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期刊论文 43

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流动化学 2

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All-in-one functional supramolecular nanoparticles based on pillar[5]arene for controlled generation,

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 307-313 doi: 10.1007/s11705-022-2216-5

摘要： The storage and controlled release of singlet oxygen (1O2) have attracted increasing attention due to the wide application and microsecond lifetime of 1O2 in water. Herein we provide an integrated nanoplatform consisting of a diphenylanthracene derivative, a water-soluble pillar[5]arene and a photosensitizer tetrakis(4-hydroxyphenyl)porphyrin (TPP), that may provide the controlled generation, storage and release of singlet oxygen. We design a new diphenylanthracene derivative with two trimethylammonium bromide groups on both ends that can be well recognized by the pillar[5]arene. The formed nanocarriers can be used to load TPP through their supramolecular self-assembly. The resulting nanoparticles show good water-solubility and uniform spherical morphology. After laser irradiation (660 nm), the nanoparticles exhibit excellent ability for the generation and storage of 1O2. When the irradiated nanoparticles are heated above 80 °C, 1O2 can be released from the system. Therefore, in this paper we pioneer the use of noncovalent interaction to integrate the diphenylanthracene derivatives and photosensitizers into one functional system, which provides a new strategy for the controlled generation, storage and release of singlet oxygen. We believe this groundbreaking strategy will have a great potential in providing necessary amounts of 1O2 for the photodynamic therapy of tumors in dark.

关键词： storage and controlled release of singlet oxygen     supramolecular nanoparticles     noncovalent interactions     pillararenes     diphenylanthracene     photosensitizers    

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Enzyme-instructed self-assembly of peptides containing phosphoserine to form supramolecular hydrogels

Jie Zhou, Xuewen Du, Jiaqing Wang, Natsuko Yamagata, Bing Xu

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 509-515 doi: 10.1007/s11705-017-1613-7

摘要： Enzyme-instructed self-assembly (EISA) offers a facile approach to explore the supramolecular assemblies of small molecules in cellular milieu for a variety of biomedical applications. One of the commonly used enzymes is phosphatase, but the study of the substrates of phosphatases mainly focuses on the phosphotyrosine containing peptides. In this work, we examine the EISA of phosphoserine containing small peptides for the first time by designing and synthesizing a series of precursors containing only phosphoserine or both phosphoserine and phosphotyrosine. Conjugating a phosphoserine to the -terminal of a well-established self-assembling peptide backbone, (naphthalene-2-ly)-acetyl-diphenylalanine (NapFF), affords a novel hydrogelation precursor for EISA. The incorporation of phosphotyrosine, another substrate of phosphatase, into the resulting precursor, provides one more enzymatic trigger on a single molecule, and meanwhile increases the precursors’ propensity to aggregate after being fully dephosphorylated. Exchanging the positions of phosphorylated serine and tyrosine in the peptide backbone provides insights on how the specific molecular structures influence self-assembling behaviors of small peptides and the subsequent cellular responses. Moreover, the utilization of D-amino acids largely enhances the biostability of the peptides, thus providing a unique soft material for potential biomedical applications.

关键词： enzyme-instructed self-assembly     phosphoserine     phosphatase     supramolecular hydrogel    

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Frontiers of Catalysis Chemistry and Technology

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 1-2 doi: 10.1007/s11705-018-1704-0

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Self-assembled bright luminescent hierarchical materials from a tripodal benzoate antenna and heptadentate Eu(III) and Tb(III) cyclen complexes

Aramballi J. Savyasachi, David F. Caffrey, Kevin Byrne, Gerard Tobin, Bruno D'Agostino, Wolfgang Schmitt, Thorfinnur Gunnlaugsson

《化学科学与工程前沿（英文）》 2019年 第13卷 第1期   页码 171-184 doi: 10.1007/s11705-018-1762-3

摘要：

The europium heptadentate coordinatively unsaturated (Eu(III)) and the terbium (Tb(III)) 1,4,7,10-tetraazacyclododecane (cyclen) complexes 1 and 2 were used in conjunction with ligand 3 (1,3,5-benzene-trisethynylbenzoate) to form the supramolecular self-assembly structures 4 and 5; this being investigated in both the solid and the solution state. The resulting self-assemblies gave rise to metal centered emission (both in the solid and solution) upon excitation of 3, confirming its role as a sensitizing antenna. Drop-cased examples of ligand 3, and the solid forms of 4 and 5, formed from both organic and mixture of organic-aqueous solutions, were analyzed using Scanning Electron Microscopy, which showed significant changes in morphology; the ligand giving rise to one dimensional structures, while both 4 and 5 formed amorphous materials that were highly dense solid networks containing nanoporous features. The surface area (216 and 119 m2·g−1 for 4 and 5 respectively) and the ability of these porous materials to capture and store gases such as N2 investigated at 77 K. The self-assembly formation was also investigated in diluted solution by monitoring the various photophysical properties of 3–5. This demonstrated that the most stable structures were that consisting of a single antennae 3 and three complexes of 1 or 2 (e.g., 4 and 5) in solution. By monitoring the excited state lifetimes of the Eu(III) and Tb(III) ions in H2O and D2O respectively, we showed that their hydration states (the q-value) changed from ~2 to 0, upon formation of the assemblies, indicating that the three benzoates of 3 coordinated directly to the each of the three lanthanide centers. Finally we demonstrate that this hierarchically porous materials can be used for the sensing of organic solvents as the emission is highly depended on the solvent environment; the lanthanide emission being quenched in the presence of acetonitrile and THF, but greatly enhanced in the presence of methanol.

关键词： self-assembly     supramolecular chemistry     lanthanides     Eu(III) and Tb(III) complexes     luminescence     metallostars    

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Role of water chemistry on estrone removal by nanofiltration with the presence of hydrophobic acids

Xue JIN,Jiangyong HU

《环境科学与工程前沿（英文）》 2015年 第9卷 第1期   页码 164-170 doi: 10.1007/s11783-014-0747-9

摘要： Hydrophobic acid organic matter (HpoA) extracted from treated effluent has been known to improve the rejection of steroid hormone estrone by reverse osmosis (RO) and nanofiltration (NF) membranes. In this study, the effects of solution chemistry (solution pH and ionic strength) on the estrone rejection by NF membrane with the presence of HpoA were systematically investigated. Crossflow nanofiltration experiments show that the presence of HpoA significantly improved estrone rejection at all pH and ionic strength levels investigated. It is consistently shown that the “enhancement effect” of HpoA on estrone rejection at neutral and alkaline pH is attributed to the binding of estrone by HpoA macromolecules via hydrogen bonding between phenolic functional groups in feed solutions, which leads to an increase in molecular weight and appearance of negative charge. The membrane exhibited the best performance in terms of estrone rejection at pH 10.4 (compared to pH 4 and pH 7) as a result of strengthening the electrostatic repulsion between estrone and membrane with the presence of HpoA. At neutral pH level, the ability of HpoA macromolecules to promote estrone rejection became stronger with increasing ionic strength due to their more extended conformation, which created more chances for the association between estrone and HpoA. The important conclusion of this study is that increasing solution pH and salinity can greatly intensify the “enhancement effect” of HpoA. These results can be important for NF application in direct/indirect potable water reuse.

关键词： indirect potable water reuse     steroid hormone     nanofiltration(NF)     rejection     water chemistry     hydrophobic acids    

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Hexavalent chromium in drinking water: Chemistry, challenges and future outlook on Sn(II)- and photocatalyst-based

Haizhou Liu, Xuejun Yu

《环境科学与工程前沿（英文）》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1267-4

摘要： Abstract • Wide occurrence of Cr(VI) in US source drinking water. • A strong dependence of occurrence on groundwater sources. • Elucidate Redox and equilibrium chemistry of Cr(VI). • Sn(II)-based and TiO2-based reductive treatments hold extreme promise. • Key challenges include residual waste, Cr(VI) re-generation and socioeconomic drivers. Chromium (Cr) typically exists in either trivalent and hexavalent oxidation states in drinking water, i.e., Cr(III) and Cr(VI), with Cr(VI) of particular concern in recent years due to its high toxicity and new regulatory standards. This Account presented a critical analysis of the sources and occurrence of Cr(VI) in drinking water in the United States, analyzed the equilibrium chemistry of Cr(VI) species, summarized important redox reaction relevant to the fate of Cr(VI) in drinking water, and critically reviewed emerging Cr(VI) treatment technologies. There is a wide occurrence of Cr(VI) in US source drinking water, with a strong dependence on groundwater sources, mainly due to naturally weathering of chromium-containing aquifers. Challenges regarding traditional Cr(VI) treatment include chemical cost, generation of secondary waste and inadvertent re-generation of Cr(VI) after treatment. To overcome these challenges, reductive Cr(VI) treatment technologies based on the application of stannous tin or electron-releasing titanium dioxide photocatalyst hold extreme promise in the future. To moving forward in the right direction, three key questions need further exploration for the technology implementation, including effective management of residual waste, minimizing the risks of Cr(VI) re-occurrence downstream of drinking water treatment plant, and promote the socioeconomic drivers for Cr(VI) control in the future.

关键词： Chromium     Chemistry     Treatment     Future outlook    

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Where physics meets chemistry: Thin film deposition from reactive plasmas

Andrew Michelmore, Jason D. Whittle, James W. Bradley, Robert D. Short

《化学科学与工程前沿（英文）》 2016年 第10卷 第4期   页码 441-458 doi: 10.1007/s11705-016-1598-7

摘要： Functionalising surfaces using polymeric thin films is an industrially important field. One technique for achieving nanoscale, controlled surface functionalization is plasma deposition. Plasma deposition has advantages over other surface engineering processes, including that it is solvent free, substrate and geometry independent, and the surface properties of the film can be designed by judicious choice of precursor and plasma conditions. Despite the utility of this method, the mechanisms of plasma polymer growth are generally unknown, and are usually described by chemical (i.e., radical) pathways. In this review, we aim to show that plasma physics drives the chemistry of the plasma phase, and surface-plasma interactions. For example, we show that ionic species can react in the plasma to form larger ions, and also arrive at surfaces with energies greater than 1000 kJ?mol (>10 eV) and thus facilitate surface reactions that have not been taken into account previously. Thus, improving thin film deposition processes requires an understanding of both physical and chemical processes in plasma.

关键词： thin films     plasma physics     plasma chemistry     functionalization     polymer    

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秦山核电厂二回路系统水化学的改进

陶钧,孔德萍

《中国工程科学》 2008年 第10卷 第1期   页码 91-96

摘要：

核电厂二回路系统的水质控制与关键重要设备蒸汽发生器的运行寿命有着密切的关系，秦山核电厂运行16年来，随着秦山核电厂二回路系统水化学管理的不断改进，二回路系统的水质不断改善。这些管理改进主要体现在管理理念的改变，二回路系统高AVT（全会法处理方式）处理、对凝结水精处理装置的优化运行以及大修及启动过程的严格控制等。通过这些改进措施的实施，电厂的WANO（世界核营运者协会）化学性能指标从1997年的1.66下降到2006年的1.00，达到了世界先进水平。二回路水化学的改善确保了蒸汽发生器传热管的结构完整性。

关键词： 二回路     水化学     WANO化学性能指标    

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Bioorthogonal chemistry based on-demand drug delivery system in cancer therapy

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 483-489 doi: 10.1007/s11705-022-2227-2

摘要： Benefiting from the advantage of taking place in biological environments without interfering with an innate biochemical process, the bioorthogonal reaction that commonly contains the “bond formation” and “bond cleavage” system has been widely used in targeted therapy for a variety of tumors. Herein, several prominent cases based on the bioorthogonal reaction that tailoring the metabolic glycoengineering tactics to modified cells for cancer immunotherapy, and the innovative tactics for reducing the metal ions’ toxic and side effects with microneedle patches will be highlighted. Based on these applications, the complexities, potential pitfalls, and opportunities of bioorthogonal chemistry in future cancer therapy will be evaluated.

关键词： bioorthogonal reaction     cancer therapy     metabolic glycoengineering     bioorthogonal catalytic patch    

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The First Attempt for Accounts of Environmental Chemistry and Technology Research

Jinyong Liu, Yin Wang, Haoran Wei

《环境科学与工程前沿（英文）》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1270-9

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Regulating surface chemistry of separator with LiF for advanced Li-S batteries

《能源前沿（英文）》 2022年 第16卷 第4期   页码 601-606 doi: 10.1007/s11708-021-0759-7

摘要： Lithium-sulfur (Li-S) batteries have attracted intensive attention owing to their ultrahigh theoretical energy density. Nevertheless, the practical application of Li-S batteries is prevented by uncontrollable shuttle effect and retarded reaction kinetics. To address the above issues, lithium fluoride (LiF) was employed to regulate the surface chemistry of routine separator. The functional separator demonstrates a great ability to suppress active S loss and protect lithium anode. This work provides a facile strategy for the development of advanced Li-S batteries.

关键词： Li-S batteries     LiF     functional separator    

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Supramolecular self-assembly of two-component systems comprising aromatic amides/Schiff base and tartaric

Xin Wang, Wei Cui, Bin Li, Xiaojie Zhang, Yongxin Zhang, Yaodong Huang

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 1112-1121 doi: 10.1007/s11705-019-1865-5

摘要： The gelating properties and thermotropic behaviors of stoichiometric mixtures of aromatic amides , and the aromatic Schiff base with tartaric acid (TA) were investigated. Among the three gelators, -TA exhibited superior gelating ability. Mixture -TA exhibits a smectic B phase and an unidentified smectic mesophase during both heating and cooling runs. The results of Fourier transform infrared spectroscopy and X-ray diffraction revealed the existence of hydrogen bonding and - interactions in -TA systems, which are likely to be the dominant driving forces for the supramolecular self-assembly. Additionally, it was established that all of the studied gel self-assemblies and mesophases possess a lamellar structure. The anion response ability of the tetrahydrofuran gel of -TA was evaluated and it was found that it was responsive to the stimuli of F , Cl , Br , I , AcO .

关键词： supramolecular self-assembly     organogel     liquid crystal     tartaric acid     hydrogen bond    

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Cadmium removal mechanistic comparison of three Fe-based nanomaterials: Water-chemistry and roles of

《环境科学与工程前沿（英文）》 2022年 第16卷 第12期 doi: 10.1007/s11783-022-1586-8

摘要：

● nZVI, S-nZVI, and nFeS were systematically compared for Cd(II) removal.

关键词： Nano zero valent iron     Sulfided zero valent iron     FeS     Cd(II) immobilization     Fe dissolution    

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compositions in sulfuric acid catalyzed isobutane/butene alkylation products: experimental and quantum chemistry

Lina Liang, Youzhi Liu, Weizhou Jiao, Qiaoling Zhang, Chao Zhang

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1229-1242 doi: 10.1007/s11705-020-2030-x

摘要： Octanes in alkylation products obtained from industrial alkylation were studied by batch experiments. More than eight octane isomers were identified and quantified by gas chromatography-mass spectrometry. Based on a classic carbenium ion mechanism, the carbocation transition states in concentrated sulfuric acid catalyzed alkylation were investigated using quantum-chemical simulations and predicted the concentration and octane isomerization products including trimethylpentane and dimethylhexane as well as the formation of heavier compounds that resulted from the oligomerization of octane and butene. The agreement between model calculations and experimental data was quite satisfactory. Calculation results indicated that composition and content of trimethylpentanes in the alkylation products were 2,2,4-trimethylpentane>2,3,3-trimethylpentane>2,3,4-trimethylpentane>2,2,3-trimethylpentane whether the 2-butene or -butene acts as olefin. Heavier compounds in the alkylate were primarily formed by the oligomerization of dimethylhexane with 1-butene. Hopefully, the carbocation transition state models developed in this work will be useful for understanding the product distributions of octane in alkylation products.

关键词： sulfuric acid catalyzed alkylation     carbocation reaction     transition state     octane compositions    

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催化裂化过程反应化学的进展

许友好,汪燮卿

《中国工程科学》 2007年 第9卷 第8期   页码 6-14

摘要：

面对催化裂化工艺所遇到的挑战，提出了催化裂化过程反应化学的多维反应结构模式。多维反应结构模式的建立是基于对烃类在酸性催化剂上反应化学认识而进行的知识创新，但多维反应结构不同于烃类在酸性催化剂上反应化学。具有多维反应结构的催化裂化工艺更具有多样性和灵活性，基于此已成功地开发了多产异构烷烃的催化裂化工艺和生产清洁汽油和多产丙烯的催化裂化工艺。

关键词： 催化裂化     反应化学     催化剂     多维反应结构     两个反应区    

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标题 作者 时间 类型 操作

All-in-one functional supramolecular nanoparticles based on pillar[5]arene for controlled generation,

期刊论文

Enzyme-instructed self-assembly of peptides containing phosphoserine to form supramolecular hydrogels

Jie Zhou, Xuewen Du, Jiaqing Wang, Natsuko Yamagata, Bing Xu

期刊论文

Frontiers of Catalysis Chemistry and Technology

期刊论文

Self-assembled bright luminescent hierarchical materials from a tripodal benzoate antenna and heptadentate Eu(III) and Tb(III) cyclen complexes

Aramballi J. Savyasachi, David F. Caffrey, Kevin Byrne, Gerard Tobin, Bruno D'Agostino, Wolfgang Schmitt, Thorfinnur Gunnlaugsson

期刊论文

Role of water chemistry on estrone removal by nanofiltration with the presence of hydrophobic acids

Xue JIN,Jiangyong HU

期刊论文

Hexavalent chromium in drinking water: Chemistry, challenges and future outlook on Sn(II)- and photocatalyst-based

Haizhou Liu, Xuejun Yu

期刊论文

Where physics meets chemistry: Thin film deposition from reactive plasmas

Andrew Michelmore, Jason D. Whittle, James W. Bradley, Robert D. Short

期刊论文

秦山核电厂二回路系统水化学的改进

陶钧,孔德萍

期刊论文

Bioorthogonal chemistry based on-demand drug delivery system in cancer therapy

期刊论文

The First Attempt for Accounts of Environmental Chemistry and Technology Research

Jinyong Liu, Yin Wang, Haoran Wei

期刊论文

Regulating surface chemistry of separator with LiF for advanced Li-S batteries

期刊论文

Supramolecular self-assembly of two-component systems comprising aromatic amides/Schiff base and tartaric

Xin Wang, Wei Cui, Bin Li, Xiaojie Zhang, Yongxin Zhang, Yaodong Huang

期刊论文

Cadmium removal mechanistic comparison of three Fe-based nanomaterials: Water-chemistry and roles of

期刊论文

compositions in sulfuric acid catalyzed isobutane/butene alkylation products: experimental and quantum chemistry

Lina Liang, Youzhi Liu, Weizhou Jiao, Qiaoling Zhang, Chao Zhang

期刊论文

催化裂化过程反应化学的进展

许友好,汪燮卿

期刊论文