ENZYME AND MICROBIAL TECHNOLOGY
·
2021
·
IF 3.493
Yue Shan,Weili Yu,Lijuan Shen,Xuan Guo,He Zheng,Jinyi Zhong,Tao Hu,Yinglun Han
Haloalkane dehalogenase DhaA catalyzes the hydrolytic cleavage of carbon-halogen bonds and produces alcohol, a proton and a halide. However, DhaA suffers from the poor environmental stability, such as sensitivity to high temperature, low pH, hypersaline and organic solvent. In order to improve the environmental stability of DhaA, DhaA was covalently conjugated with inulin, a hydrophilic polysaccharide in the present study. Each DhaA was averagely conjugated with 7∼8 inulin molecules. The conjugated inulin could form a hydration layer around DhaA, which increased the conformational rigidity and decreased the entropy of the enzyme. Conjugation of inulin maintained 75.5 % of the enzymatic activity of DhaA and slightly altered the structure of DhaA. As compared with DhaA, the conjugate (inu-DhaA) showed slightly different kinetic parameters (K m of 2.9 μmol/L and K cat of 1.0 s −1 ). Inulin conjugation could delay the structural unfolding and/or slow the protonation process of DhaA under undesirable environment, including the long-term storage, low pH, hypersaline and organic solvent stability. As a result, the environmental stability of DhaA was markedly increased upon conjugation with inulin. Thus, inulin conjugation was an effective approach to enhance the environmental stability of DhaA.
研究领域:
生物化学
·
酶工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF BIOTECHNOLOGY
·
2021
·
IF 3.307
Meiqi Wang,Weili Yu,Lijuan Shen,He Zheng,Xuan Guo,Jinyi Zhong,Tao Hu
Haloalkane dehalogenase DhaA can catalyze the hydrolytic cleavage of carbonhalogen bonds, along with production of the corresponding alcohol, a proton and a halide. However, DhaA suffers from poor environmental tolerance, such as sensitivity to high temperature, low pH and hypersaline. Arabinogalactan (AG) is a hydrophilic polysaccharide with highly branched long chains. DhaA was conjugated with AG to improve the environmental stability of DhaA in the present study. Each DhaA was averagely conjugated with 4∼5 AG molecules. Conjugation of AG essentially maintained the enzymatic activity of DhaA (91.4 %) without apparent structural alteration. The hydration layer formed by AG could reduce the solvent accessible area of DhaA and slow the protonation process, thereby improving the pH and high salt stability of DhaA. In particular, the remaining activities of the conjugate (AG-DhaA) were 35.3 % after treatment at pH4.0 for 1 h, and 80.8 % in 1 M NaCl after treatment for 16 h. As compared with DhaA, AG-DhaA showed slightly different kinetic parameters (K M of 1.90 μmol/L and k cat of 2.60 s -1).
研究领域:
生物化学
·
酶工程
·
环境生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 10
·5702-5710
·
IF 3.43
Fei Yao,Nan Gong,Wenhui Fang,Zhiwei Men
Halogen bonding, an attractive interaction that is analogous to hydrogen bonding, has been widely investigated by computational methods. However, halogen bonding in solution is hard to study by spectroscopic techniques since the intermolecular interaction often gives overlapping bands and may be difficult to interpret. The traditional interpretation of iodomethane–ethanol mixtures considered only hydrogen bonding effects and the experimental investigation was limited. Here, we employed near-infrared (NIR) spectroscopy, Raman, density functional theory calculation, and two-dimensional (2D) correlation analysis to find evidence of the halogen bonding in iodomethane–ethanol mixtures. Our results suggest that the blue-shifting C–I stretching band is probably due to the cooperative influence from halogen bonding, hydrogen bonding, and the solvent effect, while the O–H band is a cumulative band from three dimer complexes. The 2D correlation spectra further validate the hypothesis above and reveal the interaction evolution from the ethanol-rich region to the iodomethane region. These results indicate that the unique nature of the iodomethane–ethanol mixture and the larger σ-hole strengthen the halogen bond, leading to particular spectroscopic results which are different from those of the other halogenated alkanes.
研究领域:
物理化学
·
光谱学
✓ 已验证
DOI
PubMed
高影响因子
ANALYST
·
2022
·Vol. 147
·期 7
·1341-1347
·
IF 5.227
Chen-Chen Jiang,Xiao-Chong Li,Jian-Ang Fan,Jia-Ying Fu,Xu-Nan Huang-Fu,Jia-Jie Li,Ju-Fang Zheng,Xiao-Shun Zhou,Ya-Hao Wang
The electroreductive cleavage of carbon–halogen bonds has attracted increasing attention in both electrosynthesis and pollution remediation. Herein, by employing the in situ electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) technique, we have successfully investigated the electroreductive dehalogenation process of aryl halides with the thiol group on a smooth Au electrode in aqueous solution at different pH values. The obtained potential-dependent Raman spectra directly reveal a mixture of the reduction products 4,4′-biphenyldithiol (BPDT) and thiophenol (TP). The conversion ratios of the C–Cl and C–Br bonds at pH = 7 are 37% and 55%, respectively. Furthermore, quantitative analysis of the intensity variations of ν(C–Cl), ν(C–Br) and aromatic ν(CC) stretching modes suggests electroreductive dehalogenation via both direct electron transfer reduction and electrocatalytic hydrodehalogenation. Molecular evidence for the C–C cross coupling process through TP reaction with benzene free radical intermediates is found at negative potentials, which leads to the increasing selectivity of biphenyl products.
研究领域:
电化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Optical Materials
·
2025
·
IF 7.2
Chang Gu,Tao Wang,Xian Qin,Xiaogang Liu
Scintillators are essential in applications, such as homeland security, nuclear physics, and geological exploration. However, conventional scintillators often suffer from degradation under polar chemical conditions, resulting in scintillation quenching and structural decomposition. Here, a molecular engineering strategy is demonstrated to enhance scintillator stability and performance through halogen-bonded lattice reconstruction. The synthesis of a copper cluster scintillator, (X-MBA) 4 Cu 4 I 4 (X: Br or Cl, MBA: S -methylbenzylamine) is reported, where halogen bonding improves lattice symmetry and rigidity, effectively suppressing electron-phonon coupling and defect trapping. The halogenated copper clusters exhibit a photoluminescence quantum yield of ≈90%, a 13-fold increase in light yield, and an X-ray detection limit of 28.8 nGy air s −1 , outperforming halogen-free counterparts. These scintillators maintain their structural integrity and performance even after prolonged exposure to polar chemical solvents. The combination of molecular design and structural robustness enables high-resolution X-ray imaging (22 lp mm −1 ) across various chemical environments, paving the way for high-performance scintillators with exceptional durability and efficiency.
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
JOURNAL OF MOLECULAR LIQUIDS
·
2020
·
IF 5.065
Yu Chen,Honglian Liang,Xinbo Qin,Yi Liu,Shuang Tian,Yuanyuan Yang,Shujun Wang
Entrapment of hazardous radioactive iodine has attracted much attention due to the release of radioactive iodine during the application of nuclear energy, such as nuclear waste disposal and nuclear disaster. Deep eutectic solvents (DESs) are deemed as green solvents , designable solvents and solvents of the 21st century. Amino acids are cheap, highly biocompatible and highly biodegradable. Here, we for the first time develop amino acid-based DESs for iodine capture with high efficiency. Effect of structural factors (e.g., mole ratio, composition and composition) and external factors (e.g., mass, concentration and volume of iodine solution) on iodine capture is comprehensively studied. Cysteine:lactic acid (1:8) owns the highest rate and capacity for iodine capture, which shows similar efficiency with previous reports but owns lower cost and higher biodegradability . The high iodine-capturing efficiency of cysteine:lactic acid (1:8) is ascribed to the dominating halogen-bonding interaction (ca. 90%). This work opens a new route for the sustainable capture of radioactive iodine with high efficiency.
研究领域:
环境科学
·
核能工程
·
化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2024
·
IF 3.3
Jingjie Tang,Luying Xie,Jiayu Liu,Shangyu Shi,Qikun Yang,Bo Zhang,Yingying Wang,Lin Chen,Shaohui Jia,Mingfang Ma,Zengyang Xie
Highly efficient and practical carbon–chalcogen (S, Se) and amide bonds formation methodologies for the synthesis of thio- and seleno-acetamides were developed, via the base-promoted one-pot two-step reactions of 2-amino(benzo)thiazoles and aryl acetyl chlorides with dichalcogenides. This cross-coupling reaction afforded the goal products that had been chalcogenated regioselectively in moderate to good yields. Further transformations of the new synthesized compounds, DFT calculations and preliminary mechanism studies are discussed as well.
研究领域:
有机化学
·
计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Forensic Chemistry
·
2024
·
IF 2.6
Boyan Li,Qiongyao Ning,Wenyou Ye,Qianxi Wang,Haili Yu,Xuecheng Chen,Yi He
Colorimetric assays are inexpensive and attractive tools for the detection of fentanyl (FTN), yet further enhancing their sensitivity remains a major challenge. Herein, we develop a halogen-bond mediated visual competitive colorimetric assay for FTN using Erythrosine B (EB) as a probe. The addition of poly(ethylene oxide)-block-poly(propylene oxide)-block-poly(ethylene oxide (F-127) induces the EB aggregation, strongly suppressing the background signal. Upon the introduction of FTN, the subsequent competitive reaction displaces F-127 to generate EB-FTN charge-transfer complexes via N … I halogen bonds between electron-rich amine groups and electron-deficient iodine sites, accompanying a significant absorbance wavelength shift and pink-to-purple color change. The limits of detection of this approach for FTN are 2 mg·L −1 by the naked eye and 0.19 mg·L −1 by UV–vis spectroscopy, which are approximately 3.7-fold to 4 orders of magnitude more sensitive than the reported colorimetric assays. Meanwhile, the present method is well applied for FTN-spiked domestic sewage samples, and an easy-to-use smartphone-based digital image colorimetry is also fabricated. It is expected that such an assay can play a key role in alleviating the worldwide opioid overdose crisis.
研究领域:
分析化学
·
药物检测
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTAL GROWTH & DESIGN
·
2025
·
IF 3.4
Ze-Jiang Xu,Hua-Kai Li,Mei-Ling Ren,Liang-Han Shen,Xiang Zhang,Zi-Ao Qiu,Chao Shi,Li-De Yu,Na Wang,Heng-Yun Ye,Le-Ping Miao
Long-range order of electric dipoles means important physical properties such as ferroelectricity or antiferroelectricity, making materials have broad applications in information storage, sensors, switches, and optical electric devices. However, the orientation control of electric dipoles remains a great challenge on a molecular/ion level. Herein, we report the realization of ferroelectric order via Cl–Cl halogen-bond interactions in hybrid double perovskite [CH2ClN(CH3)3]2NaRuCl6 (TCNRC) derived from [(CH3)4N]2NaRuCl6 (TNRC) for the first time. TCNRC shows spontaneous polarization (Ps = 2.67 μC cm–2) and piezoelectricity (d33 = 4 pC N1–) with a Curie temperature (Tc) of 320 K. This study reveals the important role of halogen-bonding interactions to form ferroelectric orders and provides new insights into the molecular level regulatory polarity in molecular ferroelectric systems.
研究领域:
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
Soft Matter
·
2019
·Vol. 15
·期 31
·6411-6417
·
IF 3.399
Xun Tong,Yuan Qiu,Xiaoyu Zhao,Bijin Xiong,Rongzhen Liao,Haiyan Peng,Yonggui Liao,Xiaolin Xie
Photoresponsive supramolecular gels have aroused continuous attention because of their extensive applications; however, most studies utilize UV light, which inevitably brings about some health and environmental issues. The halogen bond is an important driving force for constructing supramolecules due to its high directionality, tunable strength, good hydrophobicity, and large size of the halogen atoms. Yet, it still remains a formidable challenge to utilize halogen bonds as a driving force to fabricate a visible light responsive gel. In this work, to fabricate such a gel, azopyridine-containing Azopy-Cn (n = 8, 10, 12) was selected as a halogen bond acceptor, while 1,2-bis(2,3,5,6-tetrafluoro-4-iodophenyl)diazene (BTFIPD) was chosen as both the halogen bond donor and visible light responsive moiety. The visible light response of BTFIPD resulted from the significant separation of n–π* energy levels between trans and cis isomers due to the introduction of an electron-withdrawing group (fluorine) to azobenzene at the ortho-position. Interestingly, the gel exhibited a good gel-to-sol transition behavior upon green light irradiation. At the same time, the morphologies varied from uniform narrow flakes to broad sheets with increasing illumination time. We provide an environmentally-friendly visible light-triggered method to regulate the phase transition of supramolecular materials in applications ranging from energy conversion to information storage.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2024
·
IF 15.8
Jieqing Shen,Wensheng Tian,Shuohan Liu,Hui Pan,Cheng Yang,Hengdao Quan,Shenmin Zhu
The low ionic conductivity of poly(ethylene oxide) (PEO)-based polymer electrolytes at room temperature impedes their practical applications. The addition of a plasticizer into polymer electrolytes could significantly promote ion transport while inevitably decreasing their mechanical strength. Herein, we report a supramolecular plasticizer (SMP) to break the trade-off effect between ionic conductivity and mechanical properties in PEO-based polymer electrolytes. Accordingly, the SMP is constructed by tetraethylene glycol dimethyl ether (G4) and SbF3 through halogen bonds. The SMP-plasticized PEO electrolyte (PEO/SMP) presents a simultaneously enhanced ionic conductivity of 2.4 × 10–4 S cm–1 (25 °C) and a high mechanical strength of 8.1 MPa, compared to those of pristine PEO-based electrolytes. Benefiting from the halogen bonds between G4 and SbF3, the Li–O coordination in PEO/SMP is evidently weakened, and thus rapid Li+ transport is achieved. Furthermore, the PEO/SMP electrolyte possesses a wide electrochemical stability window of 4.5 V and, importantly, derives an inorganic-rich SEI with a low interfacial resistance on a lithium metal surface. By using PEO/SMP, the lithium-metal battery with the LiNi0.5Co0.2Mn0.3O2 cathode exhibits a good rate and long-term cycling performance with a capacity retention of 75.3% (500 cycles). This work offers a rational guideline for the design of polymer electrolytes suitable for high-performance lithium-metal batteries.
研究领域:
材料科学
·
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
THIN SOLID FILMS
·
2019
·
IF 1.888
Jian He,Aisen Li,Yanchun Tao,Ning Chu,Zhixiang Wang,Shuping Xu,Jing Wang,Houyu Zhang,Jingsheng Yu,Weiqing Xu
A two-dimensional (2D) co-crystal composed of 1, 3, 5-trifluoro-2, 4, 6-triiodobenzene and 4, 4′-trimethylenedipyridine via halogen bonding (I···N) was obtained on highly-oriented pyrolytic graphite , and was characterized by scanning tunnelling microscope supplemented by the density functional theory calculation. Its special structure at the interface was further compared with its three-dimensional (3D) co-crystal structure. No orderly structures were observed when Au (111) was applied. The 2D co-crystal grown on the interface is significantly different from the 3D co-crystal. This study is of vital significance in understanding the growth mechanisms of 2D functional co-crystals.
研究领域:
材料科学
·
化学
✓ 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）