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Biodiesel Production from Euglena Sanguinea Using Catalyst Support Extracted From Steel Slag-Optimization and Kinetic Study 利用从钢渣中提取的催化剂载体从褐藻中生产生物柴油--优化和动力学研究
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-08-07 DOI: 10.1007/s10562-024-04790-z
Shriram Manikandan, Lokesh Sakthivel, Abieswar Parthiban, Roshan Cheerakkoda Baiju, Sindhu Subramanian
{"title":"Biodiesel Production from Euglena Sanguinea Using Catalyst Support Extracted From Steel Slag-Optimization and Kinetic Study","authors":"Shriram Manikandan,&nbsp;Lokesh Sakthivel,&nbsp;Abieswar Parthiban,&nbsp;Roshan Cheerakkoda Baiju,&nbsp;Sindhu Subramanian","doi":"10.1007/s10562-024-04790-z","DOIUrl":"10.1007/s10562-024-04790-z","url":null,"abstract":"<div><p>Extracting useful materials from the effluents help in cost reduction of catalyst synthesis for transesterification reaction. Hence, in this study, CaO-SiO<sub>2</sub> and MgO–SiO<sub>2</sub> catalysts were prepared in which the nano–silica was extracted from the steel slag. The properties of the slag, extracted nano-silica and synthesized catalysts were characterized in detail. Biodiesel was synthesized from <i>Euglena sanguinea.</i> Optimization of various parameters of transesterification process was done by RSM using CCD. The presence of biodiesel was confirmed with the help of <sup>1</sup>H-NMR, GC–MS and FTIR spectroscopy. The synthesized MgO–SiO<sub>2</sub> and CaO–SiO<sub>2</sub> catalyst possessed a surface area of 31 and 15 m<sup>2</sup>/g respectively. The optimized parameters obtained using CaO–SiO<sub>2</sub> were methanol to oil ratio of 9:1, catalyst weight % of 5 and duration of 3 h. The optimized parameters of the MgO–SiO<sub>2</sub> catalyst were–methanol to oil ratio of 9:1, catalyst weight % of 6 and reaction time of 5.5 h. The biodiesel yield obtained by using CaO–SiO<sub>2</sub> and MgO–SiO<sub>2</sub> corresponds to 87 and 83. 5% respectively. The loss of yield after reusing 5 times was 20 and 10% for CaO–SiO<sub>2</sub> and MgO–SiO<sub>2</sub> respectively. Kinetic models were compared with respect to their fit with experimental data. Pseudo–first order kinetics was a better fit for the experimental data using MgO–SiO<sub>2</sub>. While using CaO–SiO<sub>2</sub> as a catalyst, non-linear kinetic model was found to fit with the experimental data better.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 11","pages":"6049 - 6063"},"PeriodicalIF":2.3,"publicationDate":"2024-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141945565","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: 0
Application of Mixed Acid-Modified Hollow TS-1 Zeolite to Vapor-Phase Beckman Rearrangement Reaction 混合酸改性中空 TS-1 沸石在气相贝克曼重排反应中的应用
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-08-06 DOI: 10.1007/s10562-024-04780-1
Pengyu Yin, Jiayuan Nie, Xiangyu Wen, Zhihui Li, Dongsheng Zhang, Xinqiang Zhao, Yanji Wang
{"title":"Application of Mixed Acid-Modified Hollow TS-1 Zeolite to Vapor-Phase Beckman Rearrangement Reaction","authors":"Pengyu Yin,&nbsp;Jiayuan Nie,&nbsp;Xiangyu Wen,&nbsp;Zhihui Li,&nbsp;Dongsheng Zhang,&nbsp;Xinqiang Zhao,&nbsp;Yanji Wang","doi":"10.1007/s10562-024-04780-1","DOIUrl":"10.1007/s10562-024-04780-1","url":null,"abstract":"<div><p>ε-Caprolactam (CPL) is an important organic chemical raw material used as a monomer in the production of nylon 6. The traditional production process employs fuming sulfuric acid as a catalyst, leading to serious equipment corrosion and environmental pollution. While vapor-phase Beckman rearrangement reaction offers a solution to these issues. Unfortunately, the catalyst used is susceptible to carbon deposition and deactivation during the vapor-phase Beckman rearrangement process. Herein, a kind of mixed acid-modified hollow TS-1 zeolite was prepared in this study. It is a hollow structure of TS-1 zeolite formed by secondary crystallization, which is conducive to the shortening of the reaction path and the improvement of the anti-carbon accumulation performance. Further investigation revealed that modification of the hollow TS-1 zeolite with mixed acids facilitates the removal of non-skeletal titanium, and reduces the amount of Lewis acid in the catalyst, thereby improving its catalytic performance. Under optimal conditions, the cyclohexanone oxime (CHO) conversion rate reached 100%, with a caprolactam selectivity exceeding 98%. Notably, the catalytic activity of the catalyst remained stable after 500 h of continuous operation.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 11","pages":"6035 - 6048"},"PeriodicalIF":2.3,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141945566","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: 0
Synthesis and Investigation of Light Assisted Catalytic OER/HER Behavior of g-C3N4/Al2S3 Nanocomposite g-C3N4/Al2S3 纳米复合材料的光助催化 OER/HER 行为的合成与研究
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-08-05 DOI: 10.1007/s10562-024-04788-7
Fozia Iram, Sidra Aslam,  Javaria, Muhammad Safdar, Misbah Mirza, Muhammad Bilal Tahir, Muhammad Suleman Tahir
{"title":"Synthesis and Investigation of Light Assisted Catalytic OER/HER Behavior of g-C3N4/Al2S3 Nanocomposite","authors":"Fozia Iram,&nbsp;Sidra Aslam,&nbsp; Javaria,&nbsp;Muhammad Safdar,&nbsp;Misbah Mirza,&nbsp;Muhammad Bilal Tahir,&nbsp;Muhammad Suleman Tahir","doi":"10.1007/s10562-024-04788-7","DOIUrl":"10.1007/s10562-024-04788-7","url":null,"abstract":"<div><p>The pursuit of high-performance and cost-effective photoelectrocatalysts for water splitting stands as a focal point in sustainable energy research. In this investigation, we present the fabrication of a novel multifunctional g-C<sub>3</sub>N<sub>4</sub>/Al<sub>2</sub>S<sub>3</sub> nanocomposite as photoelectrocatalyst utilizing the co-precipitation method. Tailored for application in photoelectrochemical water splitting under alkaline conditions, the resulting nanocomposite underwent physical characterization via X-ray diffraction and scanning electron microscopy, affirming its well-defined shape, size and crystallinity. Employing a three-dimensional nickel foam substrate as a conducting support, we scrutinized the performance of the g-C<sub>3</sub>N<sub>4</sub>/Al<sub>2</sub>S<sub>3</sub> nanocomposite in the light assisted Hydrogen Evolution Reaction (HER) and Oxygen Evolution Reaction (OER). Our findings reveal the nanocomposites superiority over its pristine components (g-C<sub>3</sub>N<sub>4</sub> and Al<sub>2</sub>S<sub>3</sub>) in terms of charge transport within an alkaline medium. Additionally, the g-C<sub>3</sub>N<sub>4</sub>/Al<sub>2</sub>S<sub>3</sub> nanocomposite showcases enhanced photoelectrocatalytic efficiencies, achieving low overpotentials of 111 mV for HER and 217 mV for OER respectively, to reach a current density of 10 mA cm<sup>–2</sup>. The prepared g-C<sub>3</sub>N<sub>4</sub>/Al<sub>2</sub>S<sub>3</sub> electrocatalyst demonstrates exceptional durability in both HER and OER processes, attributed to the robust electronic coupling between g-C<sub>3</sub>N<sub>4</sub> and Al<sub>2</sub>S<sub>3</sub>. This study marks a significant advancement in the development of efficient and robust photoelectrochemical systems for water splitting, promising a brighter future for sustainable energy production.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 11","pages":"6022 - 6034"},"PeriodicalIF":2.3,"publicationDate":"2024-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141945567","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: 0
Pt/facet-Engineered Hydroxyapatite Co-Catalyst for Highly Efficient Hydrolysis of Ammonia Borane 用于高效水解氨硼烷的 Pt/facet-工程羟基磷灰石共催化剂
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-08-03 DOI: 10.1007/s10562-024-04773-0
Haruto Kamiya, Kunihiko Kato, Yunzi Xin, Yuping Xu, Takashi Shirai
{"title":"Pt/facet-Engineered Hydroxyapatite Co-Catalyst for Highly Efficient Hydrolysis of Ammonia Borane","authors":"Haruto Kamiya,&nbsp;Kunihiko Kato,&nbsp;Yunzi Xin,&nbsp;Yuping Xu,&nbsp;Takashi Shirai","doi":"10.1007/s10562-024-04773-0","DOIUrl":"10.1007/s10562-024-04773-0","url":null,"abstract":"<p>Ammonia borane (AB, NH<sub>3</sub>BH<sub>3</sub>) is a promising candidate for a hydrogen-storage material because of its high stability as a solid state at room temperature under atmospheric pressure. This study demonstrated a novel catalyst design for highly efficient hydrolysis of AB by hybridizing Pt catalyst with hydroxyapatite (HAp, Ca<sub>10</sub>(PO4)<sub>6</sub>(OH)<sub>2</sub>) as an “active support”, possessing Lewis-acidic Ca<sup>2+</sup> sites in the a-plane and Lewis-basic PO<sub>4</sub><sup>3-</sup> sites in the c-plane. Facet-engineered HAp particles were synthesized via the microwave-assisted hydrothermal reaction using Ca-EDTA chelates. Varying the Ca/P ratio of HAp precursor (from 1.5 to 1.8) affected the particle morphology, exposed facet ratio of {300} to {002}, and the percentage of phosphate anion species (PO<sub>4</sub><sup>3-</sup> and HPO<sub>4</sub><sup>2-</sup>). The rod-like HAp sole catalysts performed approximately 2-fold higher activity for the hydrolysis of AB, compared with spherical HAp with low crystallinity. Moreover, the Pt/rod-like HAp co-catalyst demonstrated superior catalytic performance with a turnover frequency (TOF) of 623 mol<sub>H2</sub> mol<sub>Pt</sub><sup>-1</sup> min<sup>-1</sup> than the Pt/spherical HAp (&lt;232 mol<sub>H2</sub> mol<sub>Pt</sub><sup>-1</sup> min<sup>-1</sup>). We proposed a possible mechanism of a synergistic effect in the significant enhancement of the hydrogen release rate from AB. Lewis basic PO<sub>4</sub><sup>3-</sup> and Lewis acidic Ca<sup>2+</sup> sites on HAp would affect preferential adsorption of electron-deficient BH<sub>3</sub> and electron-rich NH<sub>3</sub> groups in AB, catalyzing cleavage of B-N bonds. Besides, PO<sub>4</sub><sup>3-</sup> sites play a critical role in anchoring Pt particles towards electron transfer from Pt to PO<sub>4</sub><sup>3-</sup>, resulting in considerable enhancement of catalytic performance in dissociative adsorption of water molecules, which is a rate-determining step in the hydrolysis.</p>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 11","pages":"6012 - 6021"},"PeriodicalIF":2.3,"publicationDate":"2024-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10562-024-04773-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881551","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
Gel Resin Supported Ionic Liquids as Solid Acids for Esterification Reaction 凝胶树脂支持的离子液体作为酯化反应的固体酸
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-08-02 DOI: 10.1007/s10562-024-04787-8
Yulin Shao, Ping Xie, Yuning Han, Tianhao Zhong, Tao Li, Yingmin Yu, Qingshan Zhao, Zhongtao Li
{"title":"Gel Resin Supported Ionic Liquids as Solid Acids for Esterification Reaction","authors":"Yulin Shao,&nbsp;Ping Xie,&nbsp;Yuning Han,&nbsp;Tianhao Zhong,&nbsp;Tao Li,&nbsp;Yingmin Yu,&nbsp;Qingshan Zhao,&nbsp;Zhongtao Li","doi":"10.1007/s10562-024-04787-8","DOIUrl":"10.1007/s10562-024-04787-8","url":null,"abstract":"<div><p>In response to the problem that the conventional concentrated sulfuric acid catalyst for esterification reactions are prone to corrosion and generate large amounts of acid-containing wastewater, highly efficient gel resin-loaded ionic liquid solid acid (SA-ILs) catalysts were prepared by a one-pot method of loading ionic liquids onto gel resins. It is shown that the gel resin carrier has a strong water-absorbing structure, and the ionic liquids are covalently loaded on the gel resin carrier through chemical bonding, leading to SA-ILs catalysts with excellent acidity and good structural stability. With an optimal ionic liquid loading of 11% and acid density of 3.25 mmol·g<sup>−1</sup>,the synthesized SA-ILs catalysts showed good catalytic performance in the transesterification reaction between acetic acid and ethanol at 80 °C for 1.5 h. The catalyst dosage was 10 wt% of the total mass of acetic acid and ethanol, and the ethanol to acetic acid addition was at a molar ratio of 1.5:1. Ethyl acetate yields of up to 81% were achieved after the reaction. The catalyst also showed slightly decrease of the catalytic performance after reused for five cycles. The lower activation energy of the catalyst is proved to be the key to facilitate the catalytic transesterification reaction.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 11","pages":"5998 - 6011"},"PeriodicalIF":2.3,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881549","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: 0
Selective Catalytic Reduction of NOx with NH3 Over Fe Modified MOF-Derived MnOx Catalyst 在铁改性 MOF 衍生氧化锰催化剂上用 NH3 选择性催化还原氮氧化物
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-08-01 DOI: 10.1007/s10562-024-04792-x
Yao Wang, Ruiyang Chen, Jianglong Zhao, Zhiming Liu
{"title":"Selective Catalytic Reduction of NOx with NH3 Over Fe Modified MOF-Derived MnOx Catalyst","authors":"Yao Wang,&nbsp;Ruiyang Chen,&nbsp;Jianglong Zhao,&nbsp;Zhiming Liu","doi":"10.1007/s10562-024-04792-x","DOIUrl":"10.1007/s10562-024-04792-x","url":null,"abstract":"<div><p>A Fe modified MOF-derived MnO<sub>x</sub> catalyst has been synthesized and studied for the selective catalytic reduction of NO<sub>x</sub> with NH<sub>3</sub> (NH<sub>3</sub>-SCR). Compared with pure MnO<sub>x</sub>, Fe-modified MnO<sub>x</sub> showed a broader activity temperature window, enhanced N<sub>2</sub> selectivity, and improved sulfur tolerance. On one hand, the incorporation of Fe into MnO<sub>x</sub> increased acidity, thereby facilitating the adsorption of NH<sub>3</sub> as well as its activation, which plays a crucial role for the reduction of NO<sub>x</sub>. On the other hand, the presence of Fe resulted in decreased Mn<sup>4+</sup>, which contributes to improved N<sub>2</sub> selectivity. Over Fe modified MnO<sub>x</sub> catalyst, the coordinated NH<sub>3</sub>, NH<sub>4</sub><sup>+</sup>, bridging nitrate and bidentate nitrate are reactive, and participate in the NH<sub>3</sub>-SCR reaction following both “Eley–Rideal(E-R)” and “Langmuir–Hinshelwood(L–H)” mechanism. The present research provides an idea for broadening the activity temperature window and enhancing the sulfur tolerance of MnO<sub>x</sub> catalyst for the reduction of NO<sub>x</sub>, making it more suitable for practical application.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 11","pages":"5989 - 5997"},"PeriodicalIF":2.3,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141870420","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: 0
Synthesis and Characterization of AlPO4-18 Supported Mesoporous and Crystalline β-Mo2C, Ni3C, and WC Nanoparticles 以 AlPO4-18 为支撑的介孔和晶体 β-Mo2C、Ni3C 和 WC 纳米粒子的合成与表征
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-07-30 DOI: 10.1007/s10562-024-04791-y
Zinnabu T. Redda, Daniel Brennecke, Carsten Prinz, Abubeker Yimam, Mirko Barz, Steffen Kadow, Asnakech Laß-Seyoum
{"title":"Synthesis and Characterization of AlPO4-18 Supported Mesoporous and Crystalline β-Mo2C, Ni3C, and WC Nanoparticles","authors":"Zinnabu T. Redda,&nbsp;Daniel Brennecke,&nbsp;Carsten Prinz,&nbsp;Abubeker Yimam,&nbsp;Mirko Barz,&nbsp;Steffen Kadow,&nbsp;Asnakech Laß-Seyoum","doi":"10.1007/s10562-024-04791-y","DOIUrl":"10.1007/s10562-024-04791-y","url":null,"abstract":"<div><p>Developing high-efficiency, high-stability, and low-cost deoxygenation and hydrocracking catalysts could be considered one of the most significant breakthroughs in catalytic hydroprocessing. The present study utilized aluminophosphate (AlPO<sub>4</sub>-18), a zeolite-like molecular sieve, as catalyst support for producing carbon-coated β-Mo<sub>2</sub>C, Ni<sub>3</sub>C, and WC nanoparticles. The synthesis used an incipient wetness impregnation followed by a temperature-programmed reduction-carburization approach which involved cracking a hydrocarbon gas, propane, in a hydrogen environment. The synthesis parameters were a 1:7 propane/hydrogen reductive-carburizing gas stream, 15 wt.% metal loading, an 800 °C carburization temperature ramped-up at a heating rate of 10 °C min<sup>−1</sup>, a 2-h holding time, and a 1-h holding time in hydrogen. The synthesized catalysts were characterized using thermogravimetry mass spectroscopy/temperature-programmed oxidation (TPO TG-MS), nitrogen physisorption at 77 K, X-ray diffraction (XRD), and transmission electron microscopy/energy-dispersive X-ray spectroscopy (TEM EDS). TPO TG-MS, nitrogen physisorption, TEM, and XRD characterization results proved that atomic carbon was successfully incorporated into the lattice interstitials, resulting in thermally stable, well-dispersed, crystalline and mesoporous β-Mo<sub>2</sub>C/AlPO<sub>4</sub>-18, Ni<sub>3</sub>C/AlPO<sub>4</sub>-18, and WC/AlPO<sub>4</sub>-18 nanoparticles. XRD analysis showed structural evolution during reduction-carburization, with average crystallite sizes of metal-containing particles of 8.2–9.22, 6.64–8.50, and 6.03–7.56 nm for β-Mo<sub>2</sub>C/AlPO<sub>4</sub>-18, Ni<sub>3</sub>C/AlPO<sub>4</sub>-18, and WC/AlPO<sub>4</sub>-18, respectively. These values did not significantly deviate from high-resolution TEM analysis. The surface areas of the nanoparticles were categorized in decreasing order as WC/AlPO<sub>4</sub>-18 &gt; Ni<sub>3</sub>C/AlPO<sub>4</sub>-18 &gt; β-Mo<sub>2</sub>C/AlPO<sub>4</sub>-18, with values of 193.79, 169.05, and 66.57 m<sup>2</sup> g<sup>−1</sup>, respectively. In conclusion, these carbon-coated metal carbide nanoparticles with excellent thermal, structural, microscopic, and textural properties can be viable alternatives to noble metal catalysts for producing bio-jet fuel using the hydroprocessing pathway.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 11","pages":"5969 - 5988"},"PeriodicalIF":2.3,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141870367","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: 0
Theoretical Investigation of Propylene Epoxidation Using H2 and O2 Over Titanosilicate-Supported Au Catalysts 在钛硅酸盐支撑的金催化剂上使用 H2 和 O2 进行丙烯环氧化的理论研究
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-07-30 DOI: 10.1007/s10562-024-04783-y
Yasutaka Hamada, Tomohisa Yonemori, Yuhki Ishimaru, Takashi Kawakami, Shusuke Yamanaka, Mitsutaka Okumura
{"title":"Theoretical Investigation of Propylene Epoxidation Using H2 and O2 Over Titanosilicate-Supported Au Catalysts","authors":"Yasutaka Hamada,&nbsp;Tomohisa Yonemori,&nbsp;Yuhki Ishimaru,&nbsp;Takashi Kawakami,&nbsp;Shusuke Yamanaka,&nbsp;Mitsutaka Okumura","doi":"10.1007/s10562-024-04783-y","DOIUrl":"10.1007/s10562-024-04783-y","url":null,"abstract":"<div><p>Titanosilicate-supported Au-cluster catalysts can be used to selectively synthesize propylene oxide from propylene using O<sub>2</sub> and H<sub>2</sub>. However, the details of the catalytic reaction mechanism have not yet been elucidated. Thus, the reaction mechanism was investigated using density functional theory calculations. The calculation results revealed that active Ti-OOH forms on the surface Ti site, which is active as an oxidant and acts as an anchorage site for Au nanoclusters. The rate-determining step of propylene oxide synthesis on Au/titanosilicate is O insertion into propylene, with an activation energy of 1.37 eV. The propylene involved in this reaction is activated by adsorption on Au nanoclusters. Moreover, it was also found that the formation of Ti-OOH on Au/titanosilicate requires an activation energy of 0.48 eV, while it is barrierless on Au/anatase-TiO<sub>2</sub>. However, the decomposition energy of Ti-OOH on Au/titanosilicate is −0.16 eV, which is smaller than that on Au/anatase-TiO<sub>2</sub> (−1.12 eV). The results indicate that Ti-OOH decomposes more readily on Au/titanosilicate than on Au/anatase-TiO<sub>2</sub> but is easily regenerated because the reaction energy is significantly smaller than that on Au/anatase-TiO<sub>2</sub>. Therefore, these calculations are qualitatively in good agreement with the experimental results for Au/titanosilicate, which exhibited high catalytic activity at high temperatures.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 11","pages":"5948 - 5954"},"PeriodicalIF":2.3,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10562-024-04783-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141870371","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
Co-Based Bimetallic Oxide Catalysts with Abundant Vacancy Defects for Enhanced Oxidation of Toluene 具有丰富空位缺陷的共基双金属氧化物催化剂可增强甲苯氧化能力
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-07-30 DOI: 10.1007/s10562-024-04786-9
Zonglan Xie, Jiabin Zhou, Zedong Chen, Xiaohan Zhuge, Zhipu Wang
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引用次数: 0
Nickel Nanoparticles on Hydroxyl and Defect-rich Hollow Carbon Spheres as Catalysts for Efficient Selective Hydrogenation of Phenol 羟基和富缺陷中空碳球上的镍纳米颗粒作为高效选择性苯酚氢化的催化剂
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2024-07-29 DOI: 10.1007/s10562-024-04689-9
Feng Li, Yongqi Kuang, Peng Guo, Hao Li
{"title":"Nickel Nanoparticles on Hydroxyl and Defect-rich Hollow Carbon Spheres as Catalysts for Efficient Selective Hydrogenation of Phenol","authors":"Feng Li,&nbsp;Yongqi Kuang,&nbsp;Peng Guo,&nbsp;Hao Li","doi":"10.1007/s10562-024-04689-9","DOIUrl":"10.1007/s10562-024-04689-9","url":null,"abstract":"<div><p>The development and design of high-performance catalysts for selective hydrogenation of phenol to high value-added cyclohexanol is challenging. A series of hollow carbon coated Ni nanoreactor catalysts (Ni@HCS-T) were synthesized, adjusting carbonization temperature to investigate the effect of chemical microenvironment on the performance of selective hydrogenation of phenol. The results confirmed the carbonization temperature can regulate the degree of carbon skeleton defects and hydroxyl functional group content on the catalysts. The optimum catalyst (Ni@HCS-800) catalyzed phenol conversion of 99.54% and cyclohexanol selectivity of 98.53% at 120 ℃, 2 h and 1 MPa H<sub>2</sub> under the carbonization at 800 ℃. The Ni@HCS-800 catalyst is rich in defective structures which, together with neighbouring hydroxyl groups, significantly enhance substrate adsorption. Meanwhile, the abundant defects reasonably modulate the interfacial charge transfer behavior, resulting in a significantly enhanced degree of electron transfer between the metal Ni and carrier, enhancing the interaction between carbon carrier and metal. The Ni@HCS-800 catalyst showed the activation energy E<sub>a</sub> of 46.05 kJ⋅mol<sup>−1</sup> and remained stable performance after five cycles. In addition, the catalyst could effectively catalyze the conversion of a variety of lignin derivatives, showing wide applicability.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 9","pages":"5236 - 5254"},"PeriodicalIF":2.3,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141870372","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: 0
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