JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Yuxi Zhang,Yamin Deng,Jiangkai Xue,Yihan Cheng,Yulun Nie,Kunfu Pi,Yao Du,Xianjun Xie,Jianbo Shi,Yanxin Wang
The environmental fate of arsenic (As) relies substantially on its speciation, which occurs frequently coupled to the redox transformation of manganese. While trivalent manganese (Mn(III)), which is known for its high reactivity, is believed to play a role in As mobilization by iron (oxyhydr)oxides in dynamic aquifers, the exact roles and underlying mechanisms are still poorly understood. Using increasingly complex batch experiments that mimick As-affected aquifer conditions in combination with time-resolved characterization, we demonstrate that Mn(III)-NOM complexes play a crucial role in the manganese-mediated immobilization of As(III) by ferrihydrite and goethite . Under anaerobic condition , Mn(III)-fulvic acid (FA) rapidly oxidized 31.8% of aqueous As(III) and bound both As(III) and As(V). Furthermore, Mn(III)-FA exerted significantly different effects on the adsorption of As by ferrihydrite and goethite. Mn(III)-FA increased the adsorption of As by 6–16% due to the higher affinity of oxidation-produced As(V) for ferrihydrite under circumneutral conditions. In contrast, As adsorption by crystalline goethite was eventually inhibited due to the competitive effect of Mn(III)-FA. To summarize, our results reveal that Mn(III)-NOM complexes play dual roles in As retention by iron oxides , depending on the their crystallization. This highlights the importance of Mn(III) for the fate of As particularly in redox fluctuating groundwater environments.
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高影响因子
MOLECULES
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2024
·Vol. 29
·期 9
·1946
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IF 4.2
Yan Ma,Kai Wang,Sikai Liang,Zhongqing Li,Zhiyuan Wang,Jun Shen
The Mn-Fe oxide material possesses the advantages of abundant availability, low cost, and non-toxicity as an energy storage material, particularly addressing the limitation of sluggish reoxidation kinetics observed in pure manganese oxide. However, scaling up the thermal energy storage (TCES) system poses challenges to the stability of the reactivities and mechanical strength of materials over long-term cycles, necessitating their resolution. In this study, Mn-Fe granules were fabricated with a diameter of approximately 2 mm using the feasible and scalable drop technique, and the effects of Y2O3-stabilized ZrO2(YSZ) and SiO2doping, at various doping ratios ranging from 1–20 wt%, were investigated on both the anti-sintering behavior and mechanical strength. In a thermal gravimetric analyzer, the redox reaction tests showed that both the dopants led to an enhancement in the reoxidation rates when the doping ratios were in an appropriate range, while they also brought about a decrease in the reduction rate and energy storage density. In a packed-bed reactor, the results of five consecutive redox tests showed a similar pattern to that in a thermal gravimetric analyzer. Additionally, the doping led to the stable reduction/oxidation reaction rates during the cyclic tests. In the subsequent 120 cyclic tests, the Si-doped granules exhibited volume expansion with a decreased crushing strength, whereas the YSZ-doped granules experienced drastic shrinkage with an increase in the crushing strength. The 1 wt% Si and 2 wt% Si presented the best synthetic performance, which resulted from the milder sintering effects during the long-term cyclic tests.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yan Sun,Ranxin Li,Qiubo Wang,Wen-da Oh,Mingjie Huang,Xiaohui Wu,Tao Zhou
The concept of converting biowaste to energy is popular worldwide; however, overcoming the trade-off between bio-oil recovery and obtaining functional biochar remains challenging. This study investigated the effects of three transition metal ions (Mn 2+ , Cu 2+ and Fe 2+ ) throughout the entire process of recovering 5-hydroxymethylfurfural (5-HMF) from forestry waste and on the catalytic abilities of biochar derived from the oil-extracted residue. The Cu 2+ , Fe 2+ , and Mn 2+ ions significantly increased 5-HMF yields by 93- to 158-fold compared to the metal-free control. However, only marginal improvements in the catalytic ability of the residue-derived biochar for persulfate activation were observed for Cu- or Fe-doped biochar, despite the general benefit of transition metal doping for biochar functionalization. Interestingly, a dual Mn-mediated promotion was achieved beyond enhancing 5-HMF production. The Mn-doped biochar (Mn-Biochar) exhibited excellent peroxydisulfate (PDS) activation capability, enhancing the degradation of the antibiotic sulfamethoxazole (SMX) by 6.6- to 15.0-fold. Characterizations revealed that incorporated nitrogen was responsible for this enhancement. N-doping transformed the Mn species into MnO, which tripled the Mn loading capacity and enhanced the electrical conductivity of the biochar. The formed Mn-N x structure in the biochar (Mn-N-FBBC) facilitated polarization of the O O bond and cleavage of the S O bond in PDS, generating 1 O 2 for SMX degradation. Life cycle assessment (LCA) indicated that this dual Mn-mediated process for 5-HMF recovery and biochar production offers synergistic benefits, realizing the “waste-resource-material-treatment” paradigm in biomass conversion.
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Journal of the Taiwan Institute of Chemical Engineers
·
2025
·
IF 6.3
Xiaodao Liang,Yaorong He,Chao Xiong,Hongbing Ji,Yan Yang
Background Oxygen activation is a critical step in oxidation reactions for energy conversion and fine chemical synthesis, with its efficiency directly determining catalytic performance and industrial applicability. The main challenges are the high activation energy barriers and low target product selectivity caused by the inherent inertness of molecular oxygen. To address these issues, this study draws on the advantages of biomimetic catalysis using metal porphyrins and synthesizes a series of porphyrin-based organic polymers (Metal-Por-POPs) to achieve efficient aerobic epoxidation of olefins. Method A series of metalloporphyrin-based organic polymers were synthesized and thoroughly characterized using techniques such as SEM, XRD, and XPS. The catalytic performance was systematically evaluated under various conditions, including catalyst types, oxidant amount, reaction time, and temperature. Significant finding Using Mn-Por-POP as a catalyst, isobutylene was converted to the corresponding epoxide within 1 h at room temperature with a selectivity of up to 96.4 %. The catalyst also demonstrated excellent recyclability and broad substrate adaptability, maintaining over 96 % epoxide selectivity after five consecutive reaction cycles. Mechanistic studies via EPR and HRMS revealed that Mn-Por-POP promoted the generation of acyl radicals from isobutyraldehyde under aerobic conditions. These radicals subsequently reacted with molecular oxygen to form acylperoxy radicals, which facilitate the highly selective epoxidation of alkenes.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Chen Yu,Dawei Liang,Chao Qu,Na Ren,Qinghao Wu,Xiaohu Li,Jingjing Yao
Electro-oxidation is a promising technology for treating refractory organic pollutants in landfill leachate but faces challenges of high energy consumption and inefficient degradation of complex organics. This study introduces a manganese single-atom catalyst (MnSAC) doped on carbon nanotubes (CNTs) within a gas-diffusion electrode to enhance electro-oxidation performance. The bifunctional catalyst simultaneously promotes 2e oxygen reduction reaction for H 2 O 2 generation and in-situ activation of H 2 O 2 to produce reactive oxygen species, primarily hydroxyl radicals ( • OH). In a system employing a Ni-Sb-SnO 2 anode and operating under the operation conditions (initial chemical oxygen demand: 478 mg L 1 ; electrolyte: 0.1 mol L 1 Na 2 SO 4 , current density: 10 mA cm 2 , volume: 100 mL), a 90% removal rate (reduced to 49 mg L 1 ) was achieved. The core innovation lies in the unique N-coordinated MnSAC (Mn-N 4 ) sites on CNTs, identified via Density Functional Theory calculations to exhibit ΔG of −3.46 eV for H 2 O 2 activation and organic adsorption. The Mn-N-C structure modulates the d-band center to optimize electron/charge distribution and transfer. This synergistic design: 1) enhances H 2 O 2 activation and radical generation, 2) accelerates organic pollutant adsorption/degradation, and 3) improves reaction kinetics. The catalyst addresses critical issues like metal leaching and energy inefficiency, offering a robust, sustainable solution for refractory organic wastewater treatment.
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Journal of Energy Storage
·
2025
·
IF 9.8
Hongrun Qiu,Jianwei Li,Li Han,Guangqin Zhu,Min Lei,Xinhe Yang,Guofeng Jia,Min Wang
Cobalt-free manganese-based layered oxides such as LiNi 0.5 Mn 0.5 O 2 are promising cathodes for next-generation high-energy-density lithium-ion batteries owing to their high theoretical capacity. However, their structural instability in highly delithiated states leads to considerable degradation of both the surface and bulk phases during cycling, limiting their applicability. To address this structural instability, a “pinning” and “pillaring” strategy via titanium doping is proposed herein. Titanium ions act as “pillars” in highly delithiated states in the bulk structure, enhancing phase transition reversibility during cycling. In situ and ex situ X-ray diffraction analyses confirm that Titanium doping stabilizes the bulk structure within 3.0–4.8 V at room temperature. X-ray photoelectron spectroscopy reveals that Titanium ions form a “cationic barrier” at the surface, anchoring lattice oxygen and suppressing undesired phase transformations. This dual mechanism endows the 3 % Titanium-doped material with excellent cycling stability. It exhibits an initial discharge capacity of 157.7 mA h g −1 at C/2 and retains 83.45 % of this capacity after 120 cycles. This represents a 24.17 % increase in initial capacity and a 41.30 % improvement in capacity retention compared to those of undoped LiNi 0.5 Mn 0.5 O 2 . The voltage decay rate of the doped material also reduces to 1.64 mV per cycle, indicating a 90.24 % improvement. The proposed approach is a viable strategy for advancing Cobalt-free manganese-based layered oxides for use in high-energy-density lithium-ion batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Zerui Chen,Yingxinjie Wang,Jie Wang,Xiaohui Li,Guohao Li,Ziying Zhang,Zhenjun Wu,Xiuqiang Xie,Nan Zhang
Manganese-based Prussian blue analogues (PBA) have garnered widespread attention as the promising cathode materials for sodium-ion batteries. However, the inevitable Jahn-Teller distortion and the formation of unstable and uneven cathode electrolyte interphase (CEI) result in severe Mn dissolution and poor cycling stability. Herein, we report a simple MXene modification strategy cold pressing method to embed Prussian blue cathode materials into MXene nanosheets. This highly conductive protective barrier not only mitigates the Jahn-Teller distortion in Mn-PBA and maintains the integrity of the particles during charge–discharge cycles, but also partially suppresses side reactions between the electrolyte and cathode interface through surface functional groups (−F), resulting in a thin and uniform CEI. The protection of the stable CEI and MXene nanosheets simultaneously alleviate the Jahn-Teller effect and suppress the Mn dissolution during long cycling, thus allowing the cathode material to retain ∼ 80 % of its capacity after 1000 cycles at a current density of 1000 mA g −1 . This study highlights the importance of stabilizing the cathode interface and provides a novel approach for preparing highly stable manganese-based PBA cathode.
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WATER RESEARCH
·
2025
·
IF 12.4
Jung-Hyun Son,Wen-Long Wang,Peng-Hui Liu,Hang Su,Ju-Won Lee,Min-Yong Lee,Qian-Yuan Wu
This study investigates the enhancement of ozonation efficiency through the introduction of manganese ions (O 3 /Mn(II)) that significantly improve the degradation of ozone-persistent organic pollutants. Manganese ions accelerate hydroxyl radical generation by catalyzing ozone decomposition, thereby facilitating more effective oxidative reactions. The application of O 3 /Mn(II) to degrade N, N-Diethyl-3-toluamide (DEET) achieved a decomposition efficiency of 3.6 to 4.1 times higher than ozonation alone. The promotive effect was highly pH-dependent, with the observed rate constant ( k obs ) for O 3 /Mn(II) reaching 97.05 M −1 s −1 at pH 4, approximately 3.3 times greater than ozonation alone, and 686.93 M −1 s −1 at pH 7, around 1.7 times higher. O 3 oxidation contributed approximately 1% to the overall process, while hydroxyl radicals accounted for approximately 80%, and manganese species accounted for approximately 20%. Furthermore, the oxidation state of manganese significantly influenced the cooperative oxidation efficiency, with Mn(VII) achieving the highest k obs (680.87 M −1 s −1 ), while Mn(IV) exhibited the lowest (304.6 M −1 s −1 ). Additionally, intermediate products formed during DEET oxidation were identified using Orbitrap technology, elucidating various degradation pathways (such as decarboxylation, tri-hydration, and aromatic ring opening). These findings provide valuable insights into enhancing ozonation processes for environmental remediation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Mengmeng Yan,Kang Xu,Yu-Xin Chang,Zhi-Yu Xie,Sailong Xu
Environmentally friendly P2-type layered iron manganese oxides appear to be one of the most potential cathode materials for sodium-ion batteries (SIBs). However, their practical application is hindered by the unfavorable phase transitions, dissolution of transition metals, and poor air stability. One effective strategy by either single-cation doping or high-cost Li involved co-doping is used to alleviate the problems. Here, low-cost Cu/Ti co-doping is introduced to boost P2-Na 0.7 Cu 0.2 Fe 0.2 Mn 0.5 Ti 0.1 O 2 as an air and electrochemical stable cathode material for SIBs. The resulting electrode delivers an initial capacity of 130 mAh g −1 at 0.1C within 2.0–4.2 V, a reversible discharge capacity of 61.0 mAh g −1 at a high rate of 5C and a capacity retention ratio exceeding 71.1% after 300 cycles. In particular, the co-doped crystal structure is well-maintained after 1 month of exposure to air, and even 3 days of soaking in water. Furthermore, the enhancement is elucidated by the effectively mitigated P2–Z and the completely suppressed P2–P′2 phase transitions, the decreased volume variation proved by in-situ X-ray diffraction (XRD), as well as the lowered transition-metal dissolution evidenced by inductively coupled plasma optical emission spectrometer (ICP-OES) and X-ray photoelectron spectroscopy (XPS). The low-lost Cu/Ti doping strategy could thus be effective for designing and preparing environmentally friendly and high-performance cathode materials for SIBs.
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JOURNAL OF MATERIALS SCIENCE
·
2026
·
IF 4.4
Zeng Fanen,Xu Bing,Jing Chenglong,He Xiaodong,Li Chunyang,Li Guojun
High-entropy oxides (HEOs) have attracted considerable attention for energy storage applications because of their multi-principal synergistic effects and excellent structural stability. In this study, polyethylene glycol (PEG) was used as a surfactant to synthesize (CrMnFeCoNi) 3 O 4 HEOs by tuning the molar ratio of PEG to metal cations ( P / M ). The results show that PEG plays three roles during synthesis, serving simultaneously as a coordinating dispersant, a structure-directing agent, and an in situ porogen. The optimized HEO ( P / M = 4/5) exhibits a uniform nanoparticle morphology and a well-developed pore architecture, delivering a specific capacitance of 557.6 F g –1 . Kinetic analysis further indicates that its pseudocapacitive behavior is from a cooperative effect involving both capacitive-controlled and diffusion-dominated mechanisms. The assembled asymmetric supercapacitor device achieves an energy density of 64.2 Wh kg –1 at a power density of 375.3 W kg –1 and retains 81.3% of its capacitance after 10000 charge/discharge cycles. These outstanding electrochemical properties highlight the promise of PEG template (CrMnFeCoNi) 3 O 4 HEOs for advanced energy storage applications. Graphical abstract
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Journal of Environmental Chemical Engineering
·
2026
·
IF 7.5
Hang Jia,Mengyao Wang,Ruihan Li,Yanli Xie,Xing Qiao,Yuanqi Lv,Antonio Francesco Logrieco,Giuseppina Mule
A magnetic CoMn-PBA*-based adsorption–activation system was developed for mycotoxin detoxification. • Synergistic adsorption and PMS activation enabled rapid removal of AFB₁, ZEN, and OTA. • Efficient detoxification was achieved in edible oil and grape juice while maintaining acceptable quality. • The catalyst exhibited good reusability and stable performance during repeated cycles. • Zebrafish assays demonstrated reduced toxicity of degradation products and favorable preliminary biosafety. Aflatoxin B 1 (AFB 1 ), zearalenone (ZEN), and ochratoxin A (OTA) are widespread contaminants in food systems, while existing detoxification approaches often suffer from limited efficiency and poor applicability in complex matrices. Herein, a magnetic cobalt–manganese Prussian blue analogue-derived catalyst was developed by integrating adsorption with peroxymonosulfate (PMS) activation for synergistic detoxification of multiple mycotoxins. The catalyst exhibited rapid adsorption toward AFB₁ with a removal efficiency of up to 98%, while PMS activation generated reactive species, including SO₄•⁻ and •OH, which further promoted the degradation of ZEN and OTA. As a result, efficient removal of all three mycotoxins was achieved within 30 min through the combined adsorption–oxidation process. The catalyst also maintained considerable detoxification performance after four consecutive cycles, indicating acceptable reusability. Importantly, the treated edible oils and grape juice maintained comparable quality parameters to the untreated controls, indicating minimal impact on food quality and the feasibility in complex food matrices. Zebrafish assays further indicated low acute toxicity of the catalyst and treated products under the tested conditions, providing preliminary evidence of biosafety. This study provides a promising integrated adsorption–activation strategy for efficient mycotoxin detoxification in complex food matrices. Download: Download high-res image (332KB) Download: Download full-size image
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Meiling Lian,Haoquan Wang,Liuxing Chen,Da Chen,Qi Yang,Xuezhi Qiao
Electrochemical sensing devices often suffer from biofouling due to nonspecific adsorption of biomolecules and microorganisms in complex biological matrices. To address this challenge, we developed an efficient antifouling and self-sterilizing sensing interface by grafting polyethylene glycol (PEG) onto two-dimensional Ti 3 C 2 T x MXene nanosheets for the accurate detection of cardiac troponin I (cTnI), a gold-standard biomarker for acute myocardial infarction (AMI). The Mn 2+ -intercalated Ti 3 C 2 T x (Mn-Ti 3 C 2 T x ) exhibited enhanced electrochemical activity in a three-electron oxygen reduction reaction (3e - ORR), enabling in situ self-sterilization by activating molecular oxygen to generate hydroxyl radicals (•OH), which demonstrated potent antibacterial effects against both Gram-negative and Gram-positive bacteria. Density functional theory calculations revealed that Mn doping in MXene significantly reduced the free energy barrier of *OOH intermediate, promoting H 2 O 2 formation and subsequent reduction to •OH. The PEGylated Mn-Ti 3 C 2 (PEG@Mn-Ti 3 C 2 T x ) composite combined the superior hydrophilicity of PEG for effective protein repulsion with the enhanced conductivity of Mn-Ti 3 C 2 T x , enabling sensitive biosensing. Critically, the fabricated biosensor demonstrated high specificity for cTnI against common interferents and achieved reliable detection in spiked serum samples. It exhibited a broad detection range from 0.1 pg mL -1 to 500 ng mL -1 with an ultralow limit of 0.03 pg mL -1 . This work presents a novel strategy for combating biofouling and paves the way for designing robust biosensors capable of accurate and long-term operation in clinically relevant environments, holding great promise for point-of-care diagnostics.
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