INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Yujing Chi,Yuan Xu,Chenxiang Xu,Jiming Tian,Ying Li,Boxiang Gu,Haiyan Song,Han Zhang
Selective removal of 137Cs from nuclear wastewater is still a challenge due to the issues of efficient adsorbent exploitation and high concentrations of competitive ions. In this study, two-dimensional-layered Mxene Ti3C2Tx achieved the surface alkaline modification with KOH to be used as an efficient adsorbent for Cs+ removal from model wastewater. Hydroxyl-modified Ti3C2Tx obtained improved the delamination morphology and surface structure compared with the pristine Ti3C2Tx. In addition, the F species in Ti3C2Tx were efficiently removed and the hydroxyl groups were increased after modification. The adsorption efficiency of Cs+ over the hydroxyl-modified Ti3C2Tx was significantly enhanced, being attributed to the improvements in morphology, structure, and properties. 0.05 g of an optimal adsorbent achieved 90% removal of Cs+ with 5 mg·L–1 initial concentration in 50 mL of model wastewater within 5 min at ambient temperature and neutral conditions. Hydroxyl-modified Ti3C2Tx also exhibited high adsorption selectivity for Cs+ in the presence of competitive metal ions such as K+, Na+, Mg2+, and Ca2+. The mechanism study revealed that the ion exchange between [Ti–O]−H+/Cs+ mainly contributed to Cs+ adsorption, and the complexation between the oxygen-containing groups [Ti–O] in modified Ti3C2Tx and Cs was also involved. The hydroxyl-modified Ti3C2Tx was easy to regenerate and exhibited good recyclability for Cs+ adsorption.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shijian Zhou,Yuexin Shi,Guangyuan Chen,Weiguo Kong,Hao Hu,Haoran Xie,Changlai Li,Jinping Qin,Zewu Zhang,Luming Peng,Xiaokang Ke,Yan Kong
Structural design is important and challenging for the fabrication of covalent organic frameworks (COFs) in the photocatalytic applications. Hydroxyl groups have been found to be the active sites for O 2 adsorption and promote the electron-donating conjugation effects, which favorable for the oxygen reduction reaction (ORR) in photocatalytic hydrogen peroxide (H 2 O 2 ) evolution. This study reports the preparation of “fragmentized” COFs (T x H y -COFs) photocatalysts and their application in H 2 O 2 synthesis, as well as the direct hydroxylation of benzene to phenol. The results demonstrate that the functional design of surface hydroxyl (–OH) modification on fragmentized T x H y -COFs was achieved by varying the feed ratio of TAPT and THTA monomers, which greatly enhances surface hydrophilicity and effectively improves the separation and transfer of photoexcited electrons and holes. Under visible light irradiation without sacrificial agents, the fragmentized T 1 H 1.8 -COF exhibits a boosting H 2 O 2 yield of 2567 μmol g −1 h −1 , which is 4.2 times higher than the original T 1 H 1 -COF. Furthermore, the introduction of metal ions (Fe 3+ etc.) into the COF framework through the impregnation method enables the in situ activation of H 2 O 2 , allowing the direct hydroxylation of benzene to phenol in aqueous systems, with yield of 9.4 % and selectivity of 99 %. The results of this work demonstrate that the prepared photocatalyst exhibits high stability and photocatalytic activity by structural design optimization, showing great potential for industrial applications in H 2 O 2 production and direct photo-oxidation.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Qun Li,Wenyu Zhou,Chunyan Deng,Chenyang Lu,Peng Huang,Dong Xia,Luxi Tan,Cailong Zhou,Yong-Wei Zhang,Lichun Dong
In catalytic oxidation reactions, the presence of environmental water poses challenges to the performance of Pt catalysts. This study aims to overcome this challenge by introducing hydroxyl groups onto the surface of Pt catalysts using the pyrolysis reduction method. Two silica supports were employed to investigate the impact of hydroxyl groups: SiO2–OH with hydroxyl groups and SiO2–C without hydroxyl groups. Structural characterization confirmed the presence of Pt–Ox, Pt–OHx, and Pt0 species in the Pt/SiO2–OH catalysts, while only Pt–Ox and Pt0 species were observed in the Pt/SiO2–C catalysts. Catalytic performance tests demonstrated the remarkable capacity of the 0.5 wt % Pt/SiO2–OH catalyst, achieving complete conversion of benzene at 160 °C under a high space velocity of 60,000 h–1. Notably, the catalytic oxidation capacity of the Pt/SiO2–OH catalyst remained largely unaffected even in the presence of 10 vol % water vapor. Moreover, the catalyst exhibited exceptional recyclability and stability, maintaining its performance over 16 repeated cycles and a continuous operation time of 70 h. Theoretical calculations revealed that the construction of Pt–OHx sites on the catalyst surface was beneficial for modulating the d-band structure, which in turn enhanced the adsorption and activation of reactants. This finding highlights the efficacy of decorating the Pt surface with hydroxyl groups as an effective strategy for improving the water resistance, catalytic activity, and long-term stability of Pt catalysts.
研究领域:
化学
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催化科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Polymer Chemistry
·
2017
·Vol. 8
·期 17
·2630-2639
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IF 5.375
Wenjie Wang,Yang Shi,Xiao Wang,Anjun Qin,Jing Zhi Sun,Ben Zhong Tang
We report a new synthetic strategy to derive functional poly(disubstituted acetylenes) (PDSAs) through “phenol–yne click reaction”. The phenol-containing PDSA was prepared by the polymerization of the triisopropylsilane (TIPS)-protected 4-((4-fluorophenyl)ethynyl)phenol monomer and by a subsequent de-protection step. Then, different functional groups (e.g., ester and amide) were grafted onto the PDSA side chains via the highly efficient “phenol–yne click reaction”. The post-polymerization modification was carried out under mild conditions (at 40 °C, in common solvent) under an air atmosphere for a short time (4 h). The structures of the products were well characterized by GPC, NMR, and FTIR techniques and satisfactory data were collected. The data indicated that the phenol groups on the precursor PDSA were highly active to react with activated acetylenic compounds bearing functional groups intolerable to direct polymerization. This is the first example of the preparation of phenol-containing PDSA and the use of it as a precursor to prepare functional PDSAs. Besides the activated ester, thiol–ene click reaction, Michael addition reaction and Cu(I) catalysed alkyne–azide click reaction, we added a new tool in the tool-box for the synthesis of functional polymers.
研究领域:
材料化学
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高分子化学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2012
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IF 2.236
Yanjun Zhao,Li Shen,Ying Wan,Xiaoxia Zhu,Zheng Wang
Low generation poly(amidoamine) (PAMAM) dendrimers are less cytotoxic, but it is generally difficult to render them with thermosensitive properties due to the lack of surface terminal groups. Hydroxymethyl aminomethane was employed to modify PAMAM so as to increase the density of hydroxyl groups on PAMAM surface. Two types of thermosensitive units with different hydrophobicity were covalently linked to the hydroxyl groups of PAMAM surface to obtain thermosensitive PAMAM derivatives. The thermosensitivity of the surface-modified PAMAM can be precisely controlled by manipulating the hydrophobicity of the dendrimer periphery and regulating the ionization of the dendrimer interior.
研究领域:
生物化学
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纳米医学
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药物递送
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产品关联
DOI
高影响因子
POLYMER INTERNATIONAL
·
2017
·Vol. 66
·期 11
·1598-1609
·
IF 2.07
Peikun Zhang,Yang Zhou,Hui Su,Hong Lin,Saiqi Tian,Yi Chen,Jun Yan,Yazhou He,Haojun Fan
Despite being extensively implemented in research, it remains challenging but highly desirable to develop ammonium polyphosphate (APP)-based polyurethane (PU) combining excellent flame retardancy and improved mechanical properties. Herein, hydroxyl-decorated APP (OH-APP) was successfully fabricated through a facile, green, yet efficient cation exchange reaction with N -methylethanolamine, and utilized as a multifunctional reinforcing agent for solvent-free two-component PU in the curing process. Results demonstrate that the conjugation of OH-APP imparts to the resultant cured PU samples (PU/OH-APP) enhanced fire safety and smoke suppression performance, as evidenced by the considerable decrease in peak heat release rate, total heat release, peak smoke production rate and total smoke production by 75.4, 30.1, 64.3 and 14.4% over those of pure PU. Furthermore, the tensile strength of PU/OH-APP is improved by 66.5%, while the ductility is well maintained, highlighting its promising potential in industrial applications. This work is aimed at opening a new avenue for the development of APP-based PU with outstanding performances through covalent anchoring approaches. © 2017 Society of Chemical Industry
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
ACS Biomaterials Science & Engineering
·
2024
·
IF 5.4
Yucui Shen,Ye Feng,Shengjie Liang,Chunyong Liang,Baoe Li,Donghui Wang,Jianwei Sun
Developing a microenvironment-responsive drug delivery system (DDS) for the gastrointestinal system is of great interest to enhance drug efficiency and minimize side effects. Unfortunately, the rapid-flowing digestive juice in the gastrointestinal tract and the continuous contraction and peristalsis of the gastrointestinal tract muscle accelerate the elimination of drug carriers. In this study, a boric hydroxyl-modified mesoporous Mg(OH)2 drug carrier is prepared to prolong the drug retention time. Results show that the newly designed DDS presents high biocompatibility and can immediately turn the free polyhydric alcohol molecules into a gelation form. The in situ-formed gelation network presents high viscosity and can prevent the drug carriers from being washed away by the digestive juice in the gastrointestinal tract.
研究领域:
药剂学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
OPTICAL MATERIALS
·
2023
·
IF 3.9
Zihuan Wei,Lina Kong,Qiang Wang,Jianping Xu,Lan Li
Conjugated structure modification is an effective strategy for improving the photocatalytic activity of graphitic carbon nitride (g-C 3 N 4 ). Herein, we introduce p-π conjugated to g-C 3 N 4 by surface grafting of hydroxyl (-OH) groups through a facile hydrothermal process to improve the photo-carriers generation and separation. Experiments and DFT calculations indicate that the hydrothermal treatment decorated –OH groups onto the C sites of g-C 3 N 4 and formed p-π conjugated structure between the 2p orbitals of the O and the π orbitals of the tri-s-triazine unit. The extended p-π electrons delocalization of g-C 3 N 4 increases the concentration of the carriers, and the –OH groups serve as electrons transport channels facilitating the separation of the carriers. Consequently, –OH grafted g-C 3 N 4 with hydrothermal treated at 120 °C exhibits the highest and recyclable H 2 evolution rates of 2.3 mmol h −1 g −1 under simulated sunlight irradiation, which outperform pristine g-C 3 N 4 1.42 times. This work proposes a new mechanism of the p-π conjugate of –OH decorated g-C 3 N 4 for improving charge carriers formation and separation, and provides a mild strategy to engineer the other conjugated molecular structures.
研究领域:
材料科学
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光催化
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理论计算
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Qianqian Shang,Hongbing Wang,Changjie Kan,Rui Ding,Yankai Li,Shiva Pandeya,Ziliang Li,Mahesh Kumar Joshi
Exfoliation and hetero-element doping are common procedures for band gap engineering and enhancing the photocatalytic properties of g-C3N4. A novel and facile strategy for simultaneous exfoliation and hetero-element doping is still in high demand. Herein, we prepared hydroxide and fluoride doped ultrathin g-C3N4 nanosheets through the single-step solvothermal exfoliation of bulk g-C3N4 (BCN) using varying concentrations of ethanol and hydrofluoric acid (HF). The microscopic and spectroscopic analysis confirmed the doping of hydroxide groups and fluoride groups (HO−/F− groups) into g-C3N4 nanosheets (HF-CNS). The HO− groups are primarily located at the terminal amino groups of the heptazine rings in HF-CNS, while the F− groups are likely incorporated into the g-C3N4 lattice by forming C–F bonds. The UV-vis absorption spectra and DFT calculations showed that the electronic band structure, and hence charge carrier recombination, can be tuned by varying the HF amount during the exfoliation process. BET-specific surface area was increased from 18.65 m2 g−1 for BCN to 159.87 m2 g−1 for HF-CNS. The transient photocurrent increased from 5 μA to 20 μA. HF-CNS significantly improved the photocatalytic degradation of tetracycline, achieving 99% removal in 50 minutes, compared to 20% for BCN. Tetracycline degradation followed pseudo-first-order kinetics, with apparent rate constants (K) increasing from 0.0028 min−1 for BCN to 0.0793 min−1 for HF-CNS, a 30-fold enhancement. The photocatalytic hydrogen evolution for HF-CNS was 11 times higher than that of BCN. The HF-CNS exhibited remarkable stability and reusability, indicating its potential as a promising photocatalyst for green hydrogen production and degradation of organic pollutants.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2021
·
IF 5.565
Jiaqi Shi,Rui Han,Shuangchun Lu,Qingling Liu
A series of highly-hydrophobic MIL-53-Al (MIL = Materials of Institut Lavoisier) frameworks synthesized via decoration of the Al-OH groups by alkyl phosphonic acid were developed as adsorbents for removing acetone from humid gas streams. The newly prepared materials were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscope (SEM), N 2 adsorption-desorption and thermogravimetric analysis (TGA). Their adsorption behaviors toward acetone vapor under dry and wet conditions were studied subsequently. Results showed that alkyl phosphonic acid was successfully grafted into MIL-53-Al skeleton through coordinating interaction with Al 3+ generating MIL-53-Al@C x ( x = 12, 14, 18). The MIL-53-Al@C x exhibited similar crystal structure and thermal stability to parent MIL-53-Al. Furthermore, the modified materials showed significantly enhanced hydrophobicity . The water vapor uptake of MIL-53-Al@C 14 decreased by 72.55% at 75% relative humidity (RH). Dynamic adsorption experiments demonstrated that water vapor had almost no effect on the acetone adsorption performance of MIL-53-Al@C 14 . Under the condition of 90% RH, the acetone adsorption capacity of MIL-53-Al@C 14 was 102.98% higher than that of MIL-53-Al. Notably, MIL-53-Al@C 14 presented excellent adsorption reversibility and regeneration performance in 10 adsorption-desorption cycles. Taken together, the strategy of metal-OH group modification is an attractive way to improve the acetone adsorption performance over metal-organic frameworks (MOFs) under humid conditions. Besides, MIL-53-Al@C 14 would be deemed as a promising candidate for capturing acetone in high moisture environment.
研究领域:
材料化学
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环境科学
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吸附分离
·
多孔材料
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配位化学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2014
·
IF 4.331
Fa-tang Li,Ye Zhao,Qing Wang,Xiao-jing Wang,Ying-juan Hao,Rui-hong Liu,Dishun Zhao
Novel Al 2 O 3 /g-C 3 N 4 heterojunction photocatalysts were fabricated through ultrasonic dispersion method. Al 2 O 3 , obtained via solution combustion, contained amorphous ingredient with lots of defect sites and was used as active component for transferring photo-induced electrons of g-C 3 N 4 . G-C 3 N 4 was grafted surface hydroxyl groups in the presence of ammonia aqueous solution to combine with Al 2 O 3 possessing positive charges via hydrogen bond . The XRD, SEM, element map, TEM , HRTEM, FT-IR, and XPS results indicate that these synthesized materials are two-phase hybrids of Al 2 O 3 and g-C 3 N 4 with interaction. The photocatalytic results for the degradation of rhodamine B (RhB) indicate that the most active heterojunction proportion is 60 wt.% g-C 3 N 4 :40 wt.% Al 2 O 3 , the visible light photocatalytic activity of which is 3.8 times that of a mechanical mixture. The enhanced performance is attributed to the high separation efficiency of photo-induced electrons from the LUMO of g-C 3 N 4 injected into the defect sites of Al 2 O 3 , which is verified by photoluminescence spectroscopy (PL) and surface photovoltage (SPV) measurements. The electron paramagnetic resonance (EPR) signals and radical scavengers trapping experiments reveal holes (h + ) and superoxide anion radical ( O 2 − ) are the main active species responsible for the degradation of RhB.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2020
·
IF 2.369
Peixin Zhang,Yao Zhong,Qing Yao,Xing Liu,Yan Zhang,Jun Wang,Qiang Deng,Zheling Zeng,Shuguang Deng
Separation of a gas mixture achieved by the vacuum swing adsorption (VSA) technology is considered as an efficient and energy-saving method for Xe/Kr mixtures, but developing efficient and stable adsorbents remains challenging. Herein, we report an ultramicroporous metal–organic framework, namely, MIL-120 with a suitable pore size (5.4 Å × 4.7 Å), rich hydroxyl-decorated sites, and ultrahigh stability, which is capable of highly selective adsorption of xenon from krypton. Specifically, MIL-120 exhibits an excellent adsorption capacity of Xe up to 1.15 and 1.99 mmol g–1 at 298 K under 0.1 bar and 1 bar, respectively, and outstanding ideal adsorbed solution theory selectivity of 9.6 for the Xe/Kr mixture, which is comparable to those of benchmark porous materials. The isosteric heat of adsorption (Qst) and density functional theory calculations further confirm the stronger interaction of the adsorbent toward Xe than Kr. Furthermore, the cycling breakthrough experiments, hydrothermal and acid-based stability tests, and VSA assessment comprehensively demonstrate that the MIL-120 is an efficient and potent adsorbent for Xe/Kr separation under industrial conditions.
研究领域:
材料科学
·
气体分离技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）