ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Pengfei Liu,Fei Luo,Yuxin Rao,Huasong Wang,Xue Li,Miaomiao Yu,Xiang Liu,Shangquan Zhao,Shan Fang
Electrolytes play a crucial role in enhancing the cycling stability and overall lifespan of lithium metal batteries (LMBs). However, conventional electrolytes achieve ununiform and low ionic conductivity solid electrolyte interphase (SEI), leading to uncontrolled lithium dendrite growth and dead lithium formation, rendering them inadequate for meeting the performance of high energy density LMBs. Herein, a 1,2-difluorobenzene (1,2-dFBn) is introduced as antisolvent in fluorinated electrolyte which is composed of fluoroethylene carbonate (FEC) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). The low energy level of the lowest unoccupied molecular orbital (LUMO) and the high fluorine-donating ability of 1,2-dFBn jointly modify the solvation structure and electrode/electrolyte interphase chemistry. As a result, this simple electrolyte formulation enables the Li||Li symmetric cells exhibit remarkable stability, enduring 700 h of continuous cycling under 2 mA cm–2 and Li||Cu cell achieve an impressive average Coulombic efficiency (CE) of 99.76%. Moreover, the full cell assembled with electrochemically deposited lithium capacity of 5 mAh cm–2 and LiFePO4 (LFP) as cathode achieves exceptional performance, maintaining a discharge specific capacity of 134.9 mAh g–1 while retaining 95.1% capacity at 2C after 1000 cycles. This study offers a plausible ratio design for fluorinated electrolyte, which achieving high CE and long-life LMBs.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
LIQUID CRYSTALS
·
2016
·
IF 2.244
Ran Chen,Zhongwei An,Feng Li,Xinbing Chen,Pei Chen
Four series of tolane liquid crystals containing 2,3-difluorophenylene and terminated by a tetrahydropyran (THP) moiety have been synthesised via multistep reactions based on 4-alkylcyclohexanecarboxylic acids and 4-bromo-2,3-difluorophenol. Their properties were measured by differential scanning calorimetry, polarising optical microscopy, Abbe refractometer and an electrical constants instrument. The results show that the THP-based liquid crystals nT reveal a relatively high value of the birefringence, negative dielectric anisotropy, good solubility and a broad nematic mesophase. The effects of the terminal alkyl chain, the lateral fluoro substituents and the THP terminal group on the mesomorphic and physical properties are discussed. Meanwhile, density functional theory calculations of molecular conformation and polarisability were conducted to correlate the experimental findings.
研究领域:
材料科学
·
物理化学
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DOI
高影响因子
Polymers
·
2018
·Vol. 10
·期 4
·427
·
IF 2.935
Fanda Feng,Lingqian Kong,Hongmei Du,Jinsheng Zhao,Junhong Zhang
Three solution-processable D-A-type conjugated polymersP1,P2andP3were successfully synthesized via the Pd-catalyzed Stille cross-coupling copolymerization approach, with 6,8-Dibromo-3,3-bis-decyl-3,4-dihydro-2H-thieno[3,4-b][1,4] dioxepine (M1) and 2,5-Bis(trimethylstannanyl)thiophene (M3) as the donor units and 4,7-Dibromo-5,6-difluoro-2-(2-hexyl-decyl)-2H-benzotriazole (M2) as the acceptor unit, wherein the feed ratio of the three units was 1:3:4 (M1:M2:M3, the same below), 1:1:2 and 3:1:4 forP1,P2, andP3, respectively. The results obtained by our test showed that the feed ratio between the D and A units had a significant effect on both the electrochemical and the spectroelectrochemical properties of the three polymers. The copolymers exhibited a gradually deepening red color in neutral state with the increase of M1 content and then turned to a transmissive grey color in the oxidation state. Also, three copolymers showed good performance in electrochromic parameters, which mainly consists of optical contrast, response time, and coloration efficiency. In general, the excellent electrochromic performances of the copolymers make them outstanding candidates for electrochromic material applications.Keywords:D-A-type polymers;5,6-difluorobenzotriazole;propylenedioxythiophene;electrochromic property
研究领域:
材料科学
·
化学
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DOI
PubMed
高影响因子
Solar RRL
·
2023
·Vol. 7
·期 23
·2300554
·
IF 7.9
Yanqi Ren,Bowen Li,Ying Zhu,Zhihao Zhang,Qi Luo,Hongxin Weng,Xin Tan,Peng Xiang,Xinyu Tan
Perovskite solar cells have rapidly developed into the standard representative of the third generation of photovoltaic power generation due to their low energy consumption and low cost. This device faces many challenges in achieving higher efficiency and better long-term stability. The core issue is the passivation of various defects and appropriate energy-level matching. Herein, the use of potassium pentaminodifluorobenzoate (KAFA) not only improves the light transmittance of SnO 2 /ITO, but also passivates the interface defects of SnO 2 /perovskite by introducing amino, carboxyl, fluorine, and potassium ions. This allows the device to form a suitable energy-level arrangement, thereby greatly improving the performance of perovskite solar cells. Compared with 20.36% of the pristine device, the KAFA-SnO 2 -based device achieves a champion power conversion efficiency of 22.46%, with an increase in short-circuit current from 23.94 to 24.78 mA cm −2 and open-circuit voltage from 1.149 to 1.169 V. After 120 h of continuous illumination with standard sunlight under N 2 atmosphere, its initial efficiency is still as high as 88.8%, showing excellent stability.
研究领域:
材料科学
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能源技术
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DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2025
·
IF 5.2
Meiqiong Yu,Ahai Shahe,Jie Zou,Yixin Hu,Yuxuan Yang,Shucui Han,Jinbei Yang
Difluoroanilines are key fine chemical intermediates, widely used in dyestuff, pharmaceutical, and pesticides, but literature on their thermophysical properties remains limited. In this work, experimental measurements of thermophysical properties were carried out for four pure difluoroaniline isomers (2,6-difluoroaniline, 2,4-difluoroaniline, 2,5-difluoroaniline, and 3,4-difluoroaniline) at atmospheric pressure over defined temperature ranges: density (293.15–353.15 K), dynamic viscosity (293.15–353.15 K), and saturated vapor pressure (336–465 K). For each isomer, 13 data points were collected for density, 13 data points for dynamic viscosity (11 points for 3,4-difluoroaniline due to bubble formation above 343.15 K), and 22 data points for saturated vapor pressure. The instrumental uncertainties are: temperature (±0.02 K for density, ±0.005 K for dynamic viscosity, ±0.1 K for saturated vapor pressure), pressure (±0.2 kPa), density (±5 × 10 −5 g/cm 3 ), and dynamic viscosity (0.1 % relative standard uncertainty). The density-temperature dependence was successfully correlated using the DIPPR equation. Meanwhile, dynamic viscosity data were analyzed via the Litovitz, Ghatee, VFT, and Andrade models, among which the VFT model yielded the most accurate predictions. Furthermore, the Antoine and Riedel equations facilitated precise correlation of saturated vapor pressure with temperature. Additionally, the isobaric thermal expansion coefficient was derived from the density dataset, and the molar vaporization enthalpies of four of the target isomers were estimated employing the Clausius-Clapeyron equation. Collectively, the thermophysical properties of these pure components are crucial for the development and optimization of separation processes involving the four difluoroaniline isomers.
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DOI
高影响因子
ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2022
·
IF 3.858
Ling He,Wenjie Ye,Youyu Xie,Qinghai Liu,Hualei Wang,Dongzhi Wei
Bioreductions catalyzed by ketoreductases play an important role in the synthesis of chiral alcohols. However, the synthesis of (R)-2-chloro-1-(3,4-difluorophenyl)ethanol (24b), an important chiral intermediate for the synthesis of the anticoagulant ticagrelor, poses significant challenges in terms of high substrate concentration requirements that limit its production. In this study, a novel NADH-dependent, short-chain dehydrogenase, PpKR8, from Paraburkholderia phymatum STM815, exhibited excellent enantioselectivity and high activity for the production of (R)-CFPL (24b) through the reduction of 2-chloro-1-(3,4-difluorophenyl)ethanone (24a). The coexpression of PpKR8 and glucose dehydrogenase from Bacillus subtilis in Escherichia coli allowed up to 300 g/L (1.57 M) CFPO (24a) to be completely converted into 24b with 99.9% enantiomeric excess and a high space–time yield (728 g/(L day)). Substrate specificity assays demonstrated a broad substrate spectrum for PpKR8, which included 35 α/β-ketoesters, aromatic ketones, and heterocyclic ketones. Moreover, three additional optically pure chiral alcohols that are used as important drug intermediates were synthesized at high substrate concentrations (150–330 g/L), demonstrating the excellent industrial potential of PpKR8-mediated bioreductions.
研究领域:
生物化学
·
酶工程
·
制药工业
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DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Linghui Kong,Bo Fan,Yu-Cai He
( S )-2-Chloro-1-(3,4-difluorophenyl)-ethanol [( S )-CFPL] is a key chiral intermediate in the manufacture of Ticagrelor. In this study, deep eutectic solvent (DES) was used as the co-solvent, and several reaction parameters were investigated and characterized. It was observed that supplementary of DES could promote the asymmetric reduction of 2‑chloro-1-(3,4-difluorophenyl) ethanone (CFPO) to ( S )-CFPL through the biological reduction by recombinant E. coli containing a NADH-dependent reductase CmCR. The high pKa value of carboxylic acid in DES and low viscosity of DES were beneficial to increase cell membrane permeability and enhancement of biocatalytic efficiency. By supplementary of DES ChCl:LA (7.5 vol%) into the bioreaction system, the efficient bioreduction reaction of 100 mM CFPO was achieved via the biocatalysis with whole-cell at 30 °C and pH 7.0, affording ( S )-CFPL in 95.9 % yield and optical purity > 99 %. The process was environmentally friendly with high biocatalytic productivity and had potential practicability in the mass production of ( S )-CFPL.
研究领域:
生物化学
·
合成生物学
·
绿色化学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Haimin Li,Yanling Tang,Shuqian Liu,Ming Li,Hu Luo,Zheng Zhang,Haohui Li,Yuhao Wei,Bo An,Xingchong Liu,Hanyu Wang
Organic-inorganic hybrid perovskites (PVK) have aroused big enthusiasm of many researchers due to their excellent photoelectric properties. However, PVK films always inevitability demonstrate large number of defects, thus greatly affect the performance and stability of the device. Many parts of the defects are aroused from ion migrations because of the weak antibonding between Pb and I. Here, we use 4-Amino-3,5-difluorobenzonitrile (AFBN) to regulate the light-absorbing layer of perovskite films. The AFBN molecules with donor-π-acceptor (D-π-A) structure can simultaneously interact with MA + /Pb 2+ cations and I - anions in PVK, which can validly inhibit ion migration and effectively restrain non-radiative recombination, thus improves the photoelectric performance of inverted perovskite solar cells (i-PSCs). The AFBN-based device achieved a champion efficiency of 18.55%, which is a high PCE for inverted PSCs with simple structure of FTO/NiO x /perovskite/PCBM/BCP/Ag and for devices with relatively high band gap of 1.62 eV, while the control one only shows an efficiency of 16.37%. Meanwhile, the modified devices demonstrate excellent humidity stability. This work provides a new path for dipoles with donor-π-acceptor structure to inhibit ion migrations for improved efficiency and stability of reverse PSCs.
研究领域:
材料科学
·
光伏技术
·
太阳能
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DOI
高影响因子
ACS Nano
·
2022
·
IF 18.027
Haifeng Tu,Linge Li,Zhicheng Wang,Jian Wang,Hongzhen Lin,Mingchao Wang,Cheng Yan,Meinan Liu
A solid electrolyte interphase (SEI) with robust mechanical property and high ionic conductivity is imperative for high-performance lithium metal batteries since it can efficiently impede the growth of notorious lithium dendrites. However, it is difficult to form such a SEI directly from an electrolyte. In this work, a crowding dilutant modified ionic liquid electrolyte (M-ILE) has been developed for this purpose. Simulations and experiments indicate that the 1,2-difluorobenzene (1,2-dfBen) dilutant not only creates a crowded electrolyte environment to promote the interaction of Li+–FSI–, leading to abundant aggregate ion pairs (AGGs), but also participates in the reduction to construct a robust and high ionic-conductive SEI. With this M-ILE, Li/LiFePO4 cells achieve a capacity retention of 96% over 250 cycles with 9.5 mg cm–2 mass loading, and Li/LiNi0.5Co0.2Mn0.3O2 cells also deliver a discharge capacity of 132 mAh g–1 with a high retention of 88% after 100 cycles. Therefore, the use of a crowding diluent is considered to be an efficient way to construct an advanced SEI for a Li anode.
研究领域:
电化学
·
储能技术
·
材料科学
·
锂离子电池
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DOI
高影响因子
BIOORGANIC CHEMISTRY
·
2022
·
IF 5.307
Hua-Tao Liu,Chun-Yue Weng,Shen-Yuan Xu,Shu-Fang Li,Ya-Jun Wang,Yu-Guo Zheng
Traditional screening methods of enzyme engineering often require building large mutant libraries to screen for potentially beneficial sites, which are often time-consuming and labor-intensive with low mining efficiency. In this study, a novel enzyme engineering strategy was established to modify carbonyl reductase Ls CR for the synthesis of (1 S )-2-chloro-1-(3,4-difluorophenyl) ethanol (( S )-CFPL), which is a key intermediate of anticoagulant drug ticagrelor. The strategy was developed by combining HotSpot, FireProt and multiple sequence alignment, resulting in the construction of a “small and smart” mutant library including 10 mutations. Among them, 5 mutations were positive, resulting in a 50% mining accuracy of beneficial sites. Finally, a highly active mutant Ls CR M3 (N101D/A117G/F147L) was obtained by further screening through saturation mutation and iterative mutation. Compared with wild type (WT) Ls CR, the catalytic activity of Ls CR M3 was increased by 4.7 times, the catalytic efficiency k cat / K M value was increased by 2.9 times, and the half-life t 1/2 at 40 °C was increased by 1.3 times. Due to the low aqueous solubility of the substrate 2-chloro-1-(3,4-difluorophenyl) ethanone (CFPO), isopropanol was used as not only the co-substrate but also co-solvent. In the presence of 40% ( v / v ) isopropanol, Ls CR M3 completely reduced 400 g/L CFPO to enantiomerically pure CFPL (99.9%, e.e. ) in 11 h with a space–time yield (STY) as high as 809 g/L∙d.
研究领域:
酶工程
·
生物催化
·
化学生物学
·
药物化学
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DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2021
·
IF 4.759
Yuhao Han,Panpan Chen,Zhichao Li,Xiao Wang,Chenglong Sun
Ultraviolet (UV) light-catalyzed Paternò-Büchi (PB) reaction has been developed as an efficient lipid C=C double bond (DB) derivatization strategy, which can accurately assign the position of C=C bond in unsaturated lipids when coupled with tandem mass spectrometry (MS/MS). Inspired by this, here we proposed a novel visible-light induced [2+2] cycloaddition reaction combined with ESI-MS/MS and MALDI-MS/MS to identify lipid C=C position isomers. Benz[g]isoquinoline-5,10-dione (BIQD) and 6,9-difluorobenzo[g]isoquinoline-5,10-dione (DF-BIQD) were developed as a new type of [2+2] cycloaddition reagent, which can not only react with C=C bond under 254 nm UV light irradiation, but also quickly combine with lipid C=C bond under the irradiation of 405 nm visible-light and > 400 nm compact fluorescent lamp visible-light. High cycloaddition reaction conversion efficiency can be achieved by irradiating under compact fluorescent lamp light for 2 min. Moreover, we discovered that 437 nm, 489 nm, 545 nm, 581 nm, and 613 nm monochromatic light appearing in compact fluorescent lamp can individually induce the [2 + 2] cycloaddition reaction between DF-BIQD and unsaturated lipids. Using this method, we found that the expressions of lipid DB-positional isomers in rat heart, brain, lung, spleen, thymus, kidney, liver and plasma vary greatly. The relative content of FA-18:1 (Δ9) in rat heart is only 1.49 times that of FA-18:1 (Δ11), while the relative content of FA-18:1 (Δ9) in rat plasma is 5.20 times that of FA-18:1 (Δ11). The above results offer new insight into the development of photocatalytic reagent for visible-light induced [2+2] cycloaddition and structural lipidomic studies.
研究领域:
化学
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生物化学
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分析化学
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脂质组学
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DOI
PubMed
高影响因子
E-POLYMERS
·
2021
·Vol. 21
·期 1
·590-605
·
IF 2.025
Li Zhao,Xianzhi Hu,Futing Zi,Yingmei Liu,Deqiong Hu,Peng Li,Huiling Cheng
In this study, a novel functional monomer N -(1-(2,4-difluorophenyl)-2-(1 H -1,2,4-triazol-1-yl)ethyl)acrylamide (NDTEA) was designed and synthesized, and was used to prepare Ni( ii ) ion-imprinted polymers (Ni( ii )-IIPs). Sixteen kinds of Ni( ii )-IIP (Ni( ii )-IIP 1–16 ) and corresponding non-imprinted polymers (NIP 1–16 ) were prepared by precipitation polymerization method. After optimized condition experiment, Ni( ii )-IIP 5 possessed maximum adsorption capacity and better imprinting factor under optimal experimental conditions which indicated by equilibrium adsorption experiments. The morphology and structural characteristics of Ni( ii )-IIP 5 were characterized by scanning electron microscopy (SEM) and Brunauer–Emmett–Teller (BET). The adsorption selectivity of Ni( ii )-IIP 5 was analyzed by ICP-OES, and the results showed that Ni( ii )-IIP 5 had favorable selectivity recognition ability for Ni( ii ) when Cu( ii ), Co( ii ), and Cd( ii ) are used as competitive ions. The kinetic experiment indicated that the performance of Ni( ii ) adsorption on the surface of Ni( ii )-IIP 5 obeyed the pseudo-first-order model, and adsorption equilibrium was attained after 15 min. Isothermal adsorption process fitted to Langmuir and Freundlich isothermal adsorption models, simultaneously. The results showed that Ni( ii )-IIP 5 prepared by using a new functional monomer had better permeation selectivity and higher affinity for Ni( ii ), which also verified the rationality of the functional monomer design. At the same time, it also provided a broad application prospect for removal of Ni( ii ) in complex samples.
研究领域:
高分子科学
·
环境化学
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材料科学
·
分析化学
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产品关联
DOI
高影响因子
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