Heliyon
·
2024
·
IF 3.4
Yige Yan,Mohan Huang,Yongsheng Wang,Dawei He,Jiaqi He
Metal-organic frameworks (MOF) have been wildly synthesised and studied as electrode materials for supercapacitors, and bimetallic MOF of Ni and Co has been broadly studied to enhance both specific capacitance and stability of supercapacitors. Herein, a best performance (about 320 F/g) of Ni–Co bimetallic MOF was found in a uniform preparation condition by adjusting the ratio of Ni to Co. Then tiny third metal ion was introduced, and we found that the morphology of material has a significant change on the original basis. Furthermore, certain ions (Zn, Fe, Mn) introduced make a huge improvement in capacitance based on Ni–Co MOF of 320 F/g. The result shows that Zn–Ni–Co MOF, Fe–Ni–Co MOF and Mn–Ni–Co MOF perform specific capacitance of 1135 F/g, 870 F/g and 760F/g at 1 A/g, respectively. Meanwhile, the asymmetric supercapacitor (ASC) was constructed by Zn–Ni–Co MOF as positive electrode and active carbon (AC) as negative electrode. The Zn–Ni–Co MOF//AC ASC possesses a energy density of 58 Wh/kg at a power density of 775 W/kg. This research provides a new methods to regulate the morphology of MOF and a novel viewpoint for assembling high-performance, low-price, and eco-friendly green energy storage devices.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Yujia Li,Erping Bi
The metal-substituted goethite with addition of oxidants can effectively promote the degradation of antibiotics, but the usage of external agents restricts its application in in-situ remediation of antibiotic pollution. In this study, the metal-substituted goethites were prepared through co-precipitation method to investigate the effects of using manganese (Mn) or zinc (Zn) substitution alone on tetracycline (TC) degradation, combining with microscopic characterization and electrochemical methods. The results showed that the degradation rate constants of the first stage on Mn or Zn-substituted goethite were 0.299 h -1 and 0.498 h -1 , respectively, which were about 2 and 4 times of the pristine goethite (0.117 h -1 ). In the pH range of 4.0–9.0, Mn or Zn substitution significantly promoted TC degradation. Free and non-free radical pathways existed in the process of TC degradation by Mn or Zn-substituted goethite. The active site change and enhanced electron transfer ability were the main reasons for promoting degradation. Mn or Zn substitution increased oxygen vacancy (OV) content and promoted the electron transfer between TC and goethite. In Zn-substituted goethite, the coupling of OV and electron transfer produced free radicals, and in Mn-substituted goethite, the redox reaction induced mainly by electron transfer produces free radicals. This study reveals a new mechanism of efficient degradation of TC by iron minerals without the need for external oxidants, and the materials studied can be used for in-situ remediation of antibiotic contaminated groundwater.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2024
·
IF 2.2
Peng Wang,Jun-Fei Gu,Zhan Chen,Hao-Yue Ma,Xing-Chuan Li,Shuai Li,Xiang-Ya Xu,Ye Yuan,Cheng Chen,Zongkui Kou
Graphical This study develops a solid-state thermal (SST) synthesis method for the one-step preparation of MOF-derived Mn x @NC catalysts. Among these, the optimal catalyst (Mn 2.5 @NC) exhibits excellent activity, remarkable stability, and good recyclability for HMF oxidation to FDCA, achieving an FDCA yield of 94 % within 4 h at room temperature and maintaining its catalytic performance for five cycles without activity decay. Transforming the bio-based 5-hydroxymethylfurfural (HMF) into its oxidation product 2,5-furandicarboxylic acid (FDCA) offers an attractive route for synthesizing bioplastic monomers. However, significant challenges remain in developing efficient and stable non-precious metal catalysts. Here, we employed a solid-state thermal synthesis (SST) method to design and synthesize a series of metal-organic framework (MOF)-derived metal-nitrogen-carbon (M@NC) materials with gradient metal contents and low metal loadings, labeled as Mn x @NC, for converting HMF into FDCA through oxidation. Further investigations revealed that the amount of metal doping significantly influenced the catalyst structure, particularly in terms of defect quantity and specific surface area. The optimal catalyst, Mn 2.5 @NC, exhibited the largest specific surface area and the highest number of defects, achieving a 94 % FDCA yield within 4 h. Experimental results demonstrated that the recovered catalyst could be reintroduced into the reaction system and maintained selectivity comparable to that of the fresh catalyst for at least five cycles. Moreover, various characterizations of both fresh and recovered catalysts confirmed the great stability of Mn 2.5 @NC. This study provides advanced insights into the effective catalytic conversion of HMF to FDCA and highlights the importance of structural design and regulation in optimizing M@NC catalysts.
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高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Yumin Guo,Meiran Chen,Yanjie Wang,Xianglong Lu,Jingjing Wu,Xin Tang
Zinc-air batteries (ZABs) are an emerging energy technology that is environmentally friendly and has a high theoretical energy density, but their commercial application is limited by the oxygen reduction reaction (ORR). Silver-based nanocatalysts can effectively improve the ORR performance. In this paper, a nanoporous Ag–Mn (NP-AM) electrocatalyst with bicontinuous ligaments was prepared by a combination of the melt-spinning technique and dealloying method. Theoretical calculations show that Mn-doped Ag(111) indicates a shift of the d-band center toward the Fermi energy level, which improves the adsorption energy of the OOH and thus reduces the overpotential of the decision step in the ORR process. Among them, the electrocatalyst NP-AM-5 reached a half-wave potential of 0.81 V (vs reversible hydrogen electrode (RHE)) with a limiting current density of −5.63 mA cm–2. Tests showed that its ORR process almost completely undergoes 4e– transfer with higher conversion efficiency and also exhibits better long-term stability in comparison to commercial Pt/C electrocatalysts. When used as the cathode of a zinc-air battery, the maximum power density reaches 140 mW cm–2. The discharge voltage can be maintained at about 1.2 V for a long period of time by discharging at a constant current of 10 mA cm–2, and the specific capacity is calculated to be 724 mAh g–1.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiai Zhang,Rui Zhou,Ruohong Bi,Tong Wang,Qikui Fan,Hao Zhu,Zhimao Yang,Xiaofei Liu,Chuncai Kong
In this research work, flower-like MnCo 2 O 4.5 was synthesized by introducing a short-chain surfactant as a surface-active agent. This structure was utilized as a precursor, and a gas atmosphere pyrolytic deep reduction strategy was employed to construct a sea urchin-like catalyst (DTR-V o -MCO) with abundant oxygen vacancies. A series of characterizations were conducted to reveal the catalyst's microstructure and crystal phase composition. DTR-V o -MCO achieved more than 90% degradation of OTC within 10 min, and the efficiency was 1.5 times that of V p -MCO. The substantial presence of oxygen defects on the DTR-V o -MCO surface expedited charge transfer processes, resulting in a remarkable enhancement of PMS activation efficiency. Electron paramagnetic resonance spectroscopy (EPR) and radical quenching experiments indicated that the contributions of radicals to oxytetracycline (OTC) degradation were in the order of 1 O 2 > SO 4 •– > O 2 •– > • OH. 1 O 2 and SO 4 •– played dominant roles in OTC degradation. The possible oxytetracycline degradation pathways were proposed based on LC-MS analysis. In summary, this work presents an efficient method for a highly oxygen-deficient catalyst, expanding the application of binary transition metal materials in environmental remediation.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 7
·5814-5819
·
IF 2.324
Diao Chunli,Liu Hanxing,Hao Hua,Cao Minghe,Yao Zhonghua
Mn-doped barium strontium titanate Ba 0.4 Sr 0.6 TiO 3 - x mol%Mn ( x = 0, 1, 3 and 5; BSTM x ) thin films were deposited on Pt/Ti/SiO 2 /Si(100) substrates by spin-coating and annealed at 800 °C. X-ray diffraction patterns revealed that all the thin films were a typical cubic perovskite structure and no impurity peaks were observed. The effect of Mn doping on the ferroelectric properties and energy storage performance of the samples was investigated. The results showed that the recoverable energy storage density U rec and the difference ∆ P ( P max − P r ) between maximum polarization P max and remnant polarization P r firstly increased, then decreased with the increase of Mn doping amount. The optimized energy storage performance was obtained in Pt/BSTM3/Pt thin films: energy storage density of 8.48 J/cm 3 and energy storage efficiency of 42.4% at 1.63 MV/cm, electrical resistivity of 4.19 × 10 10 Ω cm and leakage current density of 7.77 × 10 −6 A/cm 2 at 163 kV/cm. Moreover, the effect of different top electrodes on energy storage performance was studied, which displayed that the energy density of Au/BSTM3/Pt films was higher than that of Pt/BSTM3/Pt films. The results indicated that Mn doping and Au electrodes could be effective ways to improve the energy storage properties of BST thin films.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Yangfan Xu,Tianze Han,Tingting Ji,Wenqian Luan,Ruiyang Zhao,Jishu Han,Lei Wang
Photocatalytic CO 2 reduction technology provides a promising approach to solve the energy and environmental problems. In this work, flower-like MnIn 2 S 4 microspheres were prepared by solvothermal method , and then calcined in air to obtain flower-like Mn doped In 2 O 3 (Mn:In 2 O 3 ) microspheres . Subsequently, Ni doped CdS (Cd 1-x Ni x S) nanocrystals were prepared and compounded with Mn doped In 2 O 3 to obtain Cd 1-x Ni x S/Mn:In 2 O 3 composite photocatalysts . It was found that Cd 0 · 96 Ni 0 · 04 S/Mn:In 2 O 3 had the best photocatalytic CO 2 reduction activity. The CO yield reached to 43.40 μmol g −1 in 3 h. The improved CO 2 reduction property were attributed to not only the increased light absorption capacity and the expanded surface area but also the enhanced charge separation efficiency that caused by the construction of Z-scheme heterostructure . The design and preparation of high-efficiency photocatalyst would be an effective way to promote the development of photocatalytic CO 2 reduction.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Wenjuan Dong,Zhuorong Fan,Ziyu Feng,Jia Shi,Xinyu Shi,Shengmei Song,Xiaojuan Gong,Wenting Liang
Phenolic compounds have increasingly serious damage to the environment, and it is imperative to develop new detection means for them. In this study, Mn-doped ZnS quantum dot (Mn/ZnS QDs) were synthesized and conjugated with horseradish peroxidase (HRP) via its ligand N-acetyl-L-cysteine (NAC) to form a bionanoconjugates with the phosphorescent response, named Mn/ZnS QDs-HRP. In the presence of a small amount of hydrogen peroxide, phenolic compounds can quench the phosphorescence of Mn/ZnS QDs-HRP, and the quenching type is speculated to be a synergistic effect of dynamic mechanism and internal filtration effect. Taking catechol as an experimental object, the phosphorescence signal of Mn/ZnS QDs-HRP showed a good linear correlation with the concentration of catechol, and the detection limit was 0.068 μM (S/N = 3). The strong anti-interference ability of room temperature phosphorescence endows the probe with excellent sensitivity, and the specific recognition performance of the enzyme makes it have excellent selectivity. Moreover, the probe exhibits good repeatability and stability. When used for actual sample detection, Mn/ZnS QDs-HRP provides stable and reliable quantification of catechol in different water samples with spiked recoveries of 92.3–104.4 %. This study provides a sensitive, convenient, and efficient phosphorescent response sensor for detecting phenolic compounds, which is of positive significance for environmental protection.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Cijun Shuai,Kangdong Wang,Shuping Peng,Jun Zan,Jiang Xiao,Shun Hu,Qi Zhong
CeO 2 nanozymes have garnered significant attention in chemodynamic therapy due to their peroxidase-like activity and ability to deplete glutathione. However, their catalytic efficiency is constrained by the low conversion rate of Ce 3+ /Ce 4+ . To overcome this limitation, the electron transfer was accelerated by introducing the transition metal Mn atom as a valence electron donor through lattice charge transfer. In detail, we introduced Ce 1-x Mn x O 2 into the poly-L-lactic acid (PLLA) scaffold fabricated by selective laser sintering. The conversion from Ce 3+ to Ce 4+ promoted the decomposition of H 2 O 2 within the tumor microenvironment to generate hydroxyl radicals with high oxidative activity, consequently inducing oxidative stress. The conversion from Ce 4+ to Ce 3+ depleted intracellular antioxidant glutathione, disrupting redox balance in tumor cells. This continuous redox cycle ultimately triggered apoptosis in tumor cells. Using a first-principles Hubbard-corrected approximate density-functional method, the analysis of the electron band structure revealed the presence of donor energy levels within the bandgap of Ce 1-x Mn x O 2 , enabling electron transfer channels around 0.645 eV. Electrochemical experiments confirmed that Ce 0.8 Mn 0.2 O 2 significantly reduced the activation overpotential from 0.907 V to 0.646 V, enhancing its redox capacity. As a result, the scaffold exhibited a threefold increase in tumor-killing rate. These findings highlight the immense potential of CeO 2 nanozymes in enhancing chemodynamic therapy for effective tumor treatment.
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ACS ES&T Water
·
2025
·
IF 4.3
Wen-Long Wang,Peng-Hui Liu,Jung-Hyun Son,Hang Su,Min-Yong Lee,Hong-Ying Hu,Qian-Yuan Wu,Uwe Hübner
The combination of ozonation and Mn(II) (O3/Mn(II)) is expected to synergistically eliminate recalcitrant organic micropollutants in water. However, the decay of O3, formation of •OH and reactive manganese species (RMnSs), and synergism in micropollutant degradation have not been comprehensively understood. Herein, the synergism of O3 and Mn(II) was observed to be pH-dependent. Compared to ozonation alone, O3/Mn(II) preferentially formed Mn(V and VI) and slightly increased •OH yield (from 0.22 to 0.30) at acidic pH 4–5, while it preferentially formed Mn(VII) and significantly increased OH yield (from 0.52 to 0.74) at circumneutral pH 6–7. Thereafter, O3/Mn(II) prominently increased RMnS exposure at acidic pH, while it dramatically diminished O3-exposurse to increase •OH exposure at circumneutral pH. As a result, O3/Mn(II) outperformed ozonation alone for the degradation of various O3-resistant micropollutants (3.7–7.9 times faster). For example, the RMnSs (82.7% contribution) and •OH (84.2% contribution) were the dominant contributors to the degradation of the isothiazolinone biocide (5-chloro-2-methyl-4-isothiazolin-3-one) at acidic and circumneutral pH, respectively. Mn(II) can enhance the removal of O3-resistant micropollutants in relatively clean waters (e.g., tap water), but its effectiveness was limited in more contaminated waters (e.g., WWTP effluent). These findings support the practice and pH optimization of the O3/Mn(II) in various water types.
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高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 13
·期 1
·399-408
·
IF 10.7
Qiangfeng Zhang,Shijie Xu,Haipeng Zhu,Zhao Chen,Libao Chen,Chunxiao Zhang,Weifeng Wei
High-voltage lithium-rich manganese-based oxides (LRMOs) are expected to become next-generation mainstream cathodes due to their higher voltage, higher specific capacity and lower cost. However, currently commercialized carbonate electrolytes still face the challenge of poor decomposition of solvents and lithium salts at high voltage, leading to serious interface side reactions and electrochemical performance degradation. Herein, we propose an interfacial chemical modification strategy based on the dual additives of fluoroethylene carbonate (FEC) and tris(trimethylsilyl)phosphate (TMSPa), to promote Li+ migration and ensure long-term cycling stability of LRMO-based batteries. Detailed characterization reveals that the dual additives FEC-TMSPa can promote the desolvation process of Li+ and reduce the adverse decomposition of electrolyte components by regulating the solvation structure of the electrolyte. Simultaneously, dual additives can facilitate the formation of a robust cathode electrolyte interphase (CEI)/solid electrolyte interphase (SEI) rich-in F/P/Si species, thereby reducing the interface side reactions, inhibiting the erosion of acidic substances on electrodes, and promoting the uniform deposition/stripping of Li+. As a result, the high-voltage LRMO-based batteries exhibit excellent rate performance and cycling stability, with a capacity retention of 82.36% after 500 cycles at 30 °C, and 86.9% after 150 cycles at a high-temperature of 55 °C, suggesting that the proposed strategy of synergistically regulating the interface chemistry with multiple additives is anticipated to facilitate the further application of high-voltage layered cathode materials.
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高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Ge Song,Yang Zheng,Minghua Zhou
The application of bimetallic catalysts in heterogeneous electro-Fenton (Hetero-EF) is limited due to its poor performance over a wide pH range. In this work, the Hetero-EF/sulfite process was constructed with FeMn@C as the catalyst to improve the degradation of pollutants under neutral pH. The removal efficiency of diclofenac (DCF) (97.8%) was significantly higher than that of Hetero-EF (15.0%) at pH 7, in which the degradation rate constant k was increased by 19.75 times. The existence and transformation process of various active species ( • OH, SO 4 •- , O 2 •- , and 1 O 2 ) in the process were verified by capture experiments and electron paramagnetic resonance (EPR) test. The possible DCF degradation pathway was also proposed. The introduction of sulfite could reduce Fe 3+ and Mn 3+ , promote the Fe(II)/Fe(III) and Mn(II)/Mn(III) cycles, strengthen the generation of active species, and thus promote the degradation of pollutants. The removal efficiency was still maintained 76.6% after five cycles. The Hetero-EF/sulfite process is a simple, feasible, and efficient method to degrade pollutants, which has a broad application prospect.
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