MOLECULES
·
2025
·Vol. 30
·期 16
·3388
·
IF 4.6
Shefeng Li,Pengyi Zhao,Ziyang Liu,Chang Wang,Linling Wang,Siyu Ding
Microwave-assisted processing has shown tremendous promise in accelerating chemical reactions and reducing energy consumption through targeted dielectric heating. This study develops MOF-derived Mn-Co and Ce-Co oxide catalysts for energy-efficient benzene oxidation via microwave catalysis. The MnCo spinel oxides (particularly MnCo11-400) exhibit superior microwave absorption and catalytic activity due to enhanced oxygen mobility and tailored dielectric properties. Microwave irradiation enables rapid benzene mineralization over the MnCo11-400 catalyst, achieving 78% conversion at 30 W and complete conversion at 50 W, demonstrating exceptional energy efficiency at low power inputs. Microwaves significantly lower the reaction temperature compared to conventional thermal catalysis (ΔT = 100–250 °C). Stability tests confirm robustness over repeated power cycling (80% conversion retained after 3 × 1 h on/off cycles). Furthermore, an adsorption–microwave oxidation synergistic strategy is demonstrated: pre-adsorbed low-concentration benzene (1.15 mmol) at ambient temperature undergoes complete mineralization within 20 min under 30 W microwave irradiation. The intermittent microwave operation achieves equivalent benzene removal to continuous thermal processing while significantly reducing energy demand. This work establishes MOF-derived spinel oxides as high-performance microwave catalysts for low-temperature VOC abatement.
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RSC Advances
·
2024
·Vol. 14
·期 48
·35993-36004
·
IF 3.9
Jinlong Zhong,Xue feng Mao,Guanyu Wang,Heng Li,Junfang Li,Sijian Qu,Jianwei Zhao
Non-homogeneous ozone-catalyzed oxidation technology is one of the effective ways of treating wastewater, the core of which lies in the development of efficient ozone oxidation catalysts. This work proposes the design and synthesis of an efficient Cu/Mn/Ce multi-metal composite oxide catalyst by metal salt precursor mixing-direct granulation. The effect of metal doping on the catalyst properties was compared using Density function theory (DFT) calculations, and the Cu/Mn/Ce co-doping showed significant charge accumulation effect with a low ozonolysis energy barrier, which is more favorable for the generation of reactive oxygen species. The successful loading of the main active metal components, such as Mn, Cu, and Ce, was clarified by systematic characterization by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) and Brunauer–Emmett–Teller's test (BET), and the chemical oxygen demand (COD) removal could reach more than 60% for the simulated wastewater. The electron paramagnetic resonance (EPR) characterization clarified that the degradation of organic pollutants was mainly dominated by the combination of single-linear oxygen and superoxide radicals in the catalytic process, and the possible catalytic oxidation mechanism was proposed. This work advances the development of non-homogeneous ozone oxidation technology.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Jing Fan,Liang Guo,Fenhong Song
This study employed the hydrothermal method to dope Mn into Sn 3 O 4 , which was then combined with g-C 3 N 4 through calcination to prepare an II-type Mn-Sn 3 O 4 -x/CN composite photocatalyst. The impact of Mn-Sn 3 O 4 loading on the photocatalytic performance was discussed. The synthesized composite catalysts exhibited remarkable hydrogen production performance under visible light, with Mn-Sn 3 O 4 -10/CN demonstrating the highest performance. Characterization techniques confirmed the successful preparation of the catalysts, and the light absorption capacity, charge separation and transport efficiency of Mn-Sn 3 O 4 -10/CN are significantly improved compared to catalysts with other ratios. This study developed a Mn-Sn 3 O 4 -x/CN composite catalyst with high stability and good hydrogen production rate. It provides further directions for the research of g-C 3 N 4 -based composite catalysts.
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Energy & Environmental Science
·
2024
·Vol. 17
·期 11
·3807-3818
·
IF 32.4
Shenyang Xu,Zhefeng Chen,Wenguang Zhao,Wenju Ren,Chenxin Hou,Jiajie Liu,Wu Wang,Chong Yin,Xinghua Tan,Xiaobing Lou,Xiangming Yao,Zhihai Gao,Hao Liu,Lu Wang,Zuwei Yin,Bao Qiu,Bingwen Hu,Tianyi Li,Cheng Dong,Feng Pan,Mingjian Zhang
As commercial cathodes with the highest practical capacity, the structural nature of Li-rich Mn-based (LMR) cathodes, composite or solid solution, is still under debate. Due to the extreme structural similarity of two layered-phase components, namely, the monoclinic phase (C2/m) and rhombohedral phase (Rm), no single tool can resolve this concern alone. Herein, we combined multiple advanced techniques to comprehensively study the structural changes during synthesis of LMR cathodes from different aspects such as the elemental distribution, local structure, long-range structure, and short-range structure, revealing a clear process from the formation of two phases to the gradual phase fusion and eventually to a nearly solid solution. Particularly, X-ray pair distribution function (PDF) analysis combined with theoretical simulations reveals for the first time that the transition metal (TM)–TM distance increases with the progress of the phase fusion, which makes the short-range structural change in TM–TM atomic pairs an effective parameter for judging the extent of phase fusion. Eventually, excellent electrochemical performance was achieved by balancing capacity and cycling stability through adjusting the phase fusion to a medium extent in lithium and sodium two layered-phase components. This study establishes an approach to investigate the structural evolution in the complicated multiple-phase system and provides valuable insights into the design and optimization of cathodes by tuning the phase fusion extent.
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Jiajia Chen,Baobao Bai,Juan Lei,Peng Wang,Shuang Wang,Jinping Li
Mn 3 O 4 catalysts have shown great potentials for toluene catalytic oxidation for the spinel structure and weak metal oxygen bonds. In this work, Mn 3 O 4 and Mn 2 O 3 catalysts were obtained by using Mn-MOFs with different ligands as precursors. It was found that the reduction of hydroxyl groups in 2,5-dihydroxyterephthalic acid was favorable for the preparation of Mn 3 O 4 under the proper temperature range. The Mn 3 O 4 -MOF-74–300 catalyst exposed the highest Mn 3+ , O ads /O latt and reducing capacity. Herein, the Mn 3 O 4 -MOFs-74–300 catalyst exhibited excellent performance for toluene oxidation, which could achieve 90% toluene conversion at 218 ℃ (toluene concentration = 1000 ppm and SV = 20000 mL·g −1 ·h −1 ). Moreover, the Mn 3 O 4 -MOFs-74–300 catalyst exhibited high stability, circulation performance and water resistance in the catalytic test.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Huixian Xie,Liping Tan,Zhuo Yao,Jiaxiang Cui,Xiaokai Ding,Zuhao Zhang,Dong Luo,Zhan Lin
Li-rich Mn-based layered oxides are proposed to be candidates for high-energy Li-ion batteries. However, their large-scale production is still hampered by poor rate capability and severe voltage decay. It was mainly attributed to the irreversible oxygen loss, which induces transition metal ion migration, electrolyte consumption, and structural evolution. Herein, we propose an effective strategy of phosphorylation, in which the phosphate ion is induced to remove the surface labile oxygen. It urges the Li2MnO3 component to transform to the spinel-like structure and promotes the anionic redox process, thus facilitating lithium-ion diffusion and improving structural stability. As a result, the Li2MnO3 component is more prone to be activated, with the capacity increased by 18% in comparison with the pristine one. It also exhibits a superior capacity retention of 86.1% after 150 extended cycles and better rate performance delivering a capacity of 148.1 mA h g–1 even at 10 C. The effective phosphorylation opens a new way to tune anion redox chemistry and obtain structurally stable materials.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Zuo Wenhua,Liu Xiangsi,Qiu Jimin,Zhang Dexin,Xiao Zhumei,Xie Jisheng,Ren Fucheng,Wang Jinming,Li Yixiao,Ortiz Gregorio F.,Wen Wen,Wu Shunqing,Wang Ming-Sheng,Fu Riqiang,Yang Yong
Layered transition metal oxides are the most important cathode materials for Li/Na/K ion batteries. Suppressing undesirable phase transformations during charge-discharge processes is a critical and fundamental challenge towards the rational design of high-performance layered oxide cathodes. Here we report a shale-like Na x MnO 2 (S-NMO) electrode that is derived from a simple but effective water-mediated strategy. This strategy expands the Na + layer spacings of P2-type Na 0.67 MnO 2 and transforms the particles into accordion-like morphology. Therefore, the S-NMO electrode exhibits improved Na + mobility and near-zero-strain property during charge-discharge processes, which leads to outstanding rate capability (100 mAh g −1 at the operation time of 6 min) and cycling stability (>3000 cycles). In addition, the water-mediated strategy is feasible to other layered sodium oxides and the obtained S-NMO electrode has an excellent tolerance to humidity. This work demonstrates that engineering the spacings of alkali-metal layer is an effective strategy to stabilize the structure of layered transition metal oxides.
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JOURNAL OF ELECTRONIC MATERIALS
·
2021
·Vol. 50
·期 5
·2725-2737
·
IF 1.938
Zhou Junxiu,Wu Tianhao,Han Yinghui,Aryana Saman
Manganese and cerium (Mn-Ce) oxides were prepared under nitrogen and high-temperature oxidation via a bath precipitation method as materials for electrode assemblies in supercapacitors. The prepared Mn-Ce oxide composite was demonstrated to have a high specific capacitance of 163.7 F g −1 with 78.4% cyclic stability after 3000 cycles at a current density of 1 A g −1 . Electrochemical impedance spectroscopy confirms that MnO 2 improves the conductivity of CeO 2 . Results from XPS analysis suggest that the introduction of MnO 2 enhances the concentrations of oxygen vacancies. Finally, band structure, density of states and Mulliken population were calculated using density functional theory, and the findings are consistent with the experimental and characterization results. Because of their excellent performances, Mn-Ce bimetallic oxides are promising electrode materials for supercapacitors. Graphic Abstract
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JOURNAL OF MATERIALS CHEMISTRY
·
2011
·Vol. 21
·期 44
·17972-17977
·
IF 5.101
Pengtao Shao,Hongzhi Wang,Qinghong Zhang,Yaogang Li
Mn-doped ZnSe nanocrystals (Mn:ZnSe d-dots) that emit white light were synthesized in aqueous media in microfluidic reactors. White light emission from Mn:ZnSe d-dots was a result of combined emission of blue light (emission from non-coordinated surface selenium sites) and yellow light (4T1 → 6A1 emission from Mn2+ ions). Emission from non-coordinated surface selenium sites was realized by adjusting the ratio of the flow volumes of [Zn]/[Mn] and the mass of stabilizer added. Photoluminescence from the Mn:ZnSe d-dots was easily tuned from 580 to 602 nm by regulating flow volume. Under the optimal experimental conditions, Mn:ZnSe d-dots that emit white light with a quantum yield of about 10.2% were fabricated.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Lili Song,Chunlian Peng,Fan Yang,Lian Wang,Yinhua Jiang,Yuqiao Wang
The charge transport between layers of layered double hydroxide (LDH) with structural stability is generally considered as a key factor in restricting electrochemical performances. Herein, we report the surface spatial confinement effect on Mn–Co LDH@carbon dots (CDs) to enhance charge transfer and the stable structure for high-performance supercapacitors. The surface confined effect should be characterized as the charge transfer and interaction between Mn–Co LDH and CDs using density functional theory calculations. CDs can improve the density of states near the Fermi level to achieve an enhanced conductivity. The geometric structure can remain stable at room temperature within 200 fs by using ab initio molecular dynamics simulations. The two-electrode device gained the energy density of 79 W h kg–1 and a power density of 666 W kg–1 at 1 A g–1. This design concept will help to design, prepare, and assemble the high-efficiency and long-lifetime electrochemical energy storage devices based on various layered materials.
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ENERGY & FUELS
·
2020
·
IF 3.421
Chunhao Wang,Xiang Xu,Yang Guo,Fan Zhou,Hongyu Chen,Haoyang Li,Zheng Zeng,Liqing Li
The cobalt carbide (Co2C) innovatively prepared from Co–Mn layered double hydroxide (CoMn LDH) has been investigated and evaluated toward its alternative synthesis conditions and different catalytic performances. Along with various characterization techniques, the preparation basically contains four steps (synthesis of CoMn LDH, calcination, reduction, and crystallization) that transform CoMn LDH to CoMn spinel and then to Co2C. Catalyst evaluation toward toluene pyrolysis was conducted. The sample with Co2C exhibited almost 100% conversion rate of toluene, where the resulting hydrogen yield (∼1.8%) is 6 times more than that of the blank test by using silica sand (∼0.3%), realizing the full transfer of hydrogen element from toluene to hydrogen molecule. Furthermore, based on the textural analysis and density functional dispersion correction calculation, which theoretically explained the easy accessibility of toluene to the crystal surface of Co2C(001) with a relatively high adsorption energy (about −280 kJ mol–1), it suggested that Co2C may expand more extensive applications in the field of catalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Boying Wang,Hao Wang,Jiantao Wang,Chaolong Li,Feng Wang,Chunli Diao,Haiwu Zheng
Dielectric thin film capacitors are expected to be a promising candidate for high-performance energy storage devices due to their high power density, fast charge/discharge speed, and excellent stability. Nevertheless, it remains a challenging endeavor to develop dielectrics with excellent energy storage density comparable to that of commercial batteries. In this work, lead-free 0.8SrTiO 3 -0.2BiFeO 3 (0.8STO-0.2BFO) thin films with coexisting amorphous and nanocrystalline structure were prepared by a sol-gel method. The heat-treatment temperature was adjusted to form polar-nano regions, thereby modulate the breakdown strength and dielectric polarization, and increase the energy storage density. The electric potential, electric field, and current density of the films with different amorphous/crystalline volume fractions were evaluated by the finite element simulation to further verify that the proper crystallization can result in the improved polarization performance and increased breakdown strength of the films, which are beneficial to the enhancement of energy storage performance. Through structural tailoring, the 0.8STO-0.2BFO film annealed at 550 °C demonstrates the optimal energy storage properties with a giant discharge energy storage density of 65 J/cm 3 and high efficiency of 75% at room temperature. Simultaneously, a broad temperature stability (20–160 °C), superb operating frequency stability (20 Hz-2 kHz), and excellent fatigue endurance (6.3 ×10 5 ) are observed without appreciable degradation of the energy storage performance. The excellent energy storage performance indicates a widespread potential of 0.8STO-0.2BFO films in pulse power applications, such as consumer electronics, microelectronics, and medical devices .
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