Processes
·
2023
·Vol. 11
·期 3
·703
·
IF 3.5
Liang Shen,Jiabao Gong,Yifang Liu,Erle Qiao
The molecular structure of cationic surfactants is closely related to their flotation performance. In this paper, three cationic surfactants with different head group structures were selected as collectors of kaolinite, and the substituent effects were studied by the DFT method. The DFT calculation results showed that increasing the number of substituents in the dodecylamine head group can significantly increase its surface and head group charge. Dodecylamine has the lowest LUMO orbital energy, so dodecylamine has the strongest electron attraction ability and the strongest interaction with kaolinite. Electron density differential showed that there was an area of electron aggregation between the collector and the surface of the kaolinite. The interaction energy of DDA on kaolinite surfaces was greater than that of the other two collectors, indicating that the adsorption of DDA on the surface of kaolinite was more stable. Flotation results showed that higher a kaolinite yield was obtained in the presence of dodecyl dihydroxyethyl methyl ammonium chloride. The calculated results of the solvent-accessible surfaces, the head group charge, and the number of bonds between the collector and the kaolinite show good consistency with the actual flotation results of the three collectors, which can be used as a screening index for kaolinite flotation collectors.Keywords:kaolinite;flotation;collector;adsorption;DFT calculation
研究领域:
化学工程
·
材料科学
·
表面化学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Wanli Zhang,Meigui Ou,Chunlin Yang
In this paper, erbium-doped gadolinium oxide rare earth oxide nanoparticles (Gd 2 O 3 :Er 3+ ) with good light absorption capacity from the visible to the infrared region were prepared by polyol method, and then compounded with TiO 2 by hydrothermal method. SEM, TEM, XPS, UV–vis and electrochemical workstation were used to study the morphology, structure, UV–vis light absorption and photoelectrochemical (PEC) properties of Gd 2 O 3 :Er 3+ /TiO 2 . The results showed that the Gd 2 O 3 :Er 3+ spherical nanoparticles with a particle size of about 15 nm were uniformly distributed on the surface of the TiO 2 nanorod array, and the Gd 2 O 3 :Er 3+ /TiO 2 nanocomposites had good light absorption capacity in the infrared region. Furthermore, the photocurrent densities of Gd 2 O 3 /TiO 2 and Gd 2 O 3 :Er 3+ /TiO 2 were 2.08 and 2.75 times higher than those of TiO 2 , respectively, manifesting that the broadening of infrared light absorption can improve the PEC property of TiO 2 . Meanwhile, the DFT calculation results showed that the energy band of Gd 2 O 3 :Er 3+ /TiO 2 was significantly narrower than that of TiO 2 , indicating that Gd 2 O 3 :Er 3+ /TiO 2 had a redshift phenomenon of UV–vis absorption. The calculation results of state density showed that the f orbital of Gd 2 O 3 :Er 3+ intersected with the d orbital of TiO 2 , indicating that there is an electron transfer between Gd 2 O 3 :Er 3+ and TiO 2 .
研究领域:
材料科学
·
光催化
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 12
·2908
·
IF 4.2
Yudong Xie,Xiaowei Wang,Jinfeng Men,Min Zhu,Chengqiang Liang,Hao Ding,Zhihui Du,Ping Bao,Zhilin Hu
The efficient segregation of radioactive nuclides from low-level radioactive liquid waste (LLRW) is paramount for nuclear emergency protocols and waste minimization. Here, we synthesized Na3FePO4CO3(NFPC) via a one-pot hydrothermal method and applied it for the first time to the selective separation of Sr2+from simulated LLRW. Static adsorption experimental results indicated that the distribution coefficientKdremained above 5000 mL·g−1, even when the concentration of interfering ions was more than 40 times that of Sr2+. Furthermore, the removal efficiency of Sr2+showed no significant change within the pH range of 4 to 9. The adsorption of Sr2+fitted the pseudo-second-order kinetic model and the Langmuir isotherm model, with an equilibrium time of 36 min and a maximum adsorption capacity of 99.6 mg·g−1. Notably, the adsorption capacity was observed to increment marginally with an elevation in temperature. Characterization analyses and density functional theory (DFT) calculations elucidated the adsorption mechanism, demonstrating that Sr2+initially engaged in an ion exchange reaction with Na+. Subsequently, Sr2+coordinated with four oxygen atoms on the NFPC (100) facet, establishing a robust Sr-O bond via orbital hybridization.
研究领域:
环境科学
·
核化学
·
理论化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Kai Zhang,Shuwei Chen,Zhaohui Guo,Yingxiong Wang,Yan Qiao
As a renewable resource, the catalytic conversion of xylose has attracted much attention. The epimerization of xylose to lyxose is an important way to obtain the rare sugar lyxose. Current approaches to xylose epimerization encounter several challenges, including the requirement for high temperatures, the use of costly catalysts and a propensity for side reactions that favor the formation of ketoses. CaCl 2 is an environmentally friendly and naturally abundant metal salt that can act as a Lewis acid in catalytic processes. Herein, we demonstrate that CaCl 2 and Et 3 N work synergistically to achieve 68 % lyxose yield under mild conditions. Compared to conventional approaches, which often require harsh conditions or expensive catalysts, our system demonstrates a cost-effective and selective strategy. Moreover, through a combined experimental and computational approach (NMR, isotope tracing and DFT), we provide unprecedented mechanistic insights into the role of calcium complexation in facilitating epimerization. Complexation between xylose and calcium ion was confirmed by NMR titration and Diffusion Ordered NMR Spectroscopy (DOSY-NMR). Isotope experiments further demonstrated that the C1-C2 migration caused the turnover of the hydroxyl group at C2 in the presence of calcium ions. The frontier orbital analysis and deprotonation energy calculation showed that the hydroxyl group at C1 had the lowest deprotonation energy, which initiated the ring-opening process. The DFT calculations reveal that the calcium ions preferentially complex with the hydroxyl groups of xylose, thereby reducing the energy barrier for the C1 proton dissociation and facilitating the epimerization. These findings offer a new perspective on xylose epimerization with Ca-based catalyst.
研究领域:
生物化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Xiongwei Tian,Qiyu Weng,Tao Lyu,Shujuan Wang,Huiqing Wang,XuSheng Wu,Yuqun Zhuo
Selenium (Se) is one of the hazardous trace elements emitted from coal-fired power plants. The Se migration behavior in wet flue gas desulfurization (FGD) slurry is still unclear, and the species of Se in FGD gypsum remains controversial. In this research, the bubbling experiments using simulated slurry with/without gypsum crystallization process were conducted. The experimental results indicated that pure gypsum has poor capability to capture Se components, and only selenite could be trapped in gypsum during its crystal growth stage. Furthermore, the DFT calculation was conducted to provide the microscopic information of Se adsorption and substitution characteristics during gypsum crystallization process. The research findings of this study could help understand the mechanism of Se migration process in FGD slurry, and facilitate the development of effective Se emission control technologies in the future.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Yaming Fan,Yuqun Zhuo,Liangliang Li
SeO 2 adsorption mechanisms on CaO surface were firstly investigated by both density functional theory (DFT) calculations and adsorption experiments. Adsorption of multiple SeO 2 on the CaO (001) surface was investigated using slab model. Based on the results of adsorption energy and surface property, a double-layer adsorption mechanisms were proposed. In experiments, the SeO 2 adsorption products were prepared in a U-shaped quartz reactor at 200 °C. The surface morphology was investigated by field emission scanning electron microscopy (FE-SEM). The superficial and total SeO 2 mass fractions were measured by X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma atomic emission spectroscopy (ICP-AES), respectively. The surface valence state and bulk structure are determined by XPS and X-Ray Diffraction (XRD). The experimental results are in good agreement with the DFT results. In conclusion, the fundamental SeO 2 chemisorption mechanisms on CaO surface were suggested.
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
·
2024
·
IF 5.3
Zhiqiang Wu,Jianhua Chen,Xiaoqin Tang,Ye Chen
Hemimorphite, as a most common Zn–O mineral, is an important source of zinc resources. Oleic acid direct flotation method is effective to recover hemimorphite. However, strong hydration of hemimorphite leads to flotation difficulties, the mechanism of hemimorphite hydration remains unclear. In this study, two hydrated surface models were established through the adsorption of H + ions and –OH groups on hemimorphite surfaces to investigate the influence of hydration on direct flotation of hemimorphite using micro-flotation tests, zeta potential analysis, FTIR measurements and DFT calculations. Experimental results show that pH severely affects direct flotation of hemimorphite. At pH < 9, the surface adsorbs H + ions; at pH > 9, –OH groups are adsorbed on the surface, leading to a rapid decrease in zeta potential. DFT results show that H adsorption shifts Zn 4s orbitals towards the Fermi energy level and leads to hemimorphite surface layer being in an electron-deficient state, promoting the stable sp 3 hybridization of oleic acid (OA) with Zn atoms to form outer-orbital complexes. However, –OH adsorption increases the steric hindrance of Zn atoms and causes an electron-enrichment state of hemimorphite surface layer, hindering the OA-Zn interaction. The study provides new insights into the mechanism of hemimorphite hydration and helps to achieve interface regulation for direct flotation of hemimorphite.
研究领域:
矿物加工
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表面化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2021
·
IF 3.196
Ting-Hong Huang,Cheng Luo,Dan Zheng,Jing-Yang Tan,Yong Liu,Jing Tang
Based on α- and β-naphthylamine, two new diphosphines, N,N-bis((diphenylphos phino)methyl)naphthalen-1-amine ( 1 ) and N,N-bis((diphenylphosphino)methyl)naphthalene -2-amine ( 2 ), have been prepared and characterized by IR, 1 H NMR, 31 P NMR, TG, UV-Vis, XRD and X-ray crystal structure analysis. Structural analysis shows that the two Ph 2 PCH 2 - groups in 1 and 2 are disposed in an anti configuration, and the change of the position of the (Ph 2 PCH 2 ) 2 N-group on the naphthalene moiety results in different spatial configurations of the two Ph 2 P- groups and different weak interactions, such as C-H … π and π–π interactions. DFT studies show that the composition of the HOMOs for 1 and 2 are almost the same (the naphthyl group with admixed N and P atoms), but the ingredients of the LUMOs for 1 are different from that for 2, coinciding with the change of Mülliken atomic charges . Moreover, the emission spectra show that the emissions of complexes 1 and 2 in acetonitrile solution are not similar to those of solid-state samples.
研究领域:
有机化学
·
计算化学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yubin Sun,Shuming Wen,Qicheng Feng,Yanyu Tang,Yongchao Miao,Xu Wang,Zhihao Shen
This work explored the application of sodium lauroyl sarcosinate (SLAS) as a green surfactant in rutile flotation systems. A detailed examination of the flotation behavior and adsorption characteristics of rutile was conducted, particularly under Pb 2+ ion-modified conditions. The experimental methodology incorporated multiple analytical techniques: micro-flotation experiments, surface potential analysis, adsorption quantification, FTIR spectroscopy, SEM-EDS characterization, XPS surface analysis, and computational DFT simulations. Micro-flotation experiments demonstrated that under the optimal conditions (SLAS concentration of 2.8 × 10 −4 mol/L, pH 3), a rutile recovery of 81.49 % was obtained. Notably, as the pH increased, the recovery of rutile exhibited a decreasing trend. Following Pb 2+ modification (8.0 × 10 −5 mol/L) combined with SLAS treatment (2.8 × 10 −4 mol/L), the rutile demonstrated consistent flotation recovery exceeding 90.02 % across a broad pH range (3 ∼ 7). The adsorption capacity experiments and SEM-EDS results indicated that multiple SLAS layers were adsorbed on the rutile. Moreover, Pb 2+ modification improved the favorability of SLAS adsorption. A combination of surface potential measurements and infrared spectroscopy confirmed the chemical adsorption mechanism of SLAS on positively charged rutile surface atoms. XPS characterization confirmed that the SLAS oxygen atoms chemically bonded with the rutile surface Ti/Pb atoms. DFT simulations demonstrated that the adsorption processes were spontaneous, with Pb 2+ and SLAS respectively, forming O − Pb and Ti − O bonds on the (110) surface. This mechanism explains how Pb 2+ enhances the SLAS adsorption capacity and subsequent flotation efficiency of the rutile. These studies proved the industrial potential of environmentally friendly collector SLAs in rutile flotation.
研究领域:
矿物加工工程
·
表面化学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Bingqiao Yang,Pengliang Huang,Qing An
A small molecular triazole derivative called AMT (3-amino-5-mercapto-1,2,4-triazole) was explored as a novel and efficient chalcopyrite depressant in the preferential flotation of chalcopyrite from molybdenite. The flotation performances were comprehensively investigated via micro-flotation tests of singe and mixed minerals with and without Cu collector. The adsorption mechanisms were determined in terms of contact angle, adsorption capacity, and zeta potential, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and DFT calculations. Single mineral flotation results illustrated that the AMT selectively depressed chalcopyrite over a wide range of pH values. Particularly, AMT was able to depress chalcopyrite even in the presence of sodium isobutyl xanthate (SIBX). The contact angle, adsorption capacity, zeta potential, and FTIR results suggested that AMT was preferentially adsorbed on chalcopyrite surface, but it barely interacted with molybdenite. XPS tests and DFT calculations demonstrated that AMT was chemically adsorbed on chalcopyrite surface through the hybridization of S (1) and N (1) 2p orbitals of AMT with the Cu (1) 3d orbital. The bonding between S (1) atom and Cu (1) was much stronger than that between N (1) and Cu (1). Thus, AMT exhibited good potential as a novel depressant due to its excellent selectivity and practicability.
研究领域:
矿物加工工程
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2020
·
IF 3.807
Taotao Fan,Li Chen,Shunguo Qiu,Chanyuan Yang,Lihua Hu,Xiong Peng,Jianwei Zhang,Zongcheng Yan
A hybrid nanocomposite of hierarchical porous zeolitic imidazolate framework-8 / three-dimensional carbon nanotubes (HP-ZIF-8/3DCNTs) has been successfully fabricated by constructing micelle by sodium dodecyl sulfate (SDS) and deep eutectic solvent (DES) aqueous solution to grow HP-ZIF-8 in situ on the 3DCNTs template. The electrochemical performance for detecting dopamine (DA) is greatly improved owing to the synergism of highly conductive CNTs and hierarchical porous ZIF-8. At the same time, the electrochemical reaction of DA on HP-ZIF-8/3DCNTs/GCE is an adsorption control process, and density function theory (DFT) calculation was performed to analysis the charge distribution and interaction force of DA and dopaminophenone in the material, forming a molecular complex with adsorption energy of −19.11 and − 25.21 kJ/mol −1 . In addition, the response current is linear when the DA content is 1.0 × 10 −7 to 1.0 × 10 −4 M, the LOD is 2.7 × 10 −8 M at S/N = 3. The electrode material has excellent selectivity, sterling reproducibility of 2.21% and satisfactory repeatability with a RSD of 1.96%, and splendid long-term stability with peak current maintained 96.03% of the initial value after 14 days. The results indicate that HP-ZIF-8/3DCNTs composite has broad application prospects in the field of electrochemical sensing, and its modification methods and theoretical concepts can potentially be applied to the research of other sensors.
研究领域:
材料科学
·
电化学传感
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
BUILDING AND ENVIRONMENT
·
2020
·
IF 4.971
Ding-Chao Zhang,JunJie Liu,Cong Wang,Yong Liu,Jia-Hua Wang,Xu Han
Given that the toxic hexanal in indoor air is primarily originated from the cooking oil fumes, it is necessary to purify hexanal in the cooking oil fumes to prevent the adverse health effects of hexanal to human beings. In this study, four typical metal-organic frameworks (MOFs), namely MIL-101 (Cr), UiO-66, ZIF-8 and Cu-BDC were synthesized and applied to purify the indoor hexanal, and their adsorption capacities to hexanal were compared with the commercial activated carbon (AC). Our results show that the adsorption capacities of hexanal follow the order of MIL-101(Cr) (135 mg g −1 )> UiO-66 (64.3 mg g −1 )> ZIF-8 (40.3 mg g −1 )> AC (35.8 mg g −1 )> Cu-BDC (32.5 mg g −1 ), and the desorption capacities (by air) follow the order of MIL-101(Cr) (55.5 mg g −1 )> UiO-66 (26.1 mg g −1 )> AC (24.5 mg g −1 )>ZIF-8 (19.3 mg g −1 )> Cu-BDC (5.5 mg g −1 ), indicating that hexanal adsorbed on MIL-101 (Cr)/UiO-66 is more appropriate than the commercial AC to be desorbed. FTIR analysis confirms that O–H in Cr–OH/Zr–OH, O–C–O and aromatic C–H in H 2 BDC in both MIL-101 (Cr) and UiO-66 are possible sites for hexanal adsorption. DFT calculations further reveal that Cr–OH/Zr–OH and aromatic C–H in H 2 BDC are important sites to interact with C O in hexanal. This study provides a possibility to purify indoor aldehyde contaminants by the highly porous MOF materials.
研究领域:
材料科学
·
环境科学
·
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）