ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Lingjia Ma,Jiongliang Yuan,Zhaotao Liu,Yiqing Luo,Yuning Su,Kunye Zhu,Zefeng Feng,Huihua Niu,Shuaishuai Xiao,Jianjun Wei,Xu Xiang
The electrocatalytic synthesis of high-value-added urea by activating N2 and CO2 is a green synthesis technology that has achieved carbon neutrality. However, the chemical adsorption and C–N coupling ability of N2 and CO2 on the surface of the catalyst are generally poor, greatly limiting the improvement of electrocatalytic activity and selectivity in electrocatalytic urea synthesis. Herein, novel hierarchical mesoporous CeO2/Co3O4 heterostructures are fabricated, and at an ultralow applied voltage of −0.2 V, the urea yield rate reaches 5.81 mmol g–1 h–1, with a corresponding Faraday efficiency of 30.05%. The hierarchical mesoporous material effectively reduces the mass transfer resistance of reactants and intermediates, making it easier for them to access active centers. The emerging space-charge regions at the heterointerface generate local electrophilic and nucleophilic regions, facilitating CO2 targeted adsorption in the electrophilic region and activation to produce *CO intermediates and N2 targeted adsorption in the nucleophilic region and activation to generate *N ═ N* intermediates. Then, the electrons in the σ orbitals of *N ═ N* intermediates can be easily accepted by the empty eg orbitals of Co3+ in CeO2/Co3O4, which presents a low-spin state (LS: t2g6eg0). Subsequently, *CO couples with *N ═ N* to produce the key intermediate *NCON*. Interestingly, it was discovered through in situ Raman spectroscopy that the CeO2/Co3O4 catalyst has a reversible spinel structure before and after the electrocatalytic reaction, which is due to the surface reconstruction of the catalyst during the electrocatalytic reaction process, producing amorphous active cobalt oxides, which is beneficial for improving electrocatalytic activity.
研究领域:
材料科学
·
电化学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Nan Jiang,Xuexin Hao,Zichen Wang,Minzhen Li,Dong Zhang,Rong Cao,Ruiqin Zhang,Haijun Zhang,Jiping Chen,Ningbo Geng
The extensive utilization of rubber-related products can lead to a substantial release of p -phenylenediamine (PPD) antioxidants into the environment. In recent years, studies mainly focus on the pollution characteristics and health risks of PM 2.5 -bound PPDs. This study presents long-time scale data of PPDs and N-(1,3-dimethylbutyl)-N′-phenyl- p -phenylenediamine quinone (6PPD-Q) in PM 2.5 and proposes the innovative use of PPDs as new markers for vehicular emissions in the Positive Matrix Factorization (PMF) source apportionment . The results indicate that PPDs and 6PPD-Q were detectable in 100 % of the winter PM 2.5 samples, and the concentration ranges of PPDs and 6PPD-Q are 15.6–2.92 × 10 3 pg·m −3 and 3.90–27.4 pg·m −3 , respectively, in which 6PPD and DNPD are the main compounds. Moreover, a competitive formation mechanism between sulfate, nitrate, ammonium (SNA) and 6PPD-Q was observed. The source apportionment results show that the incorporation of PPDs in PMF reduced the contribution of traffic source to PM 2.5 from 13.5 % to 9.5 %. In the traffic source factor profiles, the load of IPPD, CPPD, DPPD , DNPD and 6PPD reaches 91.8 %, 91.6 %, 92.9 %, 80.6 % and 87.2 %, respectively. It`s amazing that traditional markers of traffic source, which often overlap with coal burning and industrial sources, over-estimated the contribution of vehicles by one third or more. The discovery of PPDs as specific markers for vehicular emissions holds significant utility, particularly considering the growing proportion of new energy vehicles in the future. The results may prove more accurate policy implications for pollution control . Synopsis PPDs are excellent indicators of vehicle emissions, and PMF without PPDs over-estimated the contribution of traffic source to PM 2.5 .
研究领域:
环境科学
·
大气污染研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CARBON
·
2025
·
IF 11.6
Yue Liu,Zhongpan Zhang,Xiaoqiang Fan,Minhao Zhu
Covalent organic frameworks (COFs), as a well-known carbon-based material, exhibit multiple morphologies due to their controllable structure units. In this study, we proposed a molecular engineering approach utilizing the methoxy group to adjust the p -π resonance and synthesized two distinct covalent organic frameworks (COFs), designated as TATP (without methoxy) and TADM (with methoxy). These COFs exhibit significant morphological and structural disparities; TATP adopts a spherical morphology, whereas TADM forms layered structures with a high aspect ratio. The incorporation of TADM led to an excellent reduction in wear rates by 78.93 % compared to TATP (37.31 %). The exceptional interfacial lubrication performance of TADM is attributable to not only the successfully manipulated high-oriented layer structure through p -π resonance but also the formation of Fe–N bonds between the electron-rich nitrogen atoms in TADM and the electron-deficient iron atoms during the friction process.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.7
Kewei Shu,Cunguo Yang,Huizhu Niu,Xiaorui Fuyan,Shuqi Yang,Haihua Wang
GeP 3 is a promising anode material for sodium ion battery due to better conductivity, relatively high theoretical capacity and improved mechanical endurance compared to phosphorus and other phosphides. However unsatisfied rate capability and cycling stability is still an annoying issue that hinders the application of GeP 3 . Here, GeP 3 was hybridized with P doped carbon (PPC) derived from low-cost coal tar pitch to prepare composite electrode. Through ball-milling process, the GeP 3 and PPC was homogenously mixed and form fused, secondary particles as confirmed by electron microscope. The formation of P-C and P-O-C bond between GeP 3 and carbon matrix was evidenced by XPS, and prompted by P doping level and O content in PPC. The electrochemical performance of the composite electrodes was evaluated, demonstrated much enhanced properties compared to bare GeP 3 and also GeP 3 /carbon black electrode. High reversible capacity of 781 mAh/g was achieved by GeP 3 /PPC-950 at 0.05 A/g. At higher current density of 2 A/g, the capacity can maintain at 360 mAh/g, 46% of the value that obtained at 0.05 A/g. The correlation between the structure of carbon and battery performance was discussed. The improvement in battery performance can be attributed to suppressed volume expansion and good conductive network of the GeP 3 /PPC composite, which affected by P doping level and O content of PPC.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2022
·Vol. 46
·期 14
·19686-19696
·
IF 4.672
Feng Wang,Yinrong Lv,Xueli Bai,Shengjian Zhang,Huifang Wang,Baoyi Li,Aifang Liu,Xiaoping Zhang
Summary Polyhydride electrocatalysts integrated directly into metal substrates have attracted attention because they can provide high electrochemical specific surface area and excellent mechanical properties. In this work, through the classical hydrothermal method and subsequent phosphating procedure, we synthesized for the first time an electrocatalyst with a pyramid-shaped MnCO 3 as the main structure, P and Co as co-doping elements, named Co, P-MnCO 3 , and used it as hydrogen evolution reaction (HER). The experimental results show that the excellent catalytic activity in alkaline media, with current densities of 10 and 200 mA∙cm −2 at 61 mV and 158 mV and low overpotentials, which are better than P-Co (108/234 mV) and P-MnCO 3 (175 mV/340 mV), etc. it has more electrochemically active sites, faster charge transfer rate and lower resistance. The excellent electrochemical properties benefit from the unique highly active binary Co, P-MnCO 3 pyramid brick sites shortened the ion transfer distance and optimized synergistic effect between the doped metal elements (Co,P between MnCO 3 ), the porous connection between Co, P-MnCO 3 and the high conductivity substrate, increased the electron-transfer efficiency between the substrate and material, accelerating the conversion of H + to H 2 ; facilitated the release of bubbles and provided excellent mechanical properties for improved catalyst stability. This work provides a new idea for the synthesis of multi-element electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
MOLECULAR PHARMACEUTICS
·
2013
·
IF 4.57
Wenjing Li,Xinru Li,Yajie Gao,Yanxia Zhou,Shujin Ma,Yong Zhao,Jinwen Li,Yan Liu,Xinglin Wang,Dongdong Yin
The present study aimed to investigate the effect of monomethoxy poly(ethylene glycol)-block-poly(d,l-lactic acid) (mPEG-PLA) on the activity of P-glycoprotein (P-gp) in Caco-2 cells and further unravel the relationship between PLA chain length in mPEG-PLA and influence on P-gp efflux and the action mechanism. The transport results of rhodamine 123 (R123) across Caco-2 cell monolayers suggested that mPEG-PLA unimers were responsible for its P-gp inhibitory effect. Furthermore, transport studies of R123 revealed that the inhibitory potential of P-gp efflux by mPEG-PLA analogues was strongly correlated with their structural features and showed that the hydrophilic mPEG-PLA copolymers with an intermediate PLA chain length and 10.20 of hydrophilic–lipophilic balance were more effective at inhibiting P-gp efflux in Caco-2 cells. The fluorescence polarization measurement results ruled out the plasma membrane fluidization as a contributor for inhibition of P-gp by mPEG-PLA. Concurrently, mPEG-PLA inhibited neither basal P-gp ATPase (ATP is adenosine triphosphate) activity nor substrate stimulated P-gp ATPase activity, suggesting that mPEG-PLA seemed not to be a substrate of P-gp and a competitive inhibitor. No evident alteration in P-gp surface level was detected by flow cytometry upon exposure of the cells to mPEG-PLA. The depletion of intracellular ATP, which was likely to be a result of partial inhibition of cellular metabolism, was directly correlated with inhibitory potential for P-gp mediated efflux by mPEG-PLA analogues. Hence, intracellular ATP-depletion appeared to be possible explanation to the inhibition mechanism of P-gp by mPEG-PLA. Taken together, the establishment of a relationship between PLA chain length and impact on P-gp efflux activity and interpretation of action mechanism of mPEG-PLA on P-gp are of fundamental importance and will facilitate future development of mPEG-PLA in the drug delivery area.
研究领域:
药学
·
药理学
·
药物递送系统
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Haonan Zhu,Fangyuan Wang,Yingying Cao,Yuhai Yang,Siyu Yang,Zipeng Zou,Fengjie Hu,Feng Chen,Jianping Qiu,Shuang Song
Nb 2 O 5 based photocatalysts have garnered significant attention in the field of antibiotic photodegradation due to their potential. Enhancing the efficiency of carrier separation efficiency still remains a crucial factor for optimizing photocatalytic performance. Herein, a Nb 2 O 5 /Co 3 O 4 p–n heterojunction photocatalyst was synthesized by a straightforward one-step hydrothermal method. The Nb 2 O 5 /Co 3 O 4 composites effectively utilized visible light to catalytically degrade norfloxacin, achieving 89.2% degradation in 90 min. This performance was 2.68 and 7.42-fold greater than pure Nb 2 O 5 and Co 3 O 4 , respectively. Furthermore, this composite maintained its high activity through five cycles of photocatalysis. The exceptional performance was creditable to the establishment of p-n heterojunction structure between Nb 2 O 5 and Co 3 O 4 , which effectively inhibited the electron-hole recombination and distinctly broadens the visible light adsorption region. •O 2 − and h + were confirmed as the critical active species in this process. The primary degradation pathways for norfloxacin were decarboxylation and ring-opening. This study introduced an innovative method for developing and fabricating flower-like Nb 2 O 5 -based heterojunctions for enhancing photocatalytic efficiency. This approach held significant promise for the effective treatment of antibiotic-contaminated wastewater through photocatalysis.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2025
·
IF 12.1
Man Liu,Feihua Liu,Hongmei Qin,Chuanxi Xiong,Hengxue Xiang,Liping Zhu,Meifang Zhu
Polymer dielectric films are widely used in advanced electronics, hybrid vehicles, etc., however, they encounter critical challenges, including significant thermal degradation and heightened leakage currents, which severely constrain their energy density and efficiency under high-temperature conditions. Herein, a novel strategy is proposed for constructing a polyimide (PI) alloy by incorporating high-bandgap copolymer of perfluoropropyl perfluorovinyl ether and tetrafluoroethylene (P(TFE-PPVE)) and fluorinated polyimide (FPI) as a compatibilizer. The highly oriented structural PI/FPI/P(TFE-PPVE) alloy is fabricated via knife casting, which utilized high shear forces to align the P(TFE-PPVE) blocks within the polyamide acid. Simulation results indicate that the high-bandgap P(TFE-PPVE) phase (9.72 eV) with an oriented structure in the PI matrix can effectively suppress electrical tree growth. Furthermore, deep carrier trap at the PI/P(TFE-PPVE) interface (2.98 eV) further reduces leakage current and enhances breakdown strength while minimizing conduction loss. As a result, the PI/FPI/0.25P(TFE-PPVE) alloy demonstrates remarkable dielectric stability under diverse conditions, achieving a discharge energy density of 3.75 J cm −3 with 90% efficiency at 150 °C and 550 MV m −1 . This straightforward blending strategy provides an effective pathway to modulate the condensed structure of all organic polymers, offering promising potential for high-performance polymer dielectrics.
研究领域:
材料科学
·
电子工程
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Jing Xu,Xiangyi Shen,Duanli Wang,Chuxuan Zhao,Zizheng Liu,Ivan P. Pozdnyakov,Feng Wu,Jun Xia
The usage of p -arsanilic acid (ASA) in livestock and poultry farms leads to its release into the environment. The phototransformation of ASA generates toxic inorganic arsenic species and organic by-products, which affects the water security of the peripheral river basin. In this work, we have investigated the pH-dependent kinetics and mechanisms of ASA photolysis under Ultraviolet-C (UV-C) light (254 nm) irradiation in the pH range 1–11 in the absence of oxygen. The degradation rate of ASA, the ratio of the generated inorganic arsenic species, and the amount of primary organic by-products were determined under the aforesaid conditions. Our results clearly showed the pH-dependent photochemistry of ASA. The photolysis rate was low under acidic conditions, and As(III) and p -aminophenol were the main products. With increasing pH, the photolysis rate increased significantly, and As(V) and aniline became the main products. A pH-based kinetic model has been established that allows prediction of the generation rates of As(III), As(V), p -aminophenol, and aniline according to the photolysis rate of ASA.
研究领域:
环境科学
·
化学动力学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2018
·Vol. 22
·期 7
·1971-1981
·
IF 2.509
Gao Pingping,Xie Zhiyong,Ouyang Chun,Tao Tao,Wu Xiaobo,Huang Qizhong
The Ni-P/TiN/PTFE (poly tetra fluoroethylene) composite coatings were prepared by electroless plating method on Ti plate, which was used as bipolar plates of proton exchange membrane fuel cells (PEMFCs). The morphology, crystallographic texture, electrochemical corrosion, contact resistance, and hydrophobic property of the Ti bipolar plates with coatings were investigated. The results revealed that Ni-P/TiN/PTFE coating had a dense surface morphology, uniform distribution of composite particles. Ti with coating showed 0.48 μA cm 2 of corrosion current in the simulated solution of PEMFCs and 6 mΩ cm 2 of interfacial contact resistance (ICR). The hydrophobicity test showed that the coating interface was flat and the wetting angle was 112.4°. In conclusion, The Ni-P/TiN/PTFE composite coatings exhibit superior improvement in corrosion resistance, interface hydrophobicity, and conductivity to Ni-P, Ni-P/TiN, and Ni-P/PTFE coatings. The Ni-P/TiN/PTFE coating was suited for bipolar plate surface modification of bipolar plates.
研究领域:
材料科学
·
电化学
·
燃料电池技术
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2019
·Vol. 24
·期 9
·1661
·
IF 3.06
Mengmeng Xia,Yajing Fang,Weiwei Cao,Fuqiang Liang,Siyi Pan,Xiaoyun Xu
P-glycoprotein (P-gp) serves as a therapeutic target for the development of inhibitors to overcome multidrug resistance (MDR) in cancer cells. In order to enhance the uptake of chemotherapy drugs, larger amounts of P-gp inhibitors are required. Besides several chemically synthesized P-gp inhibitors, flavonoids as P-gp inhibitors are being investigated, with their advantages including abundance in our daily diet and a low toxicity. The cytotoxicity of daunorubicin (as a substrate of P-gp) to KB/MDR1 cells and the parental KB cells was measured in the presence or absence of flavonoids. A two-dimensional quantitative structure–activity relationship (2D-QSAR) model was built with a high cross-validation coefficient (Q2) value of 0.829. Descriptors including vsurf_DW23, E_sol, Dipole and vsurf_G were determined to be related to the inhibitory activity of flavonoids. The lack of 2,3-double bond, 3′-OH, 4′-OH and the increased number of methoxylated substitutions were shown to be beneficial for the inhibition of P-gp. These results are important for the screening of flavonoids for inhibitory activity on P-gp.Keywords:flavonoids;P-gp;inhibitory activity;QSAR
研究领域:
药理学
·
肿瘤学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
·
2020
·Vol. 31
·期 6
·2381-2392
·
IF 1.941
Meng Jin,Ren Mingfei,Wang Siyu,Gao Jie,Shan Xiaojing,Hu Jie
Every year, a large amount of waste water containing phenol derivatives is produced in industrial production, which causes serious pollution problem. In the present work, a dually photo- and thermo-responsive adsorbent was developed to remove p -nitrophenol in aqueous solution. N -isopropyl acrylamide was polymerized to build up the thermo-sensitive network of the adsorbent; and cyclodextrin/azobenzene supramolecular complex was grafted on the backbone to act as the photo-responsive adsorbing unit. Under low temperature and 365 nm irradiation, the adsorbent was found in swelling state. In this state, p -nitrophenol was easily caught and removed from aqueous solution by cyclodextrin cavities and azobenzene moieties grafted on the polymer chains. Most interesting, when irradiated at 430 nm, the inclusion of cyclodextrin cavities with azobenzene moieties let freedom of the p -nitrophenol molecules adsorbed previously; at this time if increasing the temperature up to 40 °C, the free p -nitrophenol molecules were forced out owing to the shrinkage of the poly( N -isopropylacrylamide) network. So, without any organic solvent, the adsorbent can be regenerated directly in water. It avoids the secondary pollution caused by traditional regenerating process of adsorbents with organic solvent, which is an important advantage for its practical application of the adsorbent.
研究领域:
环境科学
·
材料科学
✓ 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）