APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Wang Song,Qianni Cheng,Li Han,Jiawei Ji,Yandi Cai,Wei Tan,Jingfang Sun,Changjin Tang,Lin Dong
Manganese oxide-based catalysts exhibit excellent low-temperature denitration efficiency, making them potential candidates for application. Herein, the relationship between reaction stability and phase structure for MnO 2 , Mn 2 O 3 and Mn 3 O 4 was disclosed. The NO conversion for Mn 2 O 3 drastically reduced after 120 h reaction, while minor decline was detected for MnO 2 and Mn 3 O 4 . Based on dedicate qualitative and quantitative analyses on the deposits over catalyst surface, deactivation trigged by ammonium nitrate (AN) deposition was confirmed. Different from penta-coordinated Mn 4+ on MnO 2 (110) and tri-coordinated Mn 2+ , penta-coordinated Mn 4+ on Mn 3 O 4 (101), the unique tetra-coordinated Mn 3+ on Mn 2 O 3 (200) could stabilize the nitrates and make it difficult to be removed via decomposition or reaction and accumulate continuously, which resulted in the significant deactivation. This research could not only unveil the poisoning mechanism of MnO x based catalysts, but also provide new insights into the relationship between the catalytic stability and surface Mn-O microstructure.
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TALANTA
·
2025
·
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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ELECTROCHIMICA ACTA
·
2025
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IF 5.6
Dandan Han,Jialin Geng,Jingze Luan,Weiwei Jian,Lin Wu
Manganese-based oxides are promising cathodes for aqueous zinc-ion batteries but often suffer from structural instability, manganese dissolution, and poor conductivity. Herein, we propose a "dual-network synergistic construction" strategy through the in-situ derivation of a metal–organic framework to concurrently address these challenges. This strategy ingeniously constructs an oxygen-deficient network and a conductive carbon network within a hierarchical Mn₂O₃/C composite (O d -Mn₂O₃/C-400). The formed interfacial Mn–O–C bonds effectively enhance structural integrity and regulate the concentration of oxygen vacancies. As a cathode for aqueous zinc-ion batteries, the O d -Mn₂O₃/C-400 composite demonstrates exceptional electrochemical performance, delivering a remarkable specific capacity of 425 mAh·g⁻¹ at 3 A·g⁻¹. More importantly, it exhibits outstanding long-term cyclability, retaining 87.67% of its capacity (174 mAh·g⁻¹) after 5,000 cycles at a high current density of 5 A·g⁻¹. When configured into a zinc-ion hybrid supercapacitor (O d -Mn₂O₃/C-400//AC), the device achieves a high energy density of 119 Wh·kg⁻¹ at 189 W·kg⁻¹, and maintains 78.6% capacity retention with 97.5% Coulombic efficiency over 3,000 cycles. This work provides an effective material design paradigm for developing high-performance manganese-based electrodes for advanced energy storage systems.
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ACS Applied Materials & Interfaces
·
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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Advanced Energy Materials
·
2025
·Vol. 15
·期 34
·2502226
·
IF 26
Mengting Guo,Changping Wang,Yize Niu,Mingyue Ruan,Dong Yang,Fei Wang,Haonan Wang,Nankai Wang,Ying Jiang,Tianyi Li,Yan He,Qiang Li
The high-voltage spinel LiNi 0.5 Mn 1.5 O 4 (LNMO) is a promising cathode material for lithium-ion batteries due to its high energy and power densities, excellent thermal stability, low cost, and environmental benignity. However, the presence of Mn 3+ induces Jahn─Teller (J─T) distortion, leading to Mn─O bond elongation, lattice stress, and degradation of both structural and electrochemical stability during cycling. To address this,a bond-length engineering strategy is proposed by co-doping Fe at the Mn 16d sites and Sb at the vacant 16c positions to suppress the J─T effect and stabilize the crystal structure. Electron paramagnetic resonance (EPR), in situ X-ray diffraction (XRD), and density functional theory (DFT) calculations confirm that the Mn─O bond regulation strategy effectively mitigates MnO 6 octahedral distortion, reduces phase transitions, and enhances structural robustness. Moreover, Sb incorporation expands the lattice, facilitating Li + diffusion. As a result, the optimized FeSb-LNMO delivers remarkable electrochemical performance, retaining 98% of its initial capacity after 200 cycles at 1C, and achieving 85.6% capacity retention over 1000 cycles at 5C. This work introduces a novel bond-length engineering approach via multi-site doping to overcome degradation in high-voltage LNMO, enabling ultra-fast charging and long-term cycling stability.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
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IF 3.9
Xuechun Li,Ze Zhang,Yang Xu,Rongxin Xia,Yuxiang Mao,Jun Cheng
For improving the activity of low-cost non-noble metal catalysts for the oxygen evolution reaction (OER) in acidic water electrolysis, a strategy was proposed to construct atomic Mn–O–Co asymmetric units within Co3O4 to form a directional built-in electric field. Mn-doped Co3O4 catalysts (MnxCo3–xO4) were synthesized via a hydrothermal-calcination method. The computational results indicated that Mn selectively occupied the octahedral Co site, forming a directional electron transfer pathway from Mn to Co, which effectively modulated the electronic structure of both Co and O. In situ Raman spectroscopy proved that the Mn–O–Co structure accelerated the efficient conversion of oxygen-containing intermediates. DFT calculations indicated that the Mn–O–Co directional built-in electric field facilitated H2O polarization via enhancing hydrogen bonding and, by optimizing the *OOH adsorption structure, lowered the OER rate-determining step barrier by 0.05 eV. The asymmetric Mn–O–Co coordination structure lowered the p-band center of the O atom by ∼0.1 eV atom, which passivated lattice-O to improve lattice stability. XPS revealed that the Mn0.6Co2.4O4 material had the maximum built-in potential. The electrochemical testing indicated that it exhibited an overpotential of only 243 mV at a current density of 10 mA cm–2 and maintained stability for over 80 h.
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DYES AND PIGMENTS
·
2019
·
IF 4.018
Xiuquan Xu,Songmei Wang,Tongjie Hu,Xiaofeng Yu,Jiapeng Wang,Chao Jia
Co-doping has been proven to significantly enhance the photocatalytic performance of g-C 3 N 4 . Herein, Mn and O co-doped g-C 3 N 4 (Mn/O-CN) composites were constructed for the first time by a simple one-pot calcining route. The systematic characterization results of XRD , FT-IR, TEM-EDS, XPS and DRS revealed that the Mn and O elements were co-doped into the CN framework successfully as Mn 3+ / 4+ and n-π* conjugate forms, respectively. The as-prepared Mn/O-CN-2 achieved the highest visible-light-driven degradation rate constant of 0.0290 and 0.0267 min −1 for degradation of Malachite green (MG) and Amido black 10B (AB 10B), which were about 5.09 and 5.45 folds higher than that of pristine CN, respectively. The improved photocatalytic degradation property of Mn/O-CN were mainly benefited from the extended visible light utilization, the enlarged specific surface area, and the accelerated separation and transfer of photo-induced charge carriers, which were all induced by the synergistic effects of Mn and O co-doped. Finally, the active species capturing experiments proved that the superoxide radicals (·O 2 − ) and holes (h + ) acted as the predominant roles in the photocatalytic degradation process .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xi Chen,Xiaoyan Wang,Ziliang Jia,Chao Yang,Zhihong Liu,Yuexing Wei,Mengxue Wang,Meisheng Liang
K-doped Mn–Ce solid solution catalysts were synthesized using a combination of coprecipitation and hydrothermal methods, demonstrating excellent performance in benzene oxidation. The catalyst K 1 Ce 5 Mn 5 exhibited comparable activity to noble metal catalysts, achieving a 90 % benzene conversion at approximately 194 ℃. Durable tests under dry and moist conditions revealed that the catalyst could maintain its activity for 50 h at 218 ℃ and 236 ℃, respectively. Characterization results indicated that the catalyst’s enhanced activity resulted from the weakened Mn–O bonding caused by the introduction of K + , facilitating the activation of oxygen and its involvement in the reaction. CeO x , the main crystalline phase of Mn–Ce solid solutions, provided abundant oxygen vacancies for capturing and activating oxygen molecules for the weakened Mn–O structures. This conclusion was further supported by partial density of state analysis from density functional theory computations, revealing that the introduction of K + weakened the orbital hybridization of Mn3d and O2p. Finally, in situ diffuse reflectance infrared Fourier-transform spectroscopy ( in situ DRIFTS) studies on Ce 5 Mn 5 and K 1 Ce 5 Mn 5 catalysts suggested that the introduction of K + promoted the conversion of adsorbed benzene. Furthermore, intermediate products were transformed more rapidly for K 1 Ce 5 Mn 5 compared to Ce 5 Mn 5 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Pengjia Sun,Jian Xiong,Ping Sun,Yingsen Fang,Hongxia Liu,Hui Liu,Bitao Xiong,Hui Wang,Xing'ao Li
Metal-doped g-C 3 N 4 materials have been extensively investigated and utilized as catalysts in the domain of wastewater treatment. In this study, additional O was introduced in Mn-doped g-C 3 N 4 (MCN) to synthesize Mn/O co-doped material (MOCN), and a new non-radical oxidation system of periodate (PI) activation with MOCN was established for degradation of pollutants. The results indicated that additional O doping can enhance the catalytic performance of MOCN. This was primarily demonstrated by the 3.5-fold increase in the degradation rate ( k ) of sulfadiazine (SDZ) by MOCN/PI system compared to MCN/PI one. Simultaneously, density functional theory (DFT) calculations have revealed that MOCN material exhibit a higher affinity for adsorbing PI (adsorption energy E ads = −4.992 eV), resulting in an elongation of the I-O bond length ( l I-O = 1.874 Å) and facilitating bond cleavage of PI to generate reactive active species (ROS). The reaction process was confirmed to be primarily driven by non-radical singlet oxygen ( 1 O 2 ), as demonstrated by electron paramagnetic resonance (EPR) and free radical quenching experiments. In addition, possible degradation pathways of SDZ were proposed based on the identified intermediate products and the calculated Fukui constants. The MOCN/PI catalytic system was highly efficient and environmentally friendly, with great potential for development in sewage treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhikang Deng,Yongfei Ma,Jinyao Zhu,Chenyu Zeng,Rui Mu,Yifan Liu,Ping Li,Zulin Zhang
Ferrate (Fe (VI)), as a versatile oxidizer, has been widely employed for water treatment. However, the rapid self-decomposition of Fe (VI) diminishes its practical application efficiency. In this study, a novel Mn-modified sludge biochar (MSBC) was synthesized for the first time to activate Fe (VI) and generate highly reactive Fe (IV)/Fe (V) for the rapid removal of sulfamethoxazole (SMX). The results showed that MSBC (0.10 g/L) effectively activated Fe (VI) (100 μM), and 87.39 % of SMX (10 μM) and 40.26 % of total organic carbon (TOC) were removed within 10 min. Notably, raising the solution pH (e.g., from 6.0 to 11.0) would result in decreasing the reactivity of Fe (VI) and a lower removal efficiency of SMX. The quenching, electron paramagnetic resonance and probe experiments suggested that •O 2 – and high-valent iron species (Fe (V)/Fe (IV)) were identified as the major contributions to the removal of SMX. The detailed activation sites of MSBC were –OH and Mn-O, as corroborated by density functional theory (DFT) calculation and characterization. These activation sites facilitated activation of Fe (VI) through efficient electron transfer . The Fukui index indicated that the N, S, and O atom of SMX were the primary attacked sites. Subsequently, five potential degradation pathways were proposed, with the cleavage of the S-N bond being the predominant one. The toxicity of these products was examined using ECOSAR program, revealing that main products showed low toxicity or non-toxicity. The Cl - , SO 4 2- , and NO 3 – had negligible effect on SMX degradation, although excessive concentrations of HCO 3 – and humic acid (HA) showed slightly inhibition. Additionally, the Fe (VI)/MSBC system also effectively removed 87.34 % of sulfadiazine (SDZ) and 93.91 % of sulfamethoxypyridazine (SMP). Overall, this study offered a practical and cost-effective approach for the activation of Fe (VI) and provided new insights to the degradation mechanism.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 20
·9528-9538
·
IF 9.931
Yali Weng,Zhenzhang Weng,Zhiyu Liang,Haixia Lyu,Zanyong Zhuang,Yan Yu
Intricate Fenton-like catalysts composed of mixed transition metal oxides (TMOs) frequently outperform simple TMOs in scavenging organic contaminants in wastewater. Nonetheless, their activity and/or reusability may sharply decline when abundant heavy metal ions in wastewater adsorb on the catalytic surface and passivate it. This study shows that mesoporous Ca–Mn mixed oxides prepared from a facile combination of Mn and an alkaline earth metal (i.e., Ca) (denoted as CaMnx) can readily overcome this problem. CaMnx without any additive (e.g., H2O2) was able to degrade organic contaminants (e.g., indigo carmine as a model contaminant) fast within 10 seconds, outperforming many other reported heterogeneous Fenton catalysts. Besides organics, the coexisting heavy metal ions (e.g., Cu2+ and Pb2+ as indicators) were also rapidly extracted. The outstanding performance was attributed to the synergy of Ca and Mn. CaO in CaMnx efficiently extracted metal ions via an ion exchange process, and MnOx generated abundant H2O2 and degraded the organics through an uncommon Fenton-like reaction. Therein, Cu species extracted by CaO catalyzed the decomposition of H2O2 into HO˙ radicals, speeding up the degradation reaction of the organics by 81 times. Benefiting from the gradual exposure of fresh Mn-sites protected by unreacted CaO, CaMnx without regeneration treatment maintained high efficiency in scavenging organics and heavy metal ions in cycling tests. CaMnx also showed great promise in treating complex water samples containing various heavy metal ions (e.g., Pb2+, Cu2+, Cd2+, Ag+, Zn2+ and Cr3+) and organic pollutants. The findings of this work enrich the rational design of related functional nanomaterials.
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