CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Wei Chen,Xinning Dai,Zhujun Liu,Bin Du,Xinyu Zheng,Dandan Ma,Xianbin Huang
Periodate-based advanced oxidation processes (PI-AOPs) exhibited a promising future for the reduction of emerging refractory organic pollutants . However, the underlying mechanism and the sulfuretted effect of sulfide-modified metal silicate materials for PI activation were still unclear. In this study, sulfide-modified metal silicates (S-CoSi) were first synthesized and applied in the PI-AOPs system. Different from traditional metal silicate materials, sulfurization improved the catalytic performance. The enhanced degradation performance was from the increase in specific surface area and charge transfer efficiency, which derived from the sulfurization in metal silicate. DFT calculations revealed that the enhanced charge densities of Co-S bonds promoted the existence of Co (Ⅱ), which was more conducive to PI activation. Experimental and calculation results further demonstrated that Co was the active site in S-CoSi, and sulfur species strengthened the radical pathway by assisting Co (Ⅱ) regeneration (electron transfer from S to Co) rather than participating in the PI activation. Moreover, sulfurization promoted the generation of 1 O 2 (non-radical pathway) by increasing oxygen vacancy in the metal silicate. This study provided new insights into the effect of sulfurization on the radical and non-radical pathways in the metal silicates PI system.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Dongli Li,Liqin Zhou,Zongwu Wei,Xingzhen Qin,Hongbing Ji,Kungang Chai
Chlorophenols (CPs), a kind of important intermediate for fine chemicals, exists widely in the aqueous environment and poses a significant danger to humans. Therefore, developing advanced materials to enable the effective capture of CPs is highly desired. Herein, β-cyclodextrin-based porous carbon (CPAC) with exceptional capacities for CPs has been designed and tested. These porous carbon adsorbents were successfully synthesized via stepwise carbonization, affording abundant N and O functional groups, high surface area (as high as 3982 m 2 ·g −1 ) and controlled pore size to optimize for rapid CPs uptake. According to the CPs uptake measurements, CPAC exhibited exceptional CPs adsorption performance. CPAC showed high adsorption capacities (1085.08 mg · g −1 for 2,4,6-trichlorophenol) and fast adsorption kinetics for CPs. CPAC can effectively recover multi-component CPs from complex aqueous media, and the special pore structure reduces the competitive adsorption between CPs. And the recyclability studies showed that CPAC maintained its structural integrity and the initial CPs uptake capacity, highlighting its potential for practical application. Besides, DFT calculations indicate that hydrogen bonding and π-π interactions are key factors. Among them, the molecular conformation of CPs and the number of chlorine atoms on phenol play a crucial role in the adsorption behavior and adsorption energy.
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TALANTA
·
2023
·
IF 6.1
Jiaming Ling,Ting Wang,Zhoujian Xie,Xinqiao Cheng,Kungang Chai,Pengfei Li
Chromatographic stationary phases with molecular-shape selectivity are advantageous for the separation and analysis of geometric isomers. Herein, dehydroabietic acid is bonded on the surface of silica microspheres via 3-glycidoxypropyltrimethoxysilane to form a monolayer dehydroabietic-acid stationary phase (Si-DOMM) with a racket-shaped structure. Various characterization techniques indicate that Si-DOMM is successfully prepared, and the separation performance of a Si-DOMM column is evaluated. The stationary phase has a low silanol activity and metal contamination and a high hydrophobicity and shape selectivity. The resolutions of lycopene , lutein , and capsaicin on the Si-DOMM column confirm that the stationary phase exhibits high shape selectivity. The elution order of n -alkyl benzene on the Si-DOMM column indicates its high hydrophobic selectivity and suggests that the separation is an enthalpy-driven process. Repeatability experiments reveal highly stable preparation processes of the stationary phase and column and indicate that the relative standard deviations of retention time, peak height, and peak area are less than 0.26%, 3.54%, and 3.48%, respectively. Density functional theory calculations using n -alkylbenzenes, polycyclic aromatic hydrocarbons , amines, and phenols as model solutes provide an intuitive and quantitative description of the multiple retention mechanisms. The Si-DOMM stationary phase exhibits superior retention and high selectivity for these compounds via multiple interactions. The bonding phase of the monolayer dehydroabietic acid stationary phase with a racket-shaped structure has a unique affinity for benzene, strong shape selectivity, and good separation performance for geometrical isomers with different molecular shapes.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
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IF 6.2
Xiaomeng Yang,Yajiao Cui,Yingyu Qi,Luyan Fu,Armin Rezayan,Chunbao Charles Xu,Jianshe Wang,Dong Sui,Yongsheng Zhang
The rapid development of consumer electronics, electric vehicles, and smart meters demands high-performance energy storage devices. By now, supercapacitors are expected to become one of the most promising energy devices for future energy technology. In this work, NiO nanoparticles supported on activated carbon nanofibers (NiO/ACNFs) have been synthesized by atomic layer deposition technique, which is directly used as self-supporting binder-free electrodes for supercapacitors. Scanning electron microscopy, transmission electron microscopy , X-ray photoelectron spectroscopy, and Raman results show that NiO nanoparticles (3.1 nm) are uniformly coated on ACNFs. The NiO/ACNFs-600 electrodes demonstrate a specific capacitance of 870 F·g −1 (1 A·g −1 ) and good rate capability (remain 67% at 10 A·g −1 ). The asymmetric supercapacitor devices with NiO/ACNFs-600//ACNFs electrodes yield a fairly high energy density of 39.85 Wh·kg −1 at 2000 W·kg −1 and excellent capacitance retention of 87% after 10,000 cycles. The excellent electrochemical capacitance performance for NiO/ACNFs is attributed to the high conductivity and large specific surface area of ACNFs, high capacity, small size, and even dispersion of NiO as well as the synergistic effect between them. These results demonstrate that NiO/ACNFs can serve as excellent electrode materials for high-performance asymmetric supercapacitors.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 20
·e2302407120
·
IF 11.1
Ying-Jie Zhang,Jie-Jie Chen,Gui-Xiang Huang,Wen-Wei Li,Han-Qing Yu,Menachem Elimelech
Clarifying the reaction pathways at the solid–water interface and in bulk water solution is of great significance for the design of heterogeneous catalysts for selective oxidation of organic pollutants. However, achieving this goal is daunting because of the intricate interfacial reactions at the catalyst surface. Herein, we unravel the origin of the organic oxidation reactions with metal oxide catalysts, revealing that the radical-based advanced oxidation processes (AOPs) prevail in bulk water but not on the solid catalyst surfaces. We show that such differing reaction pathways widely exist in various chemical oxidation (e.g., high-valent Mn3+ and MnOX) and Fenton and Fenton-like catalytic oxidation (e.g., Fe2+ and FeOCl catalyzing H2O2, Co2+ and Co3O4 catalyzing persulfate) systems. Compared with the radical-based degradation and polymerization pathways of one-electron indirect AOP in homogeneous reactions, the heterogeneous catalysts provide unique surface properties to trigger surface-dependent coupling and polymerization pathways of a two-electron direct oxidative transfer process. These findings provide a fundamental understanding of catalytic organic oxidation processes at the solid–water interface, which could guide the design of heterogeneous nanocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Lu Zhao,Liang Liu,Xiao-Feng Bai,Ai-Yong Zhang,Shu-Chuan Peng,Chi Zhang,Hai-Hong Niu,Heng Liang
Pollutants removal by Fenton-like catalysis is of considerable interest, and the solid catalyst play governing roles. Two-dimensional MoS 2 can activate peroxymonosulfate (PMS) for radical-mediated catalysis via metallic 1T phase and/or crystal defects (i.e., sulfur vacancy). Herein, we explored the significant synergism between defective sulfur vacancy and metallic 1T rather than semiconducting 2H phase for Fenton-like catalysis on MoS 2 . This synergism was substrate-dependent during MoS 2 preparation. A series of sulfur-defected 1T-MoS 2 were prepared by H 2 O 2 oxidation, drastic structural but no morphological changes were measured. The defect-tailored 1T-MoS 2 exhibited a superior Fenton-like reactivity toward PMS activation and pollutant degradation in various water matrices. A 10.0 mg·L -1 of aqueous phenol was completely degraded in one hour, and the corresponding pseudo-first order reaction constant increased more than 12 times after defect engineering. No synergistic effect was measured between sulfur vacancy and semiconducting 2H phase on defective 2H-MoS 2 . Radical-mediated reaction mechanism was identified by ESR, scavenger inhibiting, spectroscopic analysis and electrochemical measurements. Electron transfer was accelerated within metallic 1T phase to favor PMS activation and pollutant degradation on defective sulfur vacancies serving as surface reactive sites. Our findings provided fundamental insights into PMS activation on sulfur vacancy promoted by 1T-MoS 2 in Fenton-like catalysis for water purification.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Yize Liu,Meiyu Li,Ruoyao Zhang,Tengda Zhao,Jing Han,Aibin Kang,Chunmao Chen,Hongwei Ren,Erhong Duan
With the development of the petrochemical industry , a large amount of naphthenic acids in petrochemical wastewater was accumulated in the environment, causing serious environmental pollution . Most of the commonly used methods for the determination of naphthenic acids have the characteristics of high energy consumption, complicated pretreatment , long detection cycle, and the need to send samples to analytical laboratories. Therefore, it is essential to develop an efficient and low-cost field analytical method for rapidly naphthenic acids quantify. In this study, nitrogen-rich carbon quantum dots (N-CQDs) based on natural deep eutectic solvents (NADESs) was successfully synthesized by a one-step solvothermal method. The fluorescence property of carbon quantum dots was used to achieve the quantitative detection of naphthenic acids in wastewater. The prepared N-CQDs showed excellent fluorescence and stability, showed a good response to naphthenic acids and a linear relationship in the concentration range of naphthenic acids from 0.03 to 0.09 mol‧L −1 . The effect of common interferents in petrochemical wastewater on the detection of naphthenic acids by N-CQDs was investigated. The results showed that N-CQDs had good specificity for the detection of naphthenic acids. N-CQDs was applied to the naphthenic acids wastewater, and the concentration of naphthenic acids in the wastewater was successfully calculated according to the fitting equation.
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高影响因子
ChemCatChem
·
2023
·Vol. 15
·期 13
·e202300313
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IF 4.5
Lvye Ai,Qian Wang,Fuzhi Cui,Guofang Jiang
Graphical We synthesized core-shell-structured nanospheres consisting of an Fe 3 O 4 core and a covalent triazine framework (TpMa) shell via a monomer-mediated in situ growth process. This nanocomposite was utilized as a heterojunction photocatalyst for the activation of peroxymonosulfate (PMS) in the degradation of phenol . Our findings indicate that the Fe 3 O 4 @TpMa core-shell structure promotes the utilization of light and activation of PMS, while SO 4 ⋅ − , ⋅OH, h + , O 2 ⋅ − , and 1 O 2 play crucial roles in the degradation of phenol. The development of efficient heterostructures combining covalent organic frameworks (COFs) and ideal semiconductors can significantly improve photocatalytic performance for pollutant degradation. Herein, we present the design, synthesis, and characterization of a core-shell-structured nanocomposite comprising covalent triazine framework-encased Fe 3 O 4 magnetic particles employed as a heterojunction photocatalyst for activating peroxymonosulfate (PMS) in phenol degradation. The distinctive internal structure between the TpMa shell (Tp=2,4,6-trihydroxy-1,3,5-benzenetricarboxaldehyde, Ma=melamine) and the Fe 3 O 4 core (Fe 3 O 4 @TpMa) facilitated charge transfer and accelerated charge separation. Furthermore, PMS served as an electron acceptor, enhancing photogenerated charge separation and maximizing the production of reactive oxygen species. The Fe 3 O 4 @TpMa/PMS system demonstrated remarkable photocatalytic performance and stability, achieving complete phenol degradation (10 mg L −1 ) in 40 min. The exceptional photocatalytic activity resulted from the synergistic effect of ⋅OH, SO 4 ⋅ − , O 2 ⋅ − , 1 O 2 , and h + generated in the Fe 3 O 4 @TpMa/PMS system during the degradation process. Overall, this material offers excellent potential for solar-driven pollutant degradation and enables the development of COF-based materials for wastewater treatment applications.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 25
·67758-67770
·
IF 5.8
Wang Ke,Qin Xingzhen,Chai Kungang,Wei Zongwu,Deng Fan,Liao Bingyu,Wu Jinyu,Shen Fang,Zhang Zhi
Endocrine-disrupting compounds (EDCs) are increasingly polluting water, making it of practical value to develop novel desirable adsorbents for removing these pollutants from wastewater. Here, a simple cross-linking strategy combined with gentle chemical activation was demonstrated to prepare starch polyurethane-activated carbon (STPU-AC) for adsorbing BPA in water. The adsorbents were characterized by various techniques such as FTIR, XPS, Raman, BET, SEM, and zeta potential, and their adsorption properties were investigated comprehensively. Results show that STPU-AC possesses a large surface area (1862.55 m 2 ·g −1 ) and an abundance of functional groups, which exhibited superior adsorption capacity for BPA (543.4 mg·g −1 ) and favorable regenerative abilities. The adsorption of BPA by STPU-AC follows a pseudo-second-order kinetic model and a Freundlich isotherm model. The effect of aqueous solution chemistry (pH and ionic strength) and the presence of other contaminants (phenol, heavy metals, and dyes) on BPA adsorption was also analyzed. Moreover, theoretical studies further demonstrate that hydroxyl oxygen and pyrrole nitrogen are the primary adsorption sites. We found that the efficient recovery of BPA was associated with pore filling, hydrogen-bonding interaction, hydrophobic effects, and π-π stacking. These findings demonstrate the promising practical application of STPU-AC and provide a basis for the rational design of starch-derived porous carbon.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 23
·e53932
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IF 3
Hao Dong,Xiangming Hu,Jindi Liu,Yuntao Liang,Wei Wang,Hui Tang,Fusheng Zhu,Zhenglong He,Peng Wang
In order to solve the problem of formaldehyde release from the traditional phenolic foam (PF) in the process of coal mine filling and plugging. In this paper, the effect of different factors on the efficiency of formaldehyde trapping agents were studied by adding formaldehyde trapping agents containing amino compounds after PF synthesis. The effect of formaldehyde trapping agents on the performance of resin was investigated. The results showed that the addition of formaldehyde trapping agents could greatly reduce the residual formaldehyde content in phenolic resin. Fourier-transform infrared spectroscopy (FTIR) data showed that the addition of formaldehyde trapping agent not only successfully prepared PF, but also produced a stable formaldehyde trapping agent product. Compared with the unmodified PF, the pore size and foaming rate of the modified PF decreased in varying degrees, and the foaming temperature also decreased in varying degrees. Among them, urea modified phenolic resin (PUF) had the highest formaldehyde removal efficiency. It had the t lowest heat release during combustion and the foam pore size was large and uniform. In addition, through the application of urea-modified PF in the goaf return air corner fissure sealing application, it was found that the CO concentration in the goaf maintained at the lowest state of 0.002%. It has reached the national industry standard of polymer gas plugging materials and conforms to the green development concept in the field of coal mine fire prevention.
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Polymer Chemistry
·
2021
·Vol. 13
·期 1
·80-84
·
IF 5.582
Wei Chen,Peng Liu
The ultrasound-mediated approach has attracted attention for enhanced localized drug delivery in tumor chemotherapy. Here, well-defined PEGylated dendritic polyurethane (Ph-DPU-PEG) was synthesized as unimolecular micelles with a hydrophobic core via a facile one-pot method for ultrasound-triggered localized drug delivery. The chemotherapeutic drug could be encapsulated in the hydrophobic cores, and the drug-loaded micelles (DOX@Ph-DPU-PEG) were obtained as nanomedicine, which would hardly release the drug without ultrasound, regardless of the acidity of the releasing media. However, they showed an excellent ultrasound-triggered intracellular drug release performance, with a cumulative drug release of 81.6% in the simulated tumor intracellular microenvironment within 12 h. Furthermore, the ultrasound-triggered intracellular drug release was revealed with the CLSM technique and an enhanced tumor growth inhibition was achieved on the HepG2 cells compared to free DOX.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wenyang Fu,Zhongzheng Hu,Yang Zheng,Pei Su,Qizhan Zhang,Yongli Jiao,Minghua Zhou
Compared to traditional haber–bosch process for synthetic ammonia, electrochemical reduction of nitrate to ammonia (ERNA) offers a promising and sustainable technology to generate ammonia at ambient temperature. However, the performance of ERNA is impeded by lacking of sound strategy for designing high-performance electrocatalyst. Here, a Cu based electrode with Cu 2 O/Cu interface was prepared by pulse electrodeposition and electroreduction, achieving the fast rate constant of 0.14 min −1 for reducing nitrate with a high ammonia yield rate of 2.17 mg cm -2 h −1 (faradaic efficiency: 84.36%) and ammonia selectivity of 94.4% at −0.25 V vs. RHE. Particularly, density functional theory (DFT) calculations for the adsorption energy indicated that Cu 2 O/Cu interface alleviated adsorption energy of NO 2 - from −2.02 eV (pure Cu) to −1.59 eV, improving surface diffusion of adsorbed NO 2 - . And DFT calculations for electronic structure implied that Cu 2 O/Cu interface upshifted the d band center of Cu (-2.25 eV vs. −2.48 eV of pure Cu), boosting electron transfer to NO 3 - . Additionally, in-situ infrared spectroscopic analysis confirmed vital intermediates of NO 2 - and NH 2 OH on Cu 2 O/Cu to identify reaction pathway and Gibbs free energy diagram clarified this interface decreased reaction barrier of crucial step (reducing *NO 2 to *NO) from 0.31 eV (pure Cu) to −0.77 eV for the enhancement of ERNA. Thereby, these findings demonstrated that Cu 2 O/Cu interface tunes mobility of NO 2 - and electron transfer to NO 3 - on Cu based electrocatalyst is an efficient method to promote performance of ERNA with high efficiency and rate.
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