JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Shun Qiu,Zhanxun Chen,Ling Yu,Chuying Liu,Chenghan Ji,Pengfei Shen,Sikai Cheng,Hui Qiu,Zhuoyao Fang,Xiaolin Zhang
Herein, a highly efficient As(III) purifier Ce-Mn@N201 with excellent reusability was developed by stepwise precipitating hydrated cerium(IV) oxides (HCO) and hydrated manganese(IV) oxides (HMO) inside N201, a widely-used gel-type anion exchange resin . Owing to confinement of unique nanopores in N201, the in-situ generated nanoparticles (NPs) inside Ce-Mn@N201 were highly dispersed with ultra-small sizes of around 2.6 nm. Results demonstrated that HMO NPs effectively oxidized As(III) to As(V) with the conversion of Mn(IV) to Mn(II), while the generated Mn 2+ was mostly re-adsorbed onto the negatively-charged surface of HMO NPs. During the regeneration process by simple alkaline treatment , the re-adsorbed Mn 2+ was firstly precipitated as (hydr)oxides of Mn(II) and then oxidized to HMO NPs by dissolved oxygen to fully refresh its oxidation capacity. Though HCO NPs mainly served as adsorbent for arsenic, they could partially oxidize As(III) to As(V) at the beginning, while the oxidation capacities continuously diminished with the irreversible conversion of Ce(IV) to Ce(III). In 10 consecutive adsorption-regeneration cycle, Ce-Mn@N201 efficiently decontaminated As(III) from 500 μg/L to below 5 μg/L with Mn 2+ leaching less than 0.3% per batch. During 3 cyclic fixed-bed adsorptions, Ce-Mn@N201 steadily produced 8500–9150 bed volume (BV) and 3150–3350 BV drinkable water from the synthesized and real groundwater, respectively, with Mn leaching in effluent constantly < 100 μg/L.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Wenjing Yang,Hexue Jia,Tingting Li,Yuepeng Liu,Yi Li
Superoxide radicals (·O 2 − ) has been regarded as one of the reactive oxygen species (ROS) for the elimination of complex contaminants via electro-Fenton like (EF-like) technology. However, the generation path of ·O 2 − is diverse, and the influence of the physicochemical properties of metals on the mechanism of ·O 2 − conversion is significant in the EF-like treatment of wastewater. Herein, metals (M = Mn, Cu) loaded zeolitic imidazolate frameworks catalytic materials (M–NC) were prepared for sulfamethoxazole (SMX) removal to analyze the effect of metals on the pathways of ·O 2 − generation. The removal kinetic rate of SMX by Cu–NC was 1.32 times higher than that of Mn–NC. Quenching experiments demonstrated that ·O 2 − is the most important oxidizing species to achieve SMX removal. The RRDE measurements and quantitative experiment on the concentration of H 2 O 2 experiments indicated that Mn–NC was more inclined to generate ROS through activation of H 2 O 2 and Cu–NC through other ways. Therefore, the transformation pathways of ·O 2 − in different catalytic systems were thoroughly analyzed. Electron paramagnetic resonance test and reactive oxygen species quenching experiments indicated that the pathway for ·O 2 − production of Mn–NC was O 2 → H 2 O 2 → ·O 2 − , and that of Cu–NC was O 2 → ·O 2 − . The strategy of using Mn and Cu-based catalysts to investigate the mechanism of the ·O 2 − generation pathway provided a way to efficiently utilize the conversion of ·O 2 − .
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ACS Nano
·
2025
·
IF 16
Susu Zhao,Qian Dang,Aiqing Cao,Marshet Getaye Sendeku,Hai Liu,Jian Peng,Yameng Fan,Hui Li,Fengmei Wang,Yun Kuang,Xiaoming Sun
Ruthenium (Ru)-based catalysts have demonstrated promising utilization potentiality to replace the much expensive iridium (Ir)-based ones for proton exchange membrane water electrolysis (PEMWE) due to their high electrochemical activity and low cost. However, the susceptibility of RuO2-based materials to easily be oxidized to high-valent and soluble Ru species during the oxygen evolution reaction (OER) in acid media hinders the practical application, especially under current density above 500 mA cm–2. Here, a manganese-doped RuO2 catalyst with the hydroxylated metal sites (i.e., H–Mn0.1Ru0.9O2) is synthesized for acidic OER assisted by hydrogen peroxide, where the hydroxylation results in the valence state of the Ru sites below +4. The H–Mn0.1Ru0.9O2 catalyst demonstrates an overpotential of 169 mV at 10 mA cm–2 and promising stability for an OER over 1000 h in an acidic electrolyte. A PEMWE device fabricated with the H–Mn0.1Ru0.9O2 catalyst as the anode shows a current density of 1 A cm–2 at ∼1.65 V, along with a low degradation over continuous tens of hours. Differential electrochemical mass spectrometry (DEMS) results and theoretical calculations confirm that H–Mn0.1Ru0.9O2 performs the OER through the adsorbate evolution mechanism (AEM) pathway, where the synergistic effect of hydroxylation and Mn doping in RuO2 can effectively enhance the stability of Ru sites and lattice oxygen atoms.
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Journal of Energy Storage
·
2024
·
IF 8.9
Xin Yu,Dandan Yu,Yanli Li,Huanle Niu,Tiantian Zhang,Wenyan Yang,Dongfei Sun
Aqueous zinc ion batteries (AZIBs) are gaining considerable research attention owing to their high safety and low cost. Although MnO 2 is a promising cathode, the inevitable MnO 2 dissolution and slow kinetics still limit their application in AZIBs. Herein, we propose a Fe 3+ and K + co-doping design of MnO 2 (labeled Fe-KMnO) to improve the structural stability and kinetics. Specifically, the introduction of Fe 3+ and K + can reduce the particle size and enlarge the interlayer spacing of MnO 2 , while the lattice substitution of Fe 3+ can reduce Zn 2+ diffusion barriers inside the cathode by the density functional theory calculations, leading to the good rate stability. Meantime, the TiO 2 coated Zn foil is designed to alleviate corrosion and suppress Zn dendrites, thus reduce the interfacial resistance and improve the dynamics of Zn-MnO 2 batteries. Based on the advantages of Fe-KMnO material and the effective protection of Zn anode, Fe-KMnO electrode shows excellent performance. When it is applied to the cathode material for aqueous zinc ion battery, the reversible specific capacity of 367.4 mAh g −1 is obtained at the current density of 0.1 A g −1 , superior cycle stability (a capacity of 109.5 mAh g −1 at 1 A g −1 after 5000 cycles), making it a promising cathode for high-performance AZIBs.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Li-Ming Sun,Bin Li,Ang Li,Ze-Zhou Ding,Xin-Hui Wang,Yu-Xi Huang,Chang Liu,Tong Li,Wei-Sheng Huang,Xing Zhang
The Mn–Co dual-metal oxide is recognized as an effective activator for peroxymonosulfate (PMS), but its activation mechanism remains controversial. In this study, a Co/Mn–C–N (CMCN) nanocatalyst was synthesized using a simple pyrolysis method, and its catalytic activity along with the PMS activation mechanism was comprehensively explored. The findings indicated that the synergistic effect of Mn and Co within the bimetallic composition significantly enhanced the catalytic efficiency of CMCN compared to those of individual metal oxides (Mn–C–N and Co–C–N). Bisphenol A underwent successful degradation within 3 min in a neutral environment, with a degradation kinetic rate of 1.59 min–1 and a total organic carbon removal efficiency of 63.8%. Moreover, CMCN nanoparticles demonstrated remarkable stability and reusability, maintaining their efficacy over four cycles. Employing a series of experiments and analytical characterizations, a novel activation mechanism for PMS was proposed, involving both radical and nonradical pathways. This mechanism involves the oxidation of organic pollutants through a direct electron transfer process from metastable intermediate complexes. Notably, the CMCN/PMS system exhibited a robust resistance to interference factors. This research provides novel insights into the development of bimetallic oxide composites for the effective removal of recalcitrant water pollutants.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Qing Chen,Ling Shi,Guiping Xu,Maocong Hu,Mao Peng,Zhenhua Yao
The development of low-cost and efficient bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of importance for the commercialization of green and sustainable energy conversion devices. In this work, noble metal-free XFeCoNiCu (X = Cr, Mg, and Mn) high entropy alloys were prepared with a facile pyrolytic reduction approach while the structure and composition were characterized by XRD, ICP-OES, TEM, HRTEM, and XPS. The prepared quinary alloys demonstrated excellent activity and stability for both ORR and OER, which was even superior to that of commercial Pt/C and RuO₂. Moreover, all three catalysts exhibited considerable potential for bifunctional catalysis, with a ΔE gap of 0.659 V for CrFeCoNiCu, a ΔE gap of 0.692 V for MnFeCoNiCu, and a ΔE gap of 0.727 V for MgFeCoNiCu, which was much better than that of the Pt/C+RuO 2 combination (0.723 V). The superior performance was further revealed by Density Functional Theory (DFT) calculations with projection density of states (PDOS) and free energy change. The strategy proposed in this study provides an economical approach to design and develop bifunctional electrocatalysts with exceptional performance.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Shaobo Ye,Zhentao Du,Zhengxiang Cai,Deliu Ou,Haonan Guo,Qiao Liu,Weiyou Yang,Qing Shi
Molybdenum disulfide (MoS2), a typical earth-abundant material, is an excellent candidate for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which fundamentally rely on the regulation of the morphology and electronic structure of MoS2. Herein, Mn-doped amorphous MoS2 coated on Mn-doped crystalline Ni3S2 nanorods (Mn–Ni3S2@MoS2), rationally designed core–shell nanorods, have been fabricated via a facile one-step hydrothermal method as highly efficient bifunctional activities for HER and OER in alkaline solution. The target electrodes deliver a high current density of 100 mA cm–2 at a low overpotential of 187 and 310 mV for HER and OER, respectively, outperforming most MoS2-based catalysts. Moreover, a water-splitting cell based on the Mn–Ni3S2@MoS2 electrode requires a voltage of 1.45 V to reach a current density of 10 mA cm–2, which is superior to the state-of-the-art one of those based on noble metal Pt/C–NF∥RuO2–NF and non-noble metal catalysts. The overall enhanced bifunctional catalytic performance is mainly attributed to the abundant catalytically active sites provided by the Mn-doped amorphous MoS2 and the fast pathway for electron/proton transfer facilitated by the Mn-doped crystalline Ni3S2 nanorods. The incorporated Mn dopants and assembled Ni3S2/MoS2 heterostructure effectively regulate the electronic structure with redistributed charge within the core–shell Mn–Ni3S2@MoS2 electrode.
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Materials
·
2024
·Vol. 17
·期 5
·1118
·
IF 3.1
Hanyun Xie,Runhua Chen,Yuxia Song,Yan Shen,Fengming Song,Bo He,Xiaomei Jiang,Yifan Yin,Wenming Wang
Transition metals and their oxide compounds exhibit excellent chemical reactivity; however, their easy agglomeration and high cost limit their catalysis applications. In this study, an interpolation structure of a Myriophyllum verticillatum L. biochar-supported Mn/Mg composite (Mn/Mg@MV) was prepared to degrade triphenyl phosphate (TPhP) from wastewater through the activating periodate (PI) process. Interestingly, the Mn/Mg@MV composite showed strong radical self-producing capacities. The Mn/Mg@MV system degraded 93.34% TPhP (pH 5, 10 μM) within 150 min. The experimental results confirmed that the predominant role of IO3· and the auxiliary ·OH jointly contributed to the TPhP degradation. In addition, the TPhP pollutants were degraded to various intermediates and subsequent Mg mineral phase mineralization via mechanisms like interfacial processes and radical oxidation. DFT theoretical calculations further indicated that the synergy between Mn and Mg induced the charge transfer of the carbon-based surface, leading to the formation of an ·OH radical-enriched surface and enhancing the multivariate interface process of ·OH, IO3, and Mn(VII) to TPhP degradation, resulting in the further formation of Mg PO4mineralization.
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DESALINATION
·
2024
·
IF 8.3
Yuchun Ren,Dandan Zhao,Fei Zhou,Yuan Liu,Chen Fu,Yongsheng Fu,Tao Gong,Zhenglian Wu,Xinyu Yang,Zefeng Cai
Lithium recovery from shale gas wastewater (SGW) is essential for the growth of a sustainable economy. However, traditional powder adsorbents suffer significant loss and poor recyclability, limiting their practical utility. Here, we fabricate an HMO/MXene/PSF adsorptive membrane, in which 2D MXene serves as the hydrogen bond interacting agent between H 1.33 Mn 1.67 O 4 (HMO) and polysulfone (PSF). Notably, MXene incorporation effectively mitigates Mn leaching due to the hydrogen bond interaction. Efficient lithium recovery from Sichuan Basin SGW is achieved, with a lithium adsorption capacity of 21.18 mg/g. After ten consecutive cycles of adsorption and desorption, the HMO/MXene/PSF membrane shows remarkable cyclic stability, with a negligible decrease in lithium adsorption capacity of merely 0.16 %. Filtration studies reveal that the membrane with a surface area of 12.56 cm 2 can effectively filter 160 mL of SGW. The stability of the membrane due to hydrogen bond interactions and the selective adsorption mechanism are further confirmed through DFT calculations. This work presents a novel concept for constructing a mixed matrix membrane for lithium extraction from SGW and is expected to inspire further efforts in developing LIS-based adsorbents for lithium recovery.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinran Wang,Xufeng Zang,Xin Wang,Wenjie Zhang,Yishan Fang,Bo Cui
The common detection methods of phoxim mostly rely on the output mode of single signal, which is easily disturbed by complex environmental media and causes errors. Herein, in order to improve the reliability of detection, we developed a dual-mode detection strategy based on nanozyme for the detection of phoxim. Firstly, manganese-nitrogen co-doped carbon nanozyme (Mn@NC) with peroxidase-like activity was synthesized by one-step pyrolysis, which was used to construct in the luminol-H 2 O 2 electrochemiluminescence (ECL) system with molecularly imprinted polymer (MIP) technology. Among them, Mn@NC can act as a co-reaction promoter to catalyze H 2 O 2 to produce large amounts of hydroxyl radicals ( • OH), thereby significantly amplifying the cathode signal of luminol and improving the stability of the signal. Benefiting from the specific selection of phoxim by MIP, this molecularly imprinted electrochemiluminescence (MIECL) mode has considerable sensitivity and selectivity, with a low limit of detection (LOD) of 0.011 ng/mL (S/N = 3). Moreover, the • OH produced by Mn@NC-catalyzed H 2 O 2 oxidized the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue oxidized TMB (oxTMB). Taking advantage of the fact that the simultaneous presence of acetylcholinesterase (AChE) and acetylthiocholine (ATCh) inhibited the activity of Mn@NC. A sensitive and simple colorimetric pesticide sensing platform was constructed by combining the nanozyme with the TMB-H 2 O 2 system to achieve the colorimetric detection of phoxim, with the LOD as low as 1.27 ng/mL. The dual-mode sensor was successfully applied to the determination of phoxim in agricultural products with satisfactory results, showing its great potential in the monitoring of food hazards.
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Advanced Optical Materials
·
2024
·
IF 8
Bin He,Bao Ke,Chengzhi Yang,Yijun Chen,Xianci Zhong,Weijian Li,Bingsuo Zou
The impact of magnetic coupling effects on the luminescence of 0D (zero-dimensional) perovskite materials doped with TM (transition metal) ions remains underexplored. This study synthesizes Mn 2+ -doped 0D Rb 4 CdCl 6 halide structures using a solvent-based method, with Rb + ions systematically arranged around isolated [CdCl 6 ] 4− octahedra. The resulting Rb 4 Cd 1- x Mn x Cl 6 powder exhibits stable orange-red luminescence under UV (ultraviolet) excitation, achieving a PLQY (photoluminescence quantum yield) of 88.96%. The parent Rb 4 CdCl 6 is non-luminescent, but doping with Mn 2+ induces strong luminescence due to combined emissions from d-d transitions of Mn 2+ , weakly ferromagnetically coupled Mn 2+ pairs, and STEs (self-trapped excitons). Characterization via XRD (X-ray diffraction) and DFT (density functional theory) reveals that Mn 2+ doping occurs through both substitutional and interstitial processes, facilitating magnetic coupling. Raman spectroscopy identifies strong electron-phonon coupling at a phonon mode of 112 cm −1 , supporting STEs generation. Magnetic property analysis shows significant ferromagnetic coupling between Mn 2+ pairs and paramagnetic single Mn 2+ ions, enhancing luminescence. The material demonstrates remarkable structural and thermal stability, positioning Rb 4 Cd 1- x Mn x Cl 6 as a promising candidate for optoelectronic applications.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jinghang Sun,Zhongmin Fang,Xianfa Zhang,Linjie Li,Xiaodan Zhao
Advanced oxidation processes (AOPs) based on sulfite activation have been demonstrated to achieve cost-effective and highly efficient abatement of organic pollutants. In this work, the manganese-doped γ-Fe 2 O 3 catalyst (Mn-γ-Fe 2 O 3 ) is constructed based on the properties of Mn(II) with surface oxygen vacancy regulation and as an active site for sulfite activation. The increase of the Mn(II) doping ratio is favorable for the generation of surface oxygen vacancy with the content being enhanced more than two times when the Mn(II) doping ratio is 0.09 compared with that of γ-Fe 2 O 3 . The iohexol (IOX) abatement efficacy by sulfite activation with Mn-γ-Fe 2 O 3 is positively correlated with the oxygen vacancy content, in which SO 4 •− is the major free radical responsible for IOX degradation and HO • plays a secondary role. The presence of surface oxygen vacancy on the Mn-γ-Fe 2 O 3 exhibits low electrochemical resistance. The theoretical calculations support the enhancement of the electron transfer between Mn-γ-Fe 2 O 3 and sulfite with more negative adsorption energy and strong interaction of iron and manganese atoms. By analyzing the valence variation before and after the reaction, both > Mn(II) and > Fe(III) can participate in the acceleration of sulfite autoxidation process to generate radicals. Application of surface oxygen vacancy enriched Mn-γ-Fe 2 O 3 for sulfite activation exhibits good adaptability to different real water matrices and thus have some potential for practical applications.
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