DYES AND PIGMENTS
·
2023
·
IF 4.5
Shihang Liu,Xiaodi Chen,Chao Zhang,Xingliang Liu,Shiai Xu
In this study, three typical D–π–A type heteroaromatic organic dyes containing carbazole (CBZ), phenothiazine (PTZ), and phenoxazine (POZ) moiety as electron donor cores and linked to g-C 3 N 4 with amide covalent bonds were synthesized. Thereafter, we studied the long-term photochemical stability and degradation mechanism of the associated dye-sensitised g-C 3 N 4 with covalent linkage or weak interaction. The results revealed that most of the dyes degraded and became unstable after absorption on g-C 3 N 4 under light irradiation. Interestingly, after the target dyes were linked to g-C 3 N 4 with amide covalent bonds, the photostability could be effectively promoted and improved to high levels of stability. For POZ-S dye covalent bond-linked sample g-C 3 N 4 /POZ-S, ∼90.5% percent of the dyes were reserved, whereas only ∼25.3% remained for the physically absorbed dye sample g-C 3 N 4 +POZ-S after 30 min of irradiation aging test. Moreover, the obtained g-C 3 N 4 /POZ-S sample exhibited enhanced H 2 evolution activity with photocatalytic H 2 production rates that were approximately 96- fold of that of pure g-C 3 N 4 . Then, we applied various instrumental analysis and DFT calculation to clarify the mechanism involved with dye photostability and degradation pathway. The typical decarboxylation process was confirmed, and such an unfavourable reaction process could be effectively inhibited if the target dye is linked to g-C 3 N 4 with amide covalent bond instead of the weak interaction. Overall, the existed covalent bond is the key factor for enhancing both the photochemical stability and photocatalytic activity of organic dye-sensitised g-C 3 N 4 for hydrogen evolution .
研究领域:
材料科学
·
光化学
·
催化
·
物理化学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Zhiming Liu,Dazhi Gao,Lina Hu,Hui Liu,Ying Li,Yanming Xue,Fang Liu,Jun Zhang,Chengchun Tang
High activity and stable hydrogen evolution reaction (HER) catalysts have an indispensable influence on hydrogen production . Pyrite cobalt selenide (CoSe 2 ) is considered an excellent non-noble metal compound HER catalyst due to its low price and excellent electrical conductivity . However, the HER catalytic activity of CoSe 2 is still not ideal because of the weak adsorption of hydrogen on its active Co site. The anion introduction can improve the electronic structure of the catalyst and thereby enhance the performance of HER. Here, we report that B-doped CoSe 2 nanomaterials on carbon cloth (B-CoSe 2 /CC) were successfully synthesized. Compared with CoSe 2 , B-CoSe 2 exhibits better HER performance in 1 M KOH. The overpotential of B-CoSe 2 catalyst is only 153 mV at 10 mA cm −2 . Tafel slope of B-CoSe 2 /CC sample is only 85 mV dec −1 . In addition, B-CoSe 2 /CC exhibits perfect long-term durability and cycle stability. Density functional theory (DFT) calculations illustrate that the doping of B improves the intrinsic conductivity of CoSe 2 and optimizes the hydrogen adsorption free energy (ΔG H* ) of Se and Co sites. This work not only proposes a new anion doping strategy to improve the electronic structure of cobalt-based selenides for improved HER performance, but also provides a reference for the screening and design of other transition metal compound HER electrocatalysts .
研究领域:
材料科学
·
电化学
·
催化
·
可再生能源
✓ 已验证
DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Bo Luo,Mengxing Liu,Rongrong Li,Mengnan Zhou,Fengjia Zhang,Miao Wang,Yuqing Guo,Qingsi Zhang,Xinyi Liu,Yanbing Wu,Kun Fang,Rong Wang
In the search for novel succinate dehydrogenase inhibitors (SDHIs) fungicides for managing rice sheath blight (RSB) and sclerotinia stem rot (SSR), 28 pyrazole-4-carboxamides incorporating stilbene or diphenylacetylene scaffolds were synthesized and evaluated for antifungal activities. The results showed that compound 7m exhibited the most promising antifungal efficacy against Rhizoctonia solani and Sclerotinia sclerotiorum with EC50 (half maximal effective concentration) values of 0.004 and 0.028 μg/mL, outperforming Boscalid and Fluxapyroxad. Furthermore, the detached leaf assay showed that 7m showed remarkable protective and curative efficacies against R. solani and significant inhibition of S. sclerotiorum growth on oilseed rape leaves, indicating that it had a promising application prospect for RSB and SSR management. Further SDH enzymatic inhibition assay, scanning electron microscopy (SEM), molecular docking studies, and molecular dynamics (MD) simulations revealed that compound 7m shared an antifungal mechanism similar to that of Fluxapyroxad, which was further validated by density functional theory (DFT) and electrostatic potential (ESP) calculations. These findings suggested that 7m held significant promise as a novel SDHI for the effective management of RSB and SSR, warranting further investigation.
研究领域:
农业化学
·
植物病理学
·
杀菌剂开发
·
计算化学
·
药物化学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 10
·6014-6027
·
IF 10.7
Panpan Li,Jingde Luan,Longde Jiang,Yu Zhang,Wengang Liu,Zheng Yan,Xin Ke
High pressure wet ball milling and thermal polycondensation are used to prepare W-doped O-bridge carbon nitride (WOCN) for the rapid catalytic degradation of antibiotic rifampicin (RIF). The removal of rifampicin at a concentration of 150 mg L−1 in a dark environment reached 60% within 8 minutes and 92% after 40 minutes of visible light exposure. The rapid catalytic degradation of RIF benefits from the coupling effect of dark degradation with photocatalytic degradation, including the electron replenishment theory of dark degradation and the electrophilic attack under light irradiation. In the dark degradation reaction, the abundant delocalized electrons at the tungsten-oxygen insertion surface are captured by the dissolved oxygen to produce ˙O2−, part of which directly participates in RIF degradation, whereas the other part is oxidized to 1O2 by the holes at the carbon-rich cyano group surface and then participated in RIF degradation. The electrons consumed at the reaction site are continuously replenished through the O electron bridge, allowing RIF degradation to continue. In the photocatalytic degradation reaction, photogenerated electron holes are excited using visible light, which partly participate in the degradation of RIF through the above dark reaction pathway. Meanwhile, some photogenerated holes oxidize OH− to ˙OH and degrade RIF by electrophilic attack.
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Xiaoyan Feng,Jiachen Li,Yaotian Peng,Wentai Guo,Lijun Liang,Linli Zhu,Sa Liu,Li Ren
It remains a challenge for commercial hemoperfusion adsorbents to efficiently remove multiple protein-bound toxins in the clinical treatment of liver and kidney failure. Here, polystyrene divinylbenzene microspheres (PS-DVB) were surface-modified by poly(carboxybetaine methacrylate) (poly-CBMA) through controlled polymerization, named PCBMA. PS-DVB served as a supporting backbone and provided enormous specific surface, while a layer of the poly-CBMA aimed at efficiently removing various toxins and attaining better biocompatibility. After modification, the mesoporous analysis revealed a high specific surface area of 527 m 2 /g. More notably, compared with PS-DVB, PCBMA showed an 830%, 130%, and 26% increase in the adsorption capacity of p-cresol sulfate (PCS), indoleacetic acid (IAA), and bilirubin (BR), respectively, in the presence of 40 g/L bovine serum albumin. Further molecular dynamics simulations and DFT calculations showed that poly-CBMA exhibited stronger intermolecular forces for all three toxins. The hydrogen bonds formed between the negatively charged carboxylate ions from PCBMA contributed to its excellent adsorption performance. This study not only provides a new idea to study the adsorption mechanism of toxins by zwitterionic polymers but also demonstrates the promising application of microspheres modified by zwitterionic polymers in clinical hemoperfusion therapy.
研究领域:
材料科学
·
生物医学工程
·
计算化学
·
血液透析
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaofei Zhou,Guijuan Wei,Chang Liu,Qian Zhao,Hui Gao,Wenbo Wang,Xixia Zhao,Xin Zhao,Honglei Chen
The production of hydrogen through seawater electrolysis has recently garnered increasing concern. However, hydrogen evolution reaction (HER) by alkaline seawater electrocatalysis is severely impeded by the slow H 2 O adsorption and H* binding kinetics at industrial current densities . Herein, a face-centered cubic/hexagonal close packed (fcc/hcp) NiRu alloy heterojunction was fabricated on Ni foam (N doped NiRu-inf/NF) by a low-temperature nitrogen plasma activation. Simultaneously, nitrogen atoms are introduced into the alloy to facilitate d-p hybridization. When N doped NiRu-inf/NF is integrated into a dual-electrode cell for urea-assisted seawater electrolysis, it achieves 100 mA cm −2 with an ultra-low voltage of 1.36 V and excellent stability. Density functional theory (DFT) verifies that the robust d-p hybridization among Ni, Ru and N exhibits more energy level matching for H 2 O molecule adsorption at the Ru sites, while simultaneously reducing the interaction between H* and Ni sites in N -doped NiRu-inf.
研究领域:
材料科学
·
电化学
·
能源材料
·
催化
✓ 已验证
DOI
高影响因子
Environmental Science-Advances
·
2023
·Vol. 3
·期 2
·177-185
·
IF 0
Tao Wen,Xinjie Ma,Yingzhong Huo,Ruoxuan Guo,Sai Zhang,Yanan Han,Yang Liu,Yuejie Ai,Xiangke Wang
Anthropogenic activities involving unintended uranium leakage from nuclear accidents, large-scale uranium mining, or nuclear weapon production have caused health and environmental concerns. The increasing demand for highly efficient materials to dispose of uranium may facilitate the sustainable development of nuclear power plants. Herein, a β-ketoenamine-linked covalent organic framework (COF) material, named DQTP COF, was solvothermally synthesized by an imine condensation of 1,3,5-triformylphloroglucinol (TFP) and 2,6-diaminoanthraquinone (DAAQ). The chemical and physical properties of the synthesized DQTP COF were analyzed using various advanced techniques. Additionally, the adsorption behaviors of DQTP COF for U(VI) were optimized by varying parameters, such as pH, ionic strength, contaminant concentration, and reaction temperature. The produced DQTP COF showed an enhanced adsorption capacity of 517.62 mg g−1 at pH 6.0 towards U(VI), outperforming most of the currently reported COF-based materials. Moreover, DQTP COF exhibited favorable thermodynamics and excellent anti-ion interference properties as well as good reusability. Experimental analysis and theoretical DFT calculations revealed that UO22+ ions were bound exclusively by carbonyl groups via intramolecular coordination and electrostatic interaction in DQTP COF. This work paves the way to rationally develop functionalized COFs and highlights the potential of COFs for environmental remediation.
研究领域:
环境科学
·
材料科学
·
核工程
·
理论化学
✓ 已验证
DOI
RADIOCHIMICA ACTA
·
2017
·Vol. 105
·期 7
·531-539
·
IF 1.271
Fei Chen,Congzhi Wang,Jianhui Lan,Yanqin Ji,Zhifang Chai
Two thorium organic frameworks, Th(BDC) 2 and Th(OH)(BCPBA) have been hydrothermally synthesized using 1,4-benzenedicarboxylic acid (H 2 BDC) and 3,5-bi(4-carboxyphenoxy)benzoic acid (H 3 BCPBA), respectively. The obtained two compounds were determined by single-crystal XRD, and they exhibited two new topologies. Th(BDC) 2 shows a 3-dimensional (4,4,8)-connected framework with the Schläfli symbol of (4 14 ·6 12 ·8 2 )(4 2 ·6 3 ·8)(4 4 ·6 2 ), and it is a mononuclear thorium(IV) complex. Th(OH)(BCPBA) possesses a (4,6)-connected topology with the Schläfli symbol of (4 15 ) 2 (4 6 ) 3 , and it has a dinuclear thorium(IV) asymmetric unit with the shortest Th–Th distances. Viewing along suitable directions, channels with different shapes can be found in the obtained two frameworks. Based on calculation with PLATON, the amount of void space is 21.9% and 13.5% in Th(BDC) 2 and Th(OH)(BCPBA), respectively. Density functional theory (DFT) studies revealed that the metal-ligand interactions were mainly of ionic character in both compounds and the hydroxyl ions might play an important role in the stability of dinuclear thorium(IV) of Th(OH)(BCPBA).
研究领域:
无机化学
·
材料科学
·
晶体学
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTRONIC MATERIALS
·
2022
·Vol. 52
·期 1
·547-558
·
IF 2.047
Zhou Jian,Ren Sili
The phosphor-converted white light-emitting diode (WLED) has received tremendous attention as a promising alternative to traditional light sources in lighting and displays. Herein, a novel broadband red emitter Ca 2 Sr(PO 4 ) 2 :Mn 2+ was successfully designed and synthesized based on the Sr-alloying and Mn-doping of Ca 3 (PO 4 ) 2 . The phase purity of the materials was verified by x-ray diffraction (XRD) analyses, while a scanning electron microscope (SEM) coupled with an energy-dispersive spectrometer (EDS) was employed to confirm the uniform dopant distribution. XRD Rietveld refinements were further performed to clarify the site occupation of alloying Sr and the Mn dopants. Effective site engineering confined the Mn dopants in a highly symmetric Ca5 site and excluded the immersion of Sr, leading to an extraordinarily long fluorescence lifetime. Density functional theory (DFT) simulations also revealed the good potential of the materials as host matrices for activators such as Mn 2+ . Finally, Ca 2 Sr(PO 4 ) 2 :Mn 2+ was used to fabricate a WLED prototype based on a near-ultraviolet (n-UV) commercial LED chip, which realized a warm white-light emission and high color rendering index (Ra) of 82.9. This WLED was able to survive the long-term stability test while maintaining high luminous efficacy of ~ 60 lm/W within 20 h, showing its great potential in practical applications.
研究领域:
材料科学
·
光电技术
·
照明技术
·
固体物理
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 19
·10625-10637
·
IF 14.511
Kun Wang,Xiaobing Huang,Tao Zhou,Dan Sun,Haiyan Wang,Zhi Zhang
The NASICON-type Na4MnV(PO4)3 (NMVP) possesses potential as a cathode material in SIBs, and is known for its stable 3D Na+ superconductive framework, high voltage platform, and relatively low cost and toxicity. Nevertheless, the intrinsic poor electronic conductivity and Jahn–Teller effect from Mn3+ during cycling limit its further application. Herein, to address such issues, a well-designed 3D porous spheroidal Ce3+-doped NMVP@CeO2/C cathode was constructed via a simple spraying drying-assisted route. As proved, the synergistic effect of Ce3+ doping in the crystal framework and CeO2 surface coating was achieved simultaneously, which greatly improved the electronic conductivity, facilitated the ion diffusion transfer and stabilized the crystalline structure. As a result, the as-prepared sample delivered superior discharge performance (50.3 mA h g−1 at 50C) and long circular life (91.0 mA h g−1 after 2000 cycles at 5C with 86.7% capacity retention). Furthermore, the reversible biphasic reaction for cathodes was confirmed by Galvanostatic intermittent titration technique (GITT) and ex situ XRD. The DFT calculation revealed the influence of Ce3+-doping on the crystalline framework and electrochemical properties. Finally, the optimized NMVP cathode also showed great potential for practical utilization through the successful assembly of full cells.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 40
·14046-14051
·
IF 4.174
Huanke Zhao,Pifu Gong,Xinyuan Zhang,Zheshuai Lin,Zhanggui Hu,Yicheng Wu
Two new isomorphic selenite bromides, namely Pb2GaF2(SeO3)2Br (1) and Pb2NbO2(SeO3)2Br (2), were synthesized by mild hydrothermal reactions. These two compounds crystallize in the noncentrosymmertric space group P21 and feature 3D structures consisting of 1D (Pb2Br)3+ cationic chains and 2D [Ga2F4(SeO3)4]6−/[Nb2O4(SeO3)4]6− anonic chains. As measured, 1 and 2 are phase-matchable and exhibit excellent second harmonic generation (SHG) responses of 4.5 and 1.4 times that of KDP, respectively. Moreover, these two compounds possess wide bandgaps (>3.17 eV) and high thermal stabilities (>425 °C), indicating their suitable performances as potential nonlinear optical materials. First-principle density functional theory (DFT) calculations were also performed to explicate the structure–property relationship.
研究领域:
材料科学
·
非线性光学
·
晶体学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Jianghong You,Yiming Yuan,Chen Zhang,Haoming Xu,Mingyao Chen,Ying Wang,Dongsheng Chen
The transition metal oxide of nickel cobaltite (NiCo 2 O 4 ) has gained more and more attention from battery industry for its excellent properties of high capacitance and cycling stability. However, its performance when used in supercapacitors is compromised due to its limited active sites and poor conductivity. Herein, a 3D (three-dimensional) hierarchical and high-performance material of NiCo 2 O 4 @MXene@LDH (LDH: layered double hydroxide) composite was designed and synthesized. In the material, NiCo 2 O 4 nanorods form a skeleton of nanosheet arrays on layered MXene; and on the nanosheet arrays, NiCo-LDH nanoparticles are attached to form a 3D hierarchical structure, extending the electrochemically active sites, suppressing the agglomeration of NiCo-LDH and producing hierarchical channels that promote electron and ion transport. Density functional theory (DFT) calculations and the results of Ultraviolet–visible (UV–Vis) spectrophotometry indicated that the introduction of MXene and NiCo-LDH induces a redistribution of the electronic states of NiCo 2 O 4 due to the formation of a heterointerface, thereby decreasing its bandgap by about 1.42 eV. The X-ray photoelectron spectroscopy (XPS) analysis further demonstrated the negative shift in the initial binding energies of nickel (Ni) and cobalt (Co) atoms, which is due to their transition of spin states; and this is in agreement with the high intensity of electron paramagnetic resonance (EPR) peak in the NiCo 2 O 4 @MXene@LDH composite. The in situ Raman analysis reveals that the enhanced energy storage performance originates from the accelerated formation and increased exposure of NiCoOOH active species during electrochemical cycling. The synergistic effect of MXene and NiCo-LDH introduced into NiCo 2 O 4 enhanced the supercapacitor in terms of power and energy densities. It was indicated that the supercapacitor fabricated from NiCo 2 O 4 @MXene@LDH supercapacitor exhibited a specific capacitance of 5066 F g −1 at 1 A g −1 , and a capacitance retention of 97.82 % after 10,000 charge cycles at 10 A g −1 . Moreover, an asymmetric supercapacitor (ASC) device with a NiCo 2 O 4 @MXene@LDH//AC configuration was developed. The supercapacitor presented an energy density and power density of 70.11 Wh kg −1 and 850.22 W kg −1 , respectively. The redistribution of electronic states and decreased bandgap could facilitate the creation of NiCo 2 O 4 -based materials with customized features for supercapacitors.
研究领域:
材料科学
·
电化学
·
纳米技术
·
储能技术
·
表面工程
·
固体物理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）