ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Yuwei Shen,Dingchang Shi,Liangbin Liu,Fan Liao,Wenxiang Zhu,Mingwang Shao
The electrocatalytic activity is closely associated with the electronic structure of catalysts. Electron-deficient palladium (Pd) has been proved to show better oxygen reduction reaction performance than the electrophilic one due to the downshift of the d-band center. In this work, Pd nanoparticles are uniformly dispersed in F, N-doping graphene with the assistant of silicon nanowires and hydrofluoric acid (Pd/F, N-doping G). A strong interaction between the metal and doped-graphene leads to the electron-deficiency of the modified Pd, which is beneficial for obtaining proper adsorption energy of oxygen species. The as-prepared Pd/F, N-doping G-3 catalyst shows a four-electron oxygen reduction pathway with large half-wave potential of 0.87 V and high onset potential of 0.99 V in 0.1 M KOH. In addition, the Pd/F, N-doping G-3 based zinc-air battery exhibits an open potential of 1.40 V and a high power density of 229 mW·cm–2.
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高影响因子
Nano Energy
·
2024
·
IF 16.8
Jiarun Cheng,Chaojie Lyu,Hang Lei,Xueyan Li,Hongyue Zhu,Dan Zhou,Wenjie Mai,Yiming Liu
The regulatory mechanism of strong metal-support interaction (SMSI) is of great significance in improving the electrocatalytic performance for supported electrocatalysts. Here, PtNi alloy nanoparticles were deposited on N, F-codoped graphene-like carbon nanosheets (PtNi@NFGC) to construct a highly active interface for efficient methanol oxidation reaction (MOR), which solves the problems of high cost, poor activity and easy aggregation of Pt-based catalysts. Due to the high electrophilicity, F atoms doping into the carbon lattice can not only manipulate the electron structure and the state of the carbon skeleton, but also further trigger the stronger charge transfer between metal atoms and carbon support. Compared with single-doped PtNi@NGC, N, F-codoped PtNi@NFGC possesses a lower onset potential and methanol oxidation potential, higher methanol oxidation current and stronger CO tolerance. The results of the partial density of state (PDOS) simulation display that N, F-codoping promotes the electron transfer from Pt atoms to NFGC support, and leads to the d-band center shift upward, thus strengthening the oxidation degree of Pt active sites and increasing the composition of high-valent Pt x+ . In-situ Raman analysis and density functional theory (DFT) results expound that F atoms embedding observably enhances the adsorption energy of Pt active centers to *OH intermediates, which not only significantly improves MOR catalytic activity, but also achieves efficient methanol dehydrogenation and alleviates CO poisoning. This customization of metal-support interface interaction by heteroatom doping strategy opens up opportunities for designing efficient supported catalysts.
研究领域:
电化学
·
材料科学
·
催化反应
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DOI
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·
IF 6.2
Weijia Guo,Yutian Lu,Chongyang Zhang,Zhenxing Yue
Low-loss (high- Q × f , where Q = 1/tan δ ) dielectric ceramics can help achieve efficient microwave signal transmission and reduce heat generation. In the traditional Ca-Ln-Ti-O perovskite system (where Ln = rare earth) with the general formula of Ca 1– x Ln 2 x /3 TiO 3 (CST x ), the sharp decline in the Q × f value when x > 0.5 remains unexplained, posing a challenge for designing low-loss ceramics. In this study, CST x ceramics ( x ≤ 0.7) are synthesized via the solid-state reaction method, with a focus on their structure, defects, and broadband dielectric properties. A significant discrepancy between the Q × f values in the microwave and terahertz bands is found when x ≥ 0.6, suggesting the presence of additional loss mechanisms in the microwave band beyond ion displacement depolarization. Meanwhile, the low-frequency dielectric spectra show a weak dielectric relaxation in the low-temperature region, attributed to the partially ordered A -site vacancies. Therefore, this relaxation can act on the microwave frequency band at room temperature, resulting in a sharp decline in Q × f values. Such low-frequency and low-temperature dielectric relaxation should not be ignored in the research of microwave dielectric ceramics. These findings provide a crucial theoretical reference for developing low-loss microwave dielectric ceramics.
研究领域:
材料科学
·
电子工程
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DOI
高影响因子
PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2025
·
IF 4
Benshui Shu,Yuting Huang,Xinyi Xie,Cuiting Liu,Jintian Lin,Ying Xiao,Jingjing Zhang
Azadirachtin, a highly effective botanical pesticide, demonstrated notable biological activities against Spodoptera frugiperda , including mortality induction, growth and development inhibition, and antifeedant effects. Neuropeptide F (NPF) has been shown to play a role in various physiological processes in insects. Nonetheless, the functions of Sf- NPF1 in regulating food intake and antifeedant induction by azadirachtin in S. frugiperda larvae are yet to be elucidated. In this study, the antifeedant effects induced by 0.5 and 1.0 μg/g azadirachtin treatments in S. frugiperda larvae were evaluated. The sequence of Sf-NPF1 was identified with two transcript variants, and the proteins exhibit high identity with NPFs found in lepidopteran insects. Spatiotemporal expression analysis indicated that Sf-NPF1 exhibited high expression levels in first instar larvae and male adults, while the lowest expression was observed in non-feeding stages (egg and pupa stages). Besides, Sf-NPF1 also demonstrated notable expression in the midgut tissue of larvae. Azadirachtin treatments inhibited the expression of Sf-NPF1 in the larval midgut. The injection of the Sf- NPF1a mature peptide resulted in increased larval food intake and weight gain during a two-day treatment period. The antifeedant effect induced by 1.0 μg/g azadirachtin was also mitigated by the injection of Sf- NPF1a mature peptide. Our results indicated that Sf- NPF1 may serve as a positive regulator of food intake in S. frugiperda larvae, while azadirachtin could exert an antifeedant effect in larvae via inhibiting the expression of Sf-NPF1 . These findings establish a foundation for comprehending the mechanism behind the antifeedant effect induced by azadirachtin in insect larvae and provide a potential target for developing novel insecticides.
研究领域:
昆虫学
·
分子生物学
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农药科学
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生理学
·
生物化学
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DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Xiaojun Deng,Ping Zhou,Xiayan Yan,Renjin Xiong,Huaqin Kou,Wenhua Luo
To spare the use of OSDA and fluorides, for the sake of reducing cost and environmental conservation, a green and efficient synthesis recipe of low-silica CHA zeolites has been demonstrated, without using seeds or any other zeolites. The main factors that determine the formation of CHA zeolites have been investgated systemmatically, and several rules are obtained. (i) just considering simple memallic cations acting as the SDA , K + is indispensable for the formation of CHA framework, with noting that K + can also direct to MER topology. (ii) working as catalyst or minerization agent, OH − and F − function almost identically, but when the concentration of F − has reached a really high level or even only F − was used, CHA framework can not form because the intermediate fluoride complexes are inclined to produce small melecules of fluoride salts with morderate solubility over to enter the zeolite framework. (iii) at conditions of this work, the second stirring after the RT aging should be adopted since the contrastive tests have showed the benifits of the second stirring in making fewer or smaller impurity grains. (iv) when the concentration of K + is too high in reactive gels, with the other same conditions, MER over CHA framework is preferentially to form. (v) it is reasonable to consider the as-synthesized K-CHA materials can be used to research the novel “trapdoor” effect later. The authors considered the discussions and conclusions would offer some beneficial references to the green synthesis of zeolites and further understanding of the mechanism of hydrothermal treatment .
研究领域:
材料科学
·
环境化学
·
无机化学
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DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 23
·7894
·
IF 4.6
Jia-Bin Xiong,Yong-Juan Zhou,Shi-Hui Wang,Zhang-Qi Xiong,Zi-Kun Zhang,Shan-Shan Zhang,Chen-Kunlun Zhang,Chao-Fan Xu,Guo-Qun Liu
MOF (metal organic framework) materials have been used as functional materials in a number of fields due to their diverse spatial tunability, which produces rich porous structures with stable and continuous pores and a high specific surface area. A triboelectric nanogenerator can convert trace mechanical energy into electrical energy, and the application of MOF materials to triboelectric nanogenerators has been intensively studied. In this work, we report on two MOFs with similar spatial structures, and the modulation of the end microstructures was achieved using the difference in F content. The output performance of friction power generation increases with the increase in F content, and the obtained polyacidic ligand materials can be used to construct self-powered corrosion protection systems, which can effectively protect metallic materials from corrosion.Keywords:TENG;MOF;corrosion protection;cathodic protection
研究领域:
材料科学
·
能量转换
·
腐蚀工程
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DOI
PubMed
高影响因子
SURFACE & COATINGS TECHNOLOGY
·
2025
·
IF 6.1
Huaiyin Chen,Mingzu Xu,Jinbo Wang,Congxiang Li,Xiaolin Liu,Meihua Wu,Wei Wang,Longmin Liu,Yongzhao Li,Weihe Yu,Yuekun Lai,Weilong Cai
In this work, amphiphilic Janus F-SiO 2 -NH 2 particles were prepared through step-by-step modification of SiO 2 particles inlaid in and released from paraffin microspheres by fluorosilane and aminosilane respectively, and further modified waterborne epoxy (WEP) coating. The morphology, structure, composition, and surface wettability of the prepared particles as well as the mechanical properties and corrosion resistance were investigated. The results indicate that the modified coating gained the improved mechanical properties and anti-corrosion performance. Electrochemical impedance spectroscopy tests show that after immersion in 3.5 wt% NaCl solution for 15 days, the impedance modulus at low frequency of F-SiO 2 -NH 2 modified WEP coating was above 10 6 Ω∙cm 2 , two orders of magnitude higher than that of WEP coating. The amphiphilic Janus F-SiO 2 -NH 2 particles not only improved the interfacial compatibility and penetration resistance through the good dispersibility, hydrophobic groups and cross-linking with epoxy resin matrix, but also oriented adsorbed on steel surface to form protective hydrophobic layers. This work provides a simple design approach for constructing highly corrosion-resistant waterborne coatings, which has a certain promoting effect on the development of environmentally friendly high-performance anti-corrosion coatings.
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高影响因子
RSC Advances
·
2017
·Vol. 7
·期 7
·3949-3957
·
IF 3.108
Enjie Yu,Qilong Zhang,Nuoxin Xu,Hui Yang
In this study, self-assembly flower-like TiO2 (F-TiO2) particles with an average diameter of 400 nm are synthesized via a facile one-pot solvothermal method. P(VDF-HFP)-based composites with F-TiO2 particles of different volume ratio as fillers are prepared. Microstructure and thermal analyses confirm that F-TiO2 does not change the crystallization process of the polymer matrix, but disrupts the crystallization degree of P(VDF-HFP). Dielectric properties measured at various frequencies and temperatures indicate that the addition of the F-TiO2 fillers enhances the dielectric constant of the composites, while the dielectric loss and electric conductivity do not significantly increase. The dielectric permittivity of the polymer nanocomposites is enhanced by 200% over that of the P(VDF-HFP) matrix at a filler content of 20 vol% while maintaining a rather low dielectric loss (0.043 at 1 kHz). Especially, the F-TiO2/P(VDF-HFP) composites exhibit low electric conductivity (≤10−11 S cm−1) at low frequencies. All the improved performances suggest an easy method to fabricate nanocomposites having potential electrical applications.
研究领域:
材料科学
·
电气工程
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qiang Fu,Lei Lin,Tao Wu,Qinghua Zhang,Xianjie Wang,Lingling Xu,Jun Zhong,Lin Gu,Zhihua Zhang,Ping Xu,Bo Song
Precious metals (Pt, Ir, Ru, and so on) and related compounds usually demonstrate superb catalytic activity for electrochemical hydrogen production. However, scarcity and stability are still challenges for hydrogen evolution reaction, even for single-atomic-site electrocatalysts. Herein, a fluorine (F) doping strategy is proposed to enhance the strong metal–support interaction between the F-doped Ni3N support and the loaded ruthenium (Ru) species. Via synergistically modulating both the Ru loading amount and F doping concentration, outstanding HER activity was achieved in Ru@F–Ni3N with an overpotential (η) of 115 mV at 100 mA cm–2, superior to the benchmark Pt/C (η = 201 mV). Density functional theory simulation in combination with X-ray photoelectron spectra and X-ray absorption spectroscopy characterizations convincingly demonstrate that, with the strongest electronegativity, F doping could effectively stabilize Ru atoms doped in the F–Ni3N substrate and simultaneously reduce the H bonding strength, which accelerated the desorption of H2. These findings provide a facile strategy to modulate both catalytic activities and stabilities of heteroatom-loaded catalytic materials.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Lin An,Xin Han,Yaogang Li,Hongzhi Wang,Chengyi Hou,Qinghong Zhang
Tantalic oxide (Ta 2 O 5 ), as an excellent transition metal oxide photocatalyst , has been extensively studied on fluorination or self-doped for hydrogen production , while there is little research to combine the two modifications. In this work, surface fluorination self-doped Ta 2 O 5 nanoshuttles (FTNSs) photocatalyst is synthesized successfully by a modified one-step hydrothermal method . The test results show the presence of surface fluorine ions , Ta 4+ and oxygen vacancies in the sample. The FTNSs prepared by hydrothermal method under 180 °C for 24 h exhibits the highest hydrogen evolution rate (HER). The HER is 179.2 and 19.78 μmol h −1 g −1 in the absence of any co-catalyst under full-spectrum and simulated solar light, respectively, which is higher than that of the Ta 2 O 5 nanoshuttles without fluoride and the commercial Ta 2 O 5 . The higher HER can attribute to the existence of F, Ta 4+ and oxygen vacancies, which enhance the photogenerated carrier mobility and reduce the recombination.
研究领域:
材料科学
·
能源化学
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DOI
高影响因子
NANOTECHNOLOGY
·
2025
·Vol. 36
·期 14
·145601
·
IF 2.8
Xinyu Shi,Libo Deng,Lingna Sun,Qianling Zhang,Xiangzhong Ren,Yongliang Li
Manganese dioxide (MnO2) is recognized as a promising candidate for the oxygen evolution reaction (OER); however, its practical application is hindered by limited active sites and low electrical conductivity. Fluorine (F), known for its strong electron affinity and electronegativity, can modulate the surface electronic structure and physicochemical properties of catalysts. In this study, we synthesized MnO2 nanosheets and fluorine-doped MnO2 (F-MnO2) using simple hydrothermal and ion-exchange methods. We then assessed the influence of fluorine doping on the intrinsic OER activity and stability of these catalysts, as well as their underlying catalytic mechanisms. By manipulating the amount of fluorine introduced and the fluorination temperature, we explored the relationship between varying fluorine concentrations and OER performance. The experimental results show that F-MnO2 exhibits higher OER activity than pristine MnO2. At a current density of 10 mA cm–2, the overpotential required for F-MnO2 is merely 320 mV, substantially lower than that of pristine MnO2. This enhanced performance is ascribed to fluorine doping, which leads to an increased quantity of active Mn3+ centers and oxygen vacancies, along with an expanded electrochemically active surface area. Furthermore, F-MnO2 displays improved stability during the testing period. It maintains long-term stability for over 25 h, further corroborating the catalyst's excellent anti-oxidation and anti-corrosion properties in alkaline water electrolysis.
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Genyan Hao,Tao Zhao,Qiang Fang,Yunzhen Jia,Dandan Li,Dazhong Zhong,Jinping Li,Qiang Zhao
Exploring Earth-abundant and efficient electrocatalysts to replace Ir and Ru for the acidic oxygen evolution reaction (OER) is essential to reduce the cost of clean hydrogen production. Here, we show that trace amounts of electronegative non-metallic element fluorine (F)-doped Co3O4 nanoneedles improve the activity and stability of Co3O4. The F-doped Co3O4 nanoneedles supported on carbon paper (F-Co3O4/CP) exhibit an overpotential of 350 mV at 10 mA cm−2 for the acidic OER. In addition, their performance remains consistent after continuous operation for 80 h. Detailed investigations reveal that introducing an anion promotes the enrichment of OH on the surface of Co3O4 and prevents acid corrosion, thereby enhancing the intrinsic OER activity and stability. Theoretical calculations further indicate that F doping can effectively improve electron transfer and optimize the energy barrier for the formation of *OOH intermediates, which significantly improves OER performance. This study provides guidance for designing efficient and stable non-noble metal acidic water oxidation catalysts.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）