CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Pengsen Zhao,Haizhong Zheng,Guifa Li,Yongxiang Geng,Yixin Xiao,Hongbo Guo,Ping Peng
The CaO–MgO–Al 2 O 3 –SiO 2 (CMAS) corrosion resistance of La 3+ -Yb 3+ -Ce 4+ co-doped ZrO 2 (LYZC) ceramic was systematically discussed via experiment and first-principles calculation. Results demonstrate that at the CMAS/RE-ZrO 2 interface, RE is dissolved in molten CMAS to form some RE-apatite particles, which effectively inhibits CMAS penetration. Compared with La 3+ doped ZrO 2 (LZ), LYZC owns a better ability to maintain the coating microstructure under CMAS corroded, which is conducive to alleviating CMAS penetration. This conclusion is also confirmed by the low diffusion coefficients ( D ) of RE and Zr in CMAS/LYZC(111), which are only 2.305–5.556 × 10 −8 m/s and 2.694–3.421 × 10 −8 m/s, respectively. Furthermore, the small electrostatic potential difference (Δ V = 1.578–1.654 eV) of the CMAS/LYZC(111) terminal layer suggests that molten CMAS does not easily adhere to the LYZC surface.
研究领域:
材料科学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2024
·
IF 5.9
Yongheng Ren,Yang Chen,Hongwei Chen,Lu Zhang,Jiangfeng Yang,Qi Shi,Lin-Bing Sun,Jinping Li,Libo Li
The identical molecular size and similar physical properties of carbon dioxide (CO 2 ) and acetylene (C 2 H 2 ) make their adsorptive separation extremely challenging to achieve with most adsorbents. Reports on the separation of CO 2 and C 2 H 2 mixtures by zeolites are even rarer with the mechanism of adsorptive separation requiring further exploration. In this paper, we report that ion modulation of zeolite 5A promotes the difference in kinetic diffusion of CO 2 and C 2 H 2 , realizing the inverse separation of zeolite from selective adsorption of C 2 H 2 to selective adsorption of CO 2 . Creating a compact pore space restricting the orientation of gas molecules enables charge recognition. The positive electrostatic potential at the pore openings was utilized to hinder the diffusion of C 2 H 2 between the cages while ensuring the transfer of CO 2 , increasing their diffusion differences in pore channels and leading to the CO 2 /C 2 H 2 kinetic selectivity of 31.97. Grand canonical Monte Carlo (GCMC) simulation demonstrates that the CO 2 distribution in K-5A- β is significantly higher than that of C 2 H 2 . Dynamic breakthrough experiments verify the excellent performance of material in practical CO 2 /C 2 H 2 separation, for CO 2 /C 2 H 2 (50/50 and 1/99, V/V) mixtures can be separated in one step, thus directly generating high purity C 2 H 2 (> 99.95%), which provides a promising thought for the zeolite-based separation of CO 2 and C 2 H 2 .
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Zhixue Ma,Xupeng Zong,Qiang Hong,Lijuan Niu,Tianyu Yang,Wenshuai Jiang,Dan Qu,Li An,Xiayan Wang,Zhenhui Kang,Zaicheng Sun
Although the carbon nitrides copolymers (CNs) exhibit enhanced photocatalytic performance, the essential reason remains unclear. Systematic research on incorporated molecules with structure similarity but different natures helps gain a fundamental understanding of CNs photocatalyzed reactions. A series of dihydroxyl-N-heterobenzene with a different number of N atoms and at different positions of the six-member ring are selected for constructing CNs. Structural identifications demonstrate N-heterobenzene links with heptazine of CN networks at the hydroxyl sites in the synthesized CNs. The theoretical calculation reveals that the electrostatic potential (ESP) of asymmetry pyridine strongly induces the HOMO and LUMO separation, located at different heptazine units. This is significantly different from the traditional heterojunction or D-A system. A kinetics study of CNs/triethanolamine system for photocatalysis was carried out with photovoltage spectra of CNs series. The linear- relationship between extraction charge and H 2 generation rate suggests a Volmer-Heyrovsky mechanism which is commonly acknowledged for electrocatalysis but barely mentioned in photocatalysis .
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-9
·
IF 17.694
Liu Yuan,Liu Junhui,Xiong Hanting,Chen Jingwen,Chen Shixia,Zeng Zheling,Deng Shuguang,Wang Jun
Efficient adsorptive separation of acetylene (C 2 H 2 ) from carbon dioxide (CO 2 ) or ethylene (C 2 H 4 ) is industrially important but challenging due to the identical dynamic diameter or the trace amount. Here we show an electrostatic potential compatible strategy in a nitroprusside-based Hofmann-type metal-organic framework, Cu(bpy)NP (NP = nitroprusside, bpy = 4,4’-bipyridine), for efficient C 2 H 2 separation. The intruding cyanide and nitrosyl groups in undulating one-dimensional channels induce negative electrostatic potentials for preferential C 2 H 2 recognition instead of open metal sites in traditional Hofmann-type MOFs. As a result, Cu(bpy)NP exhibits a 50/50 C 2 H 2 /CO 2 selectivity of 47.2, outperforming most rigid MOFs. The dynamic breakthrough experiment demonstrates a 99.9% purity C 2 H 4 productivity of 20.57 mmol g −1 from C 2 H 2 /C 2 H 4 (1/99, v / v ) gas-mixture. Meanwhile, C 2 H 2 can also be captured and recognized from ternary C 2 H 2 /CO 2 /C 2 H 4 (25/25/50, v/v/v ) gas-mixture. Furthermore, computational studies and in-situ infrared spectroscopy reveal that the selective C 2 H 2 binding arises from the compatible pore electro-environment generated by the electron-rich N and O atoms from nitroprusside anions.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Kai Xu,Rui Chen,Tianhua Wang,Lijie Sun,Qibo Wang,Jinkang Ma,Degao Zhong,Lifeng Cao,Bing Teng
Recent advance of the organic nonlinear optical (NLO) crystals on the design, synthesis and characterization of 2-(3,4-Dimethoxystyryl)-3-methylbenzothiazolium-benzenesulfonate (DOBS) is reported. It is found that crystal belongs to the triclinic system, with the space group P 1. The second harmonic generation efficiency is 1.8 times higher than the standard KDP. Based on density functional theory (DFT), the maximum first-order hyperpolarizability of DOBS molecule is obtained by Gaussian calculation β max is 107.7 × 10 − 30 esu. The molecular surface electrostatic potential, HOMO-LUMO orbital, ELF/LOL, Hole-electron, Hirshfeld surface and 2-D fingerprint were analyzed. The thermal stability analysis shows that DOBS crystal has a high melting point of 251 °C. In addition, UV-Vis-NIR spectra, dielectric properties and fluorescence were investigated.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
·
2021
·
IF 3.178
Rongguan Lv,Xuehua Zhang,Rong Xing,Weizhong Shi,Hongkun Zhao,Wanxin Li,Abolghasem Jouyban,William E. Acree
The intermolecular interactions and overall charge distribution of curcumin were respectively investigated by using Hirshfeld surface analysis and molecular electrostatic potential surface. The mole fraction solubility magnitudes of curcumin (I) in aprotic co-solvent blends of DMSO + water, acetone + water and acetonitrile + water ranging from 278.15 to 318.15 (333.15) K under 101.1 kPa was obtained by means of shake-flask method. Under the same conditions, e.g. identical temperature and mass fraction of DMSO (acetone or acetonitrile), the equilibrium solubility of curcumin was greater in DMSO + water blends than in acetone/acetonitrile + water blends. The lowest solubility magnitude was found in neat water at 278.15 K; and the highest one, in acetone/acetonitrile at temperature of T = 318.15 K (aqueous solutions of acetone or acetonitrile) or 333.15 K (aqueous solutions of DMSO). No crystal transition and solvate formation occurred in experimental processes as documented through X-ray power diffraction analysis. The acquired data were correlated by means of the Jouyban-Acree model, Apelblat model and modified van’t Hoff-Jouyban–Acree model. The preferential solvation at 298.15 K was investigated by the approach of inverse Kirkwood–Buff integrals. The parameters of preferential solvation for DMSO, acetone or acetonitrile were positive in the above three blends with middle and DMSO/acetone/acetonitrile-rich composition ranges, which specified that preferential solvation of curcumin was made by co-solvent. The extended Hildebrand solubility approach was further employed to describe the mole fraction solubility at 298.15 K in DMSO/acetone/acetonitrile + water blends studied in the current work and in ethanol/ n -propanol/isopropanol/PG + water blends reported previous by us, obtaining average relative deviations < 5.21%.
研究领域:
药理学
·
化学
·
药物化学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTAL GROWTH & DESIGN
·
2022
·
IF 4.01
Lan Fang,Yiming Ma,Yuntian Xiao,Zhonghua Li,Zhenguo Gao,Songgu Wu,Sohrab Rohani,Junbo Gong
The formation of multicomponent crystals depends on many factors; therefore it is extremely challenging to predict and select the appropriate coformers (CCFs) to prepare functional multicomponent crystals. In this study, we selected the 2,4-dichlorophenoxyacetic acid (2,4-D) molecule and 10 N-heterocyclic compounds with similar structures to investigate the main factors affecting the synthesis of multicomponent crystals. On screening of multicomponent crystals by solution crystallization, we obtained nine kinds of multicomponent crystals of 2,4-D with different colors, including a hydrate of the 2,4-D-PYE cocrystal. However, 1,3-bis(4-pyridyl)propane (BPP) failed to form multicomponent crystals with 2,4-D using the solution crystallization methods. The influence of CCF on the formation of multicomponent crystals was discussed from three aspects: hydrogen bond donor and acceptor capacity (molecular electrostatic potential (MEP) surface, hydrogen bond acceptor ability h_ema calculated by Molecular Operating Environment software, and interaction site-pairing energy differences (ΔEsite-pair)), thermodynamic enthalpy (the excess enthalpy ΔHex), and structural factors (molecular complementarity (MC) and molecular flexibility (Kier flex)). Molecular flexibility is the main reason no multicomponent crystals are formed between BPP and 2,4-D. A logistic regression calculation indicates that the formation of multicomponent crystals of 2,4-D is mainly affected by ΔEsite-pair and MEP values. The cases considered in this study not only expand the crystal structure landscape of the 2,4-D but also provide a reference for the effective prediction and design of multicomponent crystals, in general.
研究领域:
化学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Polymer Materials
·
2024
·
IF 4.4
Jianjun Wang,Dongning Li,Xueqing Liu,Jiao Liu,Zhichun Shi,Yu Zang,Toshiki Aoki
Nuclear energy, as an efficient and clean energy source, has been widely used in recent years, and the extraction of uranium from water resources is of great significance. Herein, a porphyrin-based hyper-cross-linked polymer with functional amidoxime groups (HCP-TPP-AO; TPP = tetraphenyl porphyrin, AO = amidoxime group) was successfully prepared and used for uranium adsorption. Owing to its abundant porous morphology and the strong chelation of amidoxime/TPP groups to uranium, HCP-TPP-AO removed 94.2% of uranium ions from aqueous solutions. The kinetic behavior of uranium adsorption on HCP-TPP-AO was comprehensively investigated and was consistent with the kinetic process dominated by chemical adsorption. HCP-TPP-AO also preferentially adsorbed U(VI) rather than other competing ions and exhibited a distribution coefficient (Kd) of up to 8.12 × 104 mL/g. Furthermore, the HCP-TPP-AO adsorbent could maintain 84.6% of its adsorption capacity after seven reuse cycles without any changes in its chemical structure or porous morphology. Electrostatic potential (ESP) analysis and adsorption calculations proved that amidoxime groups and TPP units in the polymer network of HCP-TPP-AO made a great contribution to the U(VI) adsorption capacity.
研究领域:
材料科学
·
环境科学
·
核能技术
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Kunpeng Wang,Hongjing Tian,Guosheng Li,Yingjie Dai,Jingtao Wang,Guoli Zhou,Ming Qiu,Wenpeng Li,Lijuan Wang
The separation and recovery of indium from smelting wastes is of great importance. The development of an adsorbent material with high selectivity and easy handling and recovery for the selective adsorption of In(III) remains a challenge. Polyacrylonitrile modified nanofiber membranes (P-PAN) enriched with amine and phosphonic acid groups were prepared for highly selective adsorptive separation of In(III). The adsorption capacity of the resulting membranes for In(III) in solution was 55.05 mg·g −1 , and the adsorption regeneration rate of the membranes was more than 90 % after seven cycles. The separation factors of the P-PAN nanofiber membranes for β In/Fe , β In/Cu , β In/Zn and β In/Pb in a five-member mixed solution were 209.6, 397, 462.6, and 259.6, respectively. Experimental and theoretical calculations show that the joint action of P OH and P O in the P-PAN nanofiber membranes to form an electron-rich region makes the electrostatic potential energy in this region reach the maximum negative value (−52.02 kcal/mol), which is strongly attracted to In(III). In addition, the adsorption energy of P-PAN nanofiber membranes for In(III) was −494.56 kcal/mol, which was much higher than that of competing ions such as Fe(II), Cu(II), Zn(II), and Pb(II). The findings support the feasibility of regulating the binding capacity of adsorption sites to target metal ions via the protonation of –NH, thereby enhancing selectivity towards these ions.
研究领域:
材料科学
·
环境科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
·
2024
·
IF 2.2
Haoyang Xie,Yuan Gao,Zichao Guo,Wanghua Chen
The experimental solubility of β -octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX) in binary solvent mixtures of sulfolane + (H 2 O, acetonitrile, and ethanol) was measured at temperature ranging from (298.15 K to 343.15 K) by dynamic method under atmospheric pressure. The results showed that the solubility of β -HMX monotonously increases with increasing mole fraction of sulfolane at a given temperature in the studied binary solvent mixtures. Furthermore, the experimental solubility data in binary solvents were fitted using the modified Apelblat equation, the GCM model and the Jouyban-Acree model successfully. Hirshfeld surface analysis and molecular electrostatic potential (ESP) were employed to visualize close contacts and charge distribution of β -HMX and solvents. In addition, the molar dissolution thermodynamic properties of the solution of different binary solvent mixtures, such as Gibbs free energy, enthalpy and entropy, were calculated and analyzed based on the van’t Hoff equation and the experimental solubility data. Solid-liquid surface tension and surface entropy factor of β -HMX were estimated by the experimental solubility data. The solubility of β -HMX in sulfolane based binary solvent systems will provide essential support for the further study of crystallization and spheroidization of β -HMX in industry.
研究领域:
化学工程
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
·
2023
·
IF 2.6
Fanfan Li,Yanxun Li,Yameng Wan,Hanyu Lv,Chenyang Xu,Xiaoqiang Gao,Yi Yu
As an important raw material in industrial production, the solubility studies of 1,4-cyclohexanedione (14CHD) in organic solvents may be of assistance in improving crystallization efficiency and yield in industry. Therefore, this work deeply explored the dissolution behavior of 14CHD by using the isothermal saturation method, model fitting and density functional theory (DFT) calculation. Firstly, we selected ten pure organic solvents that are environmentally friendly to measure the solubility of 14CHD at the temperature range of 278.15 ∼ 313.15 K under standard atmospheric pressure. According to the measurement results, the solubility of 14CHD increases with temperature, and there are some differences among the solubility of 14CHD in various solvents. For instance, it has a highest solubility in acetonitrile ( x 1 = 0.5331) at 313.15 K while has the lowest solubility ( x 1 = 6.757 × 10 -4 ) in cyclohexane at 283.15 K. Whereafter, the measured solubility data was correlated by Van't Hoff equation, modified Apelblat equation, λh model, Yaws model and Wilson model. Among them, Yaws model represents the most accurate fitting outcomes. At the same time, the study results of mixing thermodynamic properties on the basis of Wilson model suggest that the dissolution processes of 14CHD in ten organic solvents are entropy-driven and spontaneous. Afterwards, in order to explain the large difference in solubility of 14CHD in ten organic solvents, we found that the dissolution of 14CHD depends mostly on the polarity ( π ) and cohesive energy density (CED), viewed from the physicochemical factors of solvents. Furthermore, we further studied intermolecular interactions between 14CHD and ten solvents through molecular electrostatic potential surface (MEPS) analysis and DFT methods. Results display that alcoholic and non-alcoholic solvents molecules have different sites of action with 14CHD and the absolute values orders of interaction energies of alcoholic and non-alcoholic solvents are all consistent with corresponding solubility laws. The solvent–solute interaction plays an important role in the solubilities of 14CHD.
研究领域:
化学工程
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 17
·9768-9776
·
IF 3.119
Bo Wu,Jingmeng Huang,Zeman Lv,Ziya Cui,Guanghui Hu,Jiye Luo,Mohamed S. Selim,Zhifeng Hao
In order to search for an effective alternative to cyanide for gold plating, mercaptosuccinic acid (MSA) was selected as the complexing agent of Au+ by open circuit potential tests and gold plating compared with 1-hydroxyethylidene-1,1-diphosphonic acid and aminomethylphosphonic acid. For the first time, a novel, stable, slightly acidic and cyanide-free gold plating bath was prepared. Scanning electron microscopy, Tafel tests, and tin dipping tests showed that the Cu/Ni–P/Au coating had a fine and even grain size, no black pad, good corrosion resistance, and good weldability. Quantum chemical calculations based on density functional theory were used to further study complexants and complexes. Molecular electrostatic potential indicates that Au+ approaches MSA in the direction of CO. Frontier molecular orbital theory, atomic contribution to orbital composition, condensed local softness, and average local ionization energy indicate that the coordination capacity of the S atom in MSA is much stronger than that of other atoms. Fuzzy bond order analysis shows that the S–Au–S coordination structure is the most stable form in the plating solution. UV-visible absorption spectroscopy clarifies that the wavelength is redshifted when MSA–Au(I) ions form.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）