SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Song Gao,Xinghao Wang,Xinhao Wang,Xiru Chen,Sijia Liang,Ziyan Zhou,Shuxia Xu,Yanfen Fang,Juan Gao,Cheng Gu
Aqueous trivalent manganese [Mn(III)], an important reactive intermediate, is ubiquitous in natural surface water containing humic acid (HA). However, the effect of low-molecular-weight organic acids (LMWOAs) on the formation, stability and reactivity of Mn(III) intermediate is still unknown. In this study, six LMWOAs, including oxalic acid (Oxa), salicylic acid (Sal), catechol (Cat), caffeic acid (Caf), gallic acid (Gal) and ethylene diamine tetraacetic acid (EDTA), were selected to investigate the effects of LMWOAs on the degradation of BPA induced by in situ formed Mn(III)-L in the HA/Mn(II) system under light irradiation. The chromophoric constituents of HA could absorb light radiation and generate superoxide radical to promote the oxidation of Mn(II) to form Mn(III), which was further involved in transformation of BPA. Our results implied that different LMWOAs did significantly impact on Mn(III) production and its degradation of BPA due to their different functional group. EDTA, Oxa and Sal extensively increased the Mn(III) concentration from 50 to 100 μM compared to the system without LMWOAs, following the order of EDTA > Oxa > Sal, and also enhanced the degradation of BPA with the similar patterns. In contrast, Cat, Caf and Gal had an inhibitory effect on the formation of Mn(III), which is likely because they consumed the superoxide radicals generated from irradiated HA, resulting in the inhibition of Mn(II) oxidation and further BPA removal. The product identification and theoretical calculation indicated that a single electron transfer process occurred between Mn(III)-L and BPA, forming BPA radicals and subsequent self-coupling products. Our results demonstrated that the LMWOAs with different structures could alter the cycling process of Mn via complexation and redox reactions, which would provide new implications for the removal of organic pollutants in surface water.
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高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Shiqi Tian,Yuwei Ma,Yuanyuan Xu,Yingzi Lin,Jun Ma,Gang Wen
Dissolved Mn(III), as a potent one-electron transfer oxidant, is ubiquitous in natural waters and sediments and actively involved in the transformation of organics in biogeochemical processes and water treatment. However, the important role of Mn(III) has long been overlooked because of its short life. This study was the first to investigate the performance of Mn(III) in organoarsenic transformation and to highlight the environmental implications. Both homogeneous and heterogeneous Mn(III)-based systems were effective to remove p -arsanilic acid ( p -ASA, 15 μ M) with degradation efficiency approaching 40.4 %–98.3 %. Two degradation pathways of p -ASA were proposed, in which As-C bond and amino group were vulnerable sites to Mn(III) attack, leading to the formation of more toxic arsenate (As(V)) and nitarsone. Through transforming organoarsenic to inorganic arsenic species, the removal efficiency of total arsenic and dissolved organics were enhanced to 65.1 %–95.5 % and 16.6 %–36.6 %, respectively, by post-treatment of coagulation or adsorption, accompanied with significant reduction of cytotoxicity and environmental risks. Particularly, polymeric ferric sulfate and granular activated alumina showed superior performance in the total As removal. Moreover, oxidation efficiency of Mn(III) was hardly affected by common cations and anions (e.g., Ca 2+ , Mg 2+ , NH 4 + , NO 3 ˉ, SO 4 ˉ), halide ions (e.g., Clˉ, Brˉ) and natural organic matter, showing high robustness for organoarsenic removal under complicated water matrices. Overall, this study shed light on the significance of Mn(III) to the fate of organoarsenics in manganese-rich environments, and demonstrated the promising potential of Mn(III)-based strategies to achieve targeted decontamination in water/wastewater purification.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jing-Rui Zhang,Fa-Qiang Zhong,Lu-Bing Zhong,Zheng-Jun Dong,Quan-Bao Zhao,Zhimin Ao,Darren Delai Sun,Jia-Cheng E. Yang,Yu-Ming Zheng
An unprecedented type of 3D porous millimetric ozonation catalyst confining Mn-Ce dual-atom sites in terracotta support (MCT) was hereby reported through a feasible interface oxygen-induced ordering strategy. The utilization of cerium tailored the electron/valence state of dual-atom sites through its oxyphilic 4 f orbitals, making MCT present excellent ozone catalysis to remove model recalcitrant fulvic-like acids. The TOC removal kinetics value by MCT is 2.71 and 3.68 times higher than those of catalysts confining single Mn and Ce sites, respectively. The optimized MCT exhibited robust reusability without any regeneration (above 87% of TOC removal for each cycle), and desirable removal for the biochemical effluent organics of landfill leachate, showcasing a potential of deeply purifying saline wastewater. The electron complementary effect of cerium in dual-atom sites accelerated the electron transfer for O 3 catalysis, thus promoting the formation of reactive radicals for pollutant degradation via a thermodynamically feasible surface-adsorbed oxygen pathway. This work highlights the importance of elaborately designing dual-atom metal sites to construct reusable monolithic ozonation catalysts with electron self-cycle function for advanced wastewater purification.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2024
·
IF 4.1
Kai Lin,Zuming He,Long Shen,Jiangbin Su,Zhengyi Huang,Yongmei Xia,Yong Wang
To address the issue of poor cycling performance and capacity of Mn-based Prussian Blue analogues (PBAs) as sodium ion battery cathodes due to the solubility of Mn ions, this study utilizes the strong chelating property of EDTA 2− with Mn ions to hydrothermally modify the sodium-rich monoclinic Na 1.75 Mn[ Fe ( CN ) 6 ] 0.94 ·2.25H 2 O synthesized under high salt conditions, in order to enhance its capacity and stability. The modified Na 1.93 Mn[Fe(CN) 6 ]•2·.38H 2 O exhibits a discharge capacity of 156.16 mAh/g at 10 mA g −1 (91.86 % of the theoretical capacity), it still retains the highest discharge capacity (70.23 mAh/g) after 500 cycles at 100 mA g −1 . Based on experimental analysis, the improvement in the electrochemical performance of PBAs was attributed to three main factors: (1) enhanced Na content; (2) suppression of defects; and (3) improved crystal structure.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·Vol. 30
·期 25
·e202400088
·
IF 3.9
Xin Li,Xin Lai,Qingquan Kong,Xuguang An,Jing Zhan,Xiaolei Li,Xiaonan Liu,Weitang Yao
P2-type layered manganese-based oxides have attracted considerable interest as economical, cathode materials with high energy density for sodium-ion batteries (SIBs). Despite their potential, these materials still face challenges related to sluggish kinetics and structural instability. In this study, a composite cathode material, Na 0.67 Ni 0.23 Mn 0.67 V 0.1 O 2 @Na 3 V 2 O 2 (PO 4 ) 2 F was developed by surface-coating P2-type Na 0.67 Ni 0.23 Mn 0.67 V 0.1 O 2 with a thin layer of Na 3 V 2 O 2 (PO 4 ) 2 F to enhance both the electrochemical sodium storage and material air stability. The optimized Na 0.67 Ni 0.23 Mn 0.67 V 0.1 O 2 @5wt %Na 3 V 2 O 2 (PO 4 ) 2 F exhibited a high discharge capacity of 176 mA h g −1 within the 1.5-4.1 V range at a low current density of 17 mA g −1 . At an increased current density of 850 mA g −1 within the same voltage window, it still delivered a substantial initial discharge capacity of 112 mAh g −1 . These findings validate the significant enhancement of ion diffusion capabilities and rate performance in the P2-type Na 0.67 Ni 0.33 Mn 0.67 O 2 material conferred by the composite cathode. Graphical We propose a composite cathode material, Na 0.67 Ni 0.23 Mn 0.67 V 0.1 O 2 @Na 3 V 2 O 2 (PO 4 ) 2 F, featuring synergistic modification through doping and coating. The optimized Na 0.67 Ni 0.23 Mn 0.67 V 0.1 O 2 @5wt %Na 3 V 2 O 2 (PO 4 ) 2 F exhibited a high discharge capacity of 176 mAh g −1 within the 1.5–4.1 V range at a low current density of 17 mA g −1 . At an increased current density of 850 mA g −1 within the same voltage window, it still delivered a substantial initial discharge capacity of 112 mAh g −1 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Bolong Zhao,Yonggang Sun,Guangsuo Yu,Min Xu,Juan Zhang,Duoning Zhao,Yulong Ma
Nitrogen doping plays a crucial role in activating the Fenton catalytic activity of transition metal oxides. However, the mechanism by which nitrogen doping sites influence the properties of these oxides remains unclear. We successfully incorporated nitrogen atoms into the internal lattice of MnFe 2 O 4 spinel through thermal activation and identified two major doping sites: interstitial nitrogen (N int ) and substitutional nitrogen (N sub ). Through in-situ DIRFTS experiments and DFT calculations, we proposed a unique mechanism. Both sites can effectively activate the catalytic activity of the oxides, but N sub is particularly effective in altering the electron distribution of Mn elements within the lattice. This alteration promotes the transformation of superoxide (•O 2 – /•OOH) to H 2 O 2 , thereby further enhancing catalytic activity. Compared to un-doped MnFe 2 O 4 , experimental results obtained using MnFe 2 O 4 N 0.4 as the catalyst demonstrated that the degradation rate constant of tetracycline in simulated wastewater increased from 0.0072 min −1 to 0.2745 min −1 . Furthermore, the degradation rate of tetracycline reached 98.7 %. For real wastewater experiments, the COD removal rate was 77.4 %, and the mineralization rate was 62.5 %. This study offers new insights into the design of nitrogen-doped transition metal oxide catalysts.
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TALANTA
·
2026
·
IF 6.7
Linying Cheng,Xiang Liu,Zixin Zhang,Jing Liu,Jianru Tang,Xiaohua Zhu,Youyu Zhang,Meiling Liu
Copper ions (Cu 2+ ) are essential micronutrients but become hazardous when accumulated in excess, necessitating reliable, sensitive, and field-deployable detection methods. Herein, we report a fluorescent Mn-based MOF nanozyme (Mn-TCPP) that exhibits intrinsic oxidase-like activity, capable of catalyzing the oxidation of non-fluorescent o -phenylenediamine (OPD) to fluorescent 2,3-diaminophenazine (DAP) with an emission peak at 560 nm, while the Mn-TCPP itself displays characteristic fluorescence at 655 nm. Upon exposure to Cu 2+ , the stronger affinity of Cu 2+ toward the porphyrinic TCPP ligand displaces Mn 2+ from the framework, forming Cu-TCPP. This metal-exchange process simultaneously quenches the 655 nm fluorescence of the MOF and attenuates its oxidase-mimicking activity, whereas free Cu 2+ in solution independently catalyzes OPD oxidation, further enhancing the 560 nm emission. Leveraging this dual-response mechanism, we develop a ratiometric fluorescence sensing strategy for Cu 2+ detection based on the intensity ratio F 560 /F 655 . The calibration curve follows a linear equation: F 560 /F 655 = 0.201x-0.001 (0.2-10 μM, R 2 = 0.985) and y = 0.002x+2.061 (10-100 μM, R 2 = 0.994) with the limit of detection (LOD) of 81 nM (S/N = 3). The sensor exhibits excellent selectivity over competing metal ions, and the method reliability is validated by standard addition recovery experiments in real water and rice samples. Furthermore, the Mn-TCPP nanozyme is embedded into an agarose hydrogel matrix, enabling visual, instrument-free monitoring of Cu 2+ contamination: increasing Cu 2+ concentrations induce a discernible fluorescence color transition from orange to yellow under 365 nm illumination. This work presents a tunable MOF platform that exploits competitive targets synchronous modulation of fluorescence and enzyme-mimicking activity, providing a robust, selective, and field-deployable ratiometric sensor for Cu 2+ .
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 28
·15176-15189
·
IF 3.9
Wu Zuhao,Wu Shengji,Han Zhongxi,Li Siyue,Wang Hui,Yin Haoyong,Liu Juanjuan,Zhou Jie
Cerium-based
composite oxides have been intensively investigated
for the elimination of elemental mercury (Hg 0 ) from natural
gas and flue gas. Because of distinct operational conditions, the
required types of active oxygen species in composite oxides differ
substantially between these two atmospheric environments. Nevertheless,
the diversity of oxygen species has led to considerable debate regarding
the active sites responsible for the Hg 0 removal. The exploration
of these oxygen species is essential as it directly guides the rational
design of active sites in sorbents. In this work, we designed and
synthesized sorbents with different oxygen species and systematically
investigated the contributions of these oxygen species in the Hg 0 removal reaction. Cu–Mn–Ce (CMC) composite
oxides were successfully prepared by the coprecipitation method. Characterization
results indicate that the incorporation of Cu and Mn ions into the
CeO 2 lattice indeed significantly increases the concentration
of oxygen vacancies and releasable lattice oxygen. The Hg 0 removal efficiencies of CMC for natural gas and flue gas can be
maintained above 90.0% and 99.0%, respectively, even under a high
gas hourly space velocity of 480,000 h –1 . Furthermore,
CMC exhibits superior cyclic stability and high SO 2 resistance
for Hg 0 removal. Combined with the results from adsorption
tests and characterization, it can be concluded that the surface-active
oxygen species determine the catalytic oxidation and adsorption efficiency
of Hg 0 , while the releasable lattice oxygen species ensure
the continuous supply of active oxygen under extremely oxygen-deficient
conditions.
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MICROCHIMICA ACTA
·
2026
·Vol. 193
·期 10
·693
·
IF 5.4
Li Sirui,Wang Shanshan,Chang Guorui,Yang Yaoxing,Feng Hui,Xue Haoqian,Zhang Li,Luo Manlin,Liu Jing,Li Bowen,Xu Shuxia
To enable rapid and reliable on-site monitoring of organophosphorus pesticides a novel portable dual-mode biosensor has been developed which integrates electrochemical and colorimetric detection into a single freeze-dried bioactive capsule. This innovative design supports instrument-free operation and provides dual-signal cross-validation. The sensor is based on a newly synthesized Mn/Ce bimetallic metal-organic framework (MOF) nanozyme with high oxidase-like activity, co-immobilized with acid phosphatase (ACP) within a mannitol- and sucrose-stabilized lyophilized capsule to ensure long-term stability and field readiness. In the presence of malathion, the pesticide selectively inhibits ACP, thereby restoring the MOF's catalytic activity and enabling the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB). The resulting signal is detected both visually and through chronoamperometry after conversion to a yellow diimine product. This approach achieves a wide linear detection range of 1–2000 nM and an exceptionally low detection limit of 0.06 nM for malathion, along with high accuracy evidenced by recoveries of 93.31%-104.03% in real water samples. This work establishes a field-deployable and user-friendly sensing platform that combines innovative material design with integrated dual-mode detection, offering a robust and practical strategy for on-site environmental monitoring. Graphical
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Mining Metallurgy & Exploration
·
2026
·
IF 2.5
Wang Guangdong,Bai Ziyang,Li Maohui,Mao Xishan,Yu Jie,Su Chang,Hu Wenwen,Ma Bo,Sun Wenzhou,Lu Youjun
In response to the limitations of the traditional acid leaching process in terms of environmental impact and safety, this study developed a ternary mixed acid system (hydrochloric acid - oxalic acid - citric acid) without the use of hydrofluoric acid and nitric acid. The influence of three process parameters, namely, the concentration of the mixed acids, the liquid-solid ratio, the acid leaching temperature, and the acid leaching time, on the removal efficiency of impurities such as Fe, Mn, Al, K, and Na in quartz sand was systematically investigated. The experimental results revealed that the optimal acid leaching conditions were a hydrochloric acid concentration of 4.5 mol·L − 1 , an oxalic acid concentration of 0.03 mol·L − 1 , a citric acid concentration of 0.04 mol·L − 1 , a liquid-solid ratio (mass ratio) of 5:1, a constant temperature of 60 ℃, and a holding time of 3 h. Under these conditions, the removal rates of Fe, Mn, and Al reached 89.2%, 71.0%, and 60.1%, respectively. Moreover, K and Na were also removed to a certain extent, with removal rates of 39.6% and 25.5%, respectively. Mechanistic analysis revealed that in the ternary mixed acid system, hydrochloric acid provides an acidic environment, and the combination of oxalic acid and citric acid synergistically promotes the dissolution of impurities through complexation, reducing impurities on the surface of quartz sand, improving the cleanliness, and forming micro-porous structures. Compared with the traditional hydrogen fluoride-nitric acid leaching process, the fluorine-free ternary mixed acid system proposed in this study has a similar or even better removal efficiency for impurities such as Fe and avoids the environmental and safety risks associated with hydrogen fluoride. This system can achieve the simultaneous removal of various impurities in quartz sand under normal pressure and medium-low-temperature conditions, providing a new technical path for the development of quartz sand purification technology for safety and environmental protection.
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高影响因子
MICROCHEMICAL JOURNAL
·
2026
·
IF 5.2
Wen Qing Jia,Ting Ting Li,Jian Bing Li,Zhen Chen,Hui Xi Li,Lei Han
It is a pressing necessity to establish a valid approach for precise and sensitive monitoring of the acetylcholinesterase (AChE) activity and its inhibitor, organophosphorus pesticides (OPs), for public health and food safety. Herein, a dual-mode colorimetric sensor was designed for sensitive and accurate sensing of AChE and OPs based on Mn metal-organic gels (Mn-MOGs)-derived multifunctional nanozyme. The nanozyme was synthesized by pyrolyzing the Mn-MOGs, which show superior oxidase (OXD)-like and laccase (LAC)-like activities. It can catalyze the 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation into blue TMB (oxTMB) and 2,4-dichlorophenol to generate the red quinone imine (QI). The OXD-like and LAC-like activities can be inhibited by the thiocholine generated from AChE hydrolysis of acetylthiocholine (ATCh), causing a significant reduction in the absorption of oxTMB and QI. OPs can restrain the AChE activity, which prevents the hydrolysis of ATCh, causing the recovery of absorption of oxTMB and QI. Thus, a dual-mode colorimetric sensor was designed for sensing of AChE and OPs. Moreover, this sensor was also utilized to detect OPs in real samples with satisfactory results. This study not only provides a valid way for sensitive and accurate monitoring of AChE and OPs but also affords new insights for designing multifunctional nanozymes used to develop multimodal sensors.
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ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Miaomiao Zhang,Zhen Dai,Yongqi Wang,Xuelei Li,Zhihui Xu,Qingwen Li,Aruuhan Bayaguud
LRNM/LIC delivers 253.4 mAh g⁻ 1 at 0.1 C, outperforming LRNM/LSPSC (168.5 mAh g⁻ 1 ). • LIC forms stable In 2 O 3 passivation layer, but LSPSC has irreversible side reactions. • VGCF enables LRNM/LIC/VGCF to retain 98.72% capacity after 100 cycles at 0.2 C. Cobalt-free lithium-rich manganese-based oxides have emerged as promising cathode materials for all-solid-state lithium batteries (ASSLBs) owing to their high energy density and cost efficiency. This study systematically evaluates the interfacial compatibility between the 0.3Li 2 MnO 2 ·0.7LiNi 0.5 Mn 0.5 O 2 (LRNM) cathode and two representative solid electrolytes—namely, the sulfide electrolyte Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 (LSPSC) and the halide electrolyte Li 3 InCl 6 (LIC). The LRNM/LIC cathode achieves a high specific discharge capacity of 253.4 mAh g −1 at 0.1 C, which considerably exceeds that of the LRNM/LSPSC cathode (168.5 mAh g −1 ). Moreover, the LRNM/LIC cathode retains 87.32% of its initial capacity after 100 cycles at 0.5 C, indicating excellent cycling stability. The main reason for this improvement is that LSPSC undergoes irreversible side reactions at the interface with LRNM, generating substances such as SO 4 2- , SO 3 2- , and polysulfides. By contrast, LIC reacts with LRNM to form a stable interface layer (In 2 O 3 passivation layer), which inhibits continuous interfacial side reactions and substantially enhances interface stability. Furthermore, the influence of different conductive agents (vapor-grown carbon fiber (VGCF), carbon nanotubes, and acetylene black) on the conductivity and interfacial stability of LRNM/LIC is explored. Results indicate that the cycling stability of the LRNM/LIC/VGCF cathode is enhanced, achieving a capacity retention rate of 98.72% at 0.2 C after 100 cycles because VGCF forms a continuous three-dimensional conductive network. This study provides valuable insights for the development of low-cost LRNM-based ASSLBs with high energy density. Download: Download high-res image (227KB) Download: Download full-size image
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