ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Meicheng Zhang,Yang Li,Chiyao Bai,Xinghua Guo,Jun Han,Sheng Hu,Hongquan Jiang,Wang Tan,Shoujian Li,Lijian Ma
On the basis of high stability of phosphorus–oxygen linkage, we constructed two microporous covalent phosphazene-based frameworks (CPFs), for the first time, by choosing hexachlorocyclotriphosphazene as a core unit and polyhydroxy aromatic compounds (hydroquinone or phloroglucinol) as monomers, named CPF-D and CPF-T, respectively. Characterization studies by using Fourier transform infrared, nuclear magnetic resonance, thermal gravimetric analysis, 60Co γ-ray irradiation, and so forth, demonstrated that both of the CPF materials have excellent acid and radiation stability and relatively higher thermal stability. The results of batch adsorption experiments show that CPF-T is significantly more capable of sorbing uranium than CPF-D. In a pure uranium system with higher acidity (pH 1), the uranium sorption amount of CPF-T can reach up to 140 mg g–1. Distinctively, in mixed-metal solution with 12 coexisting cations, CPF-T shows relatively stable and excellent uranium adsorption capability over a wide range of acidity (pH 4 to 3 M HNO3), and the difference in uranium sorption amounts is less than 30% with the maximum of 0.26 mmol g–1 at pH 4 and the minimum of 0.20 mmol g–1 at 3 M HNO3, which is far superior to that of the conventional solid-phase extractant (SPE) materials previously reported. The research results suggested that the sorption model based on the speculated mechanism of size-matching plus hydrogen bond network has played a dominant role in the process of uranium adsorption. The proposed strategy for the one-pot fabrication of an acid-resistant microporous framework materials by bridging the aromatic monomers via P–O bonds provides an alternative approach for the design and synthesis of new SPE materials with size-matching function desired for effective separation of uranium or other valuable metals from highly acidic environments.
研究领域:
材料科学
·
核化学与放射化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Yan Li,Yun Liu,Ziqian Liu,Xin Wan,Hui Chen,Jinrong Zhong,Yue-Fei Zhang
Here we report an efficient strategy to separate and recycle acid blue 93 (AB93) from mixed anionic dyes selectively within sodium hydroxide activated A/CS adsorbent (N-A/CS). This work broke the common sense that the larger the specific surface area, the better the adsorption property is, which provided an alternative strategy to separate dyes. The adsorption equilibrium of AB93 could be achieved approximately within 1–2 min, and the maximum adsorption capacity was up to 2500 mg/g. Besides, it can be activated continuously and reused at least 15 times. In mixed anionic dyes, the adsorption selectivity of N-A/CS on AB93 in the mixture of AB93 and acid fuschin (AF) reached up to 99.7 %. Molecular dynamics simulation revealed that the trend of adsorption energy for dyes qualifies well with the experimental order of adsorption capacities and molecular sizes among five anionic dyes based on molecular matching effect. Thus, N-A/CS is a low-cost, easily-preparable, significantly-effective-and-reusable adsorbent, providing a promising “size-matching” strategy to adsorb multi-component dye systems.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Minlei Yin,Shiyin Huang,Yuxin Lin,Xuanjie Chen,Zhaoyang Qi,Jie Chen,Ting Qiu
Effective removal of acetaldehyde and propionaldehyde from propylene oxide is important for polyether industry but remains a significant challenge due to their similar molecular sizes and relatively close volatilities. Herein, we studied flexible molecular materials, perethylated pillar[n]arene crystals (n = 5, 6), which can be used to separate acetaldehyde and propionaldehyde in propylene oxide. Through a space size matching effect, perethylated pillar[5]arene demonstrates excellent adsorption selectivity of 95 % and 100 % for aldehydes in ternary mixture and binary mixture of propylene oxide, acetaldehyde and propionaldehyde, respectively. These impressive selective adsorption is achieved based on their differential host–guest interactions. Density functional theory calculations provide a comprehensive explanation of the adsorption process, revealing that the adsorption mechanisms of perethylated pillar[5]arene for acetaldehyde and propionaldehyde primarily involve C-H···O hydrogen bonding and C-H···π interactions. This study also provides a novel method for achieving one-step purification of propylene oxide in industrial applications.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 47
·24044-24053
·
IF 6.895
Jie Zhang,Lihong Zhou,Zhimin Jia,Xiaofeng Li,Yue Qi,Chuting Yang,Xinghua Guo,Shanyong Chen,Honghan Long,Lijian Ma
The separation and recovery of key nuclides such as uranium and plutonium from effluents related to nuclear industry is of great significance for alleviating the shortage of nuclear energy resources and protecting the environment and human health. However, the high temperature, strong acidity and radioactivity of the nuclear effluents pose a severe challenge to the separation materials used in such conditions. The diversity of structure, flexibility of design, and excellent physicochemical stability of covalent organic framework materials (COFs) provide the possibility for the directional design and preparation of adsorbents for use under harsh conditions. Herein, three COFs with similar structure, different pore sizes and connecting modules were synthesized. The ingenious structure predesign enables Dp-COF to have three carboxyl groups oriented toward the pore center and laid out in appropriate spatial positions, which builds hydrogen-bonding bridges between carboxycarbonyl and hydroxyl groups, and thus constructs for the first time a unique COF material with a double-ring pore. The inner pore size of the “double-ring” is slightly larger than the diameter of uranyl hydrate, which leads to a size-matching adsorption of uranium by Dp-COF, thus greatly reducing the effect of protonation. Even in the simulated spent fuel reprocessing liquid with pH = 1.0, the adsorption capacity of Dp-COF for uranium can reach 66.3 mg g−1, and the adsorption capacity reaches 317.3 mg g−1 at pH = 4.5, which is very rare among the reported COFs. More excitingly, the removal rate for uranium reaches up to an unprecedented 99.8% due to the size-matching effect, more than any analogous adsorbents. This study not only proposes new ideas for the design and regulation of the microscopic configuration of COF materials, but also provides an alternative approach for the preparation of efficient uranium adsorbents.
研究领域:
材料科学
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环境科学
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核能工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF INCLUSION PHENOMENA AND MACROCYCLIC CHEMISTRY
·
2011
·Vol. 73
·期 1
·237-246
·
IF 1.22
He J.
In this work, the inclusion between methyl substitute β-cyclodextrin and some linear macromolecule in supercritical carbon dioxide medium was investigated. The contributions from several factors were studied; such as the hydrogen bonding interaction between the host and guest, the hydrogen bonding interaction between the neighborhood cyclodextrin rims threaded on the polymer chain, and the matching between the host cavity and the size of the polymer axis.
研究领域:
化学
·
材料科学
·
药物传递系统
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Yansheng Liu,Yunjie Zhan,Guofu Wang,Xiaobo Jia,Jin Zhou,Hongqi Li,Haixin Chang,Zhicheng Jin,Kang Li,Zhaoxu Li
This study proposes a strategy for the highly sensitive detection of polystyrene nanoplastics (PS NPs) with varying particle sizes. Ag nanoarrays (AgNAs) with different inter-column spacings and heights are fabricated via thermal deposition of Ag in anodized aluminum oxide (AAO) templates. The size-matching effects between PS NPs and the parameters of the AgNAs (inter-column spacing and height) are investigated. Utilizing this size-matching effect, the AgNAs substrate enables sensitive detection of PS NPs with particle sizes of 130 nm, 180 nm, and 230 nm, with limits of detection (LODs) of 10 μg/mL. In real water samples (river water, rainwater, and tap water), the AgNAs substrate also demonstrates good performance, achieving a LOD of 10 μg/mL for detecting 130 nm PS NPs. Additionally, toluene is used to remove PS NPs from the AgNAs surface, allowing the substrate to be reused across multiple cycles. After at least 30 detection cycles, the surface-enhanced Raman scattering (SERS) performance of the AgNAs shows no significant decline, with a relative standard deviation (RSD) of 6.8 %. The AgNAs exhibit excellent stability and reusability in detecting PS NPs, indicating strong potential for practical applications.
研究领域:
环境科学
·
纳米技术
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Lai Qi,Pei Le,Fei Teng,Yin Ping,Pang Siping,Shreeve Jean’ne M.
Size matching molecular design utilizing host-guest chemistry is a general, promising strategy for seeking new functional materials. With the growing trend of multidisciplinary investigations, taming the metastable high-energy guest moiety in well-matched frameworks is a new pathway leading to innovative energetic materials. Presented is a selective encapsulation in hydrogen-bonded hydroxylammonium frameworks (HHF) by screening different sized nitrogen-rich azoles. The size-match between a sensitive high-energy guest and an HHF not only gives rise to higher energetic performance by dense packing, but also reinforces the layer-by-layer structure which can stabilize the resulting materials towards external mechanic stimuli. Preliminary assessment based on calculated detonation properties and mechanical sensitivity indicates that HHF competed well with the energetic performance and molecular stability (detonation velocity = 9286 m s −1 , impact sensitivity = 50 J). This work highlights the size-matched phenomenon of HHF and may serve as an alternative strategy for exploring next generation advanced energetic materials.
研究领域:
材料科学
·
化学
·
能量材料
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2013
·Vol. 38
·期 2
·845-851
·
IF 2.966
Li-Li Tan,Yumo Zhang,Bao Li,Kai Wang,Sean Xiao-An Zhang,Yanchun Tao,Ying-Wei Yang
Highly selective binding of “solvent” molecules by 1,4-dimethoxypillar[5]arene (DMP[5]A) and their host–guest complexation in solution and the solid state have been investigated by multiple methods. Enthalpy changes and the size-fit effect play an important role in the high selectivity.
研究领域:
超分子化学
·
有机化学
·
物理化学
·
材料科学
·
分析化学
✓ 已验证
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yun Chang,Xingli Zeng,Shuzhen Peng,Rong Lai,Mujing Yang,Dandan Wang,Xiaoshun Zhou,Yong Shao
Abnormal amplification of trinucleotide repeats (TNRs) is associated with neurodegenerative diseases by forming a particular hairpin bulge. It is well known that the polarity and parity of TNRs can regulate the formed hairpin structures. Therefore, there is a great challenge to efficiently discriminate the hairpin structures of TNRs with substantial selectivity. Herein, we developed a fluorescent ligand of pseudohypericin (Pse) with a beyond-size-matching (BSM) geometry to selectively sense hairpin structures of GTC and CTG TNRs. The GTC hairpin structures can bind with Pse dominantly at extreme T–T mismatches by the virtue of their most extrahelical conformations, while there is no binding event to occur with the polarity-inverted counterpart CTG hairpin structures because of the limited space provided by their intrahelical T–T mismatches. In addition, this all-or-none response with the polarity-dependent folding (PoDF) is independent of the length of these TNRs. Interestingly, the parity-dependent folding (PaDF) of GTC hairpin structures can also be resolved. Besides pure TNRs, the competency of this BSM ligand to sense the PoDF and PaDF effects was also generalized to DNAs with TNRs occurring at loop and stem end regions. To our knowledge, this is the first experimental observation with the state-of-the-art performance over the fluorescence measurement of PoDF and PaDF in TNRs. Our work provides an expedient way to elucidate the TNR folding by designing ligands having BSM features.
研究领域:
分子生物学
·
生物化学
·
神经科学
·
化学生物学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Mengdie Zhou,Guang Yang,Xiaohua Tian,Songlin Xue,Hao Li,Jianming Pan
Hybrid polymer nanosheets are promising sorbents owing to large surface area, but their complicated synthesis procedure and high cost hinder to apply in particular field of selective separation. In this work, one step Pickering oil-in-water-in-oil (O/W/O) double emulsion (DE) stabilized by palmitic chloride modified halloysite nanotubes (HNTs) were firstly designed for preparing polymer nanosheets (PMBA-PMA) by UV irradiation. Subsequently, amino ethyl benzo-12-crown ether (B12C4-NH 2 ) was covalently immobilized onto the PMBA-PMA to achieve functional hybrid polymer nanosheets (PMBA-PMA-CE) for the effective and selective recovery of lithium ion (Li + ). External metastable W/O interface produced droplets’ coalescence, and the Pickering DE droplets with irregular morphology eventually initiated the formation of polymer nanosheets. PMBA-PMA-CE exhibited cured and nanosheet-like structure constructed by HNTs and polymer networks. The batch mode experiments demonstrated that the fast adsorption equilibrium of PMBA-PMA-CE towards Li + could be reached within 100 min, and the results well followed pseudo-second-order model, confirming the chemical adsorption based on "Size-match" effect. The maximum monolayer adsorption capacity calculated from Langmuir model was 14.67 mg g −1 at 298 K. Benefiting from specific “size-match” complexation, the obtained PMBA-PMA-CE possessed an excellent selectivity towards Li + even in the presence of competitive cations, and selectivity coefficient ( α ) and relative selectivity coefficient ( α r ) were greater than 1.43 and 8.29, respectively. In addition, PMBA-PMA-CE could be simply regenerated and maintained above 90% of the initial capacity after five consecutive adsorption-desorption cycles. Furthermore, the incorporation of cheap HNTs not only endowed one step emulsion DE droplets, but also improved the sorbents’ mechanical property.
研究领域:
材料科学
·
纳米技术
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）