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Solvent-free synthesis of hierarchical Tb3+-doped Yttrium benzene-1,3,5-tricarboxylate metal organic framework nanosheets for fast and highly sensitive fluorescence detection of Fe3+ and Cr2O72− ions 无溶剂合成分级Tb3+掺杂钇苯-1,3,5-三羧酸盐金属有机骨架纳米片,用于快速高灵敏度荧光检测Fe3+和Cr2O72−离子
Pub Date : 2022-06-01 DOI: 10.1016/j.recm.2022.06.001
Ji Zhang , Jiaqiang Liu , Xianliang Li , Yan Xu

Controllable synthesis of luminescent metal-organic frameworks (MOFs) having the merits of ease preparation, outstanding sensitivity and stability is of great significance for exploring their efficient sensing applications. Herein, we report a hierarchical terbium-doped yttrium-benzene-1,3,5-tricarboxylate MOF nanosheet via solvent-free synthetic strategy with a topological structure of MIL-78. The fluorescence property of the hierarchical Tb3+-doped Y-based MOF nanosheets can be tuned by adjusting the molar ratio of Tb3+ to Y3+ ions, and the Tb0.5Y0.5-MOF nanosheet-like morphology with the optimum characteristic Tb3+ ion green emission exhibited great potential acting as fluorescence probe for highly sensitive Fe3+ and Cr2O72− detection. The Tb3+-doped Y-MOF nanosheets show a fast response time of less than 1 s for Fe3+ ions. They also have low detection limits of 0.40 and 0.26 µM toward Fe3+ and Cr2O72− ions, respectively, as well as excellent stability. This work paves the way to explore intriguing hierarchical MOF-based luminescent materials for efficient fluorescence sensing applications.

可控合成具有制备简单、灵敏度高、稳定性好的发光金属有机骨架(mof)对于探索其高效传感应用具有重要意义。本文采用无溶剂合成策略,制备了一种结构为MIL-78的分层掺铽钇-苯-1,3,5-三羧酸盐MOF纳米片。通过调整Tb3+与Y3+离子的摩尔比,可以调节Tb3+掺杂的MOF纳米片的荧光特性,具有Tb3+离子绿色发射的最佳特征的Tb0.5Y0.5-MOF纳米片具有作为高灵敏度Fe3+和Cr2O72−检测的荧光探针的巨大潜力。掺Tb3+的Y-MOF纳米片对Fe3+离子的响应时间小于1 s。它们对Fe3+和Cr2O72−离子的检出限分别为0.40µM和0.26µM,具有良好的稳定性。这项工作为探索有趣的基于mof的分层发光材料的高效荧光传感应用铺平了道路。
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引用次数: 0
Application of nanomaterials in waterborne coatings: A review 纳米材料在水性涂料中的应用综述
Pub Date : 2022-06-01 DOI: 10.1016/j.recm.2022.06.004
Hongrui Yao , Lijuan Li , Wanshen Li , Duo Qi , Wanlu Fu , Na Wang

Combining nanomaterials and waterborne resins is an effective way to obtain high-performance waterborne coatings. This paper provides a comprehensive overview on waterborne nanocomposite coatings based on the latest research progress at home and abroad. Specifically, the characteristics of zero-dimensional (0D), one-dimensional (1D), two-dimensional (2D) and binary hybrid (0D/1D, 0D/2D, 1D/2D, 2D/2D) nanomaterials and their applications in waterborne coatings are coherently reviewed. Subsequently, various modification methods of nanomaterials, especially noncovalent modification and covalent modification, are analyzed in detail. Additionally, the enhancement mechanisms of nanomaterials enhancing the corrosion resistance of waterborne nanocomposite coatings are also discussed, including physical barrier mechanism and electrochemical mechanism. Finally, based on the above discussion, the outlooks for the future design of waterborne nanocomposite coating are presented.

纳米材料与水性树脂相结合是获得高性能水性涂料的有效途径。本文根据国内外纳米复合涂料的最新研究进展,对水性纳米复合涂料进行了综述。具体地,综述了零维(0D)、一维(1D)、二维(2D)和二元杂化(0D/1D、0D/2D、1D/2D、2D/2D)纳米材料的特性及其在水性涂料中的应用。随后,详细分析了纳米材料的各种改性方法,特别是非共价改性和共价改性。此外,还讨论了纳米材料增强水性纳米复合涂层耐腐蚀性能的机理,包括物理屏障机理和电化学机理。最后,在此基础上,对未来水性纳米复合涂层的设计进行了展望。
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引用次数: 3
Zeolite-based cracking catalysts for bio-oil upgrading: A critical review 生物油升级用沸石基裂化催化剂研究进展
Pub Date : 2022-06-01 DOI: 10.1016/j.recm.2022.03.002
Nichaboon Chaihad , Surachai Karnjanakom , Abuliti Abudula , Guoqing Guan

Fast pyrolysis of biomass is an attractive way to produce bio-oil since it can convert most of biomass components directly into liquid fuel. However, the bio-oils obtained from such a fast pyrolysis process always have highly complex oxygenated compounds with high viscosity, serious corrosivity, and rather instability. Thus, before the raw bio-oils are used as fuel or chemical feedstock, they must be upgraded, especially deoxygenated. Cracking of bio-oils over porous solid catalysts such as zeolite-based catalysts at ambient pressure is considered one of effective ways for the bio-oil upgrading, especially in which hydrogen gas is not necessary. Herein, zeolite-based catalysts (mainly HZSM-5 based catalysts) for the upgrading of pyrolysis bio-oils are critically reviewed. The effects of porous structure, acidity and other parameters including biomass type, biomass/catalyst ratio and operation temperature on cracking activity, selectivity, stability and deactivation are summarized. While, the proposed mechanisms on the bio-oil upgrading over the zeolite-based catalysts and the possibility for the application of the developed catalysts in the industrial process are discussed. Furthermore, the main strategies including metal modification, construction of zeolites with a hierarchical structure and synthesis of special morphologies with hollow structure or core/shell structure and nanosheet structures for the improvement of deoxygenation property performance are introduced. It is expected to provide a guidance for the design and fabricate more excellent zeolite-based catalysts and their application for high-quality bio-oil production from fast biomass pyrolysis.

生物质快速热解是一种有吸引力的生产生物油的方法,因为它可以将大部分生物质成分直接转化为液体燃料。然而,通过这种快速热解过程得到的生物油往往含有高度复杂的含氧化合物,粘度高,腐蚀性严重,而且不稳定。因此,在原料生物油用作燃料或化学原料之前,必须对其进行升级,特别是脱氧。常压下多孔固体催化剂(如沸石基催化剂)裂解生物油被认为是生物油升级的有效途径之一,特别是在不需要氢气的情况下。本文对沸石基催化剂(主要是HZSM-5基催化剂)在热解生物油提质中的应用进行了综述。综述了多孔结构、酸度、生物质类型、生物质/催化剂比、操作温度等参数对裂化活性、选择性、稳定性和失活的影响。同时,对沸石基催化剂对生物油的提质机理及在工业上应用的可能性进行了讨论。此外,还介绍了金属改性、层叠结构分子筛的构建、中空结构、核壳结构和纳米片结构等特殊形貌的合成等提高分子筛脱氧性能的主要策略。期望为设计和制备更优的沸石基催化剂及其在生物质快速热解制取高品质生物油中的应用提供指导。
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引用次数: 17
Outside Back Cover 外封底
Pub Date : 2022-06-01 DOI: 10.1016/S2772-4433(22)00035-6
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引用次数: 0
Investigation into the hydrodynamics of liquid-solid inclined micro-fluidized beds 液固倾斜微流化床流体力学研究
Pub Date : 2022-03-01 DOI: 10.1016/j.recm.2021.12.001
Yi Zhang , Nina Ullah , Richard Law , David Reay , Vladimir Zivkovic

The inclined micro-fluidized bed (MFB) can enhance heat and mass transfer rates compared to the vertically aligned counterparts, but the increased significance of surface forces and wall effects may cause poor fluidization performance. In this paper, the effects of column inclination and different particle-to-bed ratios (dP/dB) on the solid hydrodynamics are investigated in an inclined micro-fluidized bed. The results validated the suitability of using the Ergun equation to predict minimum fluidization velocities due to small deviations between 1.01 and 1.81 times the theoretical values, for a particle-to-bed ratio ranging from 0.025 to 0.165 at inclinations between 0° and 10°. Investigation into the effects on bed expansion behavior showed that the bed contracted with an increase in bed inclination. An unexpected observation during the bed expansion was the appearance of a secondary high voidage region and the appearance of strong circulation patterns with an increase in bed inclination. A detailed analysis of this phenomenon suggested the presence of a critical angle at 6° and 10° for the 85 µm particles, 4 × 4 mm bed cross-section and 165 µm particles, 1 × 1 mm bed cross-section, respectively. However, the liquid-solid back-mixing was observed due to the modified particle trajectories resulted in the disappearance of the high voidage region. This paper gives new insights into the micro-fluidization behavior in inclined beds thus contributing to the development of micro-fluidized beds and their future applications.

与垂直排列的微流化床相比,倾斜的微流化床可以提高传热传质率,但表面力和壁面效应的增加可能导致流化性能较差。在倾斜微流化床中,研究了柱倾角和不同颗粒床比(dP/dB)对固体流体力学的影响。结果验证了用Ergun方程预测最小流化速度的适用性,因为在倾角为0°和10°时,颗粒床比在0.025到0.165之间,最小流化速度的偏差是理论值的1.01到1.81倍。对床层膨胀行为影响的研究表明,床层随床层倾角的增大而收缩。在床层膨胀过程中,出现了一个意想不到的现象,即随着床层倾角的增加,出现了一个二次高电压区和强环流模式。对这一现象的详细分析表明,85µm颗粒(4 × 4 mm床层截面)和165µm颗粒(1 × 1 mm床层截面)分别在6°和10°处存在临界角。然而,由于粒子轨迹的改变,导致高电压区消失,导致了液固回混。本文对倾斜床的微流化行为有了新的认识,有助于微流化床的发展及其未来的应用。
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引用次数: 2
Discrete particle methods for engineering simulation: Reproducing mesoscale structures in multiphase systems 工程模拟的离散粒子方法:多相系统中尺度结构的再现
Pub Date : 2022-03-01 DOI: 10.1016/j.recm.2022.01.002
Ji Xu , Peng Zhao , Yong Zhang , Junwu Wang , Wei Ge

Most natural resources are processed as particle-fluid multiphase systems in chemical, mineral and material industries, therefore, discrete particles methods (DPM) are reasonable choices of simulation method for engineering the relevant processes and equipments. However, direct application of these methods is challenged by the complex multiscale behavior of such systems, which leads to enormous computational cost or otherwise qualitatively inaccurate description of the mesoscale structures. The coarse-grained DPM based on the energy-minimization multi-scale (EMMS) model, or EMMS-DPM, was proposed to reduce the computational cost by several orders while maintaining an accurate description of the mesoscale structures, which paves the way for its engineering applications. Further empowered by the high-efficiency multi-scale DEM software DEMms and the corresponding customized heterogeneous supercomputing facilities with graphics processing units (GPUs), it may even approach realtime simulation of industrial reactors. This short review will introduce the principle of DPM, in particular, EMMS-DPM, and the recent developments in modeling, numerical implementation and application of large-scale DPM which aims to reach industrial scale on one hand and resolves mesoscale structures critical to reaction-transport coupling on the other hand. This review finally prospects on the future developments of DPM in this direction.

在化工、矿产和材料工业中,大多数自然资源都是作为颗粒-流体多相系统进行处理的,因此离散颗粒法(DPM)是工程化相关过程和设备仿真方法的合理选择。然而,这些方法的直接应用受到这些系统复杂的多尺度行为的挑战,这导致了巨大的计算成本或其他质量上不准确的中尺度结构描述。提出了基于能量最小化多尺度(EMMS)模型的粗粒度DPM (EMMS -DPM),在保持对中尺度结构的准确描述的同时,将计算成本降低了几个数量级,为其工程应用奠定了基础。在高效的多尺度DEM软件DEMms和相应的定制异构超级计算设施(图形处理单元(gpu))的支持下,它甚至可以接近工业反应堆的实时仿真。本文将简要介绍DPM的原理,特别是EMMS-DPM,以及大规模DPM的建模、数值实现和应用方面的最新进展。大规模DPM一方面旨在达到工业规模,另一方面旨在解决对反应-输运耦合至关重要的中尺度结构。最后对DPM在这一方向上的发展进行了展望。
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引用次数: 8
Development of catalysts for direct non-oxidative methane aromatization 甲烷直接非氧化芳构化催化剂的研制
Pub Date : 2022-03-01 DOI: 10.1016/j.recm.2022.01.004
Yuji Ogawa , Yuebing Xu , Zhanguo Zhang , Hongtao Ma , Yo Yamamoto

Direct catalytic conversion of methane to benzene at non-oxidative condition is considered as one of key reactions for constitution of sustainable carbon-cycling processes, since either biomethane or CO2-based synthetic methane can serve as its feed source. While this concern may motivate many researchers over the world to make their continuous effort to gain deep insight into the catalytic mechanism of this catalysis system and the essential cause of the catalyst deactivation, successful development of a catalyst with high performance, enhanced coking resistance and long-term operating stability will be the key to its industrial application. Here in this review paper, we demonstrate the high catalytic activity and stability of our two shaped Mo/HZSM-5 catalysts developed respectively for fixed-bed and fluidized-bed operations at severe reaction conditions. Thermodynamically, a possibly high aromatization temperature is required to attain a desired high benzene formation rate, but adopting such a temperature will certainly accelerate coke formation and catalyst deactivation. Therefore, the focus of the catalyst development was laid on finding various effective ways of suppressing coke accumulation and catalyst deactivation at practically required severe reaction conditions, and much effort was made to attain the purpose. As a result, a highly active and selective pelleted Mo/HZSM-5 catalyst has been successfully developed and was stably run in a fixed-bed reactor under cyclic regeneration operation mode over 1000 h. In parallel a binder-free, fluidizable Mo/HZSM-5 catalyst with certain mechanical strength has also been developed and successfully tested in a dual circulating fluidized-bed reactor system to provide a stable benzene yield of about 12% at 1073 K and 3000 ml/g/h space velocity.

甲烷在非氧化条件下直接催化转化为苯被认为是构成可持续碳循环过程的关键反应之一,因为生物甲烷或co2基合成甲烷都可以作为其原料来源。这一问题可能会促使世界各地的许多研究人员不断努力,深入了解该催化体系的催化机理和催化剂失活的根本原因,而成功开发一种高性能、抗结焦性能增强、长期运行稳定的催化剂将是其工业应用的关键。在这篇综述中,我们展示了我们分别为固定床和流化床操作开发的两种定型Mo/HZSM-5催化剂在恶劣反应条件下的高催化活性和稳定性。从热力学上讲,要达到期望的高苯生成速率,可能需要较高的芳构化温度,但采用这样的温度肯定会加速焦炭的生成和催化剂的失活。因此,催化剂开发的重点是寻找各种有效的方法来抑制实际需要的苛刻反应条件下的积炭和催化剂的失活,并为此付出了很大的努力。成功研制了一种高活性、选择性球团化Mo/HZSM-5催化剂,并在固定床反应器中循环再生运行模式下稳定运行了1000 h以上。同时,研制了一种无粘合剂、具有一定机械强度的可流化Mo/HZSM-5催化剂,并成功在双循环流化床反应器系统中进行了测试,在1073 K、3000 ml/g/h空速下,苯收率稳定在12%左右。
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引用次数: 3
Recent advance on cobalt-based oxide catalyst for the catalytic removal of volatile organic compounds: A review 钴基氧化物催化剂催化脱除挥发性有机物的研究进展
Pub Date : 2022-03-01 DOI: 10.1016/j.recm.2021.12.003
Xi Chen , Shinong Yu , Wei Liu , Shuning Zhang , Shuchen Liu , Yang Feng , Xuejun Zhang

As the main contributor to air pollution, lots of volatile organic compounds (VOCs) were emitted into the atmosphere due to the rapid urbanization and industrialization, threatening environmental safety and human health. Catalytic oxidation has been verified as an efficient approach for VOCs elimination from industrial waste gas streams. Owing to the merits of cost-effective and high activity, cobalt-based catalysts have been considered as one of the most promising candidates for VOCs degradation. This review systematically summarized the developments achieved in the design of cobalt-based catalysts for VOCs removal over the past decade. Specifically, the fabrication of single cobalt oxides, cobalt-based binary oxides and cobalt-based composites, as well as the modified cobalt-based oxides by the surface engineering strategies, such as doping technology and acid etching method are coherently reviewed. Subsequently, the corresponding kinetic models and mechanisms are also discussed. Finally, considering the enormous challenges and opportunities in this field, the perspective with respect to future research on cobalt-based catalysts is proposed.

随着城市化和工业化进程的加快,大量挥发性有机化合物(VOCs)被排放到大气中,威胁着环境安全和人类健康。催化氧化是消除工业废气中挥发性有机化合物的一种有效方法。钴基催化剂由于具有高性价比和高活性的优点,已被认为是降解挥发性有机化合物最有前途的候选材料之一。本文系统地总结了近十年来钴基催化剂在去除VOCs方面的研究进展。具体地,综述了单钴氧化物、钴基二元氧化物和钴基复合材料的制备,以及采用掺杂技术和酸蚀法等表面工程策略对钴基氧化物进行改性的研究进展。随后,讨论了相应的动力学模型和机理。最后,考虑到该领域面临的巨大挑战和机遇,对钴基催化剂的未来研究提出了展望。
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引用次数: 9
Novel Green resource material: Eucommia Ulmoides Gum 新型绿色资源材料:杜仲胶
Pub Date : 2022-03-01 DOI: 10.1016/j.recm.2022.01.005
Donghan Li , Chen Yang , Yiqi Huang , Long Li , Wenchi Han , Hailan Kang , Feng Yang , Qinghong Fang

Eucommia ulmoides gum (EUG), main composition is trans-1,4-polyisoprene, is a natural polymer extracted from Eucommia ulmoides plant tissue. Benefiting from the crystallization ability and rubber-plastic duality, it can be applied to a variety of fields, including aerospace, national defense, healthcare, transportation, sports, and construction. Herein, we summarized recent progress in EUG research concerning efficient extraction methods, crystallization characteristics and novel functional EUG materials focused on the relationship between its molecular structure, crystallization behavior, phase structure, and properties. Furthermore, the research and development directions of EUG for the development of its new materials have been outlined.

杜仲胶(EUG)主要成分为反式-1,4-聚异戊二烯,是从杜仲植物组织中提取的天然聚合物。得益于其结晶能力和橡塑双重性,可应用于航空航天、国防、医疗、交通、体育、建筑等领域。本文综述了近年来EUG在高效提取方法、结晶特性和新型功能EUG材料等方面的研究进展,重点介绍了EUG的分子结构、结晶行为、相结构和性能之间的关系。展望了EUG新材料开发的研究和发展方向。
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引用次数: 8
Advances in low-temperature extraction of natural resources using liquefied dimethyl ether 液化二甲醚低温提取自然资源的研究进展
Pub Date : 2022-03-01 DOI: 10.1016/j.recm.2022.01.001
Qingxin Zheng , Masaru Watanabe

This review summarized the valuable works on the extraction technologies using pure liquefied dimethyl ether (DME) as the organic solvent. DME is a colorless gas with a slight ether-like fragrance at room temperature and pressure. Due to some special properties, such as the strong ability for extracting organic compounds and water, high extraction rate, cheap price, low extraction temperature, and energy consumption, environmental friendliness, safety, and good compressibility, the application of liquefied DME to the extraction process shows many advantages and has strong potential market competitiveness. On the other hand, the drawbacks of liquefied DME extraction technology were also revealed, mainly on fire hazards, solvent loss, and lack of large-scale application. Furthermore, the previous studies on the application of liquefied DME extraction technology were divided into three parts based on the extracts (water, lipid/oil, and specific ingredients) and listed one by one. The research of the liquefied DME extraction process is still in development. In the future, it is expected that this technology can be continuously improved and optimized in both lab and industrial scales, together with the extension of its application range to more various natural resources.

本文综述了以纯液化二甲醚(DME)为有机溶剂的提取技术的研究进展。二甲醚是一种无色气体,在室温和常压下有轻微的醚香味。由于液化二甲醚提取有机物和水的能力强、提取率高、价格便宜、提取温度低以及能耗、环保、安全、可压缩性好等特殊性能,将其应用于提取工艺中显示出诸多优势,具有较强的潜在市场竞争力。另一方面,也揭示了液化二甲醚提取技术的缺点,主要是存在火灾隐患、溶剂损失、缺乏大规模应用等问题。此外,前人对液化二甲醚提取技术应用的研究,根据提取物(水、脂/油、特定成分)分为三部分,逐一列举。液化二甲醚提取工艺的研究仍在进行中。未来,该技术有望在实验室和工业规模上不断得到改进和优化,并将其应用范围扩展到更多的自然资源中。
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引用次数: 0
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