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Continuous deacylation of amides in a high-temperature and high-pressure microreactor

《化学科学与工程前沿（英文）》 2022年第16卷第12期页码 1818-1825 doi: 10.1007/s11705-022-2182-y

摘要： The deacylation of amides, which is widely employed in the pharmaceutical industry, is not a fast reaction under normal conditions. To intensify this reaction, a high-temperature and high-pressure continuous microreaction technology was developed, whose space-time yield was 49.4 times that of traditional batch reactions. Using the deacylation of acetanilide as a model reaction, the effects of the temperature, pressure, reaction time, molar ratio of reactants, and water composition on acetanilide conversion were carefully studied. Based on the rapid heating and cooling capabilities, the kinetics of acetanilide deacylation at high temperatures were investigated to determine the orders of reactants and activation energy. This microreaction technology was further applied to a variety of other amides to understand the influence of substituents and steric hindrance on the deacylation reaction.

关键词： amide deacylation microreactor flow chemistry reaction intensification

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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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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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瑞德西韦核碱基单元的连续流合成 Article

郭永兴, 刘敏杰, 姜梅芬, 陶媛, 程荡, 陈芬儿

《工程（英文）》 2023年第21卷第2期页码 92-100 doi: 10.1016/j.eng.2021.07.029

摘要：

本研究通过五步连续流合成了抗病毒药物瑞德西韦的核碱基单元7-溴吡咯[2,1-f][1‒2,4]三嗪-4-胺。采用间歇式合成化学方法，利用广泛可用且廉价的起始原料吡咯，通过顺序流动操作成功生产了7-溴吡咯[2,1-f][1‒2,4]三嗪-4-胺。在最佳流动条件下，7-溴吡咯[2,1-f][1‒2,4]三嗪-4-胺的分离收率为14.1%，总停留时间为79 min，通量为2.96 g∙h⁻¹,总停留时间明显短于批处理程序中消耗的总时间（大于26.5 h）。在流动中，有利地促进了涉及危险和不稳定的中间体的高度放热的Vilsmeier-Haack 和N-胺化反应、氧化液-液双相转化及需要严格低温条件的溴化反应。这种合成方法的显著特点是，通过部署专用设备和分离单元，将后处理程序完全集成到反应序列中，从而形成一个精简的连续流系统，最大限度地提高整个过程的效率。该方法是一种更环保、更可持续的高效、安全地制备核碱基单元的方法。

关键词：流动化学连续多步合成微反应技术反应分离集成

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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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电化学微反应技术的工程研究进展——一种新型有机化合物电合成方法 Review

郑思源, 闫俊妤, 王凯

《工程（英文）》 2021年第7卷第1期页码 22-32 doi: 10.1016/j.eng.2020.06.025

摘要：

电化学方法环境友好，在有机化学合成中具有独特的优势。然而，传统的电化学反应器存在复杂的传递问题，限制了电化学方法的应用。近年来，微反应技术在电合成研究中的应用缩短了离子的传递距离并增加了电极的比表面积，从而促成了高效、连续且易于规模化的电合成技术。本文从过程强化的角度讨论了在电合成中使用微通道的工程优势，分析了最近报道的电化学微反应器中的流型和传质行为，并列举了反应器放大的典型例子。作为一个相对较新的研究领域，在微反应器中进行电合成的许多科学规则和工程特征都有待研究。因此本文提出了潜在的研究重点，认为其对新型电合成技术的发展至关重要。

关键词：电化学电合成微反应器流动化学

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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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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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合成橡胶化学及技术进展

武冠英

《中国工程科学》 1999年第1卷第3期页码 79-85

摘要：

文章从合成橡胶的化学基础出发，叙述了合成橡胶工业二十世纪以来的过去、现状，并展望未来。着重讨论了合成化学基础及相应聚合工艺过程的进步这两方面的问题。指出合成橡胶化学基础中活性聚合、可控聚合，包括茂金属催化剂仍为近期的重点；气相聚合工艺将会得到较大的发展；高效聚合釜的研究仍是核心问题；环保问题应更受到重视。

关键词：合成橡胶合成化学活性/控制聚合气相聚合