SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Danni Chen,Daguang Li,Zhenjun Xiao,Zheng Fang,Xuegang Zou,Ping Chen,Tiansheng Chen,Wenying Lv,Haijin Liu,Guoguang Liu
Lead pollution has become a global concern due to its ubiquity and persistence. This study describes two Fe Mn oxide substrate adsorbents, namely, Fe Mn binary oxides (FMBO) and mesoporous Fe Mn binary oxide (MFMBO) covered with tannic acid film (FMBO@TA-Fe 3+ and MFMBO@TA-Fe 3+ ), for the treatment of Pb 2+ in water. The characterization results showed that TA was successfully coated onto the surfaces of FMBO and MFMBO. The maximum capacities of Pb 2+ on FMBO@TA-Fe 3+ and MFMBO@TA-Fe 3+ were 322.08 and 357.14 mg g −1 , respectively, which were twice those of FMBO and MFMBO. The adsorption of Pb 2+ on the adsorbents was a spontaneous, endothermic process with increasing disorder through thermodynamics studies. An overall mechanism was proposed for Pb 2+ adsorption, the improved adsorption performance of FMBO@TA-Fe 3+ and MFMBO@TA-Fe 3+ is ascribed to the mesoporous characteristics and the introduction of hydroxyl groups. Further investigation indicated the adsorption of Pb 2+ could be attributed to electrostatic interactions on FMBO@TA-Fe 3+ and MFMBO@TA-Fe 3+ , and cation exchange existed through the formation of these internal surface complexes. The Pb 2+ -loaded adsorbents could be effectively desorbed in a dilute hydrochloric acid solution, promoting recycling and reuse of the regenerated adsorbents. These results warrant the promising application of FMBO@TA-Fe 3+ and MFMBO@TA-Fe 3+ for the removal of Pb 2+ , and this work first proposed TA film-modified FMBO and MFMBO to improve its adsorption capacity in the application of environmental remediation.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Hongxin Guan,Na Wang,Xuanxuan Feng,Shaokang Bian,Wei Li,Yan Chen
The preparation of high-efficiency, stable and low-cost oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) electrocatalysts is always a challenge for new energy systems. In this work, a simple hydrothermal synthesis method was used to obtain FeMn bimetallic organic materials (FeMn-MOF/NF) grown on foamed nickel (NF) in one step. Moreover, FeMn-MOF/NF(1:1) had larger electrochemical specific surface area and unique nano-flower-like structure. The overpotentials of OER and HER in alkaline solution at a current density of 50 mA·cm −2 were 290 mV and 260 mV, respectively, and the total water splitting potential at this current density is only 1.7 V. The excellent activity and stability were attributed to the synergistic effect of FeMn. The bimetal and abundant active sites could promote the release of oxygen during the catalytic process.
研究领域:
材料科学
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电化学
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DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Ting Zhang,Yuwei Xue,Mingjun Xu,Ziqi Zhu,Qian Zhang,Junming Hong
The consumption of disinfectants increased dramatically with the outbreak of the COVID-19 epidemic. Benzalkonium chloride (DDBAC), a cationic surfactant disinfectant for import and export cargoes, is used for effective degradation method. For DDBAC effective degradation, polyhedral Fe–Mn bimetallic catalyst of Prussian blue analogue (FeMn-CA300) was novelty developed for rapid peroxymonosulfate (PMS) activation. Results showed that the Fe/Mn redox and surface hydroxyl groups in the catalyst played an important role in the DDBAC-enhanced degradation. The removal effectiveness of 10 mg L −1 DDBAC was up to 99.4% in 80 min under the initial pH = 7, catalyst dosage of 0.4 g L −1 , and PMS concentration of 15 mmol L −1 . In addition, FeMn-CA300 had a wide pH applicability range. The results indicated that hydroxyls, sulfate radicals, and singlet oxygen could effectively improve the degradation efficiency, where sulfate radicals played a crucial role. Finally, the corresponding degradation path of DDBAC was further provided according to GC-MS results. The results of this study provide new insights into the degradation of DDBAC, thereby highlighting the great potential of FeMnca300/PMS to control refractory organic compounds in the aqueous phase.
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Haiping Xiong,Xinbo Zhu,Shangmin Lu,Chunlin Zhou,Weiping Xu,Zijian Zhou
In this work, an integrated system combining non-thermal plasma (NTP) and Fe Mn catalysts was developed for ethylene oxide (EO) oxidation. The effect of Fe/Mn molar ratio on the oxidation rate of EO and energy yield of the plasma-catalytic process has been investigated as a function of specific energy density (SED). Compared with the case of using plasma alone, the combination of plasma and Fe Mn catalysts greatly enhanced the reaction performance by the factor of 25.2% to 97.6%. The maximum oxidation rate of 98.8% was achieved when Fe 1 Mn 1 catalyst was placed in the dielectric barrier discharge (DBD) reactor at the SED of 656.1 J·L −1 . The highest energy yield of 2.82 g·kWh −1 was obtained at the SED of 323.2 J·L −1 over the Fe 1 Mn 1 catalyst. The interactions between Fe and Mn species resulted in larger specific surface area of the catalyst. Moreover, the reducibility of the catalysts was improved, while more surface adsorbed oxygen (O ads ) was detected on the catalyst surfaces. Moreover, the redox cycles between Fe and Mn species facilitated consumption and supplementation of reactive oxygen species , which contributed to the plasma-catalytic oxidation reactions. The major reaction products of plasma-induced EO oxidation over the Fe Mn catalysts, including CH 3 COOH, CH 3 CHO, CH 4 , C 2 H 6 and C 2 H 4 , were observed using the FT-IR analyzer and GC–MS instrument. The reaction mechanisms of EO oxidation were discussed in terms of both gas-phase reaction and catalyst surface reaction. The redox cycles between Fe and Mn species facilitated the plasma reaction and accelerated the deep oxidation of by-products.
研究领域:
环境科学
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催化化学
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等离子体技术
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DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2022
·
IF 10.753
Qiao Li,Xinyue Ma,Chengsi Qi,Rui Li,Wei Zhang,Jiansheng Li,Jinyou Shen,Xiuyun Sun
Effective removal of Sb(III) and Sb(V) has long been an urgent task for protecting human health and environment. In this study, novel magnetic mesoporous Fe Mn binary oxides (MMFMs) were fabricated via calcinating the Mn encapsulated carboxymethyl cellulose-Fe(III) hydrogel, and the structure of MMFMs were closely related to the Fe:Mn ratio. Owing to the mesoporous structure together with synergistic effect of Fe Mn binary component, the MMFMs exhibited excellent mass transfer and adsorption ability to Sb(III) and Sb(V). MMFM 3 achieved a maximum Sb(III) and Sb(V) adsorption capacity of 281.5 and 204.6 mg/g, respectively. Co-existing anions of Cl − , NO 3 − and SO 4 2− exhibited marginal influence on the adsorption for both Sb(III) and Sb(V), except the PO 4 3− for Sb(III) and SiO 3 2− or PO 4 3− for Sb(V). X-ray photoelectron spectroscopic investigation revealed that high valence Mn(IV) was mainly responsible for the oxidation transformation of the highly toxic Sb(III) into less toxic Sb(V), while the FeO x content played major role for the adsorption of Sb(V). The generated inner-sphere Fe O Sb complex between Fe-OH groups and Sb(III/V) dominantly contributed to the removal of Sb(III/V). Overall, mesoporous structure, magnetic separation ability, excellent adsorption performance together with exceptional regeneration properties demonstrated the great potential of MMFMs for Sb(III/V) remediation.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Pijun Duan,Yuanfeng Qi,Shanshan Feng,Xiaoming Peng,Wei Wang,Yue Yue,Yanan Shang,Yanwei Li,Baoyu Gao,Xing Xu
FeMn bimetallic nanoparticles coated with nitrogen-doped graphene shells (FeMn@N-C) were prepared to decompose clothianidin (CTD) through activation of peroxymonosulfate (PMS). The redox cycles of encapsulated FeMn bimetallic nanoparticles with multiple valence states could accelerate the radical generation and ensure the stability of FeMn@N-C with continuous PMS activation. Coexisting NaH 2 PO 4 could unusually accelerate CTD degradation through facilitating reactive oxygen species (ROS) generation and decreasing bonding dissociation energies of CTD molecule. DFT calculation indicated that the C-Cl bond in CTD molecule was weakened after being surrounded by NaH 2 PO 4 . Two main degradation pathways were proposed in the absence of phosphate and a new dechlorination pathway was first reported after CTD molecule bonding with phosphate, which was confirmed by DFT. This work provides a feasible strategy of PMS activation by graphene coated bimetallic nanoparticles and give a new insight into accelerated degradation of recalcitrant pollutants with phosphate surrounding.
研究领域:
环境科学
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化学
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DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
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2022
·Vol. 48
·期 11
·4517-4536
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IF 3.134
Yang Zizhen,Wang Siya,Chen Ou,Wang Zhengwei,Xu Jundong,Zheng Shuqin
In this paper, FeMn-ZSM-5/MOR(FeMn-Z/M) catalyst was synthesized through in-situ crystallization and wet impregnation method and used as heterogeneous Fenton-like catalyst for degradation of indigo carmine (IC) in aqueous solution. The catalysts were characterized using XRD, BET, SEM, EDS, FT-IR and XPS techniques. The experimental results showed that Fe and Mn were successfully doped onto the ZSM-5/MOR(Z/M) surface. The combination of ZSM-5 and mordenite (MOR) not only enhanced the adsorption capacity of contaminant, but also had more active sites. Degradation experiments and the valence variations indicated that Fe and Mn had a significant synergistic effect. The results of IC degradation experiments under different conditions showed that the optimum conditions (FeMn mass ratio = 1:2, FeMn-Z/M = 25 mg, H 2 O 2 = 0.5 ml, pH = 3), the degradation rate of IC reaches 99% in 20 min. Reaction analyses showed that catalyst follow a first-order reaction kinetic. The degradation of IC could be divided into two stages: adsorption/oxidation (After adsorption, oxidative degradation begins) and Fenton-like reaction. Free radicals quenching studies analyzed verified that the dominant free radicals within FeMn-Z/M Fenton-like system were hydroxyl radical (·HO) and hydro-peroxy radical (·HO 2 ), ·HO 2 was the main free radical in the adsorption/oxidation stage. The possible catalytic mechanism was proposed. Finally, the synthesized FeMn-Z/M catalyst had better performance than other IC removal methods, and had good degradation efficiency and high reusability after multiple runs.
研究领域:
环境科学
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催化化学
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高影响因子
Catalysis Science & Technology
·
2019
·Vol. 9
·期 15
·3933-3946
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IF 5.726
Ting Wang,Yuebing Xu,Chengming Shi,Feng Jiang,Bing Liu,Xiaohao Liu
Direct conversion of syngas (CO/H2) into aromatics over tandem catalysts via the Fischer–Tropsch synthesis (FTS) route has attracted much attention because of its high one-pass conversion and milder reaction conditions. However, the complicated FTS product composition leads to more difficult mechanistic elucidation of aromatics formation compared to the methanol route. Herein, a series of strategies, such as covering external surface acid sites of HZSM-5 with a layer of inert SiO2, layered loading of an FeMn FTS catalyst and HZSM-5 zeolite in one reactor and two tandem reactors, and model reactions with ethylene and propylene over zeolite in a simulated FTS reaction environment, were applied to unveil the reaction mechanism and related factors affecting aromatic selectivity. It was found that different from the methanol route, the tandem FeMn–HZSM-5 catalyst produced aromatics mainly from the conversion of C5+ FT intermediates rather than light olefins (C2=–C4=). SiO2 coating could remarkably enhance the para-xylene (PX) selectivity due to hindering of its isomerization to major meta- and minor ortho-xylene (MX and OX) on the external surface acid sites of HZSM-5 by releasing the space confinement. The layered loading experiments in one reactor demonstrated that a farther distance from the FTS catalyst to zeolite largely increased the selectivity to BTX (benzene, toluene and xylene) in total aromatics from 48.3% to 68.9% on a carbon molar basis by suppressing the alkylation reaction of benzene and toluene with ethylene due to an obviously lower local ethylene concentration on HZSM-5. FeMn and HZSM-5 with layered loading in two tandem reactors confirmed that light olefins (C2=–C4=) were mainly hydrogenated and isomerized into paraffins. The model reactions with ethylene and propylene in a simulated local FTS reaction environment revealed that the presence of H2O and CO2in situ produced from the FTS reaction played a crucial role in promoting the aromatics formation at obviously lower reaction temperature which resulted from the enhancing acid strength and the driving H transfer to facilitate the cyclization and dehydrogenation reaction. This study provides a clear perspective for the aromatics formation mechanism and the tuning of the aromatic selectivity.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
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IF 7.968
Wenxue Xiong,Feng Hu,Ying Liu,Gang Nie,Ling Xiao
FeMn bimetallic nanoparticles coated with nitrogen-doped graphene shells (FeMn@NG) were prepared by calcination of cellulose supported Prussian blue analogs under N 2 flow, and used as catalysts to activate peroxymonosulfate (PMS) for the degradation of 2,4,6-trichlorophenol (2,4,6-TCP). The addition of cellulose during the formation of Prussian blue analogs reduced the agglomeration of metal particles in the subsequent carbonization process, thus increasing the specific surface area and enhancing the catalytic efficiency of the obtained catalyst. 1 O 2 and the electron transfer pathway were proved to be the main mechanisms by radical quenching experiment, electron paramagnetic resonance and chronoamperometry analysis. The metal leaching of lower than 0.1 mg L −1 and high catalytic stability were attributed to the stable core-shell structure that the metals were encapsulated and protected by graphene shells. The XPS analysis implied that a Fe/Mn redox cycle existed and played a role in balancing electrons during the PMS activation . This study shows that the PMS activator with high catalytic activity can be obtained for the degradation of pollutants by combining Prussian blue analogs with cellulose.
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
ACS Environmental Au
·
2023
·
IF 0
Lu Zheng,Jiarui Fu,Baolv Hua,Yi-nan Wu,Yifan Gu,Nianqiao Qin,Fengting Li
Effective techniques for eliminating antibiotics from water environments are in high demand. The peracetic acid (PAA)-based advanced oxidation process has recently drawn increasing attention for its effective antibiotic degrading capability. However, current applications of PAA-based techniques are limited and tend to have unsatisfactory performance. An additional catalyst for PAA activation could provide a promising solution to improve the performance of PAA. Bulky metal–organic framework gels (MOGs) stand out as ideal catalysts for PAA activation owing to their multiple advantages, including large surface areas, high porosity, and hierarchical pore systems. Herein, a bimetallic hierarchical porous structure, i.e., FeMn13BTC, was synthesized through a facile one-pot synthesis method and employed for PAA activation in ofloxacin (OFX) degradation. The optimized FeMn MOG/PAA system exhibited efficient catalytic performance, characterized by 81.85% OFX degradation achieved within 1 h owing to the specific hierarchical structure and synergistic effect between Fe and Mn ions, which greatly exceeded the performance of the only PAA-catalyzed system. Furthermore, the FeMn MOG/PAA system maintained >80% OFX degradation in natural water. Quenching experiments, electron spin resonance spectra, and model molecular degradation revealed that the primary reactive oxygen species responsible for the catalytic effect was R–O•, especially CH3C(═O)OO•, with minor contributions of •OH and 1O2. Overall, introduction of the MOG catalyst strategy for PAA activation achieved high antibiotic degradation performance, establishing a paradigm for the design of heterogeneous hierarchical systems to broaden the scope of catalyzed water treatment applications.
研究领域:
环境科学
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化学工程
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材料科学
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水处理
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DOI
Journal of Energy Storage
·
2026
·
IF 10.7
Ruolin Zhao,Lei Wang,Jianhua Yan
Steel slag-derived CaO-based composites were designed for high-performance heat storage. • Fe Mn co-modified composites retained 97% heat storage density after 20 cycles. • Fe Mn co-modification enhanced solar absorptance (82%) and compressive strength (1.26 N). • Fe Mn coexistence promoted oxygen vacancies and accelerated CO 2 uptake. CaO-based thermochemical energy storage (TCES) materials have attracted wide attention due to their high energy density, favorable reaction reversibility, and potential integration with CO 2 capture. Steel slag, as a Ca-rich solid waste naturally containing Fe and Mn, offers intrinsic advantages for developing structurally stable and solar-absorptive heat storage materials. However, current steel slag-derived TCES materials still suffer from limited understanding of the functional role of inherent transition-metal elements during repeated high-temperature cycling. In this work, Fe/Mn modified steel slag-derived CaO-based composites were rationally designed to clarify the individual and synergistic effects of Fe and Mn during high-temperature cycling. Fe/Mn containing phases formed a stable framework among CaO particles, effectively suppressing grain sintering and pore collapse. The Fe Mn co-modified sample exhibited superior overall performance. After 20 cycles, Fe Mn co-modified composite maintained a heat storage density of 1263 kJ/kg, corresponding to 97% retention of its initial capacity. The Fe Mn co-modified composite achieved a solar absorptance of 82% and a crushing strength of 1.26 N, which were 1.2 and 4.1 times higher than those of the unmodified sample, respectively. Moreover, the coexistence of Fe and Mn promoted electron transfer and oxygen vacancy formation through double-exchange interactions, thereby facilitating the carbonation reaction. This study demonstrates a targeted Fe Mn co-modification strategy based on the intrinsic Fe-rich feature of steel slag and provides new insights into the high-value utilization of steel slag for sustainable and durable TCES materials. Download: Download high-res image (156KB) Download: Download full-size image
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DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 26
·14841-14850
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IF 12.732
Zhujian Huang,Minxian Shen,Junhong Liu,Jiaer Ye,Tewodros Asefa
Advanced oxidation processes (AOPs) aided by catalysts can efficiently degrade organic pollutants and decontaminate wastewater. In this work, a highly active catalyst composed of FeMn-functionalized graphitic carbon nitride (FeMn–C3N4) for AOPs is synthesized via a green synthetic route, involving a small amount of water and no organic solvents. The synthesis also produces only minimal wastewater as a biproduct. The material contains uniformly dispersed Fe and Mn atoms in the framework of g-C3N4. It shows a unique and high catalytic activity for three AOPs, namely a Fenton-like reaction, persulfate activation and visible-light photocatalysis, while also being reusable several times afterwards. Its catalytic activity is 2.6- to 8.0-fold higher than that of g-C3N4 in all three reactions. The optimal reaction conditions for the catalyst are determined, and the mechanisms by which it drives the reactions are proposed. Notably, the Fe and Mn species present in it contribute substantially to its enhanced catalytic activity. Moreover, compared with g-C3N4, FeMn–C3N4 has a narrower band gap and helps generate more ˙OH, SO4˙− and 1O2 species during the reaction. First-principles density functional theory (DFT) calculations reveal that the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) of FeMn–C3N4 are more delocalized than those of g-C3N4. As a result, the former shows enhanced photo-induced charge carrier separation. This highly active catalyst obtained with a facile synthetic route for these three aforementioned AOPs can have great potential for water treatment and environmental remediation applications.
研究领域:
环境科学
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材料科学
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化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）