CHEMISTRY OF MATERIALS
·
2021
·
IF 9.811
Rong Wang,Qingfu Cai,Yunyang Zhu,Zhen Mi,Weijun Weng,Yicheng Liu,Jiaxun Wan,Jianhua Hu,Changchun Wang,Dong Yang,Jia Guo
Low-bandgap covalent organic frameworks (COFs) emerge as one of the most intriguing conjugated polymers for the development of electronic devices, while they often lack desirable electron affinity, thereby compromising the activity and stability in electrochemical transformation. Here, we report an n-type semiconducting two-dimensional (2D) COF, featuring a low bandgap (1.36 eV) and strong electron affinity (4.41 eV) as well as high crystallinity and porosity. The columnar stacking array of the benzobisthiadiazole moiety in 2D COFs plays a critical role in elevating electroactivity. It not only leads to the outstanding electrical conductivity and air stability upon reductive doping but also enables the boost of transformation kinetics for polysulfides on the separators of lithium–sulfur batteries causing a higher capacity and better cycling performance. The design strategy underpins the versatile development of electroactive COF materials with desirable electronic properties and promotes their applicability in energy storage and electronics.
研究领域:
材料科学
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能源存储
·
电子器件
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2020
·Vol. 11
·期 5
·1899-1913
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IF 5.721
Xiaojuan Bai,Cong Wang,Xuyu Wang,Tianqi Jia,Boxuan Sun,Shengqi Yang,Di Li,Junqi Li,Haiyan Li
Pharmaceutical and personal care products (PPCPs) are the most common hazardous environmental pollutants. Accordingly, PDI anion radicals are promising photocatalysts to transform PPCPs into non-toxic CO2 and H2O for their clean and efficient production. In the present work, we successfully synthesized an electrophilic PDI supramolecular (sEACA-PDI) compound with high electron affinity through a simple gelation process. Its electron affinity is contributed by its side chain, which enhances the electrophilicity of its perylene core edge. Consequently, sEACA-PDI tends to form anion radicals to provide a SOMO orbital, which allows sEACA-PDI to obtain electrons successively from organic pollutants. Its side chain also generates a polarized surface electric field, building an efficient pathway for electron transfer. The high flexibility and freedom of the sEACA-PDI side chain is beneficial to form a cluster structure. Numerous strongly electrophilic groups are exposed on the surface of sEACA-PDI, which further enhance its electron affinity. sEACA-PDI exhibited high photocatalytic degradation efficiency for classical organic pollutants via successive electrophilic attack, i.e. the k for DCF was 0.923 h−1. Also, sEACA-PDI achieved a k value of 0.351 h−1 for the degradation of MB. This work proposes a promising strategy for developing PDI anion radicals with high electron affinity, and also provides new insights for the treatment of environmental pollutants.
研究领域:
环境科学
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材料科学
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化学
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 24
·6951-6958
·
IF 5
Hui Zhang,Hui Han,Xuan Yang,Hongyu Ma,Zhifei Song,Xuqiang Ji
Active-site regeneration from d-band-center control engineering and electronic redistribution based on target-atom implantation is of enormous importance for efficient water oxidation. Here, low-activity Co catalytic sites of MgCo2O4 are reactivated for large-current (500 mA cm−2) and high-efficiency water oxidation through vanadium-atom electronic affinity synergy with Mg sites toward charge rearrangement around Co sites. Interestingly, very little vanadium (1.3 wt%) was implanted into MgCo2O4 to achieve atom-scale structure tailoring and electronic redistribution, reversing the Mg suppression effect on Co-site water oxidation of MgCo2O4. Vanadium-implantation-tailored MgCo2O4 coupled with MgO (V–MgCo2O4@MgO) exhibits significantly enhanced oxygen evolution reaction performance, with low overpotentials of 240 and 290 mV for 100 and 500 mA cm−2, respectively, in 1 M KOH. Operating at 500 mA cm−2, V–MgCo2O4@MgO has good catalytic stability for at least 20 hours. This work constructs excellent catalysts through atomic-level structural regulation and provides a new perspective for the principle of electronic-affinity synergy between V and Mg species toward Co–O bond optimization.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2012
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IF 2.421
Yunhui Sun,Huihui Chen,Duxia Cao,Zhiqiang Liu,Hongyu Chen,Yunlong Deng,Qi Fang
Three o -hydroxy chalcone derivatives 1–3 with carbazolyl ( 1 ), pyrene ( 2 ) and 4-nitrobenzene ( 3 ) as terminal group have been synthesized. Their crystal structures, photophysical properties in CH 3 CN and recognition properties for cyanide anions have also been examined. The research indicates that the stronger electroaffinity of the chalcone derivative's β-unit is beneficial to Michael reaction and can improve the response rate of the compound to cyanide anions. These compounds are found to be able to recognize cyanide anions with fluorescence turn-on response. Especially, compound 3 with strong electron accepting group exhibits remarkable response to cyanide anions in CH 3 CN H 2 O (1:1, v/v) solution with a ca. 40-fold intensity enhancement.
研究领域:
有机化学
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分析化学
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产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Xu Haocheng,Luo Rengan,Lv Haifeng,Liu Tianrui,Liao Qiaobo,Wang Yandong,Zhong Ziyan,Wu Xiaojun,Lei Jianping,Xi Kai
Electrochemiluminescence (ECL) is a light-emitting process in which the stability of electrochemically generated radicals has a crucial impact on the efficiency and durability of excited state generation. Therefore, deciphering a relationship between radical stability and ECL performance is highly appealing. In this work, three sp 2 carbon-conjugated covalent organic framework (COF) reticular nanoemitters compositing of same pyrene luminophores but different acrylonitrile linkers are designed with progressive electron affinities, named as CN-COF-1, 2, and 3. By precisely modulating the electron affinity of CN-COFs, a volcano relationship between ECL and radical stability is discovered with 78 folds enhancement in ECL intensity. Density functional theoretical calculations indicate that CN-COF-2 exhibits moderate radical stabilization capacity as well as efficient electron transport between the pyrene cores, facilitating ECL generation. Significantly, the appropriate radical stability of CN-COF-2 not only achieves the self-enhanced cathodic ECL but also promotes durability of the ECL intensity. The rational regulation of radical stability paves the way for developing efficient reticular nanoemitters and decoding the ECL fundamentals.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 41
·期 4
·1696-1703
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IF 3.269
Guiting Chen,Ruifeng He,Wei Yang,Bin Zhang
Two novel water-soluble π-conjugated small molecules based on dibenzothiophene-S,S-dioxide and bispyridinium salts, named FSOPyCl and FSOmiCl, were successfully synthesized. Both molecules showed deep blue light emission, with photoluminescence peaks at about 408 and 405 nm in aqueous solution, respectively. Their photoluminescence quantum yields (PLQYs) in aqueous solution were as high as 68.9% and 50.3%, respectively. Electrochemical measurements suggested that they have excellent electron affinity, with lowest unoccupied molecular orbital (LUMO) energy levels at −3.78 and −3.94 eV, respectively. Due to their unique properties including large planarity, good thermal stability, excellent electron affinity and high fluorescence efficiency, FSOPyCl and FSOmiCl may be promising construction units for preparing water/alcohol-soluble conjugated materials with good optoelectronic performance.
研究领域:
有机化学
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材料科学
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光电材料
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Xiaona Li,Hang Luo,Yuting Wan,Bo Peng,Yuan Liu,Sheng Chen,Dou Zhang
High temperature resistance is essential for electrostatic capacitors, for example, the operating temperature of capacitors used in inverters for hybrid electric vehicles is around 140–150 °C. However, the reliability of current commercial dielectrics, such as biaxial stretched polypropylene (BOPP), significantly degrades when the operating temperature exceeds 105 °C. In this work, an all-organic dielectric utilizing two mechanisms—high electron affinity and physical interaction—is designed to enhance the capacitive performance. Specifically, the molecular semiconductor 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4-TCNQ), with ultra-high electron affinity (5.24 eV) and peripheral electronegativity, is incorporated with polyetherimide (PEI). Deep electron traps are successfully constructed to capture free electrons due to the incorporation of high-electron-affinity F4-TCNQ. Moreover, it is difficult for the captured electrons to escape because of the Coulomb force between electrons in the low unoccupied molecular orbital (LUMO) of F4-TCNQ and holes in the highest occupied molecular orbital (HOMO) of PEI. From another point of view, physical interaction is formed between the peripherally electronegative groups of F4-TCNQ and the positively charged phenyls of PEI, improving the packing density among polymer chains and the Young’s modulus. Consequently, the electromechanical breakdown strength is enhanced. These two mechanisms play their part simultaneously, realizing significantly suppressed conductivity loss and increased breakdown electric field. Accompanied by an improved dielectric constant, the discharged energy density of F4-TCNQ/PEI composites is significantly increased over a wide temperature range. Especially at 150 °C, the discharged energy density ( U e ) of 0.6 wt% F4-TCNQ/PEI reaches 7.84 J/cm 3 at 670 kV/mm, which is 123 % higher than that of PEI (3.52 J/cm 3 ). The U e is still as high as 5.12 J/cm 3 even when the discharged efficiency ( η ) is over 90 %. This work exhibits a promising prospect of all-organic dielectrics in capacitive application at high temperature.
研究领域:
材料科学
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电气工程
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产品关联
DOI
高影响因子
ORGANIC ELECTRONICS
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2024
·
IF 2.7
Yanting Du,Yijia Zhou,Jiayu Li,Songhao Zhao,Haifeng Yu,Jiahui Fan,Shuhong Wang,Cheng Wang
The application of fluorinated materials in optoelectronic devices has been extensively studied, yet their potential in polymer-based memory devices still needs to be explored. The strategic manipulation of electron donors and electron acceptors to enhance the electron properties of material represents a valid approach to advancing data storage performance. The acceptor unit plays a crucial role in charge trapping, by fluorinating acceptor unit, the polymer electron affinity can be further modulated, leading to optimized carrier injection. In this work, we have synthesized three donor-acceptor-type (D-A-type) conjugated polymers, employing benzimidazole-isoindole electron acceptors substituted with different numbers of fluorine atoms. These polymers were utilized as active layers and integrated into indium-tin-oxide/active layer/aluminum devices through a straightforward fabrication process. These devices exhibit excellent ternary non-volatile memory performance and demonstrate sustained stability even after 10 3 cycle numbers. Notably, the PM4Fbzo-based device achieves impressively low threshold voltages of −0.55 V and −0.80 V, accompanied by a switching current ratio surpassing 10 4 . These exceptional outcomes show the tremendous potential of fluorinated benzimidazole-isoindole-based materials for ternary storage applications, showcasing them as one of the promising candidates for the next generation of materials.
研究领域:
材料科学
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电子工程
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DOI
高影响因子
SOLAR ENERGY MATERIALS AND SOLAR CELLS
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2022
·
IF 7.305
Ning Yang,Liubing Xie,Pingan Wang,Yanpeng Xu,Shuang Li,Xiaoming Shen,Yuechun Fu,Huan He
In this study, an InN photocathode consisting of ZnO nanowire arrays was proposed as a cathode for a photon-enhanced thermionic emission (PETE) solar energy converter. To optimize the performance of the device, we applied InN with a phonon bottleneck effect to the PETE converter. The theoretical model for PETE conversion with this complex photocathode was developed based on one-dimensional continuous equations and boundary conditions. We simulated and analyzed the conversion efficiency as a function of operating temperature, solar concentration, surface electron affinity , and operating voltage. Furthermore, we verified the feasibility of the proposed cathode through experiments on the current-voltage characteristics of the InN photocathode at different temperatures. The results of simulations and experiments indicated that InN is a promising photocathode material and may enable high-performance PETE devices.
研究领域:
材料科学
·
能源工程
·
半导体物理
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Na Zhang,Hang Zhao,Chuying Zhang,Haotong Guo,Zhi-Min Dang,Jinbo Bai
Polymer dielectrics are crucial for electrostatic energy storage and offer broad application prospects in advanced high-power electrical systems, but their energy storage performance declines considerably due to increased conductivity at elevated temperatures. This work presents a structurally-simple high-temperature composite dielectric by incorporating positively charged ultrafine UIO-66 nanoparticles into polyetherimide (PEI) matrix. Be distinguished from traditional sub-micron MOF structures that usually reported in very recently, the newly-found nanoscale effect endows the ultrafine UIO-66 (∼12.9 nm) with largely-increased active sites, surface charge density and electron affinity. These ultrafine UIO-66 nanoparticles can capture free charge through strong electrostatic interactions and introduce deeper traps in composite dielectrics, reducing conduction loss and improving energy storage property significantly at elevated temperatures. Specifically, filling only as tiny as 0.5 wt% ultrafine UIO-66 endows the PEI-based composite with ultra-high energy densities of 5.9J cm −3 and 3.7 J cm −3 accompanied by high charge–discharge efficiencies of 91.4 % and 84.1 % at 150 ℃ and 200 ℃, respectively. These obtained performance in this work surpasses those of most previously reported mono-layered composite counterparts. This study provides a straightforward and effective strategy for designing high-temperature polymer dielectrics in advanced electrical and electronic systems, offering a new route for future applications and developments.
研究领域:
材料科学
·
电气工程
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zewan Qin,Qing Guan,Yating Lu,Yu Tian,Xia Yang
The naphthalene tetracarboxdiimide (NDI) modified NH 2 -UiO-66(Zr) and NH 2 -MIL-101(Cr) (NDI/UZr and NDI/MCr for short) metal organic frameworks (MOFs) materials with strong covalent bond O C–N–C O were designed and prepared by solvothermal method. The comprehensive physical and chemical properties of the materials were characterized, and the adsorption and photocatalytic properties of the materials were evaluated by using methylene blue (MB) and Cr(VI) in single and mixture system. When the initial concentration of MB was 50 mg·L −1 , the photocatalytic degradation rate constant of NDI/MCr(2:1) was 10.3 and 13.8 times higher than that of NH 2 -MIL-101(Cr) and NDI/UZr(2:1), respectively. Additionally, NDI/MCr(2:1) exhibited 1.6 times higher reaction rate constant than that of NDI/UZr(2:1) for the removal of 10 mg∙L −1 Cr(VI). The enhanced adsorption and photocatalytic ability over NDI/MOFs were attributed to the MOFs larger specific surface area and wider spectral response, and NDI showed high electron affinity, superior charge carrier transport properties. Free radical and electron capture experiments indicated that h + , •O 2 − , and e − were the main active species in the NDI/MOFs system. Among them h + and •O 2 − played an essential role in the removal of MB, while e − and •O 2 − contributed to the photocatalytic reduction of Cr(VI). The mechanism of the photocatalytic process was discussed in detail.
研究领域:
材料科学
·
环境工程
·
化学工程
·
光催化
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2020
·
IF 16.28
Mengnan Cui,Zhihui Zheng,Jiacheng Wang,Youwei Wang,Xiaolin Zhao,Ruguang Ma,Jianjun Liu
Lithium-sulfur (Li-S) batteries show advantages for next-generation energy storage due to their high theoretical energy density and cost effectiveness. Despite tremendous efforts, rational cathode design for mitigating the shuttling of soluble lithium polysulfides (LiPSs) between electrodes and improving reversible capacity remains a challenge because effective characteristic descriptor for sulfur cathodes is not established. In this work, the surface electron affinity (defined as electron-acceptance ability of solid-state surface) is firstly established as a quantitative screening principle forcathode materials. We find that those materials with the -2.66 ~ -7.96 eV surface electron affinities do not only prevent LiPSs from dissolving but also exhibit good electronic conductivity . The design principle is verified by our comparative electrochemical characterizations that TiO (ΔV SEA = -4.42 eV) performs a lower capacity-decay rate than TiS 2 (-1.12 eV) TiC (-10.86 eV) and TiN (-14.55 eV).The design principle is verified by available experimental data reported in the previous literatures and our comparative experimental studies. The optimum binding strength of LiPSs on cathodes is identified in the range of 1.65 ~ 2.90 eV. Furthermore, differential atom electronegativity is defined as a more universal descriptor for experimentally and theoretically screening high-performance cathodes of Li-S battery . We find that divalent metal oxides (MO) with M:O = 1:1 and tetravalent transition metal sulfides, selenides and carbides (M:X = 1:2) could promote battery performance in maintaining high reversible capacity. These findings provide important insight towards the understanding of interfacial adsorption mechanism in electrochemical systems and establishing design principles for future discovery of improved cathodes for Li-S batteries.
研究领域:
能源存储
·
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）