to reach functional mesoporous molecular sieve which in-situ encapsulates two different states of highly-active FeOx inside centered core and nano-tunnel of mesoporous silica , respectively. The α-Fe 2 O 3 in-situ immobilized nanoneedles coated by the porous silica afford ∼5 nm diameter, plus highly-dispersed Fe 2 O 3 cluster-like species attachment in confined mesopore, which synergistically contributes to high activity and stabilization of catalyst. The combined iron oxides in special configuration deliver an appreciable catalytic activity in phenol hydroxylation (46.4% conversion, 87.9% benzenediol selectivity) during multiple catalytic cycles, compared to some reported results, which benefited from accelerating production of oxidative free radicals from H 2 O 2 and the tailored micrpopore (∼1.4 nm) which could enhance the catalytic selectivity of targeted products. Furthermore, the photocatalytic antimicrobial effect of Fe catalyst against Escherichia coli was also demonstrated via the constructed synergy of two FeOx nanospecies with assistance of light.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Manman Li,Kunlun Yang,Xin Huang,Shiguang Liu,Yifan Jia,Peng Gu,Hengfeng Miao
In this study, the flat microfiltration ceramic membrane (CM) was modified by wet impregnation method (Mn-Fe-CM) to catalyze ozone (O 3 ) for the oxidative degradation of trimethoprim (TMP). The conventional characterization test showed that the Mn-Fe binary oxides (Mn/FeO x ) with the crystal structure of FeMnO 3 were successfully loaded on the membrane and the catalytic performance of Mn-Fe-CM for O 3 was apparently enhanced as compared to CM. Consequently, compared with O 3 oxidation alone, the degradation and mineralization efficiencies of TMP in the O 3 /Mn-Fe-CM system were both improved and 98.6% of TMP could be removed within 10 min. The degradation efficiency of TMP decreased with the increasing pH and the addition of Cl - 、HCO 3 – 、PO 4 3- , while humic acid (HA) exhibited negative effect on the TMP removal. Radical scavenger experiment and electron paramagnetic resonance (EPR) analysis confirmed that direct oxidation by O 3 played an important role in the degradation of TMP, while hydroxyl radical (·OH) and 1 O 2 also participated. Fe(II) could act as an intermediate to transfer electrons and accelerate the transformation of Mn(III) to Mn(II) and Mn(IV) to Mn(III) during the ozonation process, which definitely strengthened the synergic catalytic effect of Mn-Fe-CM. The proposed degradation mechanism of TMP mainly contained hydroxylation , carbonylation , demethoxylation and deamination . Due to the strong catalytic ozonation performance for organic pollutants degradation, the O 3 /Mn-Fe-CM system revealed better anti-membrane fouling ability, strong cyclic usage performance and high applicability for the actual surface water treatment.
研究领域:
环境科学
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化学工程
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水处理技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Guoquan Na,Wen-Gang Cui,Hangyan Shi,Zhenglong Li,Fan Gao,Xingqiang Wang,Ke Wang,Yong Gao,Yaxiong Yang,Zichao Shen,Yanxia Liu,Jian Miao,Hongge Pan
LiBH4 has attracted significant interest due to its high-hydrogen storage capacity (18.5 wt % H2). However, its practical application is severely impeded by the high dehydrogenation temperature, sluggish hydrogen release kinetics, and poor reversibility. In this work, a graphene-supported rodlike FeF2/FeOX additive (FeF2/FeOX@G) is prepared and introduced into LiHB4 by a simple ball-milling. With an optimized LiBH4-to-FeF2/FeOX@G weight ratio of 7:3, the 7LiBH4-3(FeF2/FeOX@G) system starts dehydrogenation at a low temperature of 100 °C below and 8.7 wt % H2 is released upon heating to 400 °C, while 1.1 wt % H2 is released for pristine LiBH4. Moreover, the system releases rapidly 7.0 wt % H2 at 350 °C within 80 min, and a dehydrogenation capacity of 5.5 wt % is reached after 10 reversible hydrogen absorption and desorption cycles. The in situ formed FeB, Li3BO3, and Fe2B during the first dehydrogenation process acted as a synergistic catalysis, effectively improving the reversible hydrogen storage of LiBH4. This work provides insights into the design of unique additives to introduce multiple catalyst synergies to enhance the hydrogen storage performance of LiBH4.
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高影响因子
JOM
·
2021
·Vol. 74
·期 2
·622-633
·
IF 2.474
Liu Zhihong,Ye Fengchun,Chen Rui,Wang Hongjun,Xia Longgong
Halogen-containing organic components in waste electrical and electronic equipment have an obvious influence on the distribution behaviors of valuable metals during the smelting processes. However, the mechanism is still incomplete in the literature. The equilibration-quenching-(ICP+EPMA) experimental technique has been applied in studying the partitioning behaviors of Au, Ag, and Sn in the Cu-FeO x -SiO 2 -CaO-Al 2 O 3 smelting system in the presence of halogen elements (F, Cl, Br). The obtained results showed that: (1) 93% Au terminated into the alloy phase in CaF 2 adding experiments, and a maximum of 32% Au reported to the gas phase in CaCl 2 or CaBr 2 adding experiments; (2) 22–49% Ag entered the gas phase when adding CaF 2 into the system, and 3–34% Ag entered into the gas phase when adding CaCl 2 or CaBr 2 ; and (3) halogen elements influenced Sn dramatically, and portions of Sn in the gas phase and slag phase increased along with increasing temperature or halides dosage.
研究领域:
冶金学
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材料科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Abdul Qayum,Xiang Peng,Jianfa Yuan,Yuanduo Qu,Jianhong Zhou,Zanling Huang,Hong Xia,Zhi Liu,Daniel Qi Tan,Paul K. Chu,Fushen Lu,Liangsheng Hu
Ni-/Fe-based materials are promising electrocatalysts for the oxygen evolution reaction (OER) but usually are not suitable for the hydrogen evolution reaction (HER). Herein, a durable and bifunctional catalyst consisting of Ni-FeOx and FeNi3 is prepared on nickel foam (Ni-FeOx/FeNi3/NF) by in situ solution combustion and subsequent calcination to accomplish efficient alkaline water splitting. Density functional theory (DFT) calculation shows that the high HER activity is attributed to the strong electronic coupling effects between FeOx and FeNi3 in the Janus nanoparticles by modulating ΔGH* and electronic states. Consequently, small overpotentials (η) of 71 and 272 mV in HER and 269 and 405 mV in OER yield current densities (j) of 50 and 1000 mA cm–2, respectively. The catalyst shows outstanding stability for 280 and 200 h in HER and OER at a j of ∼50 mA cm–2. Also, the robustness and mechanical stability of the electrode at an elevated j of ∼500 mA cm–2 are excellent. Moreover, Ni-FeOx/FeNi3/NF shows excellent water splitting activities as a bifunctional catalyst as exemplified by j of 50 and 500 mA cm–2 at cell voltages of 1.58 and 1.80 V, respectively. The Ni-FeOx/FeNi3/NF structure synthesized by the novel, simple, and scalable strategy has large potential in commercial water electrolysis, and the in situ combustion method holds great promise in the fabrication of thin-film electrodes for different applications.
研究领域:
材料科学
·
电化学
·
理论计算
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产品关联
DOI
PubMed
高影响因子
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