Journal of Water Process Engineering
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2024
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IF 6.3
Huijiao Wang,Siyuan Xue,Weiyi Wang,Fan Gao,Shizuo Yi,Jiayin Li,Yuxin Yang,Erzhuo Zhao,Jianchao Wang,Jianbing Wang
In this study, an efficient Ti/SnO 2 -Sb 2 O 3 /CNT-Ce-PbO 2 electrode was fabricated for triclosan electro-oxidation by co-doping the transition metal Ce and carbon nanotubes (CNTs) into the PbO 2 active layer . Characterization results show that the co-doped Ce and CNTs present a synergistic effect on covering the obvious cracks on the Ti/SnO 2 -Sb 2 O 3 surface, decreasing the PbO 2 crystal size, increasing the electrode oxygen evolution potential from 1.60 to 2.17 V vs SCE, and reducing the charge transfer resistance by 66 %. Consequently, Ti/SnO 2 -Sb 2 O 3 /CNT-Ce-PbO 2 was the most effective and energy-efficient electrode for hydroxyl radical (•OH) generation and triclosan electro-oxidation in this study. Compared with other two electrodes (Ti/SnO 2 -Sb 2 O 3 and Ti/SnO 2 -Sb 2 O 3 /Ce-PbO 2 ), triclosan removal by Ti/SnO 2 -Sb 2 O 3 /CNT-Ce-PbO 2 was accelerated by 1.8–2.6 times, with the energy demand for abating 90 % triclosan (E EO ) decreased by 49 % – 67 %. Furthermore, triclosan degradation pathways were proposed based on density functional theory (DFT) calculation and transformation product (TP) identification, with •OH addition at C14 and C11 sites being the most favorable pathway. In addition, the estimated acute and chronic toxicities of TPs were generally decreased than their mother compound. Therefore, the results of this study suggest the feasibility and effectiveness of the Ti/SnO 2 -Sb 2 O 3 /CNT-Ce-PbO 2 electrode for triclosan electro-oxidation.
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Water
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2024
·Vol. 16
·期 14
·1994
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IF 3
Hongbin Wang,Shijie Kuang,Youlun Su,Xu Ren,Bowen Yang,Yongliang Sun
Diclofenac (DCF) is often detected in diverse aquatic bodies, and ineffective management can lead to detrimental effects on human health and ecosystems. In this study, degradation of DCF by Fe(III) and Mn(II) activating bisulfite (BS) was investigated. In the Fe(III)/Mn(II)/BS system, 93.4% DCF was degraded at 200 μM BS within 120 s, and additional research on 1000 μM BS achieved 88.4% degradation efficacy. Moreover, kinetics fitting of DCF degradation with the different BS concentrations was studied to find the two highest reaction rates (200 and 1000 μM,kobs= 0.0297 and 0.0317 s−1, respectively). Whereafter, SO4•−and Mn(III) were identified as the main active species at these two concentrations, respectively. Density functional theory (DFT) calculations, molecular frontier orbital theory, and surface electrostatic potential (ESP) forecast electrophilic attack sites. DCF degradation pathways by radical and non-radical ways were proposed by attack site prediction and thirteen intermediates identified by UPLC-QTOF-MS. ECOSAR software 2.2 was used for toxicity assessment. This work studied DCF degradation by the Fe(III)/Mn(II)/BS process in the presence of different concentrations of BS, providing a new insight into water purification.
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MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Yuanke Zhang,Siqi Wang,Li Qin,Xiaodan Li,Guixia Ling,Peng Zhang
Based on the foundation of calculations in molecular mechanics and density functional theory (DFT) for in-depth mechanistic studies, this paper proposes the sample multi-residue analysis method of five common sulfonamide antibiotics (SAs) in milk. Fe 3 O 4 nanoparticles modified magnetic graphene oxide nanoribbons (Mag-GONRs) with superior dispersibility and dispersion stability, were developed and firstly utilized to rapidly extract residual SAs from milk. Therefore, various SAs in complex samples could be simultaneously determined solely by high performance liquid chromatography-ultraviolet detector (HPLC-UV) without the need for complicated pretreatment processes. In order to obtain satisfactory extraction efficiency, indispensable investigation and optimization were conducted on some parameters influencing the extraction efficiency. And the extracted SAs were determined by. Good linearity for all analytes was achieved with appropriate correlation coefficients (R 2 higher than 0.9978). The limits of detection ranged from 0.060 to 0.075 ng·mL −1 . Recoveries of the sulfonamides in spiked milk samples were between 79.6 % and 114.6 %, with relative standard deviations within 12 %. Interestingly, with the assistant of computational chemistry, the efficient extraction of Mag-GONRs onto SAs has been validated at the molecular and quantum levels, further elucidating the adsorption mechanism based on non-covalent interactions. In the context of theoretical research and experimental results mutually supporting each other, a practical detection method with actual application value has been proposed in monitoring the residual sulfonamides in milk by the common devices.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Peilin Jia,Dongzhi Zhang,Xingyan Shao,Jieshuo Zhai,Jishun Guo,Zijian Wang,Xinyi Ji
Hydrogen (H 2 ), as a clean energy source, exhibits significant promise in the realm of new energy vehicles. Utilizing hydrogen sensors with rapid response and high selectivity is crucial for monitoring vehicles and preventing hydrogen leakage incidents. In this study, In 2 O 3 nanomaterials were synthesized via a hydrothermal approach and effectively modified with Ag/Cu bimetallic nanoparticles to fabricate high-performance hydrogen sensors. The optimal work temperature for the Ag/Cu–In 2 O 3 sensor is determined to be 300 °C. At this temperature, the sensor exhibited a response of 9.66–100 ppm H 2 , which is four times higher than the pristine In 2 O 3 sensor. Excellent H 2 selectivity and outstanding long-term stability were exhibited by the sensor in typical interference gas environments encountered in new energy vehicles. The significant enhancement in sensor performance is attributed to the electronic and chemical sensitization effects of Ag/Cu bimetals and the synergistic effects of bimetallic modification. Additionally, computational studies based on density functional theory (DFT) further elucidated the reasons for the improved H 2 gas sensing performance of Ag/Cu–In 2 O 3 nanocomposites. The Ag/Cu–In 2 O 3 nanocomposites show great potential for hydrogen detection applications in the sensor field.
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JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Hongliang Sheng,Shuainan Wang,Tao He,Xiaoben Zhao,Jinfeng Zhang,Song He,Yajun Huang
In this study, mesoporous activated carbon with high specific surface area was synthesized using lignin as the carbon source through hydrothermal pretreatment and alkali activation. The prepared activated carbon HL-4–200–800 exhibited a specific surface area as high as 3057 m²/g and a pore volume of 2.80 cm³/g. The excellent physicochemical properties were confirmed by comprehensive characterization methods including nitrogen adsorption/desorption isotherms, elemental analysis (EA), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR). Moreover, the prepared samples demonstrated outstanding adsorption performance, with a saturated adsorption capacity of 2030.13 mg/g for gaseous benzene and 140.41 mg/g for NO at 298 K. Further analysis through isotherm fitting, adsorption kinetics modeling, and ideal adsorbed solution theory (IAST) indicated that the material showed significantly better adsorption selectivity for benzene than for NO. Density functional theory (DFT) simulations revealed the competitive adsorption mechanism between benzene and NO, highlighting the crucial role of surface functional groups in enhancing adsorption efficiency.
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FUEL
·
2024
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IF 6.7
Dongdong Chen,Dongyang Liu,Liang Zhao,Jinsen Gao,Chunming Xu
Promoting hexane activation to further improve propylene selectivity has been a challenge. In this study, the activation mechanisms of hexane on Brønsted acid sites (BAS) of ZSM-5, on metal-doped Lewis acid sites (LAS) and on mixed systems with olefins have been investigated by density functional theory (DFT), microkinetics and experiments. DFT results show strong BAS are more favorable for the activation of hexane compared to weak BAS. The existence of two mechanisms for the activation of hexane under LAS. The activation of hexane to generate hexene and hydrogen on the LAS under M−I type metal doping, Ni and Cu belong to the M−I type metals, where Ni metal promotes C–H bond breaking more effectively (136.11 kJ/mol). On the other hand, under M−II type metal doping, the activation of hexane to produce hexyl carbenium ions, Co, Mn, Fe, and Zn belong to the M−II type metals, with Co metal exhibiting the highest efficiency in promoting C–H bond cleavage (18.56 kJ/mol). Among the mixed systems of olefin and hexane, the mixed system of pentene and hexane was chosen to be more effective. Microkinetics revealed that reactions occurred at lower temperatures on LAS compared to BAS. Furthermore, the capability to promote hexane activation was ranked as follows: LAS>olefin addition > BAS, which is consistent with the experimental results. To further promote hexane activation, it is necessary to dope the catalyst with Co metals and reduce the reaction temperature appropriately. Additionally, a small amount of olefin can be added in the process. This study provides a theoretical basis for the design of catalysts and optimization of operation conditions.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2025
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IF 4.6
Zijun Niu,Yingkun Shi,Sijia Liu,Yu Lv,Songlei Wang
In this study, a new electrochemical sensing platform for sulfamethazine (SDM) was prepared using MIP/CNT/MoS 2 -CoNi/GCE as an electrode modifier on a glassy carbon electrode (GCE). Firstly, theoretical simulations and quantum calculations based on density-functional theory (DFT) accelerate the prediction of the template molecule-to-functional monomer ratio. Nanocatalytic materials (CNT/MoS 2 -CoNi) loaded with metal ions Co and Ni were synthesised by a simple solvothermal method and then drop-coated onto GCE. The molecularly imprinted polymer (MIP) film with specific recognition sites can be generated on the modified electrode by electropolymerization. The successful formation of nanocatalytic materials was assessed by various characterisations such as scanning electron microscopy and X-ray diffraction. Under optimal conditions, the constructed sensor showed excellent detection efficiency for the oxidation of SDM in phosphate buffer solution (PBS, pH = 8.0) with a linear range of 0.1 μM to 800 μM and a detection limit of 0.033 μM. The sensor exhibits exceptional stability, reproducibility, and anti-interference capabilities, rendering it suitable for the detection of SDM residues in meat.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Si Duan,Yuan Gao,Guihong Lan,Haiyan Qiu,Bo Xu,Xiangming Liu,Ming Zhang,Yusong Chen
Functionalization of ligands is an effective strategy to enhance the adsorption performance of adsorbents. In this study, MIL-101(Fe)-R (R = -H, –OH, –NH 2 , and –NO 2 ) was selected as a platform for systematically studying the impact of functionalization on the adsorption behavior of chlortetracycline (CTC). A series of characterizations were conducted on the prepared MIL-101(Fe)-R to clarify the influence of organic linkers on the microscopic morphology, pore structure, and surface functionality of the adsorbents. Additionally, the effects of different functional groups on the adsorption behavior of MIL-101(Fe)-R were compared to screen for MOFs with high efficiency in removing CTC. Experimental results showed that the maximum adsorption capacities (q m ) of MIL-101(Fe), MIL-101(Fe)–NH 2 , MIL-101(Fe)–OH, and MIL-101(Fe)–NO 2 were 418.980 mg/g, 559.854 mg/g, 187.387 mg/g, and 154.131 mg/g, respectively. Among them, MIL-101(Fe)–NH 2 exhibited a higher mass transfer rate (reaching equilibrium in 15 min). Based on apparent adsorption behavior, adsorption kinetics, isotherm and thermodynamic studies, as well as FTIR and XPS characterizations before and after adsorption, the performance modulation mechanism of MIL-101(Fe)-R in CTC adsorption was discussed in detail. Combined with density functional theory (DFT) calculations, the host–guest interaction controlling the adsorption behavior was understood at the molecular level, demonstrating the optimal binding sites of the adsorbents. This study provides guidance for the design of efficient MOF adsorbents for antibiotic wastewater treatment.
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Materials Today Communications
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2024
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IF 3.7
Xianze Meng,Qianru Zhang,Xuantong Lv,Jiabo Chen,Yingzi Peng,Pengxuan Dong,Qingqing Sun
The corrosion inhibition performance of three amino acids, namely L-Phenylalanine (Phe), L-Methionine (Met) and L-Histidine (His) on 7150 Al alloy in 0.1 M HCl + 1 M NaCl solution was investigated by using electrochemical impedance spectroscopy (EIS), cyclic polarization, DFT and MD simulations. Electrochemical results indicate that all the studied amino acid inhibitors are cathodic type, and the inhibition efficiency follows the following order under all studied temperatures (25, 35 and 45 ℃): His > Met > Phe. A strong correlation between corrosion inhibition efficiency and DFT parameters is not evident, but the adsorption sites (N and O of NH 2 -COOH-, S atom of Met and two N atoms in the imidazolyl ring of His) can be determined by Fukui indices and Mulliken charges of the local atoms. In addition, MD simulations indicate that corrosion inhibition efficiency increases with the decreasing of adsorption energy.
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Toxics
·
2024
·Vol. 12
·期 1
·43
·
IF 3.9
Mingguo Peng,Yang Xu,Yao Wu,Xuewen Cai,Weihua Zhang,Lu Zheng,Erdeng Du,Jiajun Fu
Per- and Polyfluoroalkyl Substances (PFAS) bioaccumulate in the human body, presenting potential health risks and cellular toxicity. Their transport mechanisms and interactions with tissues and the circulatory system require further investigation. This study investigates the interaction mechanisms of six PFAS with Human Serum Albumin (HSA) using multi-spectroscopy, DFT and a molecular dynamics approach. Multi-spectral analysis shows that perfluorononanoic acid (PFNA) has the best binding capabilities with HSA. The order of binding constants (298 K) is as follows: “Perfluorononanoic Acid (PFNA, 7.81 × 106L·mol−1) > Perfluoro-2,5-dimethyl-3,6-dioxanonanoic Acid (HFPO-TA, 3.70 × 106L·mol−1) > Perfluorooctanoic Acid (PFOA, 2.27 × 105L·mol−1) > Perfluoro-3,6,9-trioxadecanoic Acid (PFO3DA, 1.59 × 105L·mol−1) > Perfluoroheptanoic Acid (PFHpA, 4.53 × 103L·mol−1) > Dodecafluorosuberic Acid (DFSA, 1.52 × 103L·mol−1)”. Thermodynamic analysis suggests that PFNA and PFO3DA’s interactions with HSA are exothermic, driven primarily by hydrogen bonds or van der Waals interactions. PFHpA, DFSA, PFOA, and HFPO-TA’s interactions with HSA, on the other hand, are endothermic processes primarily driven by hydrophobic interactions. Competitive probe results show that the main HSA–PFAS binding site is in the HSA structure’s subdomain IIA. These findings are also consistent with the findings of molecular docking. Molecular dynamics simulation (MD) analysis further shows that the lowest binding energy (−38.83 kcal/mol) is fund in the HSA–PFNA complex, indicating that PFNA binds more readily with HSA. Energy decomposition analysis also indicates that van der Waals and electrostatic interactions are the main forces for the HSA–PFAS complexes. Correlation analysis reveals that DFT quantum chemical descriptors related to electrostatic distribution and characteristics like ESP and ALIE are more representative in characterizing HSA–PFAS binding. This study sheds light on the interactions between HSA and PFAS. It guides health risk assessments and control strategies against PFAS, serving as a critical starting point for further public health research.Keywords:human serum albumin (HSA);per- and polyfluoroalkyl substances (PFAS);multi-spectroscopy;DFT calculations;molecular docking;molecular dynamics simulation
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PubMed
高影响因子
RARE METALS
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2025
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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
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Rui Gao,Lang Gao,Xianfa Zhang,Shan Gao,Yingming Xu,Xiaoli Cheng,Ghuanyu Guo,Qinghua Ye,Xin Zhou,Zoltán Major,Lihua Huo
ZnO@the reduced graphene oxide (rGO) nanorod arrays were grown in-situ on the ceramic tube substrate by one-step hydrothermal without any template or surfactant. The reduced graphene oxide was evenly coated around the ZnO nanorods through the controllable assembly of the rGO and ZnO heterojunction interface. rGO contributed to the improvement of material conductivity and provided more active sites to adsorb NO 2 molecules. The combination of rGO and ZnO significantly enhanced the response of the composite to NO 2 at room temperature . It showed an excellent selectivity to NO 2 and a good linear relationship in the concentration range of 0.1∼10 ppm. In order to explore the response mechanism of ZnO@rGO composite to NO 2 , the change of element composition and status was performed by XPS technology before and after the exposure of the composite to NO 2 . The gaseous products after the reaction were also tested by GC–MS technology. DFT calculations were performed based on the test results, which demonstrated that the p-n heterostructure produced by the ZnO@rGO composite had a beneficial effect on improving the gas response capability.
研究领域:
材料科学
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环境科学
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化学
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