APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Wenjuan Shuai,Cun Liu,Yuheng Wang,Fengxiao Zhu,Dongmei Zhou,Juan Gao
Diethyl phthalate ester (DEP) can be degraded in Fe 3+ -UV- aliphatic/phenolic carboxyl acids systems, and the degradation can be significantly influenced by different physical chemical properties of the organic acids. In this study, a density function theory (DFT) approach combined with multilinear regression analysis demonstrates that the lowest unoccupied molecular orbital energy ( E LUMO ) significantly negatively influenced DEP degradation. The correlation coefficient of the regression is −19.3 mM L −1 h −1 . The standardized partial correlation coefficient is −0.674. The aliphatic acids group has higher catalytic ability than the phenolic carboxyl acids group, and by shifting the dominant LUMO configuration from C 3s3d to Fe 4s3d orbitals, Fe 3+ significantly accelerates the catalytic reactions of the aliphatic acids/UV systems. Further analysis demonstrates that electron withdrawing hydroxyl group on the aliphatic acids increases the photo catalytic effects of aliphatic acids/UV system. This study highlights the important role of E LUMO of organic acids on their photocatalytic ability towards degradation of organic pollutants .
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Siyuan Chen,Haiming Cai,Xiaodong Du,Peiwen Wu,Xueqin Tao,Jiangmin Zhou,Zhi Dang,Guining Lu
Tris(2-chloroethyl) phosphate (TCEP) as a new type of flame retardant exists in various water environments, causing great risks to humans and the environment. In this study, shrimp shell was used to prepare an economical and environmental-friendly adsorbent for the efficient removal of TCEP. The systematic studies including characterization, removal performance, and adsorption mechanism of shrimp shell biochar toward TCEP were carried out. Adsorption kinetics and thermodynamics showed that fast equilibrium reached within 30 min, the maximum adsorption capacity q m was 108 μmol g −1 at 298 K, and the adsorption process is spontaneous and exothermic. The environmental factor, such as temperature, pH, inorganic anions and organic matter hardly affected the adsorption performance. Structural characterization indicated that the hierarchical porous structure of shrimp shell biochar is the key to excellent adsorption performance. The adsorption mechanisms were further revealed using density functional theory (DFT) calculations, and the hydrogen bond , van der Waals interactions, Cl–H interactions, and pi-H interactions were identified as potential interaction mechanisms between TCEP and specific biochar structures. The calculated binding energy between TCEP and simplified biochar structure suggested that oxygen-containing groups especially carboxyl, hydroxyl and aldehyde facilitate the adsorption. Our work not only provides a novel strategy for the quick remediation of organophosphate-contaminated water environments but also offers new opportunities for crustacean waste biomass valorization.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2022
·
IF 4.331
Xin Kou,Yutian Ma,Congming Pan,Yong Huang,Yulai Duan,Ying Yang
Ionic polymers have been proven to be promising adsorbents in recovering Au(III) due to their advantages of simple synthesis and high adsorption efficiency. However, the unclarity of the relationship between the adsorption ability of ionic polymers and their cationic structures hinders further optimization of their adsorption performance. This study synthesized a series of ionic polymers with pyridinium, imidazolium, piperidinium, pyrrolidinium, and triethylammonium cations to discover the effects of the cationic structure on their adsorption properties. Experimental results show that the existence of anion−π interaction between aromatic cations and [AuCl4]− makes the aromatic cations–anion interaction stronger, which does not enhance the adsorption performance of the aromatic-based ionic polymer. This is due to the charge delocalization in the aromatic ring, resulting in a lower electrostatic potential (ESP) of aromatic cations than that of aliphatic cations with a localized charge. The higher the ESP of cations, the better the adsorption performance of the corresponding ionic polymer. This study serves as a deep understanding of the cationic structure–adsorptive performance relationship of the ionic polymer at the molecular level and further provides a theoretical guidance to optimize the adsorption performance of ionic polymers.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Jingquan Wang,Min Zheng,Yang Deng,Min Liu,Ying Chen,Naiyun Gao,Erdeng Du,Wenhai Chu,Hongguang Guo
The international campaign to ban bisphenol A (BPA) has resulted in increasing application of BPA substitutes. However, investigations have mainly been confined to the removal of single contaminant from the water, resulting in an inefficient burden. Furthermore, systematic study and synthetical discussion of bisphenol analogues (BPs) kinetics and transformation pathways were largely underemphasized. Chemical oxidation of BPA and four typical alternatives (i.e., bisphenol AF, bisphenol E, bisphenol F and bisphenol S) in a UV-activated persulfate system was examined in this study. The effects of persulfate (PS) dosage, pH and water matrix constituents (i.e., bicarbonate, chloride and natural organic matter) were comprehensively examined using a combination of laboratory experiments and mathematical modeling. According to our findings, the removal characteristics of different BPs employing SO 4 • − -induced removal technology, including degradation mechanisms and influencing trends by water matrix, revealed similarly. The second order-rate constants of SO 4 • – reacting with BPs served as the main variables mediating the variation in degradation kinetics. Frontier molecular orbital theory and density functional theory suggested BPs molecules possessed the same susceptible positions to free radicals. In the UV-activated PS process, transformation pathways included hydroxylation, electron-transfer, substitution, and rearrangement triggered by ortho-cleavage, with certain intermediates exhibiting higher toxicity than the parent chemicals. The findings of this study provided valuable information to estimate potential environmental risks of using BPA alternatives.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Surfaces and Interfaces
·
2022
·
IF 6.137
Pengwei Zhao,Xiaoyuan Zhou,Yalin Huang,Yuwei Xu,Shanyong Chen,Chengbin Zheng,Yongdong Jin,Chuanqin Xia
Removal of TcO 4 − from liquid radioactive waste is urgent due to its long half-life and high mobility. Herein, two guanidine-based cationic covalent organic polymers (TG-TPAL-H and TG-TPAL-OMe) were synthesized, and were used to research for the removal of ReO 4 − . TG-TPAL-H showed high removal efficiency, its sorption capacity got to 549 mg g −1 and distribution coefficient K d was 1.17 × 10 6 mL g −1 . What impressively, the TG-TPAL-H removed 80% of ReO 4 − even there was 1000 times of competing anions (Cl − , SO 4 2− , H 2 PO 4 − ). While TG-TPAL-OMe showed a poor performance on ReO 4 − with the capacity of 317 mg g −1 and K d of 6.9 × 10 4 mL g −1 . TG-TPAL-H can remove 87% ReO 4 − from simulated Hanford LAW stream sample, while TG-TPAL-OMe just can remove 35%. The difference between the two materials can be attributed to the electron donating group (Methoxy) in TG-TPAL-OMe reduced the positive charge density of guanidine, which was demonstrated by the ESP of density functional theory (DFT) calculation.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Lingjie Zhang,Zhisheng Ke,Wenzhe Wang,Huiling Liu,Yuting Mao,Mingxue Xiang,Ping Zhang
In this study, an innovative sulfur-doped graphene-like carbon-supported layered double oxide (G/S-LDO) was developed for removing toxic heavy metal ions (HMIs; Pb(II), Cd(II), and Co(II)) that are frequently found in wastewater. In single-solute systems, the maximum adsorption capacities were 720.01 (Pb(II)), 473.11 (Cd(II)), and 170.91 (Co(II)) mg/g, which were significantly higher than that of pure LDO and other materials reported in the literature. Even in mixed systems, the outstanding adsorption performance of G/S-LDO toward HMIs was observed with high distribution coefficient values ( K d , > 100 L/g). We found that the excellent performance of G/S-LDO depended both on LDO and sulfur-doped graphene-like carbon (G/S) in a complicated manner. In detail, the released OH – from LDO as precipitate agent contributed to HMIs removal. Further, G/S enhanced the 35.42% Pb(II) adsorption, 58.19% for Cd(II) and 48.69% for Co(II) via the complexation and the cation-π interaction from graphene, and coordination and precipitation effect resulting from the doped S. Consistent with experimental results, density functional theory (DFT) calculations unveiled the essence of the enhancement by G/S, and showed that the orbital hybridization between S p and the HMIs p and d states electrons played an important role on HMIs removal. Finally, the recyclability and leaching experimental results suggested the high stability and reusability of G/S-LDO. This work provides new insights into the interactions of HMIs with G/S-based materials, which may facilitate the development of prospective HMIs capturing agents in future studies.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Qiangqiang Xue,Huilin Yi,Zhengwen Li,Zhao Jiang,Meng Chen,Yujun Wang,Binhang Yan,Guangsheng Luo
Surface modification of 600-µm-sized monodisperse gamma-alumina microspheres into magnesium–aluminum spinel, and co-impregnation-based loading of Rh–Ni (0.46 wt% Rh, 9.03 wt% Ni) were performed to synthesize catalysts for diesel-steam-reforming to hydrogen. The intimate interactions between Rh and Ni, the formation of the Rh–Ni alloy, and the Rh-doping-induced decrease in the particle size of Ni were determined. The DFT calculations results revealed that Rh-doped Ni(1 1 1) established remarkably weak bonds with oxygen-containing intermediates, and the reaction barrier of the rate-limiting step (CH 2 * + O* → CH 2 O*) on Rh–Ni(1 1 1) (0.76 eV) was lower than those of Ni(1 1 1) (1.14 eV) and Rh(1 1 1) (1.56 eV). The bimetallic catalyst shows the enhanced activity and resistance of sintering and carbon deposition compared with those of Ni-based (9.33 wt% Ni) and Rh-based (0.47 wt% Rh) catalysts. The catalytic performance of Rh–Ni-based catalyst was superior to that of physically mixed Ni-based and Rh-based catalysts at similar active metal loadings, which further confirmed the synergistic effect of Rh–Ni.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xiuqin Dong,Jianhang Tian,Junwei Lei,Yifei Chen
Copper as a non-noble metal catalyst has great prospects in the hydrogenation of acetic acid to ethanol. In this paper, Cu-MnO/SBA-15 catalysts with highly catalytic performance and stability were prepared. The mechanism was elucidated by experiments and DFT calculations . The Cu and MnO were coexistent on reduced x Cu y Mn/SBA-15. Appropriate Cu/Mn ratio was beneficial for increasing the Cu surface area and reducing the size of Cu. The rate-controlled step was found and the MnO could effectively lower the difficulty of acetaldehyde formation by dioxyethylidene. DFT calculations indicated that the formation of ethyl acetate at the Cu-MnO interface was largely prevented. The optimal catalytic hydrogenation activity was obtained for 9Cu1Mn/SBA-15, with the conversion of acetic acid and selectivity of ethanol of 99.9% and 90.1%, respectively. The catalytic activity could remain within 72 h which was more stable than the original Cu-based catalyst.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jing Deng,Cheng Ye,Anhong Cai,Linyi Huai,Shiqing Zhou,Feilong Dong,Xueyan Li,Xiaoyan Ma
As a typical iron-based oxide semiconductor with abundant reserves, α-Fe 2 O 3 has been widely used in the domain of photocatalysis and environmental remediation. Here, sulfur doped α-Fe 2 O 3 (S-α-Fe 2 O 3 ) has been successfully fabricated through coprecipitation, hydrothermal and calcination processes and applied to activate persulfate (PS) for carbamazepine (CBZ) degradation under UV irradiation. Systematic characterizations were conducted to analyze the morphology, structure and chemical composite of S-α-Fe 2 O 3 . UV/PS/S-α-Fe 2 O 3 process showed remarkably enhanced photocatalytic performance for CBZ degradation. The degradation rate constant (7.78 × 10 −2 min −1 ) was about 2.2 and 14.1 times as high as that of UV/PS/α-Fe 2 O 3 (3.60 × 10 −2 min −1 ) and UV/PS (5.53 × 10 −3 min −1 ) processes, respectively. With increasing PS concentration and photocatalyst dosage, the removal efficiency of CBZ both increased. UV/PS/S-α-Fe 2 O 3 process can efficiently and steadily operate in a wide pH range of 3.0–8.0. The introduction of water matrix species (i.e. chloride, bicarbonate, nitrate and humic acid) exerted different effects on CBZ degradation. S-dopant was doped via forming ≡Fe III -SO 4 2- bond on S-α-Fe 2 O 3 surface, and doped sulfur functioned as surface electrons trapping centers derived from DFT study. The band gap value of S-α-Fe 2 O 3 was reduced and the separation efficiency of photogenerated electrons and holes was improved. Hydroxyl radicals, sulfate radicals, superoxide radicals and holes all contributed to CBZ destruction. Furthermore, two major routes of CBZ degradation were proposed as hydroxylation and deamination, then followed by decarbonxylation, ketonization and ring cleavage based on the results of HPLC-MS and DFT calculation.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yue Sun,Yingpeng Gu,Yu Jiang
The presence of aromatic compounds with multiple functional groups such as 5-sulfosalicylic acid (SSA) in water bodies is a threat to aquatic organisms and human health. Phenol (PH) with the -OH group, benzoic acid with -COOH and benzenesulfonic acid (BSA) with -SO 3 H can be considered as SSA structural unit. In this study, three functional monomers , namely, N-methylallylamine, diallylamine, and triallylamine, with strong affinity for PH, BA, and BSA, respectively, were selected from 16 monomers by using density functional theory (DFT). Molecularly imprinted resin (MIP-4) with tri-functional groups and excellent selectivity for SSA was synthesized using a macroporous polystyrene resin (NDA-1800) as the carrier. In binary systems, MIP-4 exhibited excellent imprinting effect and adsorption selectivity for SSA. X-ray spectroscopy data and DFT calculations illustrated that the adsorption of SSA on MIP-4 was mainly dependent on the strong electrostatic interaction between the protonated amine group on the resin and -SO 3 - of SSA, as well as, the hydrogen bond between the neutral amine group and -OH and -COOH of SSA; the order of the three functional groups in identification was -OH > -COOH > -SO 3 H. In addition, the adsorption performance of MIP-4 was retained after five adsorption–desorption cycles.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Jiling Zhao,Chen Wang,Shixing Wang,Yang Zhou,Bing Zhang
Palladium wastewater is produced from various industrial activities and seriously pollutes the environment. In here, a new adsorbent (PMDA-PGMA) was manufactured by functionalizing poly(glycidyl methacrylate) microspheres with pyromellitic acid and introduced to recover Pd(II) from wastewater. The main influencing factors including pH, palladium ionic content, reaction time and temperature were evaluated. The selectivity , reusability and sorption mechanism have been systematically examined. The pH 2 was optimal for Pd(II) adsorption and only 300 min was required to reach maximum adsorption capacity about 206.71 mg/g. The experimental data were is in tune with pseudo-secondary kinetics and Langmuir model well. So, the Pd(II) adsorption process was monolayer chemical adsorption. Thermodynamic parameters indicate that Pd(II) adsorption on PMDA-PGMA was an endothermic reaction . The main adsorption mechanism is ion exchange, electrostatic attraction and coordination between palladium ions and pyromellitic acid groups. Additionally, PMDA-PGMA can be easily regenerated by 10% thiourea and can be recycled at least five times. PMDA-PGMA exhibited good selective extraction ability for Pd(II) and effectively separated Pd(II) (≥95%) from laboratory wastewater in the presence divers metal ions . Density functional theory calculations show that PMDA-PGMA combines with Pd(II) through monodentate N atoms and bidentate O groups. The application prospect of PMDA-PGMA is encouraging in removing palladium from wastewater due to its high adsorption capacity and better reusability.
✓ 已验证
产品关联
DOI
高影响因子
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）