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Titania-activated persulfate for environmental remediation: the-state-of-the-art 二氧化钛活化过硫酸盐用于环境修复:最先进的
Pub Date : 2021-11-19 DOI: 10.1080/01614940.2021.1996776
M. Sabri, A. Habibi-Yangjeh, Shima Rahim Pouran, Chundong Wang
ABSTRACT In the last decade, a considerable body of literature has been devoted to advanced oxidation processes encompassed peroxy-sulfur species owing to their capacity to generate highly active radicals. These species fulfill two main objectives in AOPs: act as electron-scavengers and give rise to sulfate radicals, which collectively facilitate the oxidation of organic pollutants. This review provides data on the recent strategies and practices aimed to enhance the photocatalytic performance of TiO2 where persulfate/peroxymonosulfate species are supplemented. The mechanism of persulfate activation, direct and interactive effects on the photoactivity of TiO2 nanostructures, and subsequent degradation efficiencies of agrochemicals, dyes, pharmaceuticals, petrochemicals, and pathogenic microorganisms were studied and thoroughly discussed. The data on several titania-based nanostructures, the best operational conditions, and the removal outputs in the presence of oxidants and electron acceptors, in particular, persulfate ions are summarized, depicted, and tabulated. As per reviewed literature, titania-persulfate integration can effectively address the environmental implications of organic pollutants.
在过去的十年中,相当多的文献已经致力于高级氧化过程,包括过氧硫物种,因为它们能够产生高活性自由基。这些物种在AOPs中实现了两个主要目标:作为电子清除剂和产生硫酸盐自由基,它们共同促进有机污染物的氧化。本文综述了近年来通过补充过硫酸盐/过氧单硫酸盐来提高TiO2光催化性能的策略和实践。研究并深入讨论了过硫酸盐活化的机理、对TiO2纳米结构光活性的直接和相互作用,以及随后对农药、染料、药品、石化产品和病原微生物的降解效率。本文总结了几种钛基纳米结构的数据,最佳操作条件,以及在氧化剂和电子受体,特别是过硫酸盐存在下的去除输出。根据文献综述,二氧化钛-过硫酸钛一体化可以有效地解决有机污染物的环境影响。
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引用次数: 81
Low-Temperature Heterogeneous Oxidation Catalysis and Molecular Oxygen Activation 低温非均相氧化催化与分子氧活化
Pub Date : 2021-10-31 DOI: 10.1080/01614940.2021.1919044
U. J. Etim, P. Bai, Oz M. Gazit, Z. Zhong
ABSTRACT Many natural oxidations are relevant to the origin and running of life but usually proceeded under mild conditions using molecular oxygen (O2) in the air as the sole oxidant and enzymes as the catalysts. In modern society, catalysis plays an essential role in many industries, such as chemical and pharmaceutical industries. However, most heterogeneous catalytic reactions need high operational reaction temperature and pressure. Research interest is redirected to green catalysis in recent years, e.g., running catalytic reactions under mild conditions, employing green solvents and green oxidants such O2, particularly air. One question always exists: can these industrial catalytic processes be ultimately run similar to the natural oxidation processes in efficiency and operation conditions? For many catalytic oxidation reactions, the greatest challenge lies in activating molecular oxygen under mild conditions. Therefore, a molecular-level understanding of the interactions of O2 molecules with catalysts or substrates is necessary and crucial. In this review, we discuss the activation of O2 to different active species (e.g., O2 2− or O2 2−) and their participation in low-temperature (≤300 oC) catalytic oxidation reactions. The challenges, recent progress, and trends in some low-temperature oxidation reactions are discussed and highlighted. The early studies on the activation of oxygen on various catalysts mainly paid attention to the interaction between the molecular oxygen and the oxygen vacancies of metal oxides. In contrast, recent studies try to fully understand the generation, measurement, and catalytic roles of the various active oxygen species. Therefore, the design of catalysts that can facilely activate O2 at low temperatures is of importance. With such catalysts, it is possible to reduce the high energy consumption, improve the selectivity of catalytic oxidations, and ultimately realize the industrial oxidation reactions at conditions as mild as possible to that of many natural oxidation processes. Finally, from the current body of knowledge, we propose future directions that can effectively utilize O2 for solving practical problems at low temperatures and help understand the oxidation catalysis at the molecular level.
许多自然氧化与生命的起源和运行有关,但通常在温和的条件下进行,以空气中的分子氧(O2)为唯一的氧化剂,酶为催化剂。在现代社会中,催化在许多工业中起着至关重要的作用,如化学和制药工业。然而,大多数非均相催化反应需要较高的操作反应温度和压力。近年来,研究方向转向绿色催化,如在温和条件下进行催化反应,使用绿色溶剂和绿色氧化剂,如O2,特别是空气。一个始终存在的问题是:这些工业催化过程最终能否在效率和操作条件上与自然氧化过程相似?对于许多催化氧化反应来说,最大的挑战在于如何在温和的条件下激活分子氧。因此,在分子水平上理解O2分子与催化剂或底物的相互作用是必要和关键的。在这篇综述中,我们讨论了O2对不同活性物质(如O2 2 -或O2 2 -)的活化及其在低温(≤300℃)催化氧化反应中的参与。讨论并强调了低温氧化反应的挑战、最新进展和发展趋势。早期对氧在各种催化剂上的活化研究主要关注的是分子氧与金属氧化物氧空位之间的相互作用。相比之下,最近的研究试图充分了解各种活性氧的产生、测量和催化作用。因此,设计能在低温下方便地活化O2的催化剂具有重要意义。有了这种催化剂,就有可能降低高能耗,提高催化氧化的选择性,最终实现工业氧化反应在尽可能温和的条件下达到许多自然氧化过程。最后,根据目前的知识体系,我们提出了未来的方向,可以有效地利用O2来解决低温下的实际问题,并有助于在分子水平上理解氧化催化。
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引用次数: 16
Nanocarbons in quantum regime: An emerging sustainable catalytic platform for organic synthesis 纳米碳在量子机制:一个新兴的可持续的有机合成催化平台
Pub Date : 2021-10-26 DOI: 10.1080/01614940.2021.1985866
A. Dandia, Pratibha Saini, Mukul Sethi, Krishan Kumar, Surendra Saini, Savita Meena, Swati Meena, Vijay Parewa
ABSTRACT Fluorescent carbon quantum dots (CQDs), specified by feature sizes of <10 nm, have become a mystic newcomers in the world of nanoscience and attracted much focus of synthetic chemists since the last decade due to their esoteric physico-chemical features. Because of these magical characteristics, carbon dots-based catalytic systems have unlocked the gateway for eco-friendly, benign, and cost-effective next-generation platform for “Nanocatalysis and Photocatalysis” in organic synthesis. The introduction of CQDs in organic synthesis allows the designing new reactions or catalysis in which unique/unprecedented connection/disconnection of chemical bonds has been implemented for the construction of new molecular architectures. This critical review presents a comprehensive study of the catalytic and photocatalytic efficiency of CQDs in organic synthesis which has initiated a more sustainable strategy in to the catalysis field. By systematic summarization and categorization of various organic transformations such as coupling reactions, oxidation reactions, reduction reactions, condensation reactions, ring-opening reactions, epoxidation, C-H activation, etc., a clear picture of all available catalytic and photocatalytic strategies for CQDs are presented and their unique role in various catalytic approaches for specific reactions are discussed in detail. Catalytic aspects of CQDs in heterocyclic synthesis are also been reviewed. Finally, challenges and future aspects associated with the green catalytic efficiency of CQDs in organic synthesis are highlighted. Herein, this review summarizes the current investigations on CQDs for various organic transformations during last 10 years. We experience that the entire potential of CQDs in organic synthesis has yet to be fully explored in organic synthesis. We hope that this review is serving as a humble urge to encourage other organic chemists for further use of CQDs as a sustainable catalyst in organic synthesis. Graphical Abstract
荧光碳量子点(CQDs)是纳米科学领域的一个神秘的新成员,其特征尺寸小于10 nm,由于其深奥的物理化学特性,近十年来引起了合成化学家的广泛关注。由于这些神奇的特性,基于碳点的催化系统为有机合成中的“纳米催化和光催化”打开了环保、良性、经济高效的下一代平台的大门。CQDs在有机合成中的引入允许设计新的反应或催化,其中独特的/前所未有的化学键连接/断开已经实现了新的分子结构的构建。本文对CQDs在有机合成中的催化和光催化效率进行了全面的研究,为催化领域开辟了一个更可持续的发展战略。通过系统总结和分类各种有机转化,如偶联反应、氧化反应、还原反应、缩合反应、开环反应、环氧化反应、C-H活化等,清晰地展示了CQDs所有可用的催化和光催化策略,并详细讨论了CQDs在各种特定反应催化方法中的独特作用。综述了CQDs在杂环合成中的催化作用。最后,强调了CQDs在有机合成中的绿色催化效率所面临的挑战和未来的发展方向。本文综述了近10年来CQDs在各种有机转化中的研究进展。我们的经验是,CQDs在有机合成中的全部潜力尚未在有机合成中得到充分挖掘。我们希望这篇综述能作为一种谦卑的敦促,鼓励其他有机化学家进一步使用CQDs作为有机合成中的可持续催化剂。图形抽象
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引用次数: 7
Progress in the application of surface engineering methods in immobilizing TiO2 and ZnO coatings for environmental photocatalysis 表面工程方法在环境光催化固定TiO2和ZnO涂层中的应用进展
Pub Date : 2021-10-06 DOI: 10.1080/01614940.2021.1983066
A. H. Navidpour, A. Hosseinzadeh, John L. Zhou, Zhenguo Huang
ABSTRACT Photocatalysis is widely used for the degradation of organic pollutants, with TiO2 and ZnO as the best candidates with unique properties. However, agglomeration and recycling are major challenges in practical photocatalysis applications. Advanced deposition processes can provide nanotubular or hierarchical structures that are more promising than suspended particles. More importantly, higher efficiency of photoelectrocatalysis than photocatalysis for the degradation of persistent organic pollutants including perfluorooctanoic acid (PFOA) necessitates catalyst immobilization. Photoelectrocatalysis exhibited remarkably higher efficiency (56.1%) than direct photolysis (15.1%), electrocatalysis (5.0%) and photocatalysis (18.1%) for PFOA degradation. This paper aims to review the progress in the application of anodizing and thermal spraying as two major industrial surface engineering processes to bridge the gap between laboratorial and practical photocatalysis technology. Overall, thermal spraying is considered as one of the most efficient methods for the deposition of TiO2 and ZnO photocatalytic films. Graphical Abstract
摘要光催化在有机污染物的降解中得到了广泛的应用,TiO2和ZnO是具有独特性能的最佳候选材料。然而,在实际的光催化应用中,团聚和回收是主要的挑战。先进的沉积工艺可以提供比悬浮粒子更有前途的纳米管或分层结构。更重要的是,在降解包括全氟辛酸(PFOA)在内的持久性有机污染物方面,光电催化比光催化效率更高,因此需要固定化催化剂。光电催化对PFOA的降解效率(56.1%)显著高于直接光解(15.1%)、电催化(5.0%)和光催化(18.1%)。本文旨在综述阳极氧化和热喷涂作为两种主要的工业表面工程工艺的应用进展,以弥合实验室与实际光催化技术之间的差距。总的来说,热喷涂被认为是制备TiO2和ZnO光催化膜最有效的方法之一。图形抽象
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引用次数: 14
Microreaction and membrane technologies for continuous single-enantiomer production: A review 连续生产单对映体的微反应和膜技术综述
Pub Date : 2021-09-28 DOI: 10.1080/01614940.2021.1977009
Z. Petrusová, Z. Slouka, Lucie Vobecká, Petr Polezhaev, P. Hasal, M. Přibyl, P. Izák
ABSTRACT Microreaction and membrane technologies offer optimal conditions for controlling enantiomer synthesis and purification processes in continuous production, with numerous advantages over batch manufacturing. One of the many forces driving the development of such technologies for the production of single optical isomers is the need for enantiomerically pure pharmaceutical drugs because enantiomers may display opposite therapeutic effects or different treatment efficacies and side effects. Yet, despite advances in asymmetric synthesis and separation techniques, preparing enantiomerically pure compounds remains a challenging task. Here, we review the progress in microfluidics and membrane chiral separation over the last two decades. In addition to describing and critically assessing the state of the art in both disciplines, we provide an overview of their beneficial properties and characteristics for developing technologies toward producing enantiomerically pure compounds. Concomitantly, we evaluate efforts to integrate synthesis and membrane separation into a microfluidic platform and pinpoint the limiting factors that must be overcome before these platforms can be fully deployed in the industry.
微反应和膜技术为连续生产中控制对映体的合成和纯化过程提供了最佳条件,与批量生产相比具有许多优势。推动这种生产单一光学异构体的技术发展的众多力量之一是对对映体纯药物的需求,因为对映体可能显示相反的治疗效果或不同的治疗效果和副作用。然而,尽管不对称合成和分离技术取得了进步,制备对映体纯化合物仍然是一项具有挑战性的任务。本文综述了近二十年来微流体和膜手性分离的研究进展。除了描述和批判性地评估这两个学科的最新进展外,我们还概述了它们的有益性质和特征,以开发生产对映异构纯化合物的技术。同时,我们评估了将合成和膜分离整合到微流控平台中的努力,并指出了在这些平台完全应用于工业之前必须克服的限制因素。
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引用次数: 3
Catalytic valorization of CO2 by hydrogenation: current status and future trends 二氧化碳加氢催化价化:现状与未来趋势
Pub Date : 2021-09-02 DOI: 10.1080/01614940.2021.1968197
I. Sancho‐Sanz, S. Korili, A. Gil
ABSTRACT Terrestrial environmental and biological systems are being threatened by the tremendous amount of human carbon dioxide emissions. Therefore, it is crucial to develop a sustainable energy system based on CO2 as chemical feedstock. In this review, an introduction to the CO2 activation and transformation has been made, together with a more comprehensive study of the catalytical reduction of CO2 to methane, methanol, and formic acid, which are currently contemplated as chemical feedstocks and/or promising energy carriers and alternative fuels.
人类排放的大量二氧化碳正威胁着陆地环境和生物系统。因此,开发以二氧化碳为化学原料的可持续能源系统至关重要。本文介绍了二氧化碳的活化和转化,并对二氧化碳催化还原为甲烷、甲醇和甲酸进行了更全面的研究,这些化合物目前被认为是化学原料和/或有前途的能源载体和替代燃料。
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引用次数: 9
One-pot amination of aldehydes and ketones over heterogeneous catalysts for production of secondary amines 多相催化剂上醛酮一锅胺化反应制备仲胺
Pub Date : 2021-09-01 DOI: 10.1080/01614940.2021.1942689
P. Mäki-Arvela, I. Simakova, D. Murzin
ABSTRACT This review summarizes the recent studies on the synthesis of secondary amines by one-pot amination of aldehydes and ketones over heterogeneous catalysts. Amines are widely applied as the key intermediates in chemical industry for the synthesis of various commodities such as agrochemicals, drugs, detergents, lubricants, food-additives and polymers. Direct catalytic reductive amination of carbonyl compounds was considered which generally includes two steps: (i) formation of imines by interactions of aldehydes or ketones with amines, and (ii) subsequent hydrogenation of imines. Synthesis of secondary amines from carbonyl compounds and amines generated in situ under reaction conditions from their progenitors, e.g., respectively, alcohols or nitro-compounds, is also discussed in detail. Recent progress in application of hydrogen sources alternative to gaseous H2, such as formic acid, NaBH4, CO and water, favored development of metal-free catalysts including solid acid catalysts. The review addresses the scope of the amination reaction with aldehydes/ketones and nitro/amine compounds of different structure, the effect of the solvent, reaction conditions and catalyst properties. In addition, catalyst regeneration and reuse, kinetic regularities and kinetic modeling with an emphasis on the continuous mode of one-pot amination have been systematically summarized and discussed. It is suggested that the future work should focus on revealing the role of the catalytically active sites addressing their acid–base properties and the correlation between catalyst properties and the reaction performance, elucidating kinetic parameters and designing feasible reactor system for further industrial implementation.
摘要综述了近年来在非均相催化下,醛酮一锅胺化法合成仲胺的研究进展。在化学工业中,胺作为关键中间体被广泛应用于合成各种商品,如农用化学品、药品、洗涤剂、润滑剂、食品添加剂和聚合物。羰基化合物的直接催化还原胺化通常包括两个步骤:(i)通过醛或酮与胺的相互作用形成亚胺,以及(ii)随后的亚胺氢化。本文还详细讨论了羰基化合物合成仲胺的方法,以及在反应条件下由它们的前体(如醇或硝基化合物)原位生成的胺的方法。近年来甲酸、NaBH4、CO和水等氢源替代氢的应用进展有利于固体酸催化剂等无金属催化剂的发展。综述了不同结构的醛/酮类和硝基/胺类化合物的胺化反应的范围、溶剂、反应条件和催化剂性能的影响。此外,还对催化剂的再生与再利用、动力学规律和动力学建模进行了系统的总结和讨论,并以一锅连续化模式为重点。建议今后的工作重点是揭示催化活性位点的作用,确定其酸碱性质以及催化剂性质与反应性能的关系,阐明动力学参数并设计可行的反应器系统,以便进一步工业化实施。
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引用次数: 7
MoS2 based ternary composites: review on heterogeneous materials as catalyst for photocatalytic degradation 二硫化钼基三元复合材料:光催化降解催化剂的多相材料研究进展
Pub Date : 2021-08-25 DOI: 10.1080/01614940.2021.1962493
S. Mohana Roopan, Mohammad Ahmed Khan
ABSTRACT Photocatalytic degradation is an upcoming technique for the removal of organic pollutants from wastewater. This topic attracts increasing interest due to its potential of utilizing “freely” available solar energy for environmental purification. In recent years, MoS2 based photocatalysts have garnered substantial attention for their graphene-like structure and suitable bandgap for visible light photocatalysis, unlike that of TiO2. However, pure MoS2 has many disadvantages like the high recombination rate of its electron-hole pairs as well as narrow bandgap, which affects its efficiency as a photocatalyst. It has been proven that heterojunction photocatalysts of MoS2 have an increased photoactivity when compared to pristine MoS2. The latest advancements in the field of MoS2 based ternary composites are summarized in this review, with a special emphasis on the application part for wastewater treatment. We have compiled relevant information for the degradation of organic pollutants using photocatalysis with the aim to further the research in this field.
光催化降解是一种新兴的去除废水中有机污染物的技术。由于其利用“免费”可获得的太阳能进行环境净化的潜力,该主题引起了越来越多的兴趣。近年来,基于MoS2的光催化剂因其与TiO2不同的类石墨烯结构和适合可见光光催化的带隙而受到广泛关注。然而,纯二硫化钼具有电子-空穴对复合率高、带隙窄等缺点,影响了其作为光催化剂的效率。实验证明,与原始的MoS2相比,MoS2异质结光催化剂具有更高的光活性。本文综述了二硫化钼基三元复合材料的最新研究进展,重点介绍了其在废水处理中的应用。我们收集了利用光催化降解有机污染物的相关资料,旨在进一步推动这一领域的研究。
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引用次数: 24
Overview of electrocatalytic treatment of antibiotic pollutants in wastewater 电催化处理废水中抗生素污染物的研究进展
Pub Date : 2021-08-19 DOI: 10.1080/01614940.2021.1960009
H. Gu, W. Xie, Ai Du, Duo Pan, Zhanhu Guo
ABSTRACT Abuse of antibiotics in animal husbandry and medicine has led to severe environmental problems especially the risk of bacterial resistance. Different from common organic pollutants, antibiotics in wastewater could not be easily removed by biological treatment because of their poor biodegradability. Electrocatalysis including electrocatalytic oxidation and reduction has gained great attention for the removal of antibiotic contaminants in wastewater due to its advantages of high efficiency, simple operation, and thorough degradation. This review summarizes the common features and synthesis methods as well as research progress of electrode materials used in the electrocatalytic process for the treatment of antibiotics in the last five years. The removal mechanism and transformation pathways of antibiotics in the electrocatalytic oxidation and reduction processes are presented, especially to avoid the second pollution. Cost aspects in the electrocatalytic process are also discussed by considering practical applications and comparison with adsorption and photocatalysis process. Finally, several developing directions of electrocatalysis in the antibiotic wastewater treatment are proposed as a guidance for further research. Graphical Abstract
畜牧业和医药中抗生素的滥用已经造成了严重的环境问题,尤其是细菌耐药性的风险。与常见的有机污染物不同,废水中的抗生素具有较差的生物可降解性,难以通过生物处理去除。电催化包括电催化氧化和电催化还原因其高效、操作简单、降解彻底等优点,在去除废水中抗生素污染物方面受到广泛关注。本文综述了近五年来用于抗生素电催化治疗的电极材料的共同特点、合成方法以及研究进展。介绍了电催化氧化还原过程中抗生素的去除机理和转化途径,特别是避免了二次污染。结合实际应用,并与吸附、光催化工艺进行比较,讨论了电催化工艺的成本问题。最后,提出了电催化在抗生素废水处理中的几个发展方向,为进一步研究提供指导。图形抽象
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引用次数: 21
A comprehensive review on catalytic O-alkylation of phenol and hydroquinone 苯酚和对苯二酚催化o -烷基化研究综述
Pub Date : 2021-06-22 DOI: 10.1080/01614940.2021.1930490
Priyanka V. Bhongale, S. Joshi, N. Mali
ABSTRACT The alkylation process involves two competitive paths of O- and C-alkylation and achieving better selectivity for desired products is a very challenging problem. The development of new process for synthesis of O-methylated products of phenol and dihydric phenols is a subject of high industrial and academic interest. Alkyl phenyl ethers, especially anisole and 4-methoxyphenol, have captivated significant interest due to their increasing applications in pharmaceutical industries. The main emphasis of the present review is to explore the recent development in two catalytic O-alkylation processes. The first process is O-methylation of phenol into anisole and another is selective mono O-methylation of hydroquinone into 4-methoxyphenol. The present article covers O-alkylation methods with methanol and dimethyl carbonate as alkylating agent over various acidic and basic catalytic systems. The catalyst systems analyzed involves Bronsted and Lewis acidic and basic ionic liquids, conventional acids, metal oxides, solid acid and basic catalysts, hydrotalcites, various zeolites and heteropolyacids. The mechanistic behavior of alkylation reactions in presence of different catalytic system is reviewed critically which is important to design new and/or modified catalyst in order to maximize the yield of desired product. Additionally, an influence of reaction parameters, role of catalyst and their active sites on product distribution is described. The review paper gives useful insight for researchers in the field of catalysis and reaction engineering of alkylation reactions. Understandings of the reaction pathways will help in developing reliable kinetic models necessary for process scale-up to industrial scale reactor system.
烷基化过程涉及到O-和c -两种相互竞争的烷基化途径,实现对所需产物更好的选择性是一个非常具有挑战性的问题。苯酚和二氢苯酚o -甲基化产物合成新工艺的开发是工业和学术界高度关注的课题。烷基苯基醚,特别是苯甲醚和4-甲氧基酚,由于它们在制药工业中的应用越来越广泛,已经引起了人们的极大兴趣。本文重点介绍了两种催化o -烷基化工艺的最新进展。第一个过程是苯酚邻甲基化成苯甲醚,另一个过程是对苯二酚选择性单邻甲基化成4-甲氧基苯酚。本文介绍了以甲醇和碳酸二甲酯为烷基化剂,在各种酸性和碱性催化体系下的o -烷基化方法。所分析的催化剂体系包括Bronsted和Lewis酸性和碱性离子液体、常规酸、金属氧化物、固体酸和碱性催化剂、水滑石、各种沸石和杂多酸。本文对不同催化体系下烷基化反应的机理行为进行了评述,这对设计新的或改性的催化剂以获得最大收率具有重要意义。此外,还讨论了反应参数、催化剂的作用及其活性位点对产物分布的影响。本文对烷基化反应的催化和反应工程领域的研究人员提供了有益的见解。对反应途径的理解将有助于建立可靠的动力学模型,为工业规模反应器系统的工艺放大提供必要条件。
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引用次数: 6
期刊
Catalysis Reviews
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