ACS Omega
·
2022
·
IF 4.132
Qingxiang Wang,Tao Huang,Jing Du,Lulu Zhou
The extraction of uranium (U)-related minerals from raw ore sands via a leaching procedure would produce enormous amounts of tailings, not only causing radioactivity contamination to surroundings but also wasting the potential U utilization. Effective recycling of U from U tailings is propitious to the current issues in U mining industries. In this study, the influence of the composite oxidation of Fe(III) and Mn(VII) intensified by microwave (MW) irradiation on the acid leaching of U from tailings was comprehensively explored in sequential and coupling systems. The U leaching activities from the tailing specimens were explicitly enhanced by MW irradiation. The composite oxidation caused by Fe(III) and Mn(VII) further facilitated the leaching of U ions from the tailing under MW irradiation in two systems. Maximum leaching efficiencies of 84.61, 80.56, and 92.95% for U ions were achieved in the Fe(III)-, Mn(VII)-, and Fe(III)–Mn(VII)-participated coupling systems, respectively. The inappropriateness of the shrinking core model (SCM) demonstrated by the linear fittings and analysis of variance (ANOVA) for the two systems explained a reverse increase of solid cores in the later stage of leaching experiments. The internal migration of oxidant ions into the particle cores enhanced by MW accelerated the dissolution of Al, Fe, and Mn constituents under acidic conditions, which further strengthened U extraction from tailing specimens.
研究领域:
环境科学
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核工程
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化学工程
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材料科学
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Fengping Zhou,Ye Xiao,Meina Guo,Yetao Tang,Weihua Zhang,Rongliang Qiu
The increasing demand for rare earth elements (REEs) motivates the development of novel strategies for cost-effective REE recovery from secondary sources, especially rare earth tailings. The biggest challenges in recovering REEs from ion-adsorption rare earth tailings are incomplete extraction of cerium (Ce) and the coleaching of iron (Fe) and manganese (Mn). Here, a synergistic process between reduction and stabilization was proposed by innovatively using elemental sulfur (S) as reductant for converting insoluble CeO2 into soluble Ce2(SO4)3 and transforming Fe and Mn oxides into inert FeFe2O4 and MnFe2O4 spinel minerals. After the calcination at 400 °C, 97.0% of Ce can be dissolved using a diluted sulfuric acid, along with only 3.67% of Fe and 23.3% of Mn leached out. Thermodynamic analysis reveals that CeO2 was indirectly reduced by the intermediates MnSO4 and FeS in the system. Density functional theory calculations indicated that Fe(II) and Mn(II) shared similar outer electron arrangements and coordination environments, favoring Mn(II) over Ce(III) as a replacement for Fe(II) in the FeO6 octahedral structure of FeFe2O4. Further investigation on the leaching process suggested that 0.5 mol L–1 H2SO4 is sufficient for the recovery of REEs (97.0%). This research provides a promising strategy to selectively recover REEs from mining tailings or secondary sources via controlling the mineral phase transformation.
研究领域:
化学工程
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环境科学
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材料科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guiyuan Cai,Yu Tian,Lipin Li,Wenxuan Zhang,Rui Huang,Jun Zhang,Qinyu Wang,Hua Xu,Yifeng Zhang
The activation of sulfite [S(IV)] by transition metals, a new generation of advanced oxidation processes, has been widely studied for water purification. However, the application of this process to oxidize and remove arsenite [As(III)] from water through Fe-based S(IV) activation and the associated mechanisms are not fully understood. In particular, rapid removal of As(III) and secondary metal contamination have presented challenges. Herein, we develop a novel sea urchin-like magnetic Fe-Mn bimetallic oxides (FeMnO)-activated S(IV) process to address these issues. Under neutral pH, the FeMnO/S(IV) system achieved a 99.2 % removal of As(III) within only 10 min with residual arsenic concentration below 10 µg/L, and the removed As(III) was fully oxidized to arsenate [As(V)]. Additionally, FeMnO was recyclable and capable of treating actual arsenic-contaminated water. Furthermore, the oxidation mechanism of non-radical active trivalent manganese [Mn(III)] was discovered during the reaction between the FeMnO/S(IV) system and As(III). The FeMnO catalyst activated S(IV) to generate oxysulfur radicals (i.e., SO 5 •– , SO 4 •– and SO 3 •– ), but they were not the primary oxidizing species for As(III). Instead, As(III) oxidation was mainly attributed to the active Mn(III) generated by the electron transfer between the FeMnO catalyst and SO 5 •– radicals. The discovery of active Mn(III) species in this work may provide a new avenue for developing novel Fe-Mn-type adsorbents to purify arsenic-contaminated water.
研究领域:
环境科学
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水处理技术
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
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IF 5.1
Wenjuan Luo,Xiunan Cai,Zhongqiu Luo,Chaochao Lai,Qian Long,Xue Yang,Limin Ning,Pingyan Wang,Xiang Zhang,Xin Fu,Xintao Zhou
Developing efficient and cost-effective processes for removing highly toxic As(III) from water is critical for environmental restoration. Herein, an amorphous Fe–Mn composite (A-CSM) rich in oxygen vacancies was synthesized via a one-pot process. Acid etching of a pretreated copper slag product created the chemical conditions that simultaneously enabled the in situ anchoring of MnO x clusters and induced a crystalline-to-amorphous transformation. The resulting strong Fe–O–Mn interfacial coupling drives interfacial electron redistribution, which upshifts the d-band center and thereby endows the material with unique capabilities for O 2 activation and arsenic adsorption. Leveraging abundant oxygen vacancies within the amorphous structure, A-CSM efficiently activates O 2 into •O 2 − radicals to drive spontaneous As(III) oxidation to As(V), while exposed unsaturated sites in amorphous FeO x domains provide rapid adsorption sites for As(V). Consequently, A‑CSM exhibits a broad pH range (3–9), rapid adsorption kinetics (achieving complete removal of 5 mg L −1 As(III) within 30 min, which is 24.7 times faster than its crystalline counterpart, CSM), the q max calculated by Langmuir model is 84 mg g −1 , and good reusability over five consecutive cycles. Mechanistic studies confirmed that the synergy between the acid etching‑induced amorphous structure and oxygen vacancies significantly reduces the O 2 adsorption energy while it upshifts the d‑band center. This effect lowers the energy barrier for As(III) oxidation/adsorption by approximately 48.9%, and substantially enhances •O 2 − generation. Adsorption primarily involves complexation, electrostatic interactions, and hydrogen bonding, which is consistent with a heterogeneous multilayer process as described by the Freundlich isotherm.
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122891
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IF 7.5
Yuankun Liu,Yuanqi Cao,Gangyi Sun,Zhiwei Zhou,Xing Li,Zhonglin Chen
Fluoxetine (FLX), a widely used antidepressant, has been increasingly detected in aquatic environments due to its high chemical stability and resistance to biodegradation, posing potential ecological risks. In this study, sludge was used as a precursor to synthesize a Fe–Mn bimetallic nitrogen-doped biochar (FeMn/NBC), enabling the resource utilization of solid waste, which was further applied for peroxydisulfate (PDS) activation to achieve efficient degradation and defluorination of FLX. The superior catalytic performance originated from the synergistic coupling between the N-doped carbon framework and Fe–Mn bimetallic active sites. Nitrogen doping enhanced adsorption and PDS activation, while the bimetallic configuration further improved radical generation efficiency, electron transfer, and catalyst stability. Under optimal conditions (FLX = 10 mg/L, PDS = 2 mM, FeMn/NBC-4 = 0.4 g/L), complete removal of FLX was achieved within 60 min. The system exhibited stable performance over a wide pH range, in the presence of coexisting anions, and in real water matrices, with low metal leaching. Quenching experiments indicated that SO₄•⁻ and •OH were the dominant reactive species. The redox cycling of Fe(II)/Fe(III) and Mn(II)/Mn(III) facilitated continuous PDS activation, while the nitrogen-doped carbon framework enhanced electron transfer. DFT calculations combined with LC–MS analysis revealed that SO₄•⁻ first oxidized FLX via electron transfer, followed by •OH weakening the stability of the C–F bond through electrophilic addition and inducing its cleavage. Toxicity evaluation indicated that the degradation intermediates exhibited reduced ecological risk. These findings provide new insights into the degradation and defluorination mechanisms of fluorinated pharmaceuticals.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Jingran Li,Longyan Cui,Chen Wang,Xuetao Liang,Mengying Wang,Han Wang,Qi Yang,Zhilin Yang
A three-dimensional particle electrode was established by integrating MoS 2 with nitrogen-doped Fe Mn biochar (MoS 2 /NFMB-1.0), enabling efficient electrochemical oxidation of tetracycline (TCH) in aqueous environments. Under optimized conditions, the MoS 2 /NFMB-1.0 achieved a TCH removal efficiency of 96.60%, substantially outperforming the two-dimensional electrode system. After five successive cycles, the degradation efficiency remained at 89.65%. The MoS 2 /NFMB-1.0 also promoted stronger mineralization, with a TOC removal of 74.31%, outperforming NFMB (65.21%), MoS 2 (38.43%). Reactive oxygen species (ROS) analysis revealed that the reaction was primarily driven by 1 O 2 (39.37%), accompanied by O 2 ·- (31.73%) and ·OH (28.90%). The incorporation of MoS 2 facilitated the Fe/Mn redox cycle and ensured continuous ROS generation throughout the reaction. The 3D/MoS 2 /NFMB-1.0 system maintained strong reactivity across a broad pH range from 3 to 11 and remained effective toward several representative antibiotics. Liquid chromatography-mass spectrometry (LC-MS) further clarified the transformation pathways of TCH, while ecotoxicity prediction confirmed that the toxicity of intermediates progressively declined as the reaction proceeded. These results highlight the significant potential of the MoS 2 /NFMB-1.0-based 3D particle-electrode system for future electrochemical water treatment.
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Yang Yang,Honghao Deng,Liying Liu,Jiahong Pan,Ping Chen,Zhicong Shi
O3-type Cu/Fe/Mn-based layered oxides are regarded as promising cathode materials for sodium-ion batteries due to the abundance of elements in the Earth's crust and the imperative for large-scale energy storage. However, these materials still encounter some challenges, including low capacity and insufficient rate performance. In this study, Al-doped, cobalt-free, and nickel-free Na 0.9 Cu 0.18 Fe 0.3 Mn 0.52-x Al x O 2 (x = 0, 0.03, 0.05, 0.08) are successfully synthesized by using the solid-state method to introduce non-electrochemically active elements to stabilize the crystal structure and enhance the electrochemical performance. The impact of Al-doping is comprehensively analyzed by using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), galvanostatic intermittent titration technique (GITT), and electrochemical impedance spectroscopy (EIS). Al-doping effectively enhances the diffusion coefficient of Na + , reduces the Jahn-Teller effect caused by Mn 3+ and mitigates the transition from O3 to P3 phase. Finally, it stops the partial phase transitions from O3 to P3, which can be found in pristine oxide without Al-doping during charge-discharge cycling. Notably, the Na 0.9 Cu 0.18 Fe 0.3 Mn 0.47 Al 0.05 O 2 electrode exhibits a reversible capacity of 123.89 mAh g −1 at 0.1 C, a capacity retention rate of 91.1 % after 200 cycles at 1 C, and a discharge capacity of 66.36 mAh g −1 at a high rate of 5 C.
研究领域:
材料科学
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能源存储与转换
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DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Anqi Huang,Dan Zhi,Yaoyu Zhou
A graphite felt (GF) cathode was firstly modified by Fe–Mn binary oxide (FMBO), active carbon (AC), carbon black (CB), and polytetrafluoroethylene (PTFE), which exhibits satisfactory ciprofloxacin (CIP) removal efficiency at neutral pH value in electro-Fenton (EF) system. Morphological data showed that modified cathodes have larger surface area and volume pore as well as more active sites. And electrochemical properties have proved stronger current response after modification. In compassion to the unmodified GF, the FMBO/AC/CB modified GF (FMBO-GF) has wider pH range and higher CIP removal efficiency due to its unique nanoparticles structure. The CIP removal efficiency achieved 95.40% in 30 min, and the removal efficiency of total organic carbon (TOC) achieved 93.77% in 2 h when conditions were optimal (25 mg/L initial CIP concentration, 2 mA/cm 2 current density, FMBO/AC: CB: PTFE of 1:1:5, and 7 initial pH value) in this study. The results of great degradation and mineralization of CIP in this study indicate that the FMBO-GF cathode has huge potential on antibiotics removals in neutral environment.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Yuting He,Hongtao Li,Yi Wang,Yufei Jia,Yongning Liu,Qiang Tan
M−N−C (M = Fe, Co, Ni, etc.) catalyst owns high catalytic activity in the oxygen catalytic reaction which is the most likely to replace the Pt-based catalysts. But it is still a challenge to further increase the active site density. This article constructs the high-efficiency FeMn-N/S-C-1000 catalyst to realize ORR/OER bifunctional catalysis by hetero-atom, bimetal (Fe, Mn) doped simultaneously strategy. When evaluated it as bi-functional electro-catalysts, FeMn-N/S-C-1000 exhibits excellent catalytic activity ( E 1/2 = 0.924 V, E j =10 = 1.617 V) in alkaline media, outperforms conventional Pt/C, RuO 2 and most non-precious-metal catalysts reported recently. Such outstanding performance is owing to N, S co-coordinated with metal to form multi-types of single atom, dual atom active sites to carry out bi-catalysis. Importantly, nitrite poison test provides the proof that the active sites of FeMn-N/S-C are more than that of single-atom catalysts to promote catalytic reactions directly. To better understand the local structure of Fe and Mn active sites, XAS and DFT were employed to reveal that FeMn-N 5 /S-C site plays the key role during catalysis. Notably, the FeMn-N/S-C-1000 based low-temperature rechargeable flexible Zn-air also exhibits superior discharge performance and extraordinary durability at −40 °C. This work will provide a new idea to design diatomic catalysts applied in low-temperature rechargeable batteries.
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高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Zhongshuai Zhang,Yuqing Liu,Zixi Liu,Hailin Li,Yaoliang Huang,Weijian Liu,Dingshan Ruan,Xin Cai,Xiaoyuan Yu
O3-type Fe/Mn-based layered oxides are considered as the competitive cathode materials for sodium-ion batteries because of environmental friendly metal elements and low cost. However, a lower capacity, poor cycling stability and irreversible phase transitions hinder their commercial application. Herein, the Cu-doped O3 biphasic Na[Mn 0.6 Fe 0.4 ] (1- x ) Cu x O 2 (NFMCu- x ) layered oxides are successfully synthesized by high temperature calcination using Fe/Mn-based Prussian blue analogues as precursor. The results indicate that the different stoichiometric of Cu 2+ substitution in P2 NaMn 0.6 Fe 0.4 O 2 can cause the transformation of P2 phase to O3 monophase or O3 biphase. The NFMCu- x samples exhibit O3 monophase at x = 0.1, 0.15, while O3 biphase coexists in the compound at x = 0.2, 0.25, and 0.3. Benefiting from the synergetic effect of Cu-doping and O3 biphasic structure, the optimized O3 biphasic NaMn 0.48 Fe 0.32 Cu 0.2 O 2 exhibits a high Na + diffusion coefficient and an excellent sodium storage performance with a high discharge specific capacity of 103.76 mAh g −1 at 24 mA g −1 and good capacity retention of 82.9% after 100 cycles. Moreover, Cu-doped O3 biphasic NaMn 0.48 Fe 0.32 Cu 0.2 O 2 features an excellent air stability. Thus, this work proposes a strategy in development of O3 Fe/Mn-based layered oxide as high-performance cathode materials for sodium-ion batteries.
研究领域:
材料科学
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电化学
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能源存储
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无机化学
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固态化学
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DOI
高影响因子
Journal of Physical Chemistry Letters
·
2024
·
IF 4.8
Yanchang Wang,Yao Xiao,Jiangnan Huang,Chunxiao Zhang,Kentaro Yamamoto,Yoshiharu Uchimoto,Weifeng Wei,Hongshuai Hou,Datong Zhang,Xiaobo Ji
For cathode materials of sodium-ion batteries, O3-type Ni/Fe/Mn-based (Na-NFM) layered oxides have garnered extensive attention because of high economic viability, environmental friendliness, and the potential for high energy density. Among them, Fe-rich compositions exhibit higher initial charge capacity and lower bill-of-material costs, while they fade rapidly and exhibit low initial coulombic efficiency, hindering their commercialization prospects. In this work, we investigate the failure of Fe-rich Na-NFM materials through X-ray absorption spectroscopy methods. The results reveal a combined failure mechanism that encompasses not only the conventional theory of Fe migration but also an abnormal Ni-redox deterioration, which has not yet been reported. More factors related to the failure of Fe-rich Na-NFM layered oxides are discussed in detail. These findings are expected to inspire targeted research efforts toward Fe-rich Na-NFM materials, thereby accelerating the practical application of sodium-ion batteries.
研究领域:
材料科学
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电化学
·
固态化学
·
储能
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DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Hao Meng,Yue Wang,Haiyan Yang,Jinglong Han,Dillirani Nagarajan,Shih-Hsin Ho,Jo-Shu Chang
Advanced oxidation processes, especially those engaging in persulfate activation, are one of the emerging technologies for the degradation of recalcitrant organic pollutants. This study used Fe and Mn-loaded Prussian blue analogs (FeMn-PBA) as precursors to synthesize a nitrogen-doped graphene shell (FeMn@NG) through calcination in a nitrogen atmosphere. This was then employed as a catalyst to initiate the degradation of sulfadiazine (SD) using persulfate. The encapsulated FeMn bimetallic nanoparticles with various oxidation states undergo redox cycling, which promotes the rapid generation of free radicals and maintains the stability of FeMn@NC by sustaining continuous persulfate (PDS) activation. The results showed that nearly 96 % of SD was degraded within 45 min. Experiments involving free radical quenching and electron paramagnetic resonance spectroscopy demonstrated that sulfate radicals (SO 4 ·− ) and superoxide radicals (O 2 ·− ) were primarily responsible for the degradation of SD. The impact of different process parameters on the degradation efficiency of SD was simultaneously investigated. The degradation products of SD were examined, and a degradation pathway was proposed according to the LC-MS findings. XPS analysis indicated the presence of Fe/Mn redox cycling, which played a role in the equilibrium electron transfer during PDS activation. This study provides insights into the rational design of efficient catalysts by combining Prussian blue analogs with FeMn, while also promoting the remediation of polluted water bodies.
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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水处理技术
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有机污染物降解
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）