Reactor

反应堆
  • 文章类型: Journal Article
    尽管使用H2O作为氢源(2N26H2O=4NH33O2)将环境N2还原为氨(NH3)被认为是Haber-Bosch工艺的有希望的替代方法,N=N键的高键能导致极低的NH3产率。在这里,我们报告了一种高效的氨合成催化系统,使用低温介质阻挡放电等离子体将惰性N2分子激活为活化的氮物种,它可以有效地与多孔金属有机框架(MOF)反应器中的受限和浓缩的H2O分子反应,Cr3+,Mn3+,Fe3+,Co2+,Ni2+和Cu2+离子。特别是,Fe基催化剂MIL-100(Fe)导致22.4mmolg-1h-1的超高NH3产率。在等离子体驱动的催化反应过程中,对MIL-100(Fe)的催化性能和系统表征的研究表明,原位生成的有缺陷的Fe-O团簇是高活性位点,并且在MIL-100(Fe)反应器内确实形成了NH3分子。理论计算表明,多孔MOF催化剂在不同的催化金属位点上对氮物种具有不同的吸附能力,其中最佳的MIL-100(Fe)对于限速*NNH形成步骤具有最低的能垒,显著提高固氮效率。
    While the ambient N2 reduction to ammonia (NH3) using H2O as hydrogen source (2N2+6H2O=4NH3+3O2) is known as a promising alternative to the Haber-Bosch process, the high bond energy of N≡N bond leads to the extremely low NH3 yield. Herein, we report a highly efficient catalytic system for ammonia synthesis using the low-temperature dielectric barrier discharge plasma to activate inert N2 molecules into the activated nitrogen species, which can efficiently react with the confined and concentrated H2O molecules in porous metal-organic framework (MOF) reactors with V3+, Cr3+, Mn3+, Fe3+, Co2+, Ni2+ and Cu2+ ions. Specially, the Fe-based catalyst MIL-100(Fe) causes a superhigh NH3 yield of 22.4 mmol g-1 h-1. The investigation of catalytic performance and systematic characterizations of MIL-100(Fe) during the plasma-driven catalytic reaction unveils that the in situ generated defective Fe-O clusters are the highly active sites and NH3 molecules indeed form inside the MIL-100(Fe) reactor. The theoretical calculation reveals that the porous MOF catalysts have different adsorption capacity for nitrogen species on different catalytic metal sites, where the optimal MIL-100(Fe) has the lowest energy barrier for the rate-limiting *NNH formation step, significantly enhancing efficiency of nitrogen fixation.
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  • 文章类型: Journal Article
    这篇综述针对空气污染控制领域的研究人员,旨在了解挥发性有机化合物(VOC)去除的最新进展。实施等离子体催化技术以去除挥发性有机化合物(VOC)导致降解产率和矿化速率显着提高,副产物形成少。等离子体-催化组合可以以两种不同的方式使用:(I)催化剂位于等离子体放电的下游,被称为“后等离子体催化配置”(PPC),和(II)催化剂位于等离子体区并直接暴露于放电,称为“在等离子体催化配置中”(IPC)。将这两种技术结合起来,尤其是对VOCs的消除近年来引起了许多研究者的兴趣。术语“协同作用”在他们的作品中被广泛报道,并与等离子体催化组合的积极作用有关。这篇综述论文研究了新发表的关于催化的论文的最新水平,光催化,非热等离子体,以及它们的组合用于VOC去除应用。重点是了解在等离子体和催化之间相互作用的不同协同源,并将其分为两个主要部分:等离子体放电对催化剂的影响和催化剂对等离子体放电的影响。这种方法具有应用于工业过程或室内环境的空气净化系统的潜力。
    This review is aimed at researchers in air pollution control seeking to understand the latest advancements in volatile organic compound (VOC) removal. Implementing of plasma-catalysis technology for the removal of volatile organic compounds (VOCs) led to a significant boost in terms of degradation yield and mineralization rate with low by-product formation. The plasma-catalysis combination can be used in two distinct ways: (I) the catalyst is positioned downstream of the plasma discharge, known as the \"post plasma catalysis configuration\" (PPC), and (II) the catalyst is located in the plasma zone and exposed directly to the discharge, called \"in plasma catalysis configuration\" (IPC). Coupling these two technologies, especially for VOCs elimination has attracted the interest of many researchers in recent years. The term \"synergy\" is widely reported in their works and associated with the positive effect of the plasma catalysis combination. This review paper investigates the state of the art of newly published papers about catalysis, photocatalysis, non-thermal plasma, and their combination for VOC removal application. The focus is on understanding different synergy sources operating mutually between plasma and catalysis discussed and classified into two main parts: the effect of the plasma discharge on the catalyst and the effect of the catalyst on plasma discharge. This approach has the potential for application in air purification systems for industrial processes or indoor environments.
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  • 文章类型: Journal Article
    有机城市固体废物的综合治理由于其对环境的直接和间接影响而备受关注。厌氧消化(AD)已被认为是废物处理的替代和环保技术,将它们转化为有机肥料和可再生能源。这项研究提出了一项实验,涉及四个装有家庭有机废物的反应器,三个用犬科动物接种,山羊,和兔子粪便,还有一个没有接种疫苗。连续30天观察实验以分析家用反应器中AD过程中涉及的pH和温度参数。统计方法,包括单向方差分析,以评估接种物类型的影响,Tukey对平均差异的同时置信区间,以及温度和粪便中μ的90%置信区间,被利用。此外,对影响平均温度和pH值的主要因素进行了分析。单因素实验结果表明,接种物的种类对pH的变化没有显著影响,而温度在整个AD过程中保持相对稳定。然而,对主要效应的分析表明,羊粪趋于稳定温度,变化最小,而在其他实验中,变异更为异质。
    The comprehensive management of organic urban solid waste is a concern due to its direct and indirect impact on the environment. Anaerobic Digestion (AD) has been recognized as an alternative and environmentally friendly technology for waste disposal, converting them into organic fertilizers and renewable energy. This research presents an experiment involving four reactors fed with household organic waste, three inoculated with canine, goat, and rabbit manure, and one without inoculum. The experiment was observed for 30 consecutive days to analyze the pH and temperature parameters involved in the AD process in domestic reactors. Statistical methodology, including one-way analysis of variance for assessing the effect of the type of inoculum, Tukey\'s simultaneous confidence intervals for mean differences, and 90 % confidence intervals for μ in temperature and manure, was utilized. Additionally, main effects analysis of the factors of average temperature and pH were conducted. The results of the one-factor experiment show that the type of inoculum does not significantly influence the variation in pH, while temperature remains relatively stable throughout the AD process. However, the analysis of main effects indicates that goat manure tends to stabilize the temperature with minimal variation, whereas variation is more heterogeneous in the other experiments.
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  • 文章类型: Journal Article
    在温和条件下通过光催化有效地将甲烷转化为有价值的化学品代表了能量储存和增值制造的可持续途径。尽管对这一领域有持续的兴趣,由于缺乏进行光催化甲烷氧化实验以及评估相应性能的标准化协议,这些成就被掩盖了。在这次审查中,我们提出了一个旨在应对这些挑战的结构化解决方案。首先,我们介绍了反应器设计的基本规范,并概述了气-固和气-固-液反应系统中的各种配置。该讨论有助于选择适合甲烷转化实验的反应器。随后,我们提供了一个全面的一步一步的协议适用于不同的甲烷转化反应。强调对产品的细致验证和准确量化,该方案强调了减少污染源和选择适当检测方法的重要性.最后,我们提出了对评估光催化甲烷转化率至关重要的标准化性能指标。通过定义这些指标,社区可以在评估不同研究的表现方面达成共识。往前走,光催化甲烷转化的未来需要进一步完善严格的实验标准和评价标准。此外,可扩展反应器的开发对于促进从实验室概念验证到潜在工业生产的过渡至关重要。
    Efficiently converting methane into valuable chemicals via photocatalysis under mild condition represents a sustainable route to energy storage and value-added manufacture. Despite continued interest in this area, the achievements have been overshadowed by the absence of standardized protocols for conducting photocatalytic methane oxidation experiments as well as evaluating the corresponding performance. In this review, we present a structured solution aimed at addressing these challenges. Firstly, we introduce the norms underlying reactor design and outline various configurations in the gas-solid and gas-solid-liquid reaction systems. This discussion helps choosing the suitable reactors for methane conversion experiments. Subsequently, we offer a comprehensive step-by-step protocol applicable to diverse methane-conversion reactions. Emphasizing meticulous verification and accurate quantification of the products, this protocol highlights the significance of mitigating contamination sources and selecting appropriate detection methods. Lastly, we propose the standardized performance metrics crucial for evaluating photocatalytic methane conversion. By defining these metrics, the community could obtain the consensus of assessing the performance across different studies. Moving forward, the future of photocatalytic methane conversion necessitates further refinement of stringent experimental standards and evaluation criteria. Moreover, development of scalable reactor is essential to facilitate the transition from laboratory proof-of-concept to potentially industrial production.
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  • 文章类型: Journal Article
    用于小型农业农场的现场厌氧消化器通常具有根据农场操作而波动的饲喂时间表。在喂养的冲击,特别是易腐烂的废物会破坏消化器的稳定运行。在四个3L反应器中以半连续模式在38°C下运行350天,水力停留时间为25天,有机负荷率(OLR)为1gVS/L/d,研究了间歇进料对废弃树莓厌氧消化的影响。在适应期(147天)期间,有机负载为每周5次饲料。然后改变两个反应器的进料方案,同时保持相同的OLR和HRT在一个反应器中每周进料一次,在另一个反应器中每周进料3次。尽管甲烷产量的每周模式差异很大,但进料方式并未显着影响特定的甲烷产量(平均369±47L/kgVS)。挥发性脂肪酸(VFA)占废水中有机物的83%以上,其余包括酚类化合物的非抑制性浓度(515-556mg没食子酸/L)。所有反应器中的微生物组成和主要群体的相对丰度是古细菌甲烷菌和甲醇菌属以及细菌门细菌和Firmicutes。在第238天将OLR提高到2gVS/L/d导致所有反应堆失效,归因于碱度不足以抵消产生的VFA,pH降低到6以下。总体结果表明,尽管喂食频率不同,但仍保持了覆盆子废物的最佳消化,但酸化可随OLR变化而发生。
    On-site anaerobic digesters for small agricultural farms typically have feeding schedules that fluctuate according to farm operations. Shocks in feeding, particularly for putrescible waste can disrupt the stable operation of a digester. The effect of intermittent feeding on the anaerobic digestion of rejected raspberries was investigated in four 3L reactors operated in semicontinuous mode for 350 days at 38 °C with a hydraulic retention time of 25 days and an organic loading rate (OLR) of 1gVS/L/d. During the acclimatisation period (147 days) the organic loading was 5 feeds per week. The feeding regime of two reactors was then changed while maintaining the same OLR and HRT to one weekly feed event in one reactor and 3 equal feeds per week in another. The feeding regime did not significantly affect specific methane yield (369 ± 47 L/kgVS on average) despite very different weekly patterns in methane production. Volatile fatty acids (VFA) comprised >83 % of the organics in the effluent, while the rest included non-inhibitory concentrations of phenolic compounds (515-556 mg gallic acid/L). The microbial composition and relative abundance of predominant groups in all reactors were the archaeal genera Methanobacterium and Methanolinea and the bacterial phyla Bacteridota and Firmicutes. Increasing the OLR to 2gVS/L/d on day 238 resulted in failure of all reactors, attributed to the insufficient alkalinity to counterbalance the VFA produced, and the pH decrease below 6. Overall results suggests that optimal digestion of raspberry waste is maintained despite variations in feeding frequency, but acidification can occur with OLR changes.
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  • 文章类型: Journal Article
    为了使用碳基固体酸催化剂进行纯结晶纤维素的水解,特别设计了具有搅拌装置的高效反应器。该催化剂包含带有SO3H的无定形碳基材料,-COOH和-OH基团。该搅拌装置具有七个涂覆有聚四氟乙烯的叶片,并且以60°偏移的规则间隔轴向布置。这个设计被证明是非常有效的,提供两倍的葡萄糖产量相比,传统的搅拌系统。本文对这种新型反应器的基本性能进行了研究和分析,并进行了讨论。
    A highly efficient reactor with a stirring device was specially designed with the intent of performing the hydrolysis of pure crystalline cellulose using a carbon-based solid acid catalyst. This catalyst comprised an amorphous carbon-based material bearing -SO3H, -COOH and -OH groups. The stirring apparatus had seven blades coated with polytetrafluoroethylene and arranged axially at regular intervals with a 60° offset. This design proved highly effective, providing double the glucose yield compared with conventional stirring systems. The basic properties of this novel reactor were investigated and analyzed and are discussed herein.
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  • 文章类型: Journal Article
    由于安全性和效率限制,用于生产活性药物成分(API)的反应性气态试剂的使用仍然是科学挑战。连续流动反应器的实施导致快速发展的气体处理技术,因为几个优点,如增加界面面积,改善质量和传热,无缝扩展。该技术能够实现用于生产药物化合物的更短和更原子经济的合成路线。在这里,我们提供了从2016年起在气体处理连续流技术的发展以及在原料药功能化中使用气体方面的文献综述。
    The use of reactive gaseous reagents for the production of active pharmaceutical ingredients (APIs) remains a scientific challenge due to safety and efficiency limitations. The implementation of continuous-flow reactors has resulted in rapid development of gas-handling technology because of several advantages such as increased interfacial area, improved mass- and heat transfer, and seamless scale-up. This technology enables shorter and more atom-economic synthesis routes for the production of pharmaceutical compounds. Herein, we provide an overview of literature from 2016 onwards in the development of gas-handling continuous-flow technology as well as the use of gases in functionalization of APIs.
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  • 文章类型: Journal Article
    脂肪酶介导的烯烃化学酶环氧化是一种绿色环保的替代工艺。然而,传统的有机-水两相反应体系引起的传质屏障和脂肪酶失活一直是研究者关注的焦点。为了克服这些问题,我们研究了反应温度和两种重要底物(H2O2和酰基供体)对环氧化反应和界面传质的影响。因此,我们确定了最佳反应条件:温度为30°C,30重量%H2O2作为氧源,和1M月桂酸作为氧载体。此外,通过模拟摇瓶反应的条件,我们设计了间歇式反应器,并添加了金属网,以有效地阻止高浓度过氧化氢与酶之间的直接接触。在这些最佳条件下,环氧化反应进行5h,产品收率最高达93.2%。此外,经过七个重复的实验,脂肪酶仍保持51.2%的相对活性。
    Chemoenzymatic epoxidation of olefin mediated by lipase is a green and environmentally friendly alternative process. However, the mass transfer barrier and lipase deactivation caused by the traditional organic-water biphasic reaction system have always been the focus of researchers\' attention. To overcome these issues, we investigated the effects of reaction temperature and two important substrates (H2O2 and acyl donor) on the epoxidation reaction and interfacial mass transfer. As a result, we determined the optimal reaction conditions: a temperature of 30 °C, 30 wt-% H2O2 as the oxygen source, and 1 M lauric acid as the oxygen carrier. Additionally, by simulating the conditions of shaking flask reactions, we designed a batch reactor and added a metal mesh to effectively block the direct contact between high-concentration hydrogen peroxide and the enzyme. Under these optimal conditions, the epoxidation reaction was carried out for 5 h, and the product yield reached a maximum of 93.2%. Furthermore, after seven repetitive experiments, the lipase still maintained a relative activity of 51.2%.
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  • 文章类型: Journal Article
    为了使用吸附工艺从合成气中纯化氢气,使用SAPO34吸附剂。由于这种吸附剂对二氧化碳的强烈吸附,不可能仅通过降低压力来回收吸附剂,并且有必要使用热操作进行回收。为此,变温吸附(TSA)工艺用于提高用于燃料电池的氢的纯度。为了研究最佳运行条件,研究了不同温度和不同压力的输入气体,以比较吸附过程的纯度和回收率。在11、22和33巴的压力下模拟TSA过程,并计算每个过程的回收率。根据获得的结果,在33巴的恢复值优于其他两个压力,但是由于操作和初始成本在高压下增加的事实;选择22巴压力来呈现剩余的结果。在这项工作中,还报告了材料的总量和摩尔比。还给出了产物和废物出口流中组分的平均纯度。因此,在温度升高阶段,产品出口流中氢气的平均摩尔分数为99.96%,99.94%,并且在用于温度降低的流中也是99.96%。
    To purify hydrogen gas from synthesis gas using a adsorption process, SAPO 34 adsorbent was used. Due to the strong adsorption of carbon dioxide in this adsorbent, it is not possible to recover the adsorbent by reducing the pressure alone, and it is necessary to use thermal operations for recovery. For this purpose, a temperature swing adsorption (TSA) process is used to increase the purity of hydrogen for use in fuel cells. To investigate the optimum operational conditions, various temperatures and different pressures of input gas were investigated to compare the purity and recovery of adsorption process. The TSA process was simulated for pressures of 11, 22 and 33 bars and the recovery percentage of each process was calculated. According to the results obtained, the recovery value at 33 bars is better than the other two pressures, but due to the fact that operational and initial costs increase at high pressures; 22 bar pressure was chosen to present the remaining results. In this work, the total amount of material and the molar rate are also reported. The average purity of the components in the product and waste outlet streams has also been presented. Accordingly, the average molar fraction of hydrogen in the product outlet stream is 99.96% in the temperature increase stage, 99.94% and in the stream used for temperature reduction is 99.96%.
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  • 文章类型: Journal Article
    为了促进Fe2+/Fe3+在共催化Fenton中的循环,增强外循环序批式填充床反应器(ECSPBR)中的传质,制备了钨硅酸(TA)修饰的超亲水性MoS2海绵(TMS),用于高效降解水溶液中的磺胺甲恶唑(SMX)抗生素。通过比较研究方法,系统研究了助催化剂亲水性对助催化Fenton的影响及ECSPBR的优越性。结果表明,超亲水性增加了Fe2+和Fe3+与TMS的接触,然后加速Fe2+/Fe3+循环。TMS共催化Fenton的最大Fe2/Fe3比(TMS/Fe2/H2O2)是疏水性MoS2海绵(CMS)共催化Fenton的1.7倍。在适宜条件下,SMX降解效率可达90%以上。TMS的结构在此过程中保持不变,Mo的最大溶解浓度低于0.06mg/L此外,TMS的催化活性可以通过简单的重新浸渍来恢复。反应器的外循环有利于提高传质性能和过程中Fe2+和H2O2的利用率。这项研究为制备可回收的亲水性助催化剂和开发用于有机废水处理的高效助催化Fenton反应器提供了新的见解。
    To promote the cycle of Fe2+/Fe3+ in co-catalytic Fenton and enhance mass transfer in an external circulation sequencing batch packed bed reactor (ECSPBR), super-hydrophilicity MoS2 sponge (TMS) modified by tungstosilicic acid (TA) was prepared for efficiently degrading sulfamethoxazole (SMX) antibiotics in aqueous solution. The influence of hydrophilicity of co-catalyst on co-catalytic Fenton and the advantages of ECSPBR were systematically studied through comparative research methods. The results showed that the super hydrophilicity increased the contact between Fe2+ and Fe3+ with TMS, then accelerated Fe2+/Fe3+ cycle. The max Fe2+/Fe3+ ratio of TMS co-catalytic Fenton (TMS/Fe2+/H2O2) was 1.7 times that of hydrophobic MoS2 sponge (CMS) co-catalytic Fenton. SMX degradation efficiency could reach over 90% under suitable conditions. The structure of TMS remained unchanged during the process, and the max dissolved concentration of Mo was lower than 0.06 mg/L. Additionally, the catalytic activity of TMS could be restored by a simple re-impregnation. The external circulation of the reactor was conducive to improving the mass transfer and the utilization rate of Fe2+ and H2O2 during the process. This study offered new insights to prepare a recyclable and hydrophilic co-catalyst and develop an efficient co-catalytic Fenton reactor for organic wastewater treatment.
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