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Recent advances in Fischer-Tropsch synthesis using cobalt-based catalysts: a review on supports, promoters, and reactors 钴基催化剂在费托合成中的最新进展:载体、促进剂和反应器的综述
Pub Date : 2020-05-18 DOI: 10.1080/01614940.2020.1762367
Z. Gholami, Z. Tišler, Vlastimil Rubáš
ABSTRACT Fischer–Tropsch (FT) process is a promising method for producing liquid fuels and other valuable chemicals through CO hydrogenation. The catalyst activity and product selectivity can be strongly affected by different parameters such as support and promoters. The physicochemical and textural properties of the support affect the metal–support interaction, crystallite size, metal dispersion, mass transfer of reactants/products, mechanical strength, and thermal stability of the catalyst. Promoters can also be used as structural, textural, electronic modifier, stabilizers, and catalyst-poison-resistant, which can improve the catalytic performance. According to the parameters mentioned above, this paper reviews the brief history of the FT process, the effect of different supports and promoters on the catalytic performance of cobalt-based catalysts. In addition to the catalyst properties, the reactor must also be designed appropriately to handle the heat of this highly exothermic reaction. The reactor types have also been reviewed and compared as a crucial part of the catalytic reactions. Graphical Abstract
费托法(FT)是一种很有前途的利用CO加氢生产液体燃料和其他有价化学品的方法。载体和促进剂等参数对催化剂活性和产物选择性有较大影响。载体的物理化学和结构性质影响着金属-载体的相互作用、晶粒大小、金属分散、反应物/产物的传质、机械强度和催化剂的热稳定性。促进剂还可以作为结构、织构、电子改性剂、稳定剂和耐催化毒性剂,提高催化性能。根据上述参数,本文回顾了FT工艺的简史,以及不同载体和促进剂对钴基催化剂催化性能的影响。除了催化剂的性能外,反应器还必须经过适当的设计,以处理这种高度放热反应的热量。作为催化反应的重要组成部分,对反应器类型进行了综述和比较。图形抽象
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引用次数: 70
Recent advances in selective catalytic reduction of NOx by carbon monoxide for flue gas cleaning process: a review 烟气净化过程中一氧化碳选择性催化还原NOx的研究进展
Pub Date : 2020-04-19 DOI: 10.1080/01614940.2020.1753972
Z. Gholami, Guohua Luo, F. Gholami, Fan Yang
ABSTRACT It is crucial to control NOx emission into the atmosphere because it can make several harmful health and environmental effects. Many techniques are available for NOx reduction, and among them, selective catalytic reduction (SCR) is one of the most efficient techniques for NOx removal in flue gas cleaning process. The reduction of NOx by CO offers a simple and low-cost technology for reducing NOx emissions from mobile or stationary sources. In this review, NOx emission, different NOx control technologies, and the challenges for the SCR process are studied. This paper reviews various types of catalysts, including supported and unsupported metal oxide catalysts as efficient catalysts for NOx reduction by CO. The reported experimental researches are analyzed to make an overview of the NOx reduction through CO-SCR process. Moreover, catalytic performances in the presence of oxygen, water steam, and sulfur dioxide, which usually exist in exhaust gases produced in the combustion process, are discussed. Moreover, this paper reviews the possible reaction mechanisms for the CO–SCR.
摘要氮氧化物排放对人体健康和环境具有多种危害,控制氮氧化物排放至关重要。NOx的还原技术有很多,其中选择性催化还原(selective catalytic reduction, SCR)是烟气净化过程中最有效的NOx脱除技术之一。一氧化碳减少氮氧化物为减少移动或固定源的氮氧化物排放提供了一种简单而低成本的技术。本文对SCR工艺的NOx排放、不同的NOx控制技术以及面临的挑战进行了研究。本文综述了各种类型的催化剂,包括负载型和非负载型金属氧化物催化剂作为CO还原NOx的有效催化剂,并对已有的实验研究进行了分析,概述了CO- scr工艺还原NOx的研究概况。此外,讨论了在氧气、水蒸气和二氧化硫存在下的催化性能,这些通常存在于燃烧过程中产生的废气中。此外,本文还对CO-SCR可能的反应机理进行了综述。
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引用次数: 50
Catalytic partial oxidation of methane to syngas: review of perovskite catalysts and membrane reactors 甲烷部分氧化制合成气:钙钛矿催化剂和膜反应器的研究进展
Pub Date : 2020-04-16 DOI: 10.1080/01614940.2020.1743420
A. H. Elbadawi, L. Ge, Zhiheng Li, Shaomin Liu, Shaobin Wang, Zhonghua Zhu
ABSTRACT Partial oxidation of methane (POM) offers a promising option to produce syngas for downstream processes such as hydrogen production and Fischer-Tropsch processes. POM in fixed-bed reactors requires an oxygen separation plant with high operation cost and safety risks. On the contrary, membrane reactors can provide an improved process by integrating both oxygen separation and catalytic reaction processes. With many advantages including high purity and efficient oxygen separation from the air at the catalytic reaction conditions, mixed ionic-electronic conducting membranes (MIEC) caught great attention in the scientific research field over the past two decades. In this review, POM using different catalysts in fixed-bed reactors was firstly summarized with emphasizing on perovskite-based catalysts, and then the material screening of MIEC membrane reactors was introduced and linked to the selection of conventional and perovskite catalysts. The catalytic activity, reaction mechanisms, and emerging challenges have been analyzed. Furthermore, future research directions have been outlined by highlighting the effect of electronic properties, continuous reduction-oxidation in the presence of oxygen flux, and chemical reaction mechanism on membrane/catalyst.
甲烷部分氧化(POM)为制氢和费托工艺等下游工艺生产合成气提供了一个很有前途的选择。固定床反应器的POM需要氧气分离装置,运行成本高,存在安全风险。相反,膜反应器可以通过整合氧分离和催化反应过程来提供改进的过程。混合离子-电子导电膜(MIEC)具有高纯度和在催化反应条件下能有效地从空气中分离氧气等优点,在过去的二十年里受到了科学研究领域的广泛关注。本文首先对固定床反应器中不同催化剂的POM进行了综述,重点介绍了钙钛矿基催化剂,然后介绍了MIEC膜反应器的材料筛选,并将其与常规催化剂和钙钛矿催化剂的选择联系起来。分析了催化活性、反应机理和新出现的挑战。强调了膜/催化剂的电子性质、氧通量下的连续还原氧化、化学反应机理等对膜/催化剂的影响,并展望了未来的研究方向。
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引用次数: 58
Solid catalysts for conversion of furfural and its derivatives to alkanediols 糠醛及其衍生物转化为烷二醇的固体催化剂
Pub Date : 2020-04-13 DOI: 10.1080/01614940.2020.1744327
Nagasuresh Enjamuri, Srinivas Darbha
ABSTRACT Alkanediols with five and six carbon atoms (1,2- & 1,5-pentanediols and 1,2- & 1,6-hexanediols, respectively) are an important class of industrial chemicals having wide application. Their production from lignocellulosic biomass-derived furfural and its derivatives using solid catalysts is a sustainable and attractive approach. Several bifunctional catalysts with metal (for hydrogenation/hydrogenolysis) and acid/base (for ring opening) functionalities have been reported. Effective and selective conversion of furfurals to a desired diol is still a challenge. This review discusses the recent advances in catalyst development for pentane- and hexanediols. The reaction pathways, active sites, and possible reaction mechanisms over the solid catalysts are discussed. A comparative catalytic activity data of the known catalysts are reported.
具有5个碳原子和6个碳原子的链二醇(分别为1,2-和1,5-戊二醇和1,2-和1,6-己二醇)是一类重要的工业化学品,具有广泛的应用。利用固体催化剂从木质纤维素生物质衍生的糠醛及其衍生物中生产糠醛是一种可持续的、有吸引力的方法。已经报道了几种具有金属(用于加氢/氢解)和酸/碱(用于开环)功能的双功能催化剂。有效和选择性地将糠醛转化为所需的二醇仍然是一个挑战。综述了近年来戊烷和己二醇催化剂的研究进展。讨论了固体催化剂的反应途径、活性位点和可能的反应机理。报道了已知催化剂的催化活性比较数据。
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引用次数: 10
Magnetic core–shell nanocatalysts: promising versatile catalysts for organic and photocatalytic reactions 磁性核壳纳米催化剂:用于有机和光催化反应的有前途的多功能催化剂
Pub Date : 2020-04-02 DOI: 10.1080/01614940.2019.1659555
Malayil Gopalan Sibi, D. Verma, Jaehoon Kim
ABSTRACT During the past decades, there have been enormous developments in catalysis in the form of great innovations such as precise structure characterization, surface functionalization, and effective utilization of active sites. In both academic and industrial sectors, the development of efficient nanosized catalysts has received considerable attention because it can improve the efficiency of the catalytic process and the selectivity of products, which can minimize the overall production cost and the amount of chemical wastes generated by improving the atomic efficiency. However, bulk-scale synthesis and utilization of nanocatalysts are hindered by the high synthetic cost, tedious synthesis procedure, and difficulty in the separation and recovery of the catalysts after the reactions. In this context, superparamagnetic nanoparticles have attracted much attention as a catalyst and as a support owing to their robust structure, low cost, environmental benignity, and easy separation under an external magnetic response. In this review, we focused on organic catalysis and photocatalysis using magnetically retrievable core–shell nanocatalysts with various functionalities. This review presents a comprehensive overview of the synthesis of magnetic core–shell nanocatalysts with suitable functionalities for catalysis, recent developments in organic and photocatalytic reactions using core–shell catalysts, and challenges to be addressed as part of future research activities. The first part summarizes the various synthetic methods of magnetic nanocores, and the second part overviews the detailed functionalization methods for the growth of shells on the surface of the magnetic nanocores, along with the merits and challenges to-date. In the last section, the efficiency, recoverability, and reusability of magnetic core–shell nanocatalysts are reviewed for a variety of organic and photocatalytic reactions.
在过去的几十年里,催化技术有了巨大的发展,比如精确的结构表征、表面功能化和活性位点的有效利用。无论是学术界还是工业界,高效纳米催化剂的开发都受到了相当大的关注,因为它可以提高催化过程的效率和产物的选择性,从而通过提高原子效率使整体生产成本和化学废物的产生量最小化。然而,纳米催化剂的大规模合成和利用受到合成成本高、合成过程繁琐、反应后催化剂分离和回收困难等问题的阻碍。在此背景下,超顺磁性纳米颗粒由于其结构坚固、成本低、环境友好、在外部磁响应下易于分离等优点,作为催化剂和载体受到了广泛的关注。本文主要介绍了磁性可回收核壳纳米催化剂在有机催化和光催化方面的应用。本文综述了具有合适催化功能的磁性核壳纳米催化剂的合成,核壳催化剂在有机和光催化反应中的最新进展,以及未来研究活动中需要解决的挑战。第一部分总结了磁性纳米核的各种合成方法,第二部分概述了磁性纳米核表面生长壳的详细功能化方法,以及迄今为止的优点和挑战。在最后一节,磁性核壳纳米催化剂的效率,可恢复性和可重复使用的各种有机和光催化反应进行了综述。
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引用次数: 24
Recent synthesis of functionalized s-tetrazines and their application in ligation reactions under physiological conditions: a concise overview 近年来功能化s-四嗪的合成及其在生理条件下结扎反应中的应用综述
Pub Date : 2020-02-15 DOI: 10.1080/01614940.2020.1726009
Li Wang, Jingwen Zhang, Jizhong Zhao, Ping Yu, Shenglin Wang, Hongmei Hu, Rui Wang
ABSTRACT Inverse electron demand Diels–Alder reactions have gained comprehensive attraction in recent years. Accordingly, the synthetic approaches for one of the coupling partners, namely s-tetrazine, have been extensively investigated. Generally, the main synthetic method of s-tetrazine relied on the condensation of two nitriles to give the corresponding symmetric/asymmetric tetrazines with moderate to excellent yields. However, the practical synthesis route and commercial/synthetic availability of the feedstock nitriles are still elusive. It is therefore probably worth summarizing the existing methods and typical biological applications that have been demonstrated in recent years. In brief, this overview will be split into three parts. First, we will summarize the typical approaches toward the synthesis of s-tetrazines till now. Then, we will provide the representative bio-orthogonal reactions by the combination of s-tetrazines with unsaturated compounds under physiological conditions. Eventually, we will propose a direction for the practical and efficient synthesis of s-tetrazine.
逆电子需求Diels-Alder反应近年来受到了广泛的关注。因此,对其中一个偶联伙伴s-四氮的合成方法进行了广泛的研究。一般来说,s-四嗪的主要合成方法是通过两个腈的缩合得到相应的对称/不对称四嗪,收率中等至优异。然而,实际的合成路线和原料腈的商业/合成可用性仍然难以捉摸。因此,可能有必要总结一下近年来已经证明的现有方法和典型的生物学应用。简而言之,本文将分为三个部分。首先,我们将总结目前合成s-四嗪的典型方法。然后,我们将在生理条件下提供具有代表性的s-四嗪与不饱和化合物结合的生物正交反应。最后,为实用高效的合成s-四氮指明了方向。
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引用次数: 6
Catalytic glycerol dehydration-oxidation to acrylic acid 催化甘油脱水氧化制丙烯酸
Pub Date : 2020-02-13 DOI: 10.1080/01614940.2020.1719611
Shuangyan Wu, Qingyan She, R. Tesser, M. Serio, C. Zhou
ABSTRACT This article provides a comprehensive and critical review of the latest studies on catalytic glycerol dehydration-oxidation to acrylic acid. The two-bed catalytic system in one or two reactors involves glycerol dehydration to acrolein and subsequent oxidation of acrolein to acrylic acid. Zeolites, metal oxides, heteropoly acids, and phosphates are effective in the dehydration of glycerol to acrolein. Mo–V–O catalysts appear active in the acrolein oxidation to acrylic acid. The glycerol can be completely converted to acrolein with 98% selectivity. In such a two-step process, the step of catalytic dehydration is thought to be critical. A few recent studies reveal that the conversion of glycerol to acrylic acid in two reactors can be also achieved via allyl alcohol as intermediate. For the one-bed catalytic glycerol oxydehydration to acrylic acid, a single catalyst must possess both active acid sites and active redox sites. Mo–V–O, W–V–O, Mo–V–W–O, W–V–Nb–O oxide catalysts, and heteropoly acid catalysts are particularly promising. Currently, a 60% yield of acrylic acid can be achieved over H0.1Cs2.5(VO)0.2(PMo12O40)0.25(PW12O40)0.75 at 340°C. However, all the catalysts rapidly deactivate due to coking. Coking usually occurs during the glycerol oxydehydration step. Optimizing reaction conditions such as increasing water and oxygen feeding, lowering reaction temperature, tuning the catalysts by finely doping, adjusting the surface acidity and enlarging pores of the solid catalysts can inhibit coking to some extent by slowing the deactivation of catalyst. Yet coking over catalysts is a major obstacle when conducting glycerol oxydehydration on a large scale. We suggest that future work should place an emphasis on revealing the essence of coking, further designing coking-resisting catalysts, and developing an efficient reaction and separation system.
本文综述了甘油催化脱水氧化制丙烯酸的最新研究进展。在一个或两个反应器中的两床催化系统涉及甘油脱水制丙烯醛和随后的丙烯醛氧化制丙烯酸。沸石、金属氧化物、杂多酸和磷酸盐在将甘油脱水成丙烯醛方面是有效的。Mo-V-O催化剂在丙烯醛氧化制丙烯酸过程中表现出活性。甘油可以完全转化为丙烯醛,选择性为98%。在这两步过程中,催化脱水的步骤被认为是至关重要的。最近的一些研究表明,在两个反应器中,也可以通过烯丙醇作为中间体将甘油转化为丙烯酸。对于单床催化甘油氧脱水制丙烯酸,单一催化剂必须同时具有活性酸位和活性氧化还原位。Mo-V-O、W-V-O、Mo-V-W-O、W-V-Nb-O氧化物催化剂和杂多酸催化剂尤其有发展前景。目前,在340°C下,在H0.1Cs2.5(VO)0.2(PMo12O40)0.25(PW12O40)0.75条件下,丙烯酸的收率可达到60%。然而,所有的催化剂都因焦化而迅速失活。焦化通常发生在甘油氧化脱水阶段。优化反应条件,如增加加水加氧、降低反应温度、通过细掺杂调整催化剂、调节表面酸度、扩大固体催化剂的孔隙等,可以减缓催化剂的失活,从而在一定程度上抑制焦化。然而,催化剂上的焦化是进行大规模甘油氧脱水的主要障碍。今后的工作重点是揭示焦化的本质,进一步设计抗焦化催化剂,开发高效的反应分离体系。
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引用次数: 17
Recent advances on TiO2-based photocatalysts toward the degradation of pesticides and major organic pollutants from water bodies 二氧化钛基光催化剂降解水体中农药和主要有机污染物的研究进展
Pub Date : 2020-01-02 DOI: 10.1080/01614940.2019.1613323
S. Kanan, Matthew A. Moyet, Robert B. Arthur, H. Patterson
ABSTRACT Pesticides and organic waste constitute a group of environmental pollutants that are widely distributed in our environment due to various human activities. Adsorptive removal and photocatalytic degradation of these pollutants from water have emerged as energy and cost-effective technologies. However, advanced oxidation technologies are gaining attention as an effective method for wastewater treatment capable of degrading a diverse spectrum of organic contaminants. Photocatalysis is a promising advanced oxidation technology to alleviate water pollution problems. Titanium dioxide (TiO2) is the most popular photocatalyst due to its low cost, nontoxicity, high oxidizing abilities, and easy immobilization on various surfaces. The current review aims to highlight recent advancements in photocatalytic degradation of pesticides and major organic pollutants using TiO2-based photocatalysts. Indeed, most of the methods, which employed potent catalysts, showed and exhibited successful degradation of the pesticides under various conditions. We believe this topic of research is extremely vital and will continue to grow in recent years, reaching ultimate desirable results and find more applications in different fields of study.
农药和有机废弃物构成了一组环境污染物,由于人类的各种活动而广泛分布在我们的环境中。从水中吸附去除和光催化降解这些污染物已成为能源和成本效益高的技术。然而,作为一种能够降解多种有机污染物的有效废水处理方法,先进的氧化技术正受到人们的关注。光催化是一种很有前途的高级氧化技术,可以缓解水污染问题。二氧化钛(TiO2)因其成本低、无毒、氧化能力强、易于固定在各种表面上而成为最受欢迎的光催化剂。本文综述了二氧化钛基光催化剂在光催化降解农药和主要有机污染物方面的最新进展。事实上,大多数使用强效催化剂的方法都显示并展示了在各种条件下农药的成功降解。我们相信这一课题的研究是非常重要的,并将在近年来继续发展,达到最终理想的结果,并在不同的研究领域找到更多的应用。
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引用次数: 153
Ag-catalyzed azide-alkyne cycloaddition: copper free approaches for synthesis of 1,4-disubstituted 1,2,3-triazoles 银催化叠氮化物-炔环加成:无铜合成1,4-二取代1,2,3-三唑的方法
Pub Date : 2020-01-02 DOI: 10.1080/01614940.2019.1673443
Jasmin Sultana, D. Sarma
ABSTRACT This review mainly focuses on purely Ag-catalyzed 1,3-dipolar azide-alkyne cycloaddition (AgAAC) so called click reaction to synthesize 1,4-regioisomers of 1,2,3-triazoles. The most established catalyst Cu (I) developed by Fokin–Sharpless and Meldal group in 2002 for AAC reaction have been further extended to different other transition metal catalysts because of certain limitations of CuAAC methods. Among different transition metal catalyzed methods, AgAAC is the most studied one having same electronic configuration, d10 (AgI) with that of CuI and shows high catalytic performance.
摘要本文主要综述了纯银催化的1,3-偶极叠氮-炔环加成反应(AgAAC)合成1,2,3-三唑的1,4-区域异构体。2002年由Fokin-Sharpless和Meldal小组开发的用于AAC反应的最成熟的催化剂Cu (I),由于CuAAC方法的某些局限性,进一步扩展到其他不同的过渡金属催化剂。在不同的过渡金属催化方法中,AgAAC是研究最多的一种,其电子构型与CuI相同,d10 (AgI),具有较高的催化性能。
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引用次数: 22
Recent advances in decarboxylative C-C bond formation using direct or in situ generated alkenyl acids 使用直接或原位生成的烯基酸脱羧C-C键的最新进展
Pub Date : 2020-01-02 DOI: 10.1080/01614940.2019.1700736
P. Kaur, Vinod Kumar, Rakesh Kumar
ABSTRACT In recent years, the reactions of abundantly available, inexpensive, and structurally diverse alkenyl acids (-C=C-COOH) with C-X (X = halogen) or C-H coupling partner have emerged as vital strategies for the streamlined synthesis of functionalized alkenes with extrusion of innocuous CO2. Various alkenyl acids such as cinnamic acids can act as stable surrogates for the polymerization prone styrenes/olefins, which otherwise need special attention for their handling and storage. Furthermore, cinnamic acids can be easily prepared through various methodologies including Knoevenagel-Doebner (KD) condensation, Heck coupling reaction, etc. Recently, various one-pot tandem methodologies involving the decarboxylative coupling of KD/Heck sequence with C-H or C-X substrate have come into fore. The present review article edifies about the recent advances, scope and limitations for C-C bond formation via (i) direct decarboxylative functionalization of C-X or C-H substrate with alkenyl acids, (ii) tandem one-pot multicomponent decarboxylative approaches (involving in situ generated alkenyl acids) e.g. coupling of KD/Heck sequences with C-X or C-H substrate. Graphical abstract
近年来,大量可用、廉价且结构多样的烯基酸(c =C-COOH)与C-X (X =卤素)或C-H偶联伙伴的反应已成为挤压无害CO2流线型合成功能化烯烃的重要策略。各种烯基酸如肉桂酸可以作为易于聚合的苯乙烯/烯烃的稳定替代品,否则需要特别注意它们的处理和储存。此外,肉桂酸可以通过Knoevenagel-Doebner (KD)缩合、Heck偶联反应等多种方法制备。最近,涉及KD/Heck序列与C-H或C-X底物脱羧偶联的各种单锅串联方法已经出现。本文综述了C-C键形成方法的最新进展、范围和局限性:(1)C-X或C-H底物与烯基酸直接脱羧功能化;(2)串联一锅多组分脱羧方法(涉及原位生成的烯基酸),例如KD/Heck序列与C-X或C-H底物的偶联。图形抽象
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引用次数: 12
期刊
Catalysis Reviews
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