SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2014
·
IF 2.129
Shuya Cui,Tao Wang,Xiaoli Hu
A new chiral ionic liquid was synthesized from (S)-1-phenylethylamine and it was studied by IR, Raman, polarimetry, NMR and X-ray crystal diffraction. Its vibrational spectral bands are precisely ascribed to the studied structure with the aid of DFT theoretical calculations. The optimized geometries and calculated vibrational frequencies are evaluated via comparison with experimental values. The vibrational spectral data obtained from IR and Raman spectra are assigned based on the results of the theoretical calculations by the DFT-B3LYP method at 6-311G(d,p) level. The computed vibrational frequencies were scaled by scale factors to yield a good agreement with observed experimental vibrational frequencies. The vibrational modes assignments were performed by using the animation option of GaussView5.0 graphical interface for Gaussian program.
研究领域:
化学
·
理论计算
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Bo He,Lixian Song,Zixuan Zhao,Weibao Liu,Yingtang Zhou,Jiangwei Shang,Xiuwen Cheng
In this study, we used the hydrothermal method and high-temperature calcination method to attach CuFe 2 O 4 to CuO for the first time. The (1 1 1) plane of CuO and (1 1 2) plane of CuFe 2 O 4 formed surface heterojunction, which acts as the interface for adsorbing PMS. Meanwhile, the most stable form of CuFe 2 O 4 /CuO, charge transfer and charge density in CuFe 2 O 4 /CuO/PMS system are proposed by combining density functional theory (DFT) and transmission electron microscope (TEM). The experimental data from electron spin resonance (ESR) determinations and active species capture demonstrated that both nonradical singlet oxygen ( 1 O 2 ) and active radicals (•OH, •SO 4 - ) participate in CIP degradation. The degradation pathways and the intermediates are proposed by Fukui index and liquid chromatography-mass spectrometry (LC-MS). Based on the T.E.S.T program (Toxicity Calculation Software), the bioaccumulation factor, acute toxicity, mutagenicity, and development toxicity of intermediates are proposed. Also, CuFe 2 O 4 /CuO demonstrated good reusability and stability. The findings within this work offered deep insights into the mechanisms of organic pollutants degradation via SR-AOP over Fe-Cu catalyst. Besides, verification of the experimental results indicated that the CIP removal of 86.67% and the mineralization efficiency of 47.17% under optimal conditions. Finally, chemical oxygen demand (COD) and fluorescence spectra in a three-dimensional excitation-emission matrix (3D EEMs) are used to characterize the potential performance of catalyst CuFe 2 O 4 /CuO-500 in medical wastewater.
研究领域:
环境科学
·
材料科学
·
计算化学
✓ 已验证
DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2023
·Vol. 415
·期 14
·2775-2780
·
IF 4.3
Jin Shanxia,Li Yaqin,Yang Liuquan,Li Wei,Zhou Ping
The affinity interactions between boronic acids and sugars have been successfully exploited in many fields, such as the sensing of saccharides, selective enrichment of glycoconjugates, and drug delivery. However, despite multiple techniques having been adopted to investigate the reaction of boronate affinity, the pathway of boronate esters formation under aqueous conditions remains controversial. We report a MALDI-MS approach to investigate the interactions between phenylboronic acid and monosaccharides in neutral aqueous solution by using polylevodopa as an innovative substrate instead of conventional matrix. A series of unusual tri-benzeneboronic esters were then revealed. The mass spectrometry data indicate that they bear a dibenzenepyroboronate cyclic ester moiety with seven-membered ring or eight-membered ring. With the aid of theoretical computations, their most likely geometrical structures are elucidated, and these tri-benzeneboronic esters are proposed to be formed via a boroxine binding monosaccharide pathway. This work provides more insight into the mechanism of boronate affinity interaction between boronic acid and sugars and proves the developed MALDI-MS approach is promising for studying interactions between small molecules. Graphical Abstract
研究领域:
分析化学
·
理论化学
·
糖化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Yingfang Nie,Yu Mei,Youcai Zhu,Yue Mu,Yulong Wu,Li Sun,ZhenHao Xi,Zhen Liu
The copolymerization of carbon dioxide (CO 2 ) and propylene oxide (PO) catalyzed by diethyl zinc/glycerol has been studied by experimental and theoretical approaches. The efficiency of the catalyst is strongly determined by the preparation methods, as the catalyst showed high activity when the catalyst was prepared by dropping glycerol into diethyl zinc. Conversely, the catalyst showed almost no activity when the dropping order was reversed. The order of dropwise addition could change the reaction between diethyl zinc and glycerol, which affects the structure of the catalyst and leads to a change in the catalytic activity. DFT calculations showed that the catalyst is self-assembled and the copolymerization follows a bimetallic coordination-push mechanism.
研究领域:
化学
·
材料科学
·
催化
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 42
·20301-20306
·
IF 6.97
Mingxing Gong,Jing Zhu,Mingjie Liu,Peifang Liu,Zhiping Deng,Tao Shen,Tonghui Zhao,Ruoqian Lin,Yun Lu,Shize Yang,Zhixiu Liang,Seong Min Bak,Eli Stavitski,Qin Wu,Radoslav R. Adzic,Huolin L. Xin,Deli Wang
Rational designing of catalysts to promote the sluggish kinetics of the cathode oxygen reduction reaction in proton exchange membrane fuel cells is still challenging, yet of crucial importance to its commercial application. In this work, on the basis of theoretical DFT calculations which suggest that order structured fct-phased PtFe (O-PtFe) with an atomic Pt shell exhibits superior electrocatalytic performance towards the ORR, the desired structure was prepared by using a scalable impregnation–reduction method. The as-prepared O-PtFe delivered enhanced activity (0.68 A mg−1Pt) and stability (73% activity retention after 10 000 potential cycles) compared with the corresponding disordered PtFe alloy (D-PtFe) and Pt. To confirm the excellent durability, in situ X-ray absorption fine structure spectroscopy was conducted to probe the local and electronic structure changes of O-PtFe during 10 000 cycle accelerated durability testing. We hope that this facile synthesis method and the in situ XAFS experiment could be readily adapted to other catalyst systems, facilitating the screening of highly efficient ORR catalysts for fuel cell application.
研究领域:
材料科学
·
催化化学
·
能源技术
✓ 已验证
DOI
高影响因子
Journal of Nano Research
·
2022
·
IF 1.78
Shui Tuan Lin,Lian Wei Shan,Cheng Guo Ma,Ming Qi Yuan,Zi Lan Fang,Yan Wei Xiao,Li Min Dong,Dan Li,Ying Kui Guo
Heterojunction semiconductor photocatalysis is an auspicious technique for clear up organic pollutants from water, and have been of valuable strategy in the area of photocatalysis. Herein, electrophoretic deposition procedure was used to prepare α-Bi2O3/CdS type-Ⅱ heterojunction photocatalysts. The results of PL, Raman, and EIS show that there is a heterojunction effect in α-Bi2O3/CdS, which is propitious to improve the separation efficiency of photogenerated electron-hole pairs. The DFT calculation reveals that the work function of CdS (4.57 eV) is higher than that of α-Bi2O3 (3.37 eV), which facilitates the migrating of e- from the CB of α-Bi2O3 to the CB of CdS, and the migrating of h+ from the VB of CdS to the VB of α-Bi2O3, thus the e--h+ pairs with high redox ability are retained. The performances were assessed by degrading methyl orange (MO), acid magenta under simulated visible light irradiation. Under simulated visible light irradiation, BC45 composite exhibited the highest degradation efficiency of 87% (MO) and 81% (acid fuchsin) for 4 h, which was about 2 times higher than that of CdS (MO) and (acid fuchsin). It is believed that the dual characteristics of H2O wettability and dye adsorption performance in α-Bi2O3/CdS composites promote photocatalytic process compared with single CdS and α-Bi2O3. The study could provide new insights to develop efficiently capable photocatalysts of the α-Bi2O3/CdS composites.
研究领域:
材料科学
·
环境科学
·
理论化学
✓ 已验证
DOI
高影响因子
HYDROMETALLURGY
·
2024
·
IF 4.8
Huaixin Hao,Yaoyang Liu,Jianhua Yuan,Xue Dong,Zhipeng Wang,Chao Xu,Jing Chen
Cerium (Ce) has become an important strategic resource in high-tech fields owing to its excellent optical, magnetic, acoustic, and electrical properties. The recovery of non-natural Ce derived from nuclear fission through spent fuel reprocessing is of potential significance for the reservation of extremely precious resources. In the present work, Ce 3+ was oxidized to Ce 4+ by NaBiO 3 and then extracted by alkyl phosphate ligands. The extraction efficiency can be enhanced by increasing acidity, raising extractant concentration and decreasing temperature. By taking the advantage of the intrinsic selectivity to tetravalent lanthanides (Ln) by alkyl phosphates, highly efficient and selective extraction of Ce 4+ from other trivalent lanthanides with remarkable separation factor ( SF ) over 10 3 was achieved. Meanwhile, the back extraction of Ce could be accomplished through reducing Ce 4+ to Ce 3+ by H 2 O 2 . Further studies on structure-property relationship by spectroscopic methods and DFT calculations revealed that alkyl substituent groups with more C atoms enhanced the complexation between Ce 4+ and the ligand, while steric hindrance effect could weaken the extractability of Ce 4+ . Moreover, a shorter Ce O bond and a stronger covalent interaction in the Ce 4+ complex, as compared to the Ln 3+ complex, contributed to the excellent selectivity to Ce 4+ over Ln 3+ .
研究领域:
化学工程
·
材料科学
·
核能技术
✓ 已验证
产品关联
DOI
高影响因子
RARE METALS
·
2025
·
IF 11
Pan Jia-Xin,Zhao Long-Sheng,Li Zheng,Feng Zong-Yu,Liu De-Peng,Chen Jun,Huang Xiao-Wei
To achieve selective leaching of ion adsorption rare earth, it is necessary to thoroughly reveal the differences in the adsorption mechanisms of aluminum and rare earth elements. In this study, we investigated the adsorption processes of Dy and Al on the surface of K–homoionic kaolinite using batch experiments and sequential chemical extractions. The results revealed that the adsorption of Dy and Al, as well as the desorption of K, followed the Langmuir model. The maximum ion-exchangeable capacity of Dy was higher (9.39 mmol·kg −1 ) than that of Al (6.30 mmol·kg −1 ). The ion exchange stoichiometry ratios of Dy–K and Al–K derived from the Langmuir model were 2.0 and 2.6. The analysis of X-ray absorption fine structure (XAFS) and density functional theory (DFT) revealed that Dy and Al were adsorbed onto kaolinite as outer-sphere hydrated complexes via hydrogen bonds. Dy was adsorbed as [Dy(H 2 O) 10 ] 3+ , and Al was adsorbed as [Al(OH) 2 (H 2 O) 4 ] + . In particular, the adsorption of Al resulted in protonation of the hydroxyl groups on the surface of the kaolinite. Based on the above insights, the higher ion exchange stoichiometry ratios are attributed to closer adsorption distances (6.04 Å for Dy and 3.69 Å for Al) and lower adsorption energies (− 223.72 kJ·mol −1 for Dy and − 268.33 kJ·mol −1 for Al). The maximum ion-exchangeable capacity is related to the change of the surface electrical properties of kaolinite. The zeta potential was increased to − 7.3 mV as the protonation resulted from aluminum adsorption, while Dy adsorption had a minor effect, maintaining a value of − 17.5 mV. Graphical abstract
研究领域:
矿物学
·
环境科学
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2019
·
IF 6.044
Chunfu Shao,Qiang Shao,Xiaoyi Wang,Jun Ling,Xiao Guo,Yulin Ning,Yujie Dai,Shiru Jia,Yuanyuan Qiao,Changwen Li,Kai Zhao
The OH induced cellulose degradation was examined by analyzing the reaction products of Fenton’s regents with cellobiose. Many degradation products including C2-C5 compounds such as oxaldehyde, malonaldehyde and 2-hydroxysuccinaldehyde were detected by GC MS analysis. Four reaction pathways for the formation of some degradation products were obtained from ReaxFF kinetics simulation and validated by the DFT quantum chemistry calculation at B3LYP/6-31+g(d,p) level. It was found that the H-abstraction from OH of the glucose unit by OH can cause saccharide ring open and breakage of the glycosidic bond. Pathways 1–4 showed that the glucose unit can react with OH consecutively to produce small molecular products with carbon atoms less than 6. This study indicated that ReaxFF reaction kinetics is a powerful tool for the exploration of the degradation mechanism of cellulose induced by OH at room temperature, which correlated well with the experimental results and was validated by DFT calculation.
研究领域:
生物化学
·
计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION B-A JOURNAL OF CHEMICAL SCIENCES
·
2024
·
IF 0.8
Chao Feng,Linlin Zhu,Jing-Jing Guo
A novel 1D Mn(II) coordination polymer, namely, [Mn 3 (bpz) 2 (MeCN) 2 Cl 6 ]
n
( 1 ) was synthesized by a solvothermal method based on bpz and MnCl 2 , where bpz is di(1 H -pyrazol-1-yl)methane. The X-ray diffraction data show that the crystal structure of complex 1 is a one-dimensional polymer with two different coordination modes of the Mn(II) ions. The structure was modelled with Density Functional Theory (DFT) calculations and the intermolecular interactions were analyzed using the Hirshfeld surface method.
研究领域:
化学
·
材料科学
·
理论化学
✓ 已验证
DOI
高影响因子
Journal of CO2 Utilization
·
2023
·
IF 7.7
Xianyao Yan,Chenyu Duan,Shuihua Yu,Bing Dai,Chaoying Sun,Huaqiang Chu
The calcium looping is a promising technology to achieve industrial CO 2 capture, and the introduction of oxygen vacancy can promote the CO 2 capture reactivity of CaO-based sorbents. In this work, DFT calculations were performed to investigate the CO 2 adsorption by CaO in the presence of oxygen vacancy defect. The presence of oxygen vacancy reduces the band gap of CaO surface, which results from the delocalization of Ca 2p orbital. Besides, the electron accumulation at the oxygen vacancy occurs due to the unsaturated Ca-O bonds, and the reaction possibility is promoted neighbouring the defect. The top site of oxygen vacancy defect of CaO is favourable for CO 2 adsorption. The adsorption energy of CO 2 on CaO with oxygen vacancy achieves − 2.52 eV, which is 1.81 times as high as that on pristine CaO. Due to strong interaction between CO 2 and CaO with oxygen vacancy, CO 2 migration from this site is more difficult, while the following diffusion is more prone to occur. In the presence of steam, CO 2 adsorption energy is enhanced to − 2.70 eV on CaO with oxygen vacancy, and the distance from CO 2 radical to surface is intuitively reduced, which results from the electrons donated from defect and neighbouring Ca atoms, while CO 2 diffusion difficulty is increased. This work provides an incisive investigation for structural, electronic, and thermodynamic characteristics of CO 2 adsorption and diffusion on CaO in the presence of oxygen vacancy defect, and it can shed light on rational synthesis and functional design of surface-active sites of CaO-based sorbents.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 41
·94740-94756
·
IF 5.8
Zhao Xiaoben,Chen Guanyu,He Song,Sheng Hongliang,Sun Junwei,Wu Xiya,Tian Fuliang,Zhang Xiaoqian
The cyclohexane is the common toxic volatiles emitted from the various industry in worldwide leading to environmental degradation and human illnesses. Hence, there is a requirement for an efficient and stable adsorbent for adsorbing these toxic molecules to safeguard human health and the air atmosphere. Hollow carbon spheres (HCS) are a new type of carbon nanomaterial with large specific surface area, low density, and good chemical and thermal stability. In this study, DFT simulations and static-dynamic adsorption studies of cyclohexane were carried out using HCS as the adsorbent material. Among them, static adsorption focuses on adsorption/desorption isotherm, adsorption isotherm model fitting and isosteric heat of adsorption. Dynamic adsorption was mainly studied the effect of initial concentrations, gas flow rate, and ambient temperature on adsorption performance. The results showed that HCS exhibited very good performance in cyclohexane adsorption.
研究领域:
环境科学
·
材料科学
·
化学工程
·
计算化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）