COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Weifan Du,Xianbo Li
The flotation separation of dolomite and fluorapatite is difficult due to the similar surface properties. In this study, carboxymethyl cellulose (CMC) was introduced as a depressant for flotation of dolomite and fluorapatite, the adsorption mechanism of CMC on the mineral surfaces was clarified by DFT calculations, XPS analysis , zeta potential and contact angle measurements. The results showed that CMC exhibited a strong inhibitory effect for dolomite under alkaline conditions due to the surface adsorption. Compared with the adsorption of CMC on two Ca sites or two Mg sites of dolomite (104) surface, CMC preferred to simultaneously adsorb at Ca site and Mg site to form a more stable bridge adsorption, the two O in carboxyl group of CMC could bond with Ca and Mg to form chemical adsorption . However, CMC could not be adsorbed on the surface of fluorapatite, and the presence of CMC did not affect the adsorption of collector on fluorapatite surface to make it hydrophobic. Thus, CMC can be used as an alternative depressant for the selective flotation separation of dolomite and fluorapatite.
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MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Jingxuan Han,Yan Zhang,Zhenfei Chen,Ao Zhang,Xuerong Shi
The rational design and fabrication of high-performance electrochemical sensors for the determination of environmentally hazardous substances, such as fenitrothion, is of great significance and remains a great challenge. Understanding the interaction between fenitrothion and substrates is critical to inform the design of electrochemical sensors. Herein, we have developed an electrochemical sensor based on nitrogen and sulfur co-doped holey graphene (NS-HG) for fenitrothion. NS-HG with high levels of nitrogen and sulfur leaded to excellent conductivity and a fast electron transfer rate. NS-HG modified electrode showed high electrochemical activity towards fenitrothion. The results were supported by density functional theory (DFT) calculations. The adsorption energy calculations and density of states analysis (DOS) showed that NS-HG exhibited strengthened fenitrothion adsorption and fast electron transfer rate by nitrogen and sulfur co-doping. The fenitrothion sensor based on NS-HG showed an excellent analytical response with high sensitivity, low LOD (0.062 ng·ml −1 ), excellent selectivity, stability, and satisfactory recoveries for real samples. This research provides new insights into understanding the synergetic effect of co-dopant, and new opportunities for the rational design of electrochemical sensors.
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Environmental Science-Nano
·
2022
·Vol. 9
·期 9
·3562-3580
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IF 9.473
Zhengwen Wei,Xiang-fei Lü,Wei Wang,Giuseppe Mele,Zhen-Yi Jiang
Owing to the more significant health and environmental risks of 9-phenanthrol (9-PROL) compared to phenanthrene, it is imminent to solve the 9-PROL pollution issue. Herein, Fe3O4-0.75-4,4′-biphenyldicarboxaldehyde (Fe3O4-0.75BIPHENY) was synthesized via a silane coupling reaction and condensation reaction and employed as an efficient nanocomposite for the removal of 9-PROL. The magnetic core provided the possibility for its fast and convenient separation and the aromatic rings on the BIPHENY shell contributed to improving the capturing ability of 9-PROL molecules via the formation of π–π interactions. Multiple characterization techniques were employed to obtain a comprehensive understanding of the prepared magnetic adsorbents. Fe3O4-0.75BIPHENY not only exhibited an excellent adsorption performance towards 9-PROL, but also showed a relatively excellent regeneration performance. The homogeneous surface of Fe3O4-0.75BIPHENY provided adsorption sites for the adsorption of 9-PROL molecules, which adhered in monolayer molecular form. Importantly, density functional theory calculations provided novel deep insights into the most possible adsorption bonding mode and verified that π–π interactions existed in the offset stacking form. Furthermore, the visible electrostatic potential and energy orbital distribution plots demonstrated the validity of the adsorption reaction and stability of a specific configuration. This study provides guidance for the assembly of novel magnetic nanocomposites for alleviating traditional and secondary pollution caused by polycyclic aromatic hydrocarbons.
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ENERGY CONVERSION AND MANAGEMENT
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2022
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IF 11.533
Donghua Xu,Junhao Lin,Shichang Sun,Rui Ma,Mingliang Wang,Jinlong Yang,Juan Luo
Microwave pyrolysis of nitrogen-rich biomass for bio-oil is a green and sustainable pathway to realize energy conversion and produce high-value nitrogenous chemicals. This work selected three typical amino acids (serine (Ser), glutamic acid (Glu), and phenylalanine (Phe)) as nitrogenous model compounds for biomass, and the distribution characteristics and formation mechanisms of the nitrogenous chemicals in bio-oil were studied in depth. Results showed that the amino acid structure and pyrolysis temperature were the crucial factors affecting the distribution and selectivity of nitrogenous chemicals. The nitrogenous chemicals were mainly produced at 200–500 °C from the model amino acids, and the nitrogen in Ser was more prone to accumulating in bio-oil compared with Glu and Phe. At 300 °C, the model amino acids generated numerous amines and cyclic amides through decarboxylation, decarbonylation, and dehydration. Higher temperatures (400 and 500 °C) promoted amines/amides to form nitriles and N-heterocycles, with the releasing of H 2 . Nitriles (including propionitrile and phenylacetonitrile) were typically produced by the straight-chain dehydrogenation of amines. Ser, Glu, and Phe produced N-heterocycles (including pyrazine, pyrrole, 2-pyrrolidone, and indole) based on the cyclization and dehydration between carbonyl and amino compounds, intramolecular dehydration, and cyclization dehydrogenation of phenethylamine, respectively. Finally, the possible formation pathways of the main nitrogenous chemicals were proposed, and the kinetics and thermodynamic analyses were performed through density functional theory (DFT) calculations. The findings could provide theoretical support for the nitrogenous chemicals production from microwave pyrolysis of amino acids and biomass.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Yiqun Chen,Jiandeng Ruan,Baitian Zeng,Wei Jiang,Liting Luo,Qing Shao,Zizheng Liu
This paper offers novel insights into the recently reported cobalt(II) sulfide (CoS) activated sulfite (S(IV)) process. After adding 0.5 g/L CoS and 0.4 mM S(IV) at pH 9.0, 83.1% of acetaminophen (ACP) was removed in 10 min. However, this effect was subject to the inhibition of coexisting chloride or humic acid . Dissolved O 2 played an important role in the reaction. The interactive impacts between S(IV) concentration and initial pH were found the most significant. The CoS/S(IV) system involved synchronous homogeneous and heterogeneous catalysis, which demonstrated sizable ACP degradation. The generated sulfate radical (SO 4 •− ) and hydroxyl radical (HO • ) were primarily responsible for ACP degradation. DFT-based first-principle calculations show the electrons transferred from sulfite to the CoS surface in heterogeneous activation. The pathway of ACP degradation was determined to primarily comprise addition and substitution reactions based on the detected intermediates. Besides, the CoS/S(IV) system demonstrated good reusability and was successful in degrading the other five organics: bisphenol A, metoprolol, estriol, atenolol, and imipramine. The ACP removal performance under real water background was also acceptable. As a result, the CoS/S(IV) system is expected to be a reliable approach for water treatment .
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Kean Chen,Binxian Chu,Qiuju Qin,Xuemei Ou,Runqi Zhao,Xiaoling Wei,Huan Wu,Bin Li,Lihui Dong
As an ideal substitute for the precious metals in the selective catalytic reduction of NO by CO, transition metal oxides perform very well. Thus, a series of CuO - Co 3 O 4 symbiotic oxide porous nanosheet catalysts are prepared with a CTAB-assisted hydrothermal method. Cu5 with the ratio of Cu and Co is 5 : 10, has the best activity on the premise of maintaining the nanosheet structure. Reduction pretreatment of Cu5 with H 2 is carried out, and the surface will be rapidly oxidized in air. In this period, Cu, CuO and Co 3 O 4 were produced and coexisted on surface. Cu5-re-163 exhibits greatly higher N 2 selectivity but a little inferior NO conversion. Further DFT calculation and characterizations proved that [N] free radicals exist during the reaction. The reaction on Cu5 and Cu-re-163 follow L-H and E-R mechanism respectively. [N] radicals on the latter are much easier to desorb, so that they are easy to combine with each other to form N 2 rather than with NO to generate N 2 O, as the reason why Cu5-re-163 has better selectivity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Lingchao Kong,Jun Zhang,Yi Wang,Qinlin Yan,Jiayu Xu,Xi Quan,Charles B. Andrews,Zuotai Zhang,Chunmiao Zheng
Hazardous oxyanions in water bodies are potentially toxic to aquatic life, and the coexistence of multiple anions aggravates the toxicity. Herein, bowknot-like Zr/La bimetallic organic frameworks (Zr/La-BTC) were developed with superior hazardous oxyanion adsorption capacities, i.e., approximately 102 mg/g for arsenate and 159 mg/g for phosphate, respectively. The molar ratio of Zr to La in Zr/La-BTC plays a significant role in the structure and the adsorption efficiencies. Notably, the experiment-derived adsorption capacities of various Zr/La-BTC samples were consistent with their adsorption energies calculated by density-function theory (DFT). Further mechanism analysis revealed that coordination of Zr/La atoms with the target anion groups occurred during adsorption. The positive shift of binding energies in La 3d and Zr 3d XPS spectra and Bader charge analysis unveiled that back-donation interactions dominated the adsorption process . The reliable adsorption selectivity and reusability of 0.1Zr/La-BTC were verified with anion competition experiments and four adsorption-desorption cycles. Overall, this study provides significant insight into the design of high-performance bimetallic organic frameworks for the enhanced removal of hazardous oxyanions from water.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Yingli Zhu,Xiangcheng Li,Pingan Chen,Boquan Zhu
Strong absorption, thin thickness, wide-bandwidth as well as lightweight of microwave absorption materials (MAMs) are highly desirable. In this study, the mesoporous silica skeleton embedded by FeRu/(Fe, Ru) 3 O 4 magnetic nanoparticles (FR/FRO- m SiO 2 ) were designed and fabricated by vacuum impregnation and reduction sintering methods. The minimum reflection loss (RL min ) of the FR/FRO- m SiO 2 composite with a metal mass ratio of 46% was −61.1 dB at a thickness of 2.0 mm, and the covered absorption bandwidth (RL < −10 dB) reached 6.8 GHz. In combination of Density functional theory (DFT) calculation, microstructure characterizations and electromagnetic characteristics, we found that the interface polarization and magnetic enhancement at the interfaces of FeRu-(Fe, Ru) 3 O 4 , the local dipole moment, and the abundant propagation channels for the incident microwaves, endowed by the unique component and construction of FR/FRO- m SiO 2 , contributed together to the excellent microwave absorption capability of FR/FRO- m SiO 2 . This work provides a promising porous structure to broaden efficient bandwidth and strengthen microwave absorption intensity with lightweight.
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HYDROMETALLURGY
·
2023
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IF 4.7
Hongrui Xiang,Zhihui Yang,Xiaobo Min,Yanjie Liang,Cong Peng,Xiaoyun Liu,Rui Yuan,Qingwei Wang,Feiping Zhao
The recovery of germanium (Ge) from zinc residue leachate has attracted increasing attention. Herein, this study report on the development of a tartaric acid functionalized chitosan (TA-CS) material serving as an efficient adsorbent for Ge(IV). The introduction of TA resulted in abundant protonatable hydroxyl and carboxyl groups , which endows materials with excellent buffering capacity under acidic conditions. Adsorption kinetics and isotherms showed a fast and efficient adsorption capacity of 57.28 mg/g for Ge(IV). In binary systems, Ge(IV) was preferentially adsorbed over Zn(II), a major coexisting ion, with a separation factor of 3.22. The SEM–EDS FT-IR, XPS and DFT results revealed that mechanisms in combination, including electrostatic adsorption, complexation, hydrogen bonding, and ion exchange, promoted the immobilization of Ge(IV) on TA. The TA-CS material also exhibited great reusability with an adsorption efficiency of 70% after 3 recycles. For the recovery of Ge(IV) in practical zinc residue leachate, the TA-CS material showed superior affinity toward Ge(IV) and a 10-fold higher of adsorption capacity compared to that of pristine chitosan. Together, TA-CS demonstrates that it is a viable and economical material for the separation and preconcentration of Ge(IV) from zinc residue leachate.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2023
·Vol. 415
·期 14
·2775-2780
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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
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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.
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Arabian Journal of Chemistry
·
2023
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IF 6
Hong Shen,Changwei Zhang,Hao zhou,Chuan Li,Hua Yuan,Jianxin Jiang,Chengzhang Wang
Chlorophyll compounds (Chls) from Ginkgo biloba leaves (GBL) are non-toxic natural pigments characterized by highly conjugated molecules and special spectra, making them ideally potential photosensitizers (PSs) in photodynamics therapy (PDT). In this study, 4 Chls were isolated from Ginkgo biloba polyprenols (GBPPs) wastes by using silica gel column separation and high performance liquid chromatography (HPLC). In addition, two new chlorophyll derivatives were successfully synthesized with chlorin e6 as the primary raw material. To evaluate and identify superior chlorophyll PSs, Density Functional Theory (DFT) and Density Functional Theory (TD-DFT)were employed to decode the microscopic and spectral properties of Ginkgo biloba Chls (GBChls). The spectral absorption, optical stability and reactive oxygen species (ROS) production of GBChls were further analyzed through comparisons of their frontier molecular orbital layout, charge distribution and excitation energy properties. Our results show that about 63 % absorption in the Q band for 14 GBChls comes from the π⇢π* transition from the highest occupied orbital (HOMO) to the lowest unoccupied orbital (LUMO), indicating the favorable delocalization effect of these GBChls. In particular, those GBChls with the long chain of the phytyl group exhibited higher total electron energy and thus could significantly increase the light stability. However, the large spatial volume and hydrophobicity of these compounds with the phytyl group chain was unfavorable for cellular uptake, leading to low ROS in cells. The electronegativity of porphin macrocycles in GBChls positively correlates with the intracellular ROS production rate, meaning that the former likely promotes the energy transfer between PSs and molecular oxygen during type II photoreaction. Among the GBChls, chlorin e6 demonstrated the highest ROS yields in DMF, while purpurin 18 compounds displayed long-wavelength absorption (698 nm), strong Q-band absorption, good optical stability, and high intracellular ROS production. Our findings highlight that chlorin e6 and purpurin 18 are most potential PSs anticancer drugs and offer new research perspectives for the processing and utilization of GBL resources.
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