CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Xinwei Zhu,Jimin Shen,Jing Kang,Pengwei Yan,Lei Yuan,Yizhen Cheng,Binyuan Wang,Shengxin Zhao,Zhonglin Chen
Developing highly efficient and anti-interference catalysts was still a challenge for the practical application of heterogeneous catalytic ozonation (HCO) in water decontamination. Herein, a magnetic Fe 3 C decorated biochar (Fe 3 C/BC) was prepared for HCO to achieve efficient degradation of 2,4-dichlorophenoxyacetic acid (2,4-D). The Fe 3 C/BC catalytic ozonation system promoted the degradation ratio of 2,4-D from 58.7% (ozonation alone) to 90.0% within 10 mins when the ozone dosage was 1.0 mg/L. And the observed degradation rate constant ( k obs ) of 2,4-D under catalytic ozonation system was 2.58 times that of ozonation alone. Fe 3 C/BC exhibited negligible adsorption on 2,4-D but with a significant enrichment to ozone, which realized the cooperating process of “adsorption-catalysis” at the solid–liquid interface, thus avoiding the ineffective decomposition of ozone. The dissociative adsorption of ozone molecules on the surface Fe 3 C generated surface atomic oxygen species (O* and O 2 *), which mediated the in-situ formation of hydroxyl radicals (·OH). ATR-FTIR, in-situ Raman, isotope tracing tests, and theoretical calculations were used to disclose the interface reaction processes and reveal the ·OH formation mechanism. Free radical reactions at the interface efficiently avoid the interference of coexisting ions dissolved in water. The presence of 3 mM (183 mg/L) bicarbonate had essentially little effect on the degradation of 2,4-D. The consecutive use of Fe 3 C/BC did not influence its catalytic performance and stable structure. This study provided new insight into the ·OH-dominated interfacial reaction in the HCO process.
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jie Li,Hua Yin,Haoyu Luo,Yingchao Li,Xufa Rong,Zhi Dang
Polychlorinated biphenyls (PCBs) degradation by peroxymonosulfate (PMS) activation through •OH and SO 4 •– radical oxidation process was the effective technology in the last decades; however, there were few research focusing on removing PCBs by O 2 •– and 1 O 2 induced by PMS activation. In this work, 90.86% of 2,4,4-trichlorodiphenyl (PCB 28) was degraded by 0.3 g/L Fe 3 C@Fe-800 activated 0.5 mM PMS system under the synergistic action of O 2 •– and 1 O 2 . The structures of Fe 3 C@Fe-800 were identified by Scanning electron microscope (SEM), High resolution-transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET), Raman spectra and Fourier transform infrared (FT-IR) spectra. Electron paramagnetic resonance (EPR) measurements and quenching tests verified that O 2 •– and 1 O 2 were the primary reactive species in Fe 3 C@Fe-800/PMS/PCB 28 ternary reaction system. Density functional theory (DFT), Linear sweep voltammetry (LSV), and chronoamperometry test revealed that electron-deficient Fe atoms on Fe 3 C were the main active sites in Fe 3 C@Fe-800 for PMS activation to generate 1 O 2 . Unlike the reported •OH and SO 4 •– mediated degradation induced by the iron-based catalyst, both O 2 •– and 1 O 2 contributed to PCB 28 degradation： nucleophilic dichlorination reaction by O 2 •- and then ring-open oxidation process by 1 O 2 . Fe 3 C@Fe-800/PMS system had excellent catalytic performance under different reaction conditions and possessed desirable inorganic salt and natural organic matter resistance. This work elucidated the important role of Fe 3 C in PMS activation to generate O 2 •- and 1 O 2 for PCB 28 decontamination by nonradical way and provided a clue to design rationally catalysts in polychlorinated biphenyl pollution remediation.
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高影响因子
Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 17
·3311-3319
·
IF 7.571
Rui Li,Xiaohong Qiao,Huijun Ma,Hanmei Li,Cong Li,Lihua Jin
In this work, we reported new Fe3C embedded Fe–N-doped carbon nanomaterials (Fe3C@Fe–N-CMs) generated in situ by the facile pyrolysis of Fe–Zn ZIF precursors. The resulting Fe3C@Fe–N-CMs were equipped with several desirable nanozyme features, including multiple efficient intrinsic active sites (i.e. Fe–Nx, Fe3C@C, and C–N moieties), large specific surface area and abundant mesoporous structures. As a result, these Fe3C@Fe–N-CMs displayed exceptional ability to mimic three enzymes: peroxidase, catalase and oxidase, while the Fe3C@Fe–N-CMs pyrolyzed at 800 °C, named CMs-800, showed the best enzyme-like properties. After systematically investigating the catalytic mechanism, we further explored the application of the oxidase-like properties of CMs-800 in the detection of the total antioxidant capacity (TAC) in beverages and tablets. This study not only provided a new approach to construct multifunctional carbon-based nanozymes, but also expanded the application of carbon nanozymes in the field of food quality and safety.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wanlu Hua,Yifei Pu,Jie Xu,Baichuan Zhuang,Jing Zhang,Jifei Zhuo,Xiaoli Xie,Xin Tian,Xiangnan Chen,Tengfei Qu,Guo Li,Guangjun Gou
Heterointerface engineering has been widely proven effective for designing composite materials with high-efficiency microwave absorption (MA) capabilities. However, challenges persist in regulating the interface structures of MA materials at the microscale and nanoscale. In this study, a novel N/S-codoped multi-interfacial porous carbon composite (Fe 7 S 8 /Fe 2 S/Fe 3 C@C) is successfully prepared by chemical foaming and vulcanization. Concretely, when the carbonization and vulcanization temperature were both 600 °C, the mass ratio of carbonized sample to sulfur (carbon: sulfur) was 1:2 (PF-2), which exhibited exceptional electromagnetic wave attenuation properties. Notably, the composite achieved a minimum reflection loss ( RL min ) of −48.83 dB at 1.85 mm thickness, and an effective absorption bandwidth (EAB) value reaching 6 GHz (12–18 GHz) at 2 mm, while the proportion of paraffin wax was only 20 wt%. The significantly improved MA performance primarily originated from the synergistic effects between dielectric/magnetic heterostructures and heterointerfaces. In addition, PF-2 exhibits excellent antibacterial properties, with antibacterial rates against Escherichia coli and Staphylococcus aureus both exceeding 99.999 % under no light and 808 nm light conditions. Overall, this research provides a pathway through heterointerface engineering for designing a new generation of multifunctional electromagnetic wave absorbing materials.
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高影响因子
CARBON
·
2024
·
IF 10.5
Longsen Wang,Guanghao Li,Chen Chen,Haonan Zhang,Lin Fang,Zixun Wang,Xinbo Tu,Zhongzhu Wang,Peihong Wang,Wen He
Portable and wearable electronics demand flexible, multifunctional films with electromagnetic interference (EMI) shielding and thtaermal management capabilities. However, the preparation of flexible films with suitable performance is still a challenge. Here, we constructed the flexible, stretchable, and multifunctional patch with a multistage structure composed of Fe 3 C–C (FC) fibrous film, MXene , and polystyrene-polyisoprene-polystyrene (SIS), which exhibited outstanding EMI shielding effectiveness total (SE T ) of 56 dB. Due to the package of the SIS layer, the EMI SE of the as-prepared patch remains almost unchanged after 3000 cycles of bending test or placing in the air for one month. Furthermore, the multistage structure film shows excellent Joule heating performance and can maintained for a long time. This work provides a simple and effective strategy for the preparation of multifunctional flexible patches, which have great application potential in the fields of EMI shielding and thermal management.
研究领域:
材料科学
·
电子工程
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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Lei Zhuang,Mingyuan Jian,Ruifang Xue,Nan Li,Jie Chen,Yanghe Fu,De–Li Chen,Weidong Zhu,Fumin Zhang
Developing efficient heterogeneous catalysts for the aerobic oxidation of C–H bonds using oxygen molecule as an oxidant to produce value–added aryl ketones is a challenging task. In this study, a series of cementite–iron–carbon composites (referred to as Fe–C–T, where T represents the pyrolysis temperature) were synthesized using a metal–organic–framework–mediated sacrificial template strategy. The Fe–C–T composites consist of highly dispersed Fe/(Fe 3 C or Fe 2 O 3 ) nanoparticles surrounded by graphitic carbon on porous carbon supports. Under mild reaction conditions (1 atm of O 2 pressure, 353 K, 12 h), with tert–butyl hydroperoxide (0.25 equiv.) as the initiator in a green solvent water, the prepared Fe–C–973 achieved a high conversion of 98.4 % for ethylbenzene and a selectivity of 98.7 % for acetophenone . This performance was markedly superior to the comparable Fe–C–873 and Fe–C–1073, as well as the commercially available Fe–based catalysts. Kinetic studies revealed that the catalytic system followed first–order kinetics for the substrate ethylbenzene, and the activation energy over Fe–C–973 was remarkably low of 40.4 kJ/mol. The highly distributed Fe 3 C nanoparticles embedded in the porous carbon framework were identified as the most active sites for the reaction.
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高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 22
·11340-11347
·
IF 8.867
Lei Cao,Zhen-huan Li,Yu Gu,Dao-hao Li,Kun-mei Su,Dong-jiang Yang,Bo-wen Cheng
Zn–air battery, as a low cost, high energy density, and safe energy device, has received significant attention in recent years. However, its wide application has been hindered due to the low oxygen reduction reaction (ORR) activity in air electrodes without excellent catalysts. Herein, N-doped porous and highly graphitic carbon nanobox-supported Fe-based nanoparticles (Fe–N-CNBs), which were synthesized from fructose, NH3, and FeCl3 by a self-propagating high-temperature synthesis (SHS) process followed by a heat treatment process, were used as ORR catalysts. Fe–N-CNBs calcined at 600 °C (Fe–N-CNBs-600) showed higher ORR activity (onset and half-wave potentials of 1.03 and 0.85 V vs. RHE, respectively), better electrochemical stability, and higher methanol tolerance than Pt/C under alkaline conditions. The outstanding ORR performance of Fe–N-CNBs-600 was attributed to the synergistic effect of Fe, Fe2N, and Fe3C nanoparticles, which was unambiguously confirmed by HRTEM and XRD characterization. Furthermore, Fe–N-CNBs-600 also exhibited higher electrochemical properties than the currently used expensive Pt/C catalyst in Zn–air batteries.
研究领域:
材料科学
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电化学
·
能源技术
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yuying Chen,Caiwen Wu,Haiyang Xie,Zhaoyan Deng,Yiming Liu,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
Iron-based catalysts have garnered great attention as alternatives for Fenton-like catalysts in the degradation of organic compounds. However, there is a demand for the synthesis of highly efficient iron-based catalysts that can solve the problems of iron dissolution and poor stability. Herein, nitrogen-doped graphitic carbon-supported Fe-Co/Fe 3 C dual active sites catalyst (Fe-Co/Fe 3 C-NC) is successfully prepared by ball milling method combined with subsequent high-temperature self-reduction. 0.5 wt%-Fe-Co/Fe 3 C-NC shows high efficiency in the activation of peroxymonosulfate (PMS) for the ultrafast degradation of high concentration Rhodamine B (200 mg/L of RhB is completely degraded within 8 min and the degradation rate constant is as high as 0.5066 min −1 ), as well as high stability and good reproducibility, attributing to the synergistic mechanism between the dual active sites (Fe-Co and Fe 3 C) and the adsorption sites (Fe 3 C and pyrrolic-N). Chemical quenching experiments and electron paramagnetic resonance indicate that the prepared 0.5 wt%-Fe-Co/Fe 3 C-NC exhibits outstanding activation for PMS by generating reactive oxygen species (SO 4 •− , • OH, 1 O 2 ) and high-valent FeCo=O species. This work shows useful insights into the synthesis of iron-based dual active sites catalysts, providing exciting chances for the highly efficient degradation of high concentration organic wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chao Zhang,Mengxiang Ye,Huaimeng Li,Zhenzhen Liu,Zhen Fu,Haimin Zhang,Guozhong Wang,Yunxia Zhang
Heterogeneous electro-Fenton is a promising technology for the degradation of organic contaminants. To ensure its effectiveness, it is in urgent demand to design cathode materials with the integrated capability of sufficient H 2 O 2 generation and subsequent activation into reactive oxygen species (ROS) together with catalytic stability. Herein, a composite constituted by Fe/Fe 3 C nanoparticles embedded into N-doped porous carbon (NPC), designated as Fe/Fe 3 C@NPC, was successfully fabricated from Fe 3+ -loaded poly(imine dioxime) (PIDO) membrane via the thermal treatment in N 2 atmosphere and employed as the heterogeneous electro-Fenton catalyst to degrade bisphenol A (BPA). By optimizing the pyrolysis temperature and loading level of iron species, the catalyst obtained at 800 °C (i.e. Fe/Fe 3 C@NPC-800) achieved almost 100% of BPA removal efficiency within 120 min via the electro-Fenton system, accompanied by 69.2% of the total organic carbon (TOC) removal rate. Furthermore, the proposed composite catalyst also exhibited satisfactory reusability and stability, as reflected by low decrease in removal efficiency after six successive degradation tests and limited iron leaching (<0.5 mg/L). This work might provide valuable instruction for the rational design of highly efficient and stable heterogeneous electro-Fenton catalysts for organic pollutant control.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Tangying Liu,Yanyan Xiang,Zhengjie Tan,Wei Hong,Zhimin He,Jilan Long,Bin Xie,Rong Li,Xinglong Gou
Ni 3 Fe-Fe 3 C heterostructures well encapsulated in N-doped carbon nanotubes (Ni 3 Fe-Fe 3 C@NCNTs) were fabricated by a facile one-step pyrolysis-growth approach. Thanks to the merits of abundant active sites, multiple heterogeneous interfaces, large electrochemical active surface area, robust structure, self-supporting configuration and remarkable synergistic effect, Ni 3 Fe-Fe 3 C@NCNTs exhibits excellent bifunctional catalytic activity and stability toward both HER and OER in alkaline media. Moreover, the Ni 3 Fe-Fe 3 C@NCNTs||Ni 3 Fe-Fe 3 C@NCNTs electrolyzer requires an ultralow voltage of 1.80 V for overall water splitting to reach a current density of 300 mA cm −2 , and it keeps stable over 300 h for continuous hydrogen generation with 100% Faradaic efficiency, surpassing Pt/C||RuO 2 electrolytic cell and showing great promise for industrial application in green hydrogen production.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Wen Wen Xie,Tong Zhen Tian,Min Yang,Nian Wu Li,Le Yu
Rational design of effective bifunctional inexpensive oxygen electrocatalyst is highly important for Zn-air batteries (ZABs), which can accelerate both oxygen reduction/evolution reactions at the oxygen electrode. Herein, we present the formation of hierarchical hollow frameworks of dual-sided Fe/Fe 3 C@N-doped carbon nanotubes (FNCHFs) through a template-engaged method. Benefitting from the synergistic effect between the robust hollow frameworks and in-situ grown dual-sided N-doped carbon nanotubes, the FNCHF electrocatalyst presents enhanced mass/electron transport with high structural stability. As a result, the FNCHFs based bifunctional oxygen electrode demonstrates a desirable oxygen electrocatalytic activity and stability with a half-wave potential of 0.863 V for oxygen reduction and an overpotential of 340 mV to reach the current density of 10 mA cm −2 for oxygen evolution. The corresponding ZAB exhibits a high peak power density of 206 mW cm −2 , a high specific capacity of 781 mAh g Zn −1 , and a good cycling stability more than 300 h.
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Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 9
·3636-3645
·
IF 6.482
Xiaoqin Li,Taotao Gao,Qilin Liu,Yanxue Xu,Jing Li,Dan Xiao
Fiber-shaped energy storage devices (FESDs) are indispensable for developing portable and wearable electronic products. Aqueous rechargeable Ni/Fe batteries are an appropriate candidate due to the cost-effectiveness, high ionic conductivity, and great safety. However, their energy density is still far from satisfactory, hindering further practical applications. Herein, we focused on studying binder-free fibrous electrodes for high-performance FESDs based on rechargeable Ni/Fe batteries. A fast microwave-assisted synthesis method was adopted to grow active materials with a 3D conductive network which is constructed from carbon nanotubes decorated with Fe–Fe3C nanoparticles. Due to the heterogeneous structure, the active materials depicted improved electron/ion transfer, boosting the electrochemical performance of the anode. A flexible Ni/Fe battery is successfully fabricated using the aforementioned anode coupled with a NiCoO-based cathode which is synthesized by electrodeposition and a post-annealing process. Thanks to the special structure of the active materials and the fast redox reaction, the assembled flexible Ni/Fe battery achieved high electrochemical properties with a maximum volumetric specific capacity of 1.61 mA h cm−3 and energy density of 1.28 mW h cm−3. The cycling stability and mechanical flexibility were also tested, which demonstrated the prospects for practical application.
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