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Iridium Nanodisks Intercalated Between Graphite Layers: Iridium Loading and Metal Particle Size 嵌入石墨层之间的铱纳米片:铱负载和金属粒度
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-09-20 DOI: 10.1007/s10563-022-09369-5
Masayuki Shirai, Sakura Kudo, Tomoki Sobu, Mika Sodeno, Shusuke Kato, Etty N. Kusumawati, Hidetaka Nanao

Iridium nanoparticles were synthesized between graphite layers by thermal treatment of the mixture of iridium chloride (IV) and graphite powder under chlorine atmosphere followed by hydrogen reduction (Ir-GIC). In Ir-GIC samples with 1–6 wt% iridium metal loadings, all iridium nanoparticles with disk-shape (iridium nanodisks) were located between graphite layers; however, iridium nanoparticles on graphite surface were also formed in addition to iridium nanodisks in the Ir-GIC samples with 8 and 10 wt% iridium metal loadings. Iridium nanodisks between graphite layers were highly active for cinnamaldehyde hydrogenation and selective to cinnamyl alcohol compared with the iridium particles on graphite surfaces.

Graphical Abstract

Iridium nanoparticles with disk-shape structure were synthesized between graphite layers by thermal treatment of the mixture of iridium chloride and graphite under chlorine pressure followed by hydrogen reduction.

将氯化铱(IV)与石墨粉混合在氯气气氛下进行热处理,再进行氢还原(Ir-GIC),在石墨层间合成了铱纳米颗粒。在1-6 wt%铱金属负载的Ir-GIC样品中,所有具有圆盘状的铱纳米颗粒(铱纳米盘)都位于石墨层之间;然而,在含有8 wt%和10 wt%铱金属的Ir-GIC样品中,除了铱纳米盘外,石墨表面还形成了铱纳米颗粒。与石墨表面的铱颗粒相比,石墨层间的铱纳米片对肉桂醛的加氢活性和对肉桂醇的选择性均较高。摘要将氯化铱和石墨的混合物在氯压下进行热处理,再进行氢还原,在石墨层间合成了具有圆盘状结构的纳米铱。
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引用次数: 1
Rice Husk Ash Derived SiO2 for Template Free Synthesis of H-ZSM-5 Support for Ni Catalyst: Investigation on Non-Oxidative CH4 Cracking for Clean H2 Production 稻壳灰衍生SiO2无模板合成H-ZSM-5 Ni催化剂载体:清洁制氢非氧化CH4裂解研究
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-09-13 DOI: 10.1007/s10563-022-09365-9
Manasa Kandula, Naresh Gutta, Hari Padmasri Aytam, Vijayanand Perupogu, Kalpana Manda, Venugopal Akula

H-ZSM-5(RH) was synthesized using rice husk without an organic reagent and explored it as a support for Ni in the catalytic cracking of methane (CCM). Detailed investigations of the fresh and used catalysts analysed by using XRD, SEM, TEM, H2-TPR, DT/TGA and CO pulse chemisorption techniques revealed that the high CCM activity was due to enhanced Ni dispersion and increased Cu-Ni interactions. Among the Ni/H-ZSM-5(RH) and bimetallic (Ni-M/H-ZSM-5(RH) M = Zn, Co, Fe, Cu) catalysts, the Cu-Ni/H-ZSM-5(RH) demonstrated a hydrogen yield of ~ 275 Nm3/molNi which was explained by a high degree of graphitization confirmed by Raman spectroscopic analysis.

以稻壳为原料合成了H-ZSM-5(RH),并探讨了其作为Ni在甲烷(CCM)催化裂化中的载体作用。利用XRD、SEM、TEM、H2-TPR、DT/TGA和CO脉冲化学吸附技术对新催化剂和旧催化剂进行了详细的研究,结果表明,高CCM活性是由于Ni分散增强和Cu-Ni相互作用增强所致。在Ni/H-ZSM-5(RH)和双金属(Ni-M/H-ZSM-5(RH) M = Zn, Co, Fe, Cu)催化剂中,Cu-Ni/H-ZSM-5(RH)催化剂的产氢率为~ 275 Nm3/molNi,这与拉曼光谱分析证实的高石墨化程度有关。
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引用次数: 0
Recent Advances in Catalytic Conversion of C5/C6 Alkanes to Olefins: A Review C5/C6烷烃催化转化烯烃的研究进展
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-09-12 DOI: 10.1007/s10563-022-09367-7
Xin Wang, Youhao Xu

Light naphtha (C5–C6 alkanes) is commonly used as a feedstock for steam cracking or catalytic cracking to produce ethylene and propylene. This paper summarizes the progress of C5/C6 alkanes steam cracking and catalytic cracking, but the key problem of the above method is the high yield of low-value C1–C3 alkanes. When C5/C6 olefin is used as the feedstock of catalytic cracking, the ethylene and propylene yields are high, while the C1–C3 alkanes yield is low. It is of scientific value to dehydrogenate the C5/C6 alkanes into the corresponding olefins, and effectively convert the olefins into ethylene and propylene. This paper reviews recent progress of direct catalytic dehydrogenation and oxidative dehydrogenation of C5/C6 alkanes, and points out that the key is to develop C5/C6 alkanes dehydrogenation catalyst for selective preparation of corresponding mono-olefins. The main issues about how to develop highly selective C5/C6 alkanes dehydrogenation catalysts are proposed.

轻石脑油(C5-C6烷烃)通常用作蒸汽裂化或催化裂化生产乙烯和丙烯的原料。综述了C5/C6烷烃蒸汽裂化和催化裂化的研究进展,指出上述方法的关键问题是低价值C1-C3烷烃的高产率。以C5/C6烯烃为原料催化裂化时,乙烯和丙烯收率高,C1-C3烷烃收率低。将C5/C6烷烃脱氢为相应的烯烃,并将烯烃有效地转化为乙烯和丙烯,具有一定的科学价值。综述了近年来C5/C6烷烃直接催化脱氢和氧化脱氢的研究进展,指出开发C5/C6烷烃选择性脱氢催化剂是制备相应单烯烃的关键。提出了开发高选择性C5/C6烷烃脱氢催化剂的主要问题。
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引用次数: 0
Synthesis, Spectroscopic and Catalytic Properties of FeOx/Al2O3 Nanopowders Prepared by CO2 Laser Vaporization CO2激光汽化法制备FeOx/Al2O3纳米粉体的合成、光谱及催化性能
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-08-25 DOI: 10.1007/s10563-022-09366-8
Mark G. Baronskiy, Anton I. Kostyukov, Aleksey V. Zhuzhgov, Nadezhda A. Zaitseva, Svetlana V. Cherepanova, Tatyana V. Larina, Valeriy N. Snytnikov

Nanostructured powders xFe/nano-Al2O3 with the Fe loading of x = 0.0 – 5.0 wt% were obtained using laser vaporization by CO2 laser. XRF, XRD, HRTEM, PL and UV–Vis DRS techniques were employed to investigate physicochemical, structural and optical properties of the synthesized nanopowders with the average particle size of 9 nm. Nanopowders xFe/nano-Al2O3 as model catalysts were tested in isobutane dehydrogenation reaction. The results obtained were compared with similar data for the xFe/γPb-Al2O3 systems synthesized by the conventional sol–gel method. According to XRD and UV–Vis DRS data, in the series of xFe/nano-Al2O3 samples a great part of Fe3+ ions is in the disordered environment of subsurface layers of Al2O3 nanocrystallites, predominantly in the tetrahedral coordination. In distinction to samples of the xFe/γPb-Al2O3 series, in the case of nanostructured xFe/nano-Al2O3 powders the formation of Fe2O3 phase does not occur at any concentrations of iron or conditions of testing. The analysis of the PL spectra of xFe/nano-Al2O3 powders also showed the presence of surface sites of Fe3+ ions, which were not detected for xFe/γPb-Al2O3. Catalytic testing of the xFe/nano-Al2O3 series samples in isobutane dehydrogenation revealed the formation of the iron active sites that ensure catalytic activity of the samples. Differences in the catalytic properties of FeOx/Al2O3 samples obtained by the sol–gel method and laser vaporization are related to different states of Fe3+ ions. Thus, the xFe/nano-Al2O3 nanopowders, in contrast to xFe/γPb-Al2O3, contain a large amount of active Fe3+ sites. These sites, being involved in the dehydrogenation reaction, are present predominantly on the surface of the nanopowders.

采用CO2激光汽化法制备了铁含量为x = 0.0 ~ 5.0 wt%的xFe/nano-Al2O3纳米粉体。采用XRF、XRD、HRTEM、PL和UV-Vis DRS等技术对合成的平均粒径为9 nm的纳米粉体进行了理化、结构和光学性能表征。采用纳米粉末xFe/纳米al2o3作为模型催化剂,对异丁烷脱氢反应进行了实验研究。所得结果与常规溶胶-凝胶法制备的xFe/γPb-Al2O3体系的相似数据进行了比较。XRD和UV-Vis DRS数据表明,在xFe/nano-Al2O3系列样品中,大部分Fe3+离子处于Al2O3纳米晶亚表面层的无序环境中,以四面体配位为主。与xFe/γPb-Al2O3系列样品不同,在纳米结构xFe/纳米al2o3粉末的情况下,在任何铁浓度或测试条件下都不会形成Fe2O3相。对xFe/γ - pb - al2o3粉末的PL光谱分析表明,xFe/γ - pb - al2o3粉末表面存在Fe3+离子,而xFe/γ - pb - al2o3粉末表面没有Fe3+离子。对xFe/纳米al2o3系列样品在异丁烷脱氢过程中的催化测试表明,铁活性位点的形成保证了样品的催化活性。溶胶-凝胶法和激光汽化法制备的FeOx/Al2O3样品的催化性能差异与Fe3+离子的不同状态有关。因此,与xFe/γPb-Al2O3相比,xFe/nano-Al2O3纳米粉末含有大量的活性Fe3+位点。这些参与脱氢反应的位点主要存在于纳米粉体的表面。
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引用次数: 1
Towards Extraordinary Catalysts for Aromatization of Biomass and Low-Cost C5 Streams 面向生物质芳构化和低成本C5流的特殊催化剂
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-07-20 DOI: 10.1007/s10563-022-09364-w
Ahmad Galadima, Ahmad Masudi, Oki Muraza

The production of aromatics with fuel properties from either biomass resources or low-cost refinery streams such as C5 is an important industrial interest. However, the strategic design of reliable catalysts with commercial compatibilities remained a challenge. Several investigations were carried out in this direction. This review accordingly presents a comprehensive analysis of the literature on the catalysis-based strategies adopted for aromatization of the feeds. Valorization of furans and allied oxygenates derived from biomass into aromatics was initially covered. The review examined strategies for C5 streams aromatization, co-upgrading of furans with hydrocarbons and methanol and discussed how biomass-derived bio-oils could be valorized into aromatics. In addition to discussion on the influence of catalytic textural, acidity and topological properties, the paper provided substantial updates on the associated reaction mechanisms. A perspective for further investigations in aromatization was also provided.

从生物质资源或低成本的炼油流(如C5)中生产具有燃料特性的芳烃是一个重要的工业兴趣。然而,具有商业相容性的可靠催化剂的战略设计仍然是一个挑战。在这方面进行了几项调查。这篇综述相应地提出了一个综合分析的文献上的催化为基础的策略采用的芳香化饲料。最初涵盖了从生物质中提取的呋喃和相关含氧化合物转化为芳烃的增值。综述了C5流芳构化、呋喃与烃类和甲醇共升级的策略,并讨论了生物质衍生生物油如何转化为芳烃。除了讨论了催化结构、酸度和拓扑性质的影响外,本文还对相关的反应机理进行了大量的更新。并对芳构化的进一步研究提出了展望。
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引用次数: 3
Effect of Shell Thickness on the Properties of Multi-Pd Cores-Hollow Carbon Shell Catalyst mPd@HCS 壳层厚度对多钯芯-空心碳壳催化剂性能的影响mPd@HCS
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-07-04 DOI: 10.1007/s10563-022-09362-y
Feifei Hu, Chengbing Fu, Chenchen Zhao, Peng Liu, Wei Tian, Bo Chen, Hongyan Pan, Qian Lin

Traditional catalysts with one core and one shell structure have few active sites and shell structure parameters are difficult to be regulated. In order to solve these two problems, it is presented herein a multi-Pd-core and porous carbon shell catalyst mPd@HCS, where multiple Pd nuclei provide more active sites for the reaction, the shell structure parameters are tuned by the adjustment of shell thickness, and the influence of shell thickness on the performance of H2O2 direct synthesis was mainly investigated. The results showed that the selectivity and yield of H2O2 changed volcanically with the increase of carbon crust thickness because of the compromise between reactants diffusion and product degradation, and the selectivity (87%) and productivity (1938 mmol gPd−1 h−1) of the sample with middle shell thickness (10.18 nm) were the highest.

传统的一核一壳结构催化剂活性位点少,壳结构参数难以调控。为了解决这两个问题,本文提出了一种多钯核多孔碳壳催化剂mPd@HCS,其中多钯核为反应提供了更多的活性位点,通过调整壳层厚度来调整壳层结构参数,并主要研究了壳层厚度对H2O2直接合成性能的影响。结果表明,H2O2的选择性和产率随碳壳厚度的增加呈火山状变化,这是由于反应物扩散和产物降解之间的折衷,其中,中壳厚度(10.18 nm)样品的选择性(87%)和产率(1938 mmol gPd−1 h−1)最高。
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引用次数: 0
Review: Graphite Phase Carbon Nitride Photo-Fenton Catalyst and its Photocatalytic Degradation Performance for Organic Wastewater 综述:石墨相氮化碳光fenton催化剂及其对有机废水的光催化降解性能
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-06-20 DOI: 10.1007/s10563-022-09363-x
Jingpeng Luo, Xu Du, Qingying Ye, Dong Fu

The catalytic properties and applications of Fenton and Fenton-like catalysts based on graphitic carbon nitride (g-C3N4) are reviewed. Compared with semiconductor photocatalytic, the synergistic system of photocatalysis and Fenton-like oxidation has a stronger ability to degrade organic wastewater, but there are still some shortcomings, such as high recombination rate of photogenerated carriers and serious agglomeration of metals on the catalyst surface, and its catalytic performance still needs to be further improved. The development of heterogeneous photo-Fenton-like catalysts based on g-C3N4 and their Fenton-like mechanism will be the focus of future research.

综述了氮化石墨碳(g-C3N4)基Fenton及类Fenton催化剂的催化性能及应用。与半导体光催化相比,光催化与类芬顿氧化协同体系对有机废水的降解能力更强,但仍存在光生载体复合率高、金属在催化剂表面团聚严重等缺点,其催化性能有待进一步提高。基于g-C3N4的非均相光fenton类催化剂的开发及其fenton类机理将是未来研究的重点。
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引用次数: 3
Wild Olive Oil as a Novel and Sustainable Feedstock for Biodiesel Production: Overviewed Various Feedstock, Methodologies and Reaction Mechanisms of Different Catalysts 野生橄榄油作为生物柴油生产的新型可持续原料:各种原料、方法和不同催化剂的反应机理综述
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-06-03 DOI: 10.1007/s10563-022-09361-z
Ihtisham Wali Khan, Abdul Naeem, Muhammad Farooq, Tahira Mahmood, Tooba Saeed, Fouzia Parveen, Tabassum Malik

The over-consumption of petroleum fuel due to the progressive increase in population, transportation, industrialization, modernization as well as improvement in the lifestyle of the society leads to the fast declining of non-renewable resources. Therefore, it is important to discover low cost, environmentally friendly and sustainable surrogates of petroleum fuels. In this regard, biodiesel production is one of the gorgeous solutions for the research community. Contrary to the benefits, the high cost of the biodiesel is the main disadvantage, greatly reliant on the feedstock. In this sense, wild olive oil was explored for the first time as a suitable and novel feedstock for biodiesel technology development. The fatty acid composition was identified by GC–MS analysis whereas various physiochemical properties were determined by ASTM and EN methods. Furthermore, this review paper conveys a detailed overview of biodiesel production technologies, various generation feedstocks and types of catalyst along with their plausible mechanism.

由于人口、交通、工业化、现代化以及社会生活方式的不断提高,石油燃料的过度消耗导致了不可再生资源的快速减少。因此,寻找低成本、环保、可持续的石油燃料替代品具有重要意义。在这方面,生物柴油生产是研究界的华丽解决方案之一。与优点相反,生物柴油的主要缺点是成本高,严重依赖原料。从这个意义上说,野生橄榄油首次被探索为一种适合生物柴油技术发展的新型原料。脂肪酸组成采用气相色谱-质谱法鉴定,理化性质采用ASTM和EN法测定。此外,本文还详细介绍了生物柴油的生产技术、各种生产原料和催化剂类型及其可能的机理。
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引用次数: 0
Catalytic Oxidation of Ethyl Lactate to Ethyl Pyruvate over Au-Based Catalyst Using Authentic Air as Oxidant 真实空气作氧化剂在金基催化剂上催化氧化乳酸乙酯制丙酮酸乙酯
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-05-21 DOI: 10.1007/s10563-022-09359-7
Shiyao Lu, Jian Zhang, Zhiyi Wu, Zerui Su, Jianbin Huang, Yehao Liang, Feng-Shou Xiao

Highly dispersed Au nanoparticles supported on Ni–Al mixed metal oxides (Au/NiAl-MMO) were prepared by a facile method, which is significantly efficient for the aerobic oxidation of ethyl lactate using authentic air as the oxidant, achieving 72.6% ethyl lactate conversion and 88.3% selectivity to ethyl pyruvate at 240 °C in a continuous fixed-bed reactor. The catalyst retained its catalytic performance during a long-term stability test. Characterization and experimental studies on the kinetic dependence sequence of the reactants and elementary reaction steps confirmed that the Au/NiAl-MMO catalyst followed the Mars–van Krevelen mechanism, with the activation of O2 as the elementary step. The quasi in situ X-ray photoelectron spectroscopy spectra demonstrated that the active sites in the Au/NiAl-MMO catalyst were Au nanoparticles. This work may provide a novel technique for developing more efficient supported metal catalysts for the aerobic oxidation of ethyl lactate using authentic air as the oxidant.

Graphical abstract

Highly dispersed Au nanoparticle catalyst was facilely prepared for the efficient catalytic oxidation of ethyl lactate with authentic air.

采用简便方法制备了负载在Ni-Al混合金属氧化物(Au/NiAl-MMO)上的高度分散的Au纳米颗粒,该纳米颗粒在真实空气为氧化剂的条件下对乳酸乙酯的好氧氧化效果显著,在240℃的连续固定床反应器中乳酸乙酯转化率为72.6%,丙酮酸乙酯选择性为88.3%。该催化剂在长期稳定性试验中保持了其催化性能。对反应物和基本反应步骤的动力学依赖顺序进行表征和实验研究,证实Au/NiAl-MMO催化剂遵循Mars-van Krevelen机理,以O2活化为基本反应步骤。准原位x射线光电子能谱分析表明,Au/NiAl-MMO催化剂的活性位点为Au纳米粒子。本研究为开发以真实空气为氧化剂的负载型金属催化剂制备乳酸乙酯的好氧反应提供了一种新技术。摘要制备了分散的金纳米颗粒催化剂,用于乳酸乙酯在真实空气中的高效催化氧化。
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引用次数: 0
2-Pyridyl-benzimidazole-Pd(II)/Pd(0) Supported on Magnetic Mesoporous Silica: Aerobic Oxidation of Benzyl Alcohols/Benzaldehydes and Reduction of Nitroarenes 磁性介孔二氧化硅负载的2-吡啶-苯并咪唑-Pd(II)/Pd(0):苯甲醇/苯甲醛的好氧氧化和硝基芳烃的还原
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-05-10 DOI: 10.1007/s10563-022-09360-0
Mohammad Sajedi, Yagoub Mansoori, Ayat Nuri, Somayeh Fekri, Dolores Esquivel, Mª Angeles Navarro

2-(2-Pyridyl)benzimidazole (PyBzIm) was supported onto magnetic mesoporous silica, Fe3O4@SiO2@SBA-15 via the click chemistry. The supported ligand was treated with Na2PdCl4 in methanol to afford Fe3O4@SiO2@SBA-PyBzIm-Pd(II) as a magnetically retrievable supported catalyst. The catalyst was fully characterized by conventional methods. X-ray photoelectron spectroscopy (XPS) studies confirmed some C = N nitrogen atoms interact with palladium in the + 2 oxidation state. The prepared catalyst was found to catalyze the aerobic oxidation of benzyl alcohols and benzaldehydes to the corresponding benzoic acids, and excellent conversions were obtained. The magnetic catalyst showed a very low metal leaching (3.9%) in the first run. Fe3O4@SiO2@SBA-PyBzIm-Pd(II) was then treated with aqueous NaBH4 to give Fe3O4@SBA-PyBzIm-Pd(0). The obtained catalyst was found to catalyze the transfer hydrogenation of nitroarenes to the corresponding anilines in the presence of hydrazine, and excellent yields were obtained. The prepared catalysts present an excellent recycling efficiency over seven consecutive runs without significant loss of catalyst reactivity.

Graphical abstract

通过点击化学将2-(2-吡啶基)苯并咪唑(PyBzIm)负载在磁性介孔二氧化硅Fe3O4@SiO2@SBA-15上。负载配体用Na2PdCl4在甲醇中处理,得到Fe3O4@SiO2@ sba - pybzem - pd (II)作为磁性可回收负载催化剂。用常规方法对催化剂进行了表征。x射线光电子能谱(XPS)研究证实了一些C = N的氮原子与钯以+ 2氧化态相互作用。所制备的催化剂能催化苯甲醇和苯甲醛的好氧氧化生成苯甲酸,并取得了良好的转化率。在第一次运行中,磁性催化剂的金属浸出率很低(3.9%)。Fe3O4@SiO2@SBA-PyBzIm-Pd(II)用NaBH4水溶液处理得到Fe3O4@SBA-PyBzIm-Pd(0)。结果表明,该催化剂能在肼存在下催化硝基芳烃的转移加氢反应生成相应的苯胺,收率较高。制备的催化剂在连续七次运行中表现出优异的回收效率,而催化剂的反应性没有明显损失。图形抽象
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引用次数: 4
期刊
Catalysis Surveys from Asia
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