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Effects of Hydroxy Groups in Anthraquinone Dyes on Photocatalytic Activity of Visible-light-sensitized Pt-TiO2 for Hydrogen Evolution 蒽醌染料中羟基对可见光敏化Pt-TiO2析氢光催化活性的影响
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-10-20 DOI: 10.1007/s10563-022-09370-y
Fumiaki Amano, Yasukazu Akaki, Akira Yamakata

Alizarin (1,2-dihydroxyanthraquinone) is a stable red photoredox sensitizer. We explored the effect of the hydroxy substituents of 9,10-anthraquinone (AQ) molecules on the photocatalytic hydrogen evolution over a dye-sensitized Pt-TiO2 system under visible-light irradiation. The 2-hydroxy group in AQ dyes was necessary to induce photocatalytic H2 evolution. By contrast, the 1-hydroxy group was the anchoring group to increase the adsorption amount of the dyes on the TiO2 surface. Using time-resolved infrared spectroscopy, we found that the 2-hydroxy group enhances the electron injection and suppresses the back electron transfer from TiO2 particles to the dye.

茜素(1,2-二羟基蒽醌)是一种稳定的红色光氧化还原敏化剂。研究了9,10-蒽醌(AQ)分子羟基取代基对可见光下染料敏化Pt-TiO2体系光催化析氢的影响。AQ染料中的2-羟基是诱导光催化析氢所必需的。1-羟基为锚定基团,增加染料在TiO2表面的吸附量。利用时间分辨红外光谱,我们发现2-羟基增强了电子注入,抑制了TiO2粒子向染料的反向电子转移。
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引用次数: 1
A Novel Dual Z-Scheme Visible Light Catalyst PCN/BiOCl/CdS with Oxygen Vacancies for Benzylamine Oxidative Coupling Reaction 具有氧空位的双Z-Scheme可见光催化剂PCN/BiOCl/CdS用于苯胺氧化偶联反应
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-10-07 DOI: 10.1007/s10563-022-09372-w
Li Qin, Yefeng Chen, Zhuhan Wang, Huicai Zheng, Wen Li, Guichuan Xu, Limei Zhou

Here we report a strategy to prepare a novel ternary dual Z-scheme PCN/BiOCl/CdS photocatalyst by in-situ introducing bismuth oxychloride (BiOCl) on porous carbon nitride (PCN) and then depositing cadmium sulfide (CdS). The synthesized PCN/BiOCl/CdS not only has the porous structure of PCN and the wide visible-light absorption range of CdS, but a special morphology and abundant oxygen vacancies of BiOCl under the action of the structure-directing agent ethylene glycol. Through the modulation of oxygen vacancies, the BiOCl in the PCN/BiOCl/CdS can be excited under visible light, thereby further improving its optical properties. The PCN/BiOCl/CdS exhibited excellent photocatalytic activity in oxidative coupling reaction of benzylamine under visible light. The excellent catalytic performance of PCN/BiOCl/CdS photocatalyst was due to high charge separation efficiency, oxygen vacancies and visible light absorption. Finally, we proposed a feasible photocatalytic mechanism for the PCN/BiOCl/CdS in oxidative coupling reaction of benzylamine.

本文报道了在多孔氮化碳(PCN)上原位引入氯化铋(BiOCl),然后沉积硫化镉(cd),制备新型三元双Z-scheme PCN/BiOCl/CdS光催化剂的策略。合成的PCN/BiOCl/CdS不仅具有PCN的多孔结构和CdS的宽可见光吸收范围,而且在结构导向剂乙二醇的作用下具有BiOCl的特殊形态和丰富的氧空位。通过对氧空位的调制,PCN/BiOCl/CdS中的BiOCl可以在可见光下被激发,从而进一步改善其光学性能。PCN/BiOCl/CdS在可见光下对苄胺的氧化偶联反应表现出优异的光催化活性。PCN/BiOCl/CdS光催化剂具有较高的电荷分离效率、氧空位和可见光吸收性能。最后,我们提出了PCN/BiOCl/CdS在苯胺氧化偶联反应中的可行光催化机理。
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引用次数: 1
Acetoacetate Production from CO2 and Acetone with Acetone Carboxylase from Photosynthetic Bacteria Rhodobacter Capsulatus 光合细菌荚膜红杆菌丙酮羧化酶催化CO2和丙酮生产乙酰乙酸
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-10-06 DOI: 10.1007/s10563-022-09371-x
Yu Kita, Yutaka Amao

Carbon capture and utilization (CCU) technology is the process of capturing and converting CO2 into useful materials for further usage. The CCU aims to convert the captured CO2 into more valuable materials while maintaining the carbon neutrality of the production process. In this work, we have demonstrated the acetoacetate production from acetone and NaHCO3 using acetone carboxylase (AC) in cell extract from photosynthetic bacteria Rhodobacter capsulatus strain SB1003 (Rb. capsulatus SB1003) cultured in a medium containing acetone and bicarbonate under anaerobic photoheterotrophic conditions as a catalyst in the presence of ATP. Steady acetoacetate production due to the carboxylation of acetone with NaHCO3 was accomplished in the presence of ATP by using cell extract including AC from Rb. capsulatus SB1003. Moreover, steady acetoacetate production from acetone and gaseous CO2 also was attained by using cell extract.

碳捕获与利用(CCU)技术是将二氧化碳捕获并转化为有用材料以供进一步利用的过程。CCU旨在将捕获的二氧化碳转化为更有价值的材料,同时保持生产过程的碳中和。在这项工作中,我们证明了利用丙酮羧化酶(AC)在光合细菌荚膜红杆菌SB1003 (Rb)的细胞提取物中由丙酮和NaHCO3生产乙酰乙酸。SB1003)在含丙酮和碳酸氢盐的培养基中厌氧光异养条件下作为ATP存在下的催化剂培养。在ATP存在的条件下,利用含有Rb的AC的细胞提取物,用NaHCO3使丙酮羧化,从而稳定地生产乙酰乙酸。capsulatus SB1003。此外,利用细胞萃取物还可实现丙酮和气态CO2的稳定生产乙酰乙酸。
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引用次数: 0
Short Review on CO Combustion Promoters for FCC Regenerator FCC蓄热器CO助燃剂的研究进展
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-09-30 DOI: 10.1007/s10563-022-09368-6
Snehalkumar Parmar, T. M. Sankaranarayanan, Gopal Ravichandran

Fluidized Catalytic Cracking (FCC) is one of the key processes of any petroleum refinery as it produces gasoline, Liquefied Petroleum Gas (LPG) and valuable petrochemical feedstock viz. ethylene and propylene. FCC is a catalytic process where zeolite (USY and ZSM-5) based catalysts are being used, contain a high concentration of acidic sites, which are responsible for cracking heavy hydrocarbon molecules into smaller ones. During these cracking reactions, significant coke formation occurs over the catalyst surface and blocks the pores, thus resulting drop in catalytic activity. To regain the catalyst activity, the coke on the catalyst is burned in the FCC regenerator unit and provides heat demand for the FCC riser bed where the cracking reaction takes place and the cycle continues. The temperature of the FCC regenerator reaches around 700 °C due to the combustion of coke on the catalyst. Due to incomplete combustion of coke on catalyst produces CO which burns above the catalyst bed, which is denoted as a dilute bed. The heat of reaction of CO combustion needs to be realized on catalysts bed and also to avoid the heat loss in the regenerator dilute bed. Higher dilute bed temperature damages the FCC regenerator internals, which is to be avoided. Conventionally, additives named CO Combustion Promoters (COPs) have been used for the promotion of CO to CO2 in the catalyst bed which helps in improving regeneration of FCC equilibrium catalysts. The present article covers the concept and various types of COP reported in the literature. Different preparation methodologies, physico-chemical properties and evaluation results have been discussed. These insights would be helpful to understand the structure–property–activity relationship of COP. Further, it can also help to select the right COP for the desired commercial applications.

流化催化裂化(FCC)是任何炼油厂生产汽油、液化石油气(LPG)和有价值的石化原料乙烯和丙烯的关键工艺之一。催化裂化是一种使用沸石(USY和ZSM-5)催化剂的催化过程,含有高浓度的酸性位点,负责将重烃分子裂解成较小的分子。在这些裂化反应中,催化剂表面会形成大量的焦炭,堵塞了气孔,从而导致催化活性下降。为了恢复催化剂的活性,催化剂上的焦炭在催化裂化再生装置中燃烧,并为催化裂化提升床提供热需求,裂化反应在这里发生,循环继续。由于焦炭在催化剂上的燃烧,催化裂化蓄热器的温度达到700℃左右。由于焦炭在催化剂上的不完全燃烧产生CO, CO在催化剂床上燃烧,称为稀床。CO燃烧的反应热既要在催化剂床上实现,又要避免再生器稀床的热损失。较高的稀床温度会损坏FCC再生器内部,这是必须避免的。在催化床层中,通常使用CO助燃剂(cop)来促进CO向CO2的转化,从而提高催化裂化平衡催化剂的再生能力。本文涵盖了文献中报道的缔约方会议的概念和各种类型。讨论了不同的制备方法、理化性质和评价结果。这些见解将有助于理解COP的结构-性能-活性关系。此外,它还可以帮助为所需的商业应用选择合适的COP。
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引用次数: 0
In-situ One-Pot Synthesis of Ti/Cu-SSZ-13 Catalysts with Highly Efficient NH3-SCR Catalytic Performance as Well as Superior H2O/SO2 Tolerability 一锅原位合成具有高效NH3-SCR催化性能和耐H2O/SO2性能的Ti/Cu-SSZ-13催化剂
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-09-29 DOI: 10.1007/s10563-022-09374-8
Jie Wan, Jiawei Chen, Yijun Shi, Yiyan Wang, Yanjun Liu, Jin Zhang, Gongde Wu, Renxian Zhou

Series of Ti/Cu-SSZ-13 zeolite catalysts with variable Ti content were prepared via convenient in-situ one-pot synthesizing strategy. Systematic evaluations of the NH3-SCR catalytic performance over the obtained catalysts were conducted. Results show that Ti/Cu-SSZ-13 with appropriate Ti content (in the current work Ti0.81/Cu2.15-SSZ-13) could serve as capable candidate for NH3-SCR application, as it exhibits highly efficient catalytic activity with expanded operation temperature window width from 140 to 540 °C, nearly 100% N2 selectivity, as well as superior tolerability against water vapor and SO2. Further structural/physicochemical characterizations demonstrate that the obtained Ti/Cu-SSZ-13 catalysts possess well-crystallized characteristic chabazite (CHA) structure. Isolated Cu2+ and monomeric Ti4+ are recognized as the primary active species, as the former mainly contributes to SCR reaction at low temperatures, while the latter are conducive for improving the high temperature SCR activity. Ti over doping would result in partial destruction of the zeolite structure, occupation of Cu2+ cation sites and formation of surface aggregated TiOx, thus leading to unsatisfactory NH3-SCR performances. Moreover, formation of agglomerated CuOx species during hydrothermal ageing and blockage of surface active sites by sulfate species formed during SO2 pretreatment are considered responsible for activity deterioration in the tolerability tests.

采用原位一锅法制备了一系列可变钛含量Ti/Cu-SSZ-13分子筛催化剂。对所得催化剂的NH3-SCR催化性能进行了系统评价。结果表明,Ti含量合适的Ti/Cu-SSZ-13(目前的研究为Ti0.81/Cu2.15-SSZ-13)具有高效的催化活性,其工作温度窗宽从140°C扩大到540°C, N2选择性接近100%,对水蒸气和SO2具有良好的耐受性,可以作为NH3-SCR应用的候选材料。进一步的结构/物理化学表征表明,所制备的Ti/Cu-SSZ-13催化剂具有良好结晶的特征恰辉石(CHA)结构。分离Cu2+和单体Ti4+被认为是主要的活性物质,前者主要参与低温SCR反应,而后者则有利于提高高温SCR活性。Ti过掺杂会导致沸石结构部分破坏,占据Cu2+阳离子位点,形成表面聚集的TiOx,从而导致NH3-SCR性能不理想。此外,水热老化过程中形成的CuOx团块和SO2预处理过程中形成的硫酸盐堵塞表面活性位点被认为是耐受性试验中活性下降的原因。
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引用次数: 1
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。
{"title":"Iridium Nanodisks Intercalated Between Graphite Layers: Iridium Loading and Metal Particle Size","authors":"Masayuki Shirai,&nbsp;Sakura Kudo,&nbsp;Tomoki Sobu,&nbsp;Mika Sodeno,&nbsp;Shusuke Kato,&nbsp;Etty N. Kusumawati,&nbsp;Hidetaka Nanao","doi":"10.1007/s10563-022-09369-5","DOIUrl":"10.1007/s10563-022-09369-5","url":null,"abstract":"<div><p>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.</p><h3>Graphical Abstract</h3><p>\u0000Iridium 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.</p><figure><div><div><div><picture><source><img></source></picture></div></div></div></figure></div>","PeriodicalId":509,"journal":{"name":"Catalysis Surveys from Asia","volume":"27 1","pages":"107 - 114"},"PeriodicalIF":3.0,"publicationDate":"2022-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4809866","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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。
{"title":"Recent Advances in Catalytic Conversion of C5/C6 Alkanes to Olefins: A Review","authors":"Xin Wang,&nbsp;Youhao Xu","doi":"10.1007/s10563-022-09367-7","DOIUrl":"10.1007/s10563-022-09367-7","url":null,"abstract":"<div><p>Light naphtha (C<sub>5</sub>–C<sub>6</sub> alkanes) is commonly used as a feedstock for steam cracking or catalytic cracking to produce ethylene and propylene. This paper summarizes the progress of C<sub>5</sub>/C<sub>6</sub> alkanes steam cracking and catalytic cracking, but the key problem of the above method is the high yield of low-value C<sub>1</sub>–C<sub>3</sub> alkanes. When C<sub>5</sub>/C<sub>6</sub> olefin is used as the feedstock of catalytic cracking, the ethylene and propylene yields are high, while the C<sub>1</sub>–C<sub>3</sub> alkanes yield is low. It is of scientific value to dehydrogenate the C<sub>5</sub>/C<sub>6</sub> 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 C<sub>5</sub>/C<sub>6</sub> alkanes, and points out that the key is to develop C<sub>5</sub>/C<sub>6</sub> alkanes dehydrogenation catalyst for selective preparation of corresponding mono-olefins. The main issues about how to develop highly selective C<sub>5</sub>/C<sub>6</sub> alkanes dehydrogenation catalysts are proposed.</p></div>","PeriodicalId":509,"journal":{"name":"Catalysis Surveys from Asia","volume":"26 4","pages":"245 - 260"},"PeriodicalIF":3.0,"publicationDate":"2022-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10563-022-09367-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4814186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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
期刊
Catalysis Surveys from Asia
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