PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 10
·5702-5710
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IF 3.43
Fei Yao,Nan Gong,Wenhui Fang,Zhiwei Men
Halogen bonding, an attractive interaction that is analogous to hydrogen bonding, has been widely investigated by computational methods. However, halogen bonding in solution is hard to study by spectroscopic techniques since the intermolecular interaction often gives overlapping bands and may be difficult to interpret. The traditional interpretation of iodomethane–ethanol mixtures considered only hydrogen bonding effects and the experimental investigation was limited. Here, we employed near-infrared (NIR) spectroscopy, Raman, density functional theory calculation, and two-dimensional (2D) correlation analysis to find evidence of the halogen bonding in iodomethane–ethanol mixtures. Our results suggest that the blue-shifting C–I stretching band is probably due to the cooperative influence from halogen bonding, hydrogen bonding, and the solvent effect, while the O–H band is a cumulative band from three dimer complexes. The 2D correlation spectra further validate the hypothesis above and reveal the interaction evolution from the ethanol-rich region to the iodomethane region. These results indicate that the unique nature of the iodomethane–ethanol mixture and the larger σ-hole strengthen the halogen bond, leading to particular spectroscopic results which are different from those of the other halogenated alkanes.
研究领域:
物理化学
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光谱学
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DOI
PubMed
高影响因子
Science China-Chemistry
·
2024
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IF 10.4
Tai Bo,Li Baoyu,He Linwei,Ma Zhonglin,Lin Shujing,Zhang Mingxing,Chen Junchang,Wu Fuqi,Chen Long,Dai Xing,Ma Fuyin,Chai Zhifang,Wang Shuao
The development of adsorbent materials for effective capture of radioactive iodomethane (CH 3 I) from the off-gas of used nuclear fuel reprocessing, remains a significant and challenging line of research because currently state-of-art adsorbents still suffer from low binding affinity with CH 3 I. Here, we proposed a brand-new adsorption topological structure by developing a 2D interdigitated layered framework, named SCU-20, featuring slide-like channel with multiple active sites for CH 3 I capture. The responsive rotating-adaptive aperture of SCU-20 enables the optimal utilization of all active sites within the pore for highly selective recognition and capture of CH 3 I. A record-breaking CH 3 I uptake capacity of 1.84 g/g was achieved under static sorption conditions with saturated CH 3 I vapor. Both experimental and theoretical findings demonstrated that the exceptional uptake of SCU-20 towards CH 3 I can be attributed to the confined physical electrostatic adsorption of F sites, coupled with the chemical nitrogen methylation reaction with uncoordinated N atoms of pyrazine. Moreover, dynamic CH 3 I uptake capacity potentially allows for the capture of CH 3 I in simulated real-world off gas reprocessing conditions. This study highlights the potential of SCU-20 as a promising candidate for efficient capture of iodine species and contributes to the development of effective solutions for radioactive iodine remediation.
研究领域:
化学
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环境科学
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核能工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Man He,Hui Zhu,Guoren Li,Tao Duan,Jiehong Lei
Radioactive iodine (I₂) and methyl iodine (CH₃I), as common and dangerous volatile fission products in nuclear waste streams, pose a serious threat to the environment and human health due to their long-term radioactivity. Here, we aim to achieve effective co-capture of I₂ and CH₃I through the synthesis of a nitrogen-rich porous organic polymer (CTP-BPA) based on triazine through the Schiff base reaction. Various characterizations have confirmed that the material has a rich mesoporous structure and nitrogen active sites. The material exhibits excellent performance under both static and dynamic conditions: it can achieve a high equilibrium capacity (4996.5 mg/g for I₂ and 621.5 mg/g for CH₃I gas), and more importantly, in dynamic penetration experiments, it has significant absorption capacity (1052.3 mg/g for I₂ and 377.8 mg/g for CH₃I) at low concentrations (3.83 ppm for I₂ and 3.39 ppm for CH₃I). Crucially, CTP-BPA can still maintain its capturing effect in simulated harsh environments, resisting strong acids (1 M HNO₃), high temperatures (up to 500°C), and high humidity (80 % relative humidity). Comprehensive experiments and DFT theoretical analysis indicate that the high-density nitrogen active sites effectively activate and fix iodine through strong charge transfer interactions, thereby achieving the chemical sequestration of harmful iodine substances. This research provides a promising strategy and advanced materials for the safe and long-term management of radioactive iodine in environmental remediation.
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高影响因子
LANGMUIR
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2020
·
IF 3.557
Xinting Han,Junyan Peng,Shaohua Jiang,Jian Xiong,Yu Song,Xiao Gong
Good mechanical and chemical stabilities are the key factors for the wide application of superhydrophobic surfaces. In this work, we first prepared raspberry-like hollow structured SnO2 nanoparticles using a simple hydrothermal method, followed by an annealing step. Then, the intrinsic raspberry-like hollow SnO2 nanoparticles were combined with hydrophilic SiO2 nanoparticles to construct rough surfaces with suitable hierarchical structures, and 1H,1H,2H,2H-perfluorodecyltriethoxysilane (FAS-17) was used as a hydrophobic modifier of SnO2, while epoxy resin was used as an adhesive to prepare a superamphiphobic coating with good stability and durability. Such a coating can be applied on various substrates using a simple spray-coating or drop-coating method. The water contact angle and diiodomethane contact angle of the coating could reach up to ∼165 and ∼151°, respectively. After various chemical and mechanical stability tests including hot water treatment, salt water corrosion, strong adhesive tape peeling, and kneading, the coatings still remained amphiphobic. The facile fabrication of the robust superhydrophobic coating has great potential for applications in real life and industrial production.
研究领域:
材料科学
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表面化学
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纳米技术
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涂层与薄膜
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2024
·Vol. 22
·期 1
·1-15
·
IF 10.6
Chen Can,Huang Baoxing,Zhang Ruru,Sun Chaoping,Chen Lei,Ge Jianxian,Zhou Dandan,Li Yueping,Wu Shuwang,Qian Zhiyuan,Zeng Jianfeng,Gao Mingyuan
Background The general sluggish clearance kinetics of functional inorganic nanoparticles tend to raise potential biosafety concerns for in vivo applications. Renal clearance is a possible elimination pathway for functional inorganic nanoparticles delivered through intravenous injection, but largely depending on the surface physical chemical properties of a given particle apart from its size and shape. Results In this study, three small-molecule ligands that bear a diphosphonate (DP) group, but different terminal groups on the other side, i.e. , anionic, cationic, and zwitterionic groups, were synthesized and used to modify ultrasmall Fe 3 O 4 nanoparticles for evaluating the surface structure-dependent renal clearance behaviors. Systematic studies suggested that the variation of the surface ligands did not significantly increase the hydrodynamic diameter of ultrasmall Fe 3 O 4 nanoparticles, nor influence their magnetic resonance imaging (MRI) contrast enhancement effects. Among the three particle samples, Fe 3 O 4 nanoparticle coated with zwitterionic ligands, i.e. , Fe 3 O 4 @DMSA, exhibited optimal renal clearance efficiency and reduced reticuloendothelial uptake. Therefore, this sample was further labeled with 99m Tc through the DP moieties to achieve a renal-clearable MRI/single-photon emission computed tomography (SPECT) dual-modality imaging nanoprobe. The resulting nanoprobe showed satisfactory imaging capacities in a 4T1 xenograft tumor mouse model. Furthermore, the biocompatibility of Fe 3 O 4 @DMSA was evaluated both in vitro and in vivo through safety assessment experiments. Conclusions We believe that the current investigations offer a simple and effective strategy for constructing renal-clearable nanoparticles for precise disease diagnosis. Graphical Abstract
研究领域:
医学影像学
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纳米医学
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生物材料
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DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
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IF 11.4
Ning Gan,Yuqing Lin,Baolong Wu,Yulong Qiu,Haopan Sun,Jingwen Su,Jianguo Yu,Qian Lin,Hideto Matsuyama
Ion-selective membranes (ISM) with sub-nanosized pore channels hold significant potential for applications in saline wastewater treatment and resource recovery. Herein, novel synergistic ion channels featuring bi-periodic structures were constructed through the coordination of functional Cyclen (quaternary_1,4,7,10-tetraazacyclododecane, Q_Cyclen) and Cu 2+ -m-Phenylenediamine (Cu 2+ -MPD) to develop supramolecular membranes for lithium extraction. The exterior quaternary ammonium-rich sites exhibit a significant Donnan exclusion effect, resulting in tremendous mono/divalent (Li + /Mg 2+ ) ion selectivity; while the interior regular-confined channels of Cyclen yield a fast vehicular pathway, facilitating water molecules and Li + ion-selective transport. The optimized membrane exhibited an increased water permeance of 19.2 L·m -2 ·h -1 ·bar -1 and simultaneously promoted Li + /Mg 2+ selectivity (achieving a selectivity of 18.5 under a Mg 2+ /Li + mass ratio of 30), surpassing the trade-off limit of conventional nanofiltration membranes. Due to the acquired excellent Li + /Mg 2+ selectivity, lithium extraction from simulated salt-lake brines was successfully achieved through a two-stage nanofiltration process, reducing the Mg 2+ /Li + mass ratio from 40 to 1.1. This work validates the applicability of macrocyclic with intrinsic sub-nanosized channels and desired multifunctionality for developing high-performance ISM for efficient lithium separation and beyond.
研究领域:
材料科学
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环境工程
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEDICINAL CHEMISTRY
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2024
·
IF 6.8
Chao Zhao,Wanlu Sun,Yanyan Zhu,Xiaoyan Huang,Ye Sun,Hai-Yan Wang,Yi Pan,Yi Liu
Photodynamic therapy (PDT) is an innovative and promising method for treating tumors that has attracted significant interest but still faces several challenges, such as a lack of selectivity, deep penetration of light, and efficient ROS generation. To address these challenges, we optimized and synthesized a series of photosensitizers and successfully developed a heavy-atom-free near-infrared FUCL photosensitizer NFh-NMe-2. This photosensitizer can generate singlet oxygen (1O2) and induce cellular apoptosis under 808 nm light. For the safe ablation of microtumors in vivo, an activatable FUCL photosensitizer NFh-NTR was developed based on the overexpression of nitroreductase (NTR). NFh-NTR could be activated by NTR, leading to the release of the photosensitizer NFh-NMe-2, restoring the fluorescence signal, and effectively killing tumor cells under 808 nm light irradiation. This work opens new possibilities in the chemical design of an FUCL photosensitizer for cancer treatment.
研究领域:
生物医学工程
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肿瘤学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
·
IF 5.3
Xiaoxiao Gu,Dongmei Li,Haoyang Yuan,Cailing Li,Dinghua Yu,Guowei Wang,Shuang Li
Baicalin is a flavonoid compound extracted from the Scutellaria baicalensis plant. It possesses strong free radical scavenging ability and has a wide range of medical applications in antibacterial, anti-inflammatory, and anti-tumor fields. However, its limited solubility in water restricts its application. In this study, we prepared SL-DMEA by the amidation of acidic sophorolipids and N, N-dimethylethanolamine, while SL-TMEAI was synthesized via the quaternization of SL-DMEA with iodomethane. The structures of SL-DMEA and SL-TMEAI were confirmed by 1 H NMR, FT-IR, and Mass spectra. Surface tension and micelle microenvironment indicated that SL-DMEA and SL-TMEAI exhibit superior surface activity. Furthermore, the solubility of baicalin in aqueous solutions containing SL-DMEA and SL-TMEAI was approximately 70 mg/L and 75 mg/L, while it was only 18 mg/L in SL-COOH solution, which were significantly higher than the solubility in pure water (4 mg/L). Similarly, SL-DMEA and SL-TMEAI can enhance the antioxidant activity of baicalin. Specifically, in the SL-TMEAI aqueous solution, the free radical scavenging rate of baicalin was increased by 10 %–20 %. Density functional theory calculations revealed that SL-DMEA and SL-TMEAI formed stable hydrogen bonds with baicalin molecules, which can increase the solubility of baicalin in water and expose the groups that react with free radicals in the solution, thereby enhancing the antioxidant activity. These results demonstrated that SL-DMEA and SL-TMEAI could significantly enhance the solubility and antioxidating of baicalin in water through a hydrotropy mechanism.
研究领域:
生物化学
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药物化学
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材料科学
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产品关联
DOI
高影响因子
npj Flexible Electronics
·
2024
·Vol. 8
·期 1
·1-10
·
IF 12.3
Lei Yutian,Yin Mengying,Shi Chang,Wu Lingxi,Peng Guoqiang,Xu Youkui,Wang Haoxu,Tang Rongbing,Li ZhenHua,Jin Zhiwen
The emerging pseudohalide metal-free perovskite (pseudohalide–MFPs) X-ray detector caters to the demands of timely mobile diagnosis owing to its lightweight, flexibility, and cost-effectiveness. However, the performance of these devices is severely limited by poor X-ray absorption, ultra-wide band gap, relative instability, and their unknown biotoxicity. Herein, we construct heavy atom covalent bonds (C–Br/Cl) on the A-site organic cation to reinforce component coordination to modulate X-ray absorption and band gap in pseudohalide–MFPs and further enhance its stability. Molecular dynamics simulations demonstrate that the introduction of halogen atoms can strengthen hydrogen bonding interactions, thereby improving the coordination between different components. The resultant (MDABCOBr)–NH 4 (BF 4 ) 3 (MDABCO = N-methyl-N’-diazabicyclo[2.2.2]octonium) single crystal significantly increases X-ray absorption cross-section and crystalline density (from 1.728 to 1.950 g cm −3 ), and synergistically realizes the band nature modulation (from 7.4 to 5.5 eV) and enhanced ionic migration inhibition (628 meV) with optimized stability. As such, our X-ray detectors realized a sensitivity of 2377 μC Gy air −1 cm −2 , an ultralow detection limit of 50.1 nGy air s −1 , and impressive operation stability. Moreover, cytotoxicity assay confirmed the compatibility of pseudohalide metal-free perovskite. Finally, within this framework, we successfully fabricate the (MDABCOBr)–NH 4 (BF 4 ) 3 -based flexible device to create an ideal in vitro wearable X-ray detection.
研究领域:
材料科学
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物理学
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生物医学工程
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放射学
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产品关联
DOI
高影响因子
BIOMACROMOLECULES
·
2025
·
IF 5.4
Yu Sun,Yushuang Shang,Xinyu Zhang,Zhaoyan Ge,Fengni Liu,Jian Shen,Jiang Yuan
Mimicked by the structure of dimethyl sulfoxide propionate (DMSP), a novel zwitterion monomer of N-methylacryloyl S-methyl l-cysteine methyl sulfonium salt (NMASMCMS) was synthesized and characterized for the first time through three steps using l-cysteine as a starting material. Poly(NMASMCMS) brushes were constructed on PET sheets via surface-initiated reversible addition–fragmentation chain-transfer (SI-RAFT) polymerization. The physical and chemical structures were characterized by water contact angle (WCA), attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), X-ray photoelectron spectroscopy (XPS), and atomic force microscopy (AFM). The polymer brush grafted sheets (PET-B) had good hydrophilicity and high lubricity. Moreover, PET-B sheets exhibited excellent antifouling and hemocompatible properties with low protein adsorption, bacterial adhesion, platelet adhesion, and hemolysis.
研究领域:
材料科学
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生物医学工程
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高分子化学
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产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2024
·
IF 15.8
Jiayi Bian,Yingjie Xu,Minghao Sun,Zerui Ma,Hao Li,Changrui Sun,Fei Xiong,Xiaopeng Zhao,Wenjing Yao,Yue Chen,Yuanyuan Ma,Xikuang Yao,Shenghong Ju,Wenpei Fan
Accurate imaging and precise treatment are critical to controlling the progression of pancreatic cancer. However, current approaches for pancreatic cancer theranostics suffer from limitations in tumor specificity and invasive surgery. Herein, a pancreatic cancer-specific phototheranostic modulator (AuHQ) dominated by aggregation-induced emission (AIE) luminogens-tethered gold nanoparticles is meticulously designed to facilitate prominent fluorescence-photoacoustic bimodal imaging-guided photothermal immunotherapy. Once reaching the pancreatic tumor microenvironment (TME), the peptide Ala-Gly-Phe-Ser-Leu-Pro-Ala-Gly-Cys (AGFSLPAGC) linkage within AuHQ can be specifically cleaved by the overexpressed enzyme Cathepsin E (CTSE), triggering the dual self-assembly of AuNPs and AIE luminogens. The aggregation of AuNPs mediated by enzymatic cleavage results in potentiated photothermal therapy (PTT) under near-infrared (NIR) laser irradiation, induced immunogenic cell death (ICD), and enhanced photoacoustic imaging. Simultaneously, AIE luminogen aggregates formed by hydrophobic interaction can generate AIE fluorescence, enabling real-time and specific fluorescence imaging of pancreatic cancer. Furthermore, coadministration of an indoleamine 2,3-dioxygenase 1 (IDO1) inhibitor with AuHQ can address the limitations of PTT efficacy imposed by the immunosuppressive TME and leverage the synergistic potential to activate systemic antitumor immunity. Thus, this well-designed phototheranostic modulator AuHQ facilitates the intelligent enzymatic dual self-assembly of imaging and therapeutic agents, providing an efficient and precise approach for pancreatic cancer theranostics.
研究领域:
生物医学工程
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癌症治疗
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纳米技术
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成像科学
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免疫学
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产品关联
DOI
PubMed
高影响因子
CARBOHYDRATE POLYMERS
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2024
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IF 10.7
Wan-Qi Deng,Shao-Wei Han,Si-Yuan Shao,Shuai Li
Pseudobulbs of Pleione bulbocodioides have been used as traditional Chinese medicine for a long time to treat cancers through decoction with water. However, as its main water-soluble ingredient, the structure of polysaccharide has not been elucidated yet. To obtain its polysaccharide with antitumor activity, a series of isolation, structural identification and antitumor evaluation experiments were performed. As a result, a newly discovered glucomannan, named PBP, was isolated and purified from the pseudobulbs of P. bulbocodioides . The molecular weight of PBP is 1.11 × 10 5 Da. Its monosaccharide composition comprises mannose and glucose at a molar ratio of 5:3. The fine structure of PBP was confirmed as a linear glucomannan backbone primarily comprising repeating →4)-β- d -Glc-(1 → 4)-β- d -Man-(1 → 4)-β- d -Glc-(1 → 4)-β- d -Man-(1 → 4)-β- d -Glc-(1 → 4)-β- d -Man-(1→4)-β- d -Man-(1 → 4)-β- d -Man-(1 → via a combination of analytical techniques and enzymolysis methods. PBP effectively inhibited the growth of 4T1 tumors with low toxicity in vivo . Furthermore, a noteworthy augmentation in the expression levels of CD4+ and CD8+ T cells suggested the existence of an elevated immune response. In summary, a new glucomannan with anti-breast tumor activity was obtained, which has the potential to contribute to breast cancer therapy.
研究领域:
药用植物学
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肿瘤学
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免疫学
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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）