JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Ruipeng Yuan,Jinyu Zhao,Xu Chen,Xiaoming Qiu,Xiaomin Wang
Cobalt-nitrogen-carbon (CoN x C) materials are regarded as promising low-cost electrocatalysts for the oxygen reduction reaction (ORR). However, their susceptibility to deactivation and poor stability in acidic media limits their practical applications. In this study, we develop cobalt (Co) and manganese (Mn) embedded in nitrogen-doped carbon (CoMnN x C) dual-site catalysts by incorporating Mn into CoN x C and leverage a synergistic dual-catalysis strategy to optimize both activity and stability. The dynamic evolution of *OOH intermediate on the catalyst surface is monitored via in situ Raman spectroscopy, confirming that Mn introduction modulates the reaction pathway. Due to electron transfer from Mn to the Co-N x center in CoMnN x C, *OOH activation on the surface is enhanced, and the two-electron ORR process is inhibited. Consequently, the CoMnN x C catalyst exhibits excellent ORR activity (E 1/2 = 0.76 V vs. reversible hydrogen electrode) and a very low hydrogen peroxide (H 2 O 2 ) yield (<2.9 %) in acidic electrolyte. Additionally, the dynamic evolution of *OH on the Mn-N x site confirms that Mn-N x can serve as a potential catalytic site for the hydrogen peroxide reduction reaction (HPRR), facilitating H 2 O 2 decomposition. Differential electrochemical mass spectrometry (DEMS) demonstrates that this parallel catalytic pathway effectively weaks the oxidative corrosion of H 2 O 2 on the carbon carrier. The results indicate that the negative half-wave potential shift of CoMnN x C catalysts in acidic electrolyte after 10,000 accelerated durability tests (ADT) is only 11 mV. The synergistic dual-catalytic strategy proposed in this work offers a novel approach for designing high-efficiency and stable transition metal-nitrogen-carbon catalysts.
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Surfaces and Interfaces
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2024
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IF 5.7
Ping Lu,Zixing Gu,Zihan Zhang,Huaneng Su,Qiang Ma,Chunsheng Li,Lei Wei,Qian Xu
The all-in-one E-fueled solar flow battery system that can be recharged with liquid fuel is a new type of power system. It can continuously convert solar energy into liquid fuel without relying on external power supply equipments. However, the interface between the photoanode and the electrolyte often exhibits unsteady behavior, resulting in poor performance of the system. In this work, the {201} facets are selected and the impact of two doping treatment strategies for TiO 2 {201} photoanode on the performance of the E-fueled solar flow battery system is systematically studied through the I-t curve, linear sweep voltammetry, Mott-Schottky plot. The results show that the un-biased photocharging current of bulk-doped TiO 2 can reach 2.7 mA·cm −2 in the battery system test, only relying on the self-built electric field at the interface, and the energy conversion efficiency approaches 2.67 %. In addition, the performance is analyzed by the combination of transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy and other characterizations, with the aim of distinguishing the effects of bulk- and surface-doped Mn and accurately revealing the mechanism of their influences from the outside to the inside. Finally, the optimization rules of the un-biased light charging mode of the system are explored.
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Journal of Water Process Engineering
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2024
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IF 6.3
Meijuan Gao,Hong Wei,Ruijie Teng,Junqi Song,Xuetong Huang,Guizhen Wang,Huaien Li
The Ni/Co/Mn ternary catalysts were fabricated through a one-step calcination process using the cathode material (CM) derived from spent lithium-ion batteries. The morphological and structural properties of the Ni/Co/Mn catalysts calcined at various temperatures (labeled as CM-450, CM-550 and CM-650) were characterized. CM-650 demonstrated the lowest concentration of metal leaching, excellent stability, and efficient activation performance for peroxymonosulfate (PMS) in the degradation of iopamidol (IPM). The catalytic activity of ternary CM-650 was obvious higher than the respective cathode material. Radical quenching experiments, electron paramagnetic resonance (EPR), and electrochemical characterization analysis indicated that both radical (·OH, SO 4 •− , ·O 2 − ) and non-radical pathways ( 1 O 2 , electron transfer) were involved in the CM-650/PMS system. The conversion between Ni(III)/Ni(II) and Co(III) /Co(II) as well as Mn(III)/Mn(II), Mn(IV)/Mn(III) redox couples on the surface of CM-650 facilitated the activation of PMS and a synergistic effect among Ni, Co and Mn existed. Liquid chromatography-mass spectrometry (LC-MS) and density functional theory (DFT) calculations were employed to analyze the degradation intermediates and reaction pathways of IPM. ECOSAR analysis indicated that some intermediates posed certain ecological risks. In summary, the one-step calcination of Ni/Co/Mn ternary catalysts exhibited a sustainable, cost-effective, and environmentally friendly approach for converting waste materials into valuable, high activating-performance materials.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Huating Huang,Weiqing Li,Xixi Chen,Zhiming Yang,Minggang Chen,Anhong Zhang,Chun He,Shuanghong Tian
The strong metal–support interaction (MSI) has been widely attributed to enhanced catalytic activity. However, this attribution might be wrong in catalytic ozonation, since MSI that is too strong might impede the activation of electron-poor ozone molecules. Herein, we reported a strategy to subtly modulate the Mn–O–Si interaction by intercalating the carbon film between the silica support and active manganese oxide. When using MnOx/0.5C/SiO2 with the moderate MSI as a catalyst in the catalytic ozonation of refractory paracetamol (PCM), 91.1 ± 2.4% of PCM was removed within 30 min, about 30% higher than that using the catalyst of MnOx/SiO2 with a strong MSI. Moreover, the reaction rate reached 8.01 × 10–2 min–1, 2.2 and 1.3 times that with MnOx/SiO2 and MnOx/1C/SiO2, respectively. Importantly, further integration of MnOx/0.5C/SiO2 into membrane filtration achieved high rejections of PCM (>94.3%) under various realistic water scenarios during a continuous 12 h operation, demonstrating strong resistance to environmental matrices interference. Experimental and theoretical evidence revealed that the moderate MSI resulted in the high dispersion of active MnOx nanoclusters in the size of 2.3–4.4 nm and promoted the adsorption of ozone over MnOx and its dissociation into surface *O, •OH, •O2–, and 1O2 for decontamination. As a constructive work, this study revealed the significance of MSI in catalytic ozonation and offered a simple regulation method for constructing active interfaces of metal-supported catalysts.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Haishuo Wang,Jie Zhang,Zhichun Li,Bin Shi,Shiyin Li,Heyong Huang
Microcystin-LR (MCLR) is a highly toxic pollutant widely distributed in eutrophic waters. The interplay between dissolved organic matter (DOM) and metal ions has been extensively reported; however, the impact of DOM-metal complexes on MCLR remains to be thoroughly studied. In this research, equilibrium dialysis was employed to study the kinetics and isotherms of MCLR adsorption by DOM, meanwhile the Density functional theory (DFT) calculations provided insights into the theoretical mechanisms of Fe(II)/Mn(II) involvement in the adsorption process. The adsorption kinetics revealed that the process is physicochemical, with chemisorption being the critical factor controlling the adsorption rate. The adsorption isotherms confirmed that Fe(II) alters the spatial arrangement of adsorption sites on the superficies of DOM, with the complexes of Fe(II) and DOM from the macrophyte-dominated regions of Lake Taihu (MDR-Fe(II)) showing the uppermost adsorption capacity of 6193.965 µg/g among all combinations. The influence of different cations (K + , Ca 2+ , Na + , Mg 2+ ) on the adsorption of MCLR to DOM is divergent, with metals either reducing MCLR adsorption through competition for adsorption sites or increasing it by forming ternary complexes. The pH decrease reduced the affinity of DOM to metal ions while simultaneously enhancing MCLR adsorption through changes in its ionization state. DFT calculations demonstrated that Fe(II)/Mn(II) reduces the resistance to interaction between functional groups on DOM and MCLR, with carboxyl-Fe(II)-carboxyl interactions showing the highest binding energy (ΔG = −7.253 eV). Overall, Fe(II)/Mn(II) enhances the adsorption of MCLR via altering the structure and surface electrostatic potential distribution of DOM. This research indicates that the ultimate fate of MCLR in aquatic ecosystems is affected by DOM and metal ions.
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RARE METALS
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2025
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IF 11
Dong Qi,Li Wen-Bin,Zhang Jian-Hua,Yang Hao-Fei,Wu Yu-Mei,Pei Jing-Jie,Huang Xing,Wang Jing-Jing,Li Xi-Fei
Layered V 2 O 5 ·H 2 O (vanadium pentoxide hydrate) is a highly promising cathode material for aqueous zinc-ion batteries owing to its large interlayer space, variable V valence states, and unique interlayer H 2 O. However, the low electronic conductivity and easily exfoliated lattice layers lead to its poor charge transport kinetics and lattice stability. In this regard, we develop a ternary transition metal ions pre-intercalation strategy, where ternary Ni/Mn/Cu cations are successfully pre-intercalated into V 2 O 5 ·H 2 O by one-step hydrothermal method. It is revealed that Mn cation activates the additional Mn 4+ /Mn 3+ redox reaction, and ternary Ni/Mn/Cu cations cause the strong ion column effect, induce the highest p-band center of O, and improve the electrical conductivity, thus simultaneously enhancing the lattice stability and charge transport kinetics. As a result, the energy density of 391 Wh kg −1 at 0.1 A g −1 and the high-rate capability with a capacity of 240 mAh g −1 at 3 A g −1 after 600 cycles are achieved. Besides, the electrochemical reaction mechanism is revealed to be H + intercalation at high potentials, and followed Zn 2+ intercalation at low potentials, and Zn 2+ intercalation contributes most of the capacity (> 65%) and H + intercalation promotes the optimization of electrochemical performance. Graphical abstract
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Materials Today Chemistry
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2025
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IF 6.7
Chengzhi Yang,Bao Ke,Qilin Wei,Biling Zheng,Yijun Chen,Weijian Li,Bingsuo Zou
Low-dimensional metal halides are promising photoelectric materials due to outstanding luminescence efficiency, diverse components and stability. Customizing and precisely adjusting their microscopic interactions and optical response is crucial for expanding their potential applications. Doping strategies, especially those involving transition metal (TM) ions with spins, have been widely employed to reach above target. In this study, two isomers of phenylenediamine were selected as cations to regulate the dimensions of two organic-inorganic hybrid cadmium halides with varied dimensionality through organic π-π stacking interaction, spin-spin coupling and electron-phonon coupling. In two-dimensional structures the phonon zone folding effect expands the electron-phonon coupling range, which can lead to magnetic polarons covering different layers with the multi-phonon coupling promotion, although local excitons are preferentially present in a polyhedral of one-dimensional or two-dimensional structures. The different binding energy and size of the magnetic polaron within a layer (chain) determine its temperature of the highest emission intensity and related PL efficiency. Moreover, the antiferromagnetic (AFM) coupling between layers (chains) can also affect the range and coefficient of electron-phonon coupling, thereby influencing the emission efficiency. Therefore, the magnetic coupling and electron-phonon interaction in varied structures contribute to the modulation of the spatial zone, binding energy and transition processes of the polaronic exciton states in low-dimensional metal halides, which holds great significance for further material designs, luminescence optimizations and applications.
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MICROCHEMICAL JOURNAL
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2025
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IF 5.1
Rong Hu,Gui-Xin Guo,Jun-An Chen,Qing Li
The development of dual-mode biosensors for the accurate detection of acid phosphatase (ACP) activity and the screening of its inhibitors is of vital importance in clinical diagnostics and environmental monitoring. In this work, we report the synthesis of Mn–Ce co-doped carbon dots (Mn&Ce@CDs) exhibiting both oxidase-mimetic catalytic activity and intrinsic fluorescence. The nanozymes efficiently catalyze the oxidation of colorless o -phenylenediamine (OPD) to produce a yellow chromogen, 2,3-diaminophenazine (DAP), characterized by a distinct absorption peak. Significantly, the excitation spectrum of DAP overlaps with the emission wavelength of Mn&Ce@CDs, resulting in an inner filter effect (IFE) that quenches the blue fluorescence of the carbon dots while simultaneously enhancing DAP's emission. This mechanism establishes a robust ratiometric fluorescence signal. The enzymatic hydrolysis of ascorbyl-2-phosphate by ACP yields ascorbic acid, which inhibits the nanozyme-catalyzed oxidation of OPD. Consequently, this leads to a decrease in DAP formation, diminishing both its characteristic absorption and the IFE-induced fluorescence quenching, thus producing a dual-signal response. Quantitative ACP detection exhibited a linear range of 0.5–15 U/L with limits of detection of 0.037 U/L in fluorescence mode and 0.49 U/L in colorimetric mode. The platform demonstrated high selectivity and reliability, showing recovery rates of 97.7–109.3 % (fluorescence) and 97.9–107.5 % (colorimetric) in spiked serum samples. Additionally, smartphone-based RGB analysis enables rapid on-site detection. The system was successfully applied for screening ACP inhibitors, with chlorpyrifos exhibiting IC 50 values of 50.45 μg/mL (fluorescence) and 43.77 μg/mL (colorimetric). This integrated dual-mode approach offers a powerful, reliable tool for clinical diagnostics and environmental assessment.
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DESALINATION
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2025
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IF 9.8
Songlin Yang,Wei Qin,Shijia Lu,Zheng Li,Chi Ma,Yafei Guo,Tianlong Deng
Rubidium (Rb), a critical rare alkali metal, is widely used in high-tech fields for its unique properties. With growing demand, liquid mineral resources (e.g., brines) require efficient green extraction. This study introduces a novel electrochemical ion exchange (EIE)-electrodialysis (ED) coupling technology for rubidium salt production. A manganese-based Prussian blue@carbon nanotube electrode enabled selective Rb + extraction via EIE, achieving 243.72 mg/g adsorption capacity and 97 % desorption efficiency. Batch tests and DFT calculations validated performance under varying conditions. In real brine, the system showed high selectivity ( α K Rb =206 and α Na Rb =521), reducing Rb + : Na + : K + from 1:258:610 to 1:0.49:2.96 via cyclic adsorption. Coupled ED concentrated a 9 L desorption solution to 450 mL in 90 min using alternating membranes, minimizing waste/emissions versus traditional evaporation. Evaporation yielded crude salts with 16.35 % Rb purity as in RbCl, achieving a brine-to-product breakthrough. This EIE-ED technology offers a selective, sustainable paradigm for rubidium enrichment from Salt Lakes, with industrial promise for rare metal extraction.
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JOURNAL OF THE INDIAN CHEMICAL SOCIETY
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2025
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IF 3.4
Honghui Teng,Meng Zhang,Hongxue Du,Yuanqi Fang,Mingyue Piao
Three-dimensional (3D) electrochemical oxidation has emerged as a promising advanced oxidation process for wastewater treatment, owing to its high efficiency, environmental compatibility, and operational advantages. In this study, we developed a novel Fe/Mn co-loaded activated carbon (Fe/Mn-AC) particle electrode for the electrochemical oxidation of ammonium nitrogen NH 4 + -N) in wastewater. The as-prepared catalyst was systematically characterized through multiple analytical techniques including SEM-EDS, XRD, FTIR, XPS, and BET surface area analysis. Post-impregnation, SEM revealed maintained surface smoothness but reduced pore sizes, while BET measurements confirmed decreased surface area (from 732.38 to 650.83 m 2 /g), pore diameter (from 2.6 to 2.18 nm), and pore volume (from 0.43 to 0.37 cm 3 /g). XRD and XPS analyses identified iron and manganese oxides (Fe 2 O 3 , Fe 3 O 4 , Mn 2 O 3 , Mn 3 O 4 ) as the active phases. FTIR spectra exhibited characteristic bands of O–H (3462 cm −1 ), C–O (1571 cm −1 ), and C–C (1384 cm −1 ) in both AC and Fe/Mn-AC, with observable intensity variations after metal loading. Under optimized conditions (pH = 7, applied voltage = 14 V, Fe/Mn loading = 1 %, initial NH 4 + -N concentration = 100 mg/L), the 3D electrochemical system achieved an NH 4 + -N removal efficiency of 87.64 % with an energy consumption of 6.2 kW h/kg NH4+-N after 8 h of treatment. Radical quenching experiments confirmed the in-situ generation of hydroxyl radicals and electrons during the electrochemical process. The degradation mechanism study revealed that NH 4 + -N was primarily removed through indirect electro-oxidation pathways, with N 2 identified as the dominant end product.
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TALANTA
·
2025
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IF 6.1
Xin Xu,Ting Ying,Zhanghuan Yang,Ze Zhang,Liang Hu,Tong Shen,Dejian Li,Rui Zhu,Dong Chang
The development of portable exosome detection platforms is crucial for noninvasive early diagnosis of lung cancer, particularly in resource-limited settings. Herein, we engineered a paper-based colorimetric biosensor utilizing a MnO 2 /CeO 2 heterojunction nanozyme for visual quantification of plasma exosomes. The heterojunction synergistically integrates the high surface area of CeO 2 (45.689 m 2 /g) with the nanorod shaped MnO 2 , generating an interfacial electron transfer pathway that enhances peroxidase-like activity by 1.77 and 5.87 fold (K m = 1.197 mM, V max = 0.884 M/min) compared to individual components. Molecular recognition was achieved through dual-target immobilization: exosome-specific aptamers and anti-CD63/FGG/FGB antibodies conjugated on a chitosan-modified cellulose substrate. A smartphone-based hue-saturation-value (HSV) analysis system embedded in the platform enabled rapid on-site screening within 15 min, followed by microplate scanning of suspected high-risk samples, achieving a detection range of 10 2 –10 8 particles/μL with an ultralow detection limit of ∼2 particles/μL. Integration of a logistic regression model incorporating CD63, FGG, and FGB absorbance values further improved classification robustness. Clinical validation using 194 plasma samples demonstrated exceptional diagnostic accuracy in discriminating malignant from benign pulmonary nodules (AUC = 0.996), with a 95 % confidence interval ranging from 0.797 to 1.05, with 98.51 % sensitivity and 95.52 % specificity. This work establishes a multimodal strategy combining heterojunction nanozyme catalysis, paper-based microfluidics, smartphone-assisted imaging, and machine learning, offering a scalable paradigm for liquid biopsy applications in primary healthcare.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Mingyu Chang,Jingcheng Lv,Lianhui Sun,Aihong Chen,Fengbo Zhang,Guangjian Fan,Zhanliang Liu,Jun Li,Hongliang Shen,Mingjun Shi,Yinong Niu,Ye Tian,Xijian Liu,Boyu Yang
Benign prostatic hyperplasia (BPH) presents a significant clinical challenge, with conventional therapies carrying substantial risks, including urinary retention, sexual dysfunction, and prolonged recovery. To address the urgent need for safer, ultra-minimally invasive alternatives, we developed a sonosensitizing nanoplatform using copper–manganese-doped mesoporous silica nanoparticles (Cu–Mn@SiO2) for ultrasound-induced sonodynamic therapy (SDT). Here, we demonstrate that this innovative strategy provides highly effective and precisely targeted therapy for BPH. In vitro studies revealed that Cu–Mn@SiO2-mediated SDT significantly amplified intracellular reactive oxygen species (ROS) generation, triggering oxeiptosis characterized by PGAM5 cleavage, mitochondrial membrane depolarization, and mitochondrial damage in both BPH-1 epithelial and WPMY-1 stromal cells. In a testosterone-induced BPH rat model, a Cu–Mn@SiO2-combined, localized SDT treatment resulted in a substantial 60% reduction in prostatic weight and a marked improvement in urinary function. Thermal imaging confirmed prostate-specific hyperthermia without affecting the surrounding tissues. Histopathology revealed reduced collagen deposition and restored glandular morphology with comprehensive biosafety assessments showing no systemic toxicity. By precisely inducing localized oxeiptosis within hyperplastic prostatic tissue via focused ultrasound activation, this Cu–Mn@SiO2-based nanoplatform represents a clinically translatable, ultra-minimally invasive therapeutic strategy offering a superior safety profile for BPH management.
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