Pub Date : 2024-02-01DOI: 10.1016/j.catcom.2024.106874
Lucas David Biondo , Christian Manera , Cesar Aguzzoli , Marcelo Godinho
Methane decomposition for hydrogen production is classified as blue turquoise, an intermediate between green and blue hydrogen. It does not generate greenhouse gas (GHG) emissions and does not require installation of carbon capture, utilization, and storage (CCUS) processes, becoming environmentally competitive among technologies, as the only byproduct is solid carbon. This research contributes to optimize temperature and gas hourly space velocity parameters for methane conversion adopting design of experiment (DoE) concept to collect data and identify significant factors through a 32 factorial design. Highest methane conversion, considering thermodynamic equilibrium limit of reaction, was obtained at 900 K and 6000 mL.h−1.g−1. The catalyst used was characterized by SEM, BET, and XRD.
{"title":"DoE-driven thermodynamic assessment of COX-free hydrogen production from methane decomposition","authors":"Lucas David Biondo , Christian Manera , Cesar Aguzzoli , Marcelo Godinho","doi":"10.1016/j.catcom.2024.106874","DOIUrl":"10.1016/j.catcom.2024.106874","url":null,"abstract":"<div><p>Methane decomposition for hydrogen production is classified as blue turquoise, an intermediate between green and blue hydrogen. It does not generate greenhouse gas (GHG) emissions and does not require installation of carbon capture, utilization, and storage (CCUS) processes, becoming environmentally competitive among technologies, as the only byproduct is solid carbon. This research contributes to optimize temperature and gas hourly space velocity parameters for methane conversion adopting design of experiment (DoE) concept to collect data and identify significant factors through a 3<sup>2</sup> factorial design. Highest methane conversion, considering thermodynamic equilibrium limit of reaction, was obtained at 900 K and 6000 mL.h<sup>−1</sup>.g<sup>−1</sup>. The catalyst used was characterized by SEM, BET, and XRD.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106874"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000347/pdfft?md5=218fd30ab70bb6b574b766fa7282d613&pid=1-s2.0-S1566736724000347-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139816772","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A novel bimetallic central covalent coupling catalytic system (Porp.Co@Zn-C6) based on Tris(4-Cl)(4-OH)Co and Tris(4-Cl)(4-OH)Zn was established to improve cycloalkanes oxidation. In particular, the partially-oxidized product's selectivity rose from 86.4% to 97.5% and the cyclohexane conversion was boosted from 3.80% to 4.41%. Simultaneously achieved improvements in conversion and selectivity. In this system, Co(II) was employed to activate molecular oxygen, Zn(II) was utilized to strengthen the utilization of cyclohexyl hydroperoxide and to be avoided its thermal decomposition in disorder state. This proposal can be very suitable for other cycloalkanes as well, which will improve the conversion and selectivity concurrently.
{"title":"Cycloalkanes oxidation with O2 catalyzed by a novel metalloporphyrin-based covalent coupling structure with bimetallic catalytic centers through synergistic mode","authors":"Jia-Ye Ni, Yan-Bo Ding, Jing Sun, Hong-Ke Wu, Hai-Min Shen, Yuan-Bin She","doi":"10.1016/j.catcom.2024.106876","DOIUrl":"10.1016/j.catcom.2024.106876","url":null,"abstract":"<div><p>A novel bimetallic central covalent coupling catalytic system (Porp.Co@Zn-C6) based on Tris(4-Cl)(4-OH)Co and Tris(4-Cl)(4-OH)Zn was established to improve cycloalkanes oxidation. In particular, the partially-oxidized product's selectivity rose from 86.4% to 97.5% and the cyclohexane conversion was boosted from 3.80% to 4.41%. Simultaneously achieved improvements in conversion and selectivity. In this system, Co(II) was employed to activate molecular oxygen, Zn(II) was utilized to strengthen the utilization of cyclohexyl hydroperoxide and to be avoided its thermal decomposition in disorder state. This proposal can be very suitable for other cycloalkanes as well, which will improve the conversion and selectivity concurrently.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106876"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000360/pdfft?md5=637c64fd64077690f6c55455185f5fa0&pid=1-s2.0-S1566736724000360-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139824303","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01DOI: 10.1016/j.catcom.2024.106882
Sethumathavan Vadivel , P. Sujita , Bappi Paul , B. Vidhya , Anju Sebastian , R. Selvarajan
Here in, we have fabricated a composite of SiC and g-C3N5 to form a noble-metal-free heterostructure as SiC/g-C3N5 for electrochemical HER activity. More than a few characterization techniques were investigated for their structural properties, such as the XRD, UV- DRS, FT-IR, FE-SEM, HR-TEM, and XPS measurements respectively. The HER reaction of SiC/g-C3N5 heterostructure with an overpotential obtained from Tafel slope of 81 mV/dec vs RHE at 10 mA/cm2 which is much better than that of the pristine SiC material. This work entitles that the effective approach for the rational design of g-C3N5-based electrocatalysts, for future developments in metal-free electrocatalysts.
在此,我们制备了 SiC 和 g-C3N5 的复合材料,形成了一种不含惰性金属的异质结构 SiC/g-C3N5,用于电化学 HER 活性。研究人员采用了多种表征技术,如 XRD、UV- DRS、FT-IR、FE-SEM、HR-TEM 和 XPS 测量等,对其结构特性进行了研究。在 10 mA/cm2 的条件下,SiC/g-C3N5 异质结构的 HER 反应的过电位为 81 mV/dec vs RHE,远高于原始 SiC 材料的过电位。这项工作为合理设计基于 g-C3N5 的电催化剂提供了有效方法,有助于未来无金属电催化剂的发展。
{"title":"Enhanced electrocatalytic HER performances of metal free SiC/g-C3N5 heterostructures","authors":"Sethumathavan Vadivel , P. Sujita , Bappi Paul , B. Vidhya , Anju Sebastian , R. Selvarajan","doi":"10.1016/j.catcom.2024.106882","DOIUrl":"10.1016/j.catcom.2024.106882","url":null,"abstract":"<div><p>Here in, we have fabricated a composite of SiC and g-C<sub>3</sub>N<sub>5</sub> to form a noble-metal-free heterostructure as SiC/g-C<sub>3</sub>N<sub>5</sub> for electrochemical HER activity. More than a few characterization techniques were investigated for their structural properties, such as the XRD, UV- DRS, FT-IR, FE-SEM, HR-TEM, and XPS measurements respectively. The HER reaction of SiC/g-C<sub>3</sub>N<sub>5</sub> heterostructure with an overpotential obtained from Tafel slope of 81 mV/dec vs RHE at 10 mA/cm<sup>2</sup> which is much better than that of the pristine SiC material. This work entitles that the effective approach for the rational design of g-C<sub>3</sub>N<sub>5</sub>-based electrocatalysts, for future developments in metal-free electrocatalysts.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106882"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000426/pdfft?md5=63ad123bfc7bd10ffd24786392bec422&pid=1-s2.0-S1566736724000426-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139924439","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01DOI: 10.1016/j.catcom.2024.106884
Haoran Liu , Hanlin Zhou , Luowen Yang , Yixian Pan , Xin Zhao , Fengliang Wang , Ruiqi Fang , Yingwei Li
Solar-driven CO2 reduction to CO production is often hampered by the kinetically sluggish water photooxidation and fast recombination of photocarriers. Herein, we report a photoredox system of CO2 reduction coupled with biomass-based amines oxidation. Double-shelled CdS nanocages (CdS DSNC) are synthesized by a successive etching‑sulfuration strategy, which delivers impressive CO and difurfurylamine yields of 1226.4 and 5526.5 μmol·g−1·h−1, respectively. Mechanism studies uncover that the double-shelled structure endows CdS DSNC with high accessibility of active sites and short transfer distance for photocarriers. Besides, furfurylamine serves as both the electron donor and the capturer of CO2, thus boosting the photoredox performance.
{"title":"Photocatalytic CO2 reduction coupled with biomass-based amines oxidation over double-shelled CdS nanocages","authors":"Haoran Liu , Hanlin Zhou , Luowen Yang , Yixian Pan , Xin Zhao , Fengliang Wang , Ruiqi Fang , Yingwei Li","doi":"10.1016/j.catcom.2024.106884","DOIUrl":"10.1016/j.catcom.2024.106884","url":null,"abstract":"<div><p>Solar-driven CO<sub>2</sub> reduction to CO production is often hampered by the kinetically sluggish water photooxidation and fast recombination of photocarriers. Herein, we report a photoredox system of CO<sub>2</sub> reduction coupled with biomass-based amines oxidation. Double-shelled CdS nanocages (CdS DSNC) are synthesized by a successive etching‑sulfuration strategy, which delivers impressive CO and difurfurylamine yields of 1226.4 and 5526.5 μmol·g<sup>−1</sup>·h<sup>−1</sup>, respectively. Mechanism studies uncover that the double-shelled structure endows CdS DSNC with high accessibility of active sites and short transfer distance for photocarriers. Besides, furfurylamine serves as both the electron donor and the capturer of CO<sub>2</sub>, thus boosting the photoredox performance.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106884"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S156673672400044X/pdfft?md5=07c989a8f409b20f352707c34cdb80c9&pid=1-s2.0-S156673672400044X-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139954361","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01DOI: 10.1016/j.catcom.2024.106885
Hikmet Beyza Erdem, Sevil Çetinkaya
Catalytic efficiency in hydrogenation reactions can be increased due to the stability achieved with nanomaterials prepared by homogeneously immobilizing multiple metal nanoparticles onto porous solid materials. Herein, porous carbon (PC)-supported bimetallic (AgNi/PC) and trimetallic nanoparticles (AgNi/PC@Mn) were developed and evaluated as catalysts in the NaBH4-mediated reduction of 4-nitrophenol to 4-aminophenol. AgNi/PC@Mn catalysts were synthesized using a two-step synthesis strategy. The highest and excellent catalytic efficiency under ambient conditions was obtained by the trimetallic catalyst. Both catalysts proved to be easily separated from the reaction medium and usable for up to five consecutive cycles without losing their catalytic activity.
{"title":"AgNi/PC bimetallic and AgNi/PC@Mn trimetallic nanocatalysts for the efficient reduction of 4-nitrophenol","authors":"Hikmet Beyza Erdem, Sevil Çetinkaya","doi":"10.1016/j.catcom.2024.106885","DOIUrl":"10.1016/j.catcom.2024.106885","url":null,"abstract":"<div><p>Catalytic efficiency in hydrogenation reactions can be increased due to the stability achieved with nanomaterials prepared by homogeneously immobilizing multiple metal nanoparticles onto porous solid materials. Herein, porous carbon (PC)-supported bimetallic (AgNi/PC) and trimetallic nanoparticles (AgNi/PC@Mn) were developed and evaluated as catalysts in the NaBH<sub>4</sub>-mediated reduction of 4-nitrophenol to 4-aminophenol. AgNi/PC@Mn catalysts were synthesized using a two-step synthesis strategy. The highest and excellent catalytic efficiency under ambient conditions was obtained by the trimetallic catalyst. Both catalysts proved to be easily separated from the reaction medium and usable for up to five consecutive cycles without losing their catalytic activity.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106885"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000451/pdfft?md5=71540cb5163eac9347fb93de88c43381&pid=1-s2.0-S1566736724000451-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139954471","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01DOI: 10.1016/j.catcom.2024.106892
Jinfei Lu , Shaohua Wang , Yanheng Hao , Lu Lin , Fan Bai , Wenhao Cui , Juan Wang , Qingda An , Peng Tian , Jifeng Pang , Wenhao Luo
The impact of binder selection on catalytic performance of real catalyst extrudates is still limitedly shown in biomass catalysis. Herein, we have prepared two zeolite-based bifunctional extrudates (Ni/LaY-Al2O3 and Ni/LaY-SiO2). Compared with Ni/LaY-Al2O3, Ni/LaY-SiO2 shows a markedly enhanced durability and sustained performance for 936 h in the continuous liquid-phase hydrogenation of γ-valerolactone into methyl pentanoate. Complementary characterization studies reveal that choosing SiO2 as binder could efficiently mitigate metal agglomeration, coke formation and support dealumination during catalysis. These findings showcase that binder selection is essential for catalyst durability in the development of the industrial-level bifunctional catalysts for biomass valorization.
{"title":"Influence of binder selection on the catalytic performance of zeolite-based bifunctional catalysts for biomass catalysis","authors":"Jinfei Lu , Shaohua Wang , Yanheng Hao , Lu Lin , Fan Bai , Wenhao Cui , Juan Wang , Qingda An , Peng Tian , Jifeng Pang , Wenhao Luo","doi":"10.1016/j.catcom.2024.106892","DOIUrl":"10.1016/j.catcom.2024.106892","url":null,"abstract":"<div><p>The impact of binder selection on catalytic performance of real catalyst extrudates is still limitedly shown in biomass catalysis. Herein, we have prepared two zeolite-based bifunctional extrudates (Ni/LaY-Al<sub>2</sub>O<sub>3</sub> and Ni/LaY-SiO<sub>2</sub>). Compared with Ni/LaY-Al<sub>2</sub>O<sub>3</sub>, Ni/LaY-SiO<sub>2</sub> shows a markedly enhanced durability and sustained performance for 936 h in the continuous liquid-phase hydrogenation of γ-valerolactone into methyl pentanoate. Complementary characterization studies reveal that choosing SiO<sub>2</sub> as binder could efficiently mitigate metal agglomeration, coke formation and support dealumination during catalysis. These findings showcase that binder selection is essential for catalyst durability in the development of the industrial-level bifunctional catalysts for biomass valorization.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106892"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000529/pdfft?md5=11700240203d5ad1c3def2381ec4ba18&pid=1-s2.0-S1566736724000529-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140045599","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01DOI: 10.1016/j.catcom.2024.106914
A. Muhammad Afdhal Saputra , Averroes Fazlur Rahman Piliang , Dellyansyah , Marpongahtun , Andriayani , Ronn Goei , Risky Ramadhan H.T.S. , Saharman Gea
This review highlights Carbon Quantum Dots (CQDs) as promising photocatalysts for breaking down organic pollutants, particularly in advancing CQDs-based systems for degrading organic dyes. CQDs, used alone or combined with semiconductors, enhance performance. In scenarios with narrow bandgaps, CQDs assist in separating charges, whereas in wider bandgaps, they enable visible/NIR activity through up-conversion luminescence. When integrated into Z-scheme heterostructures, CQDs reduce recombination by facilitating electron transfer. Synthesis methods—both top-down and bottom-up—are explored along with crucial physicochemical properties. Furthermore, modifying CQDs through doping and integrating functional groups on their surface adjusts their characteristics, promising more effective CQDs-modified photocatalysts in future research.
{"title":"Synthesis, properties, and utilization of carbon quantum dots as photocatalysts on degradation of organic dyes: A mini review","authors":"A. Muhammad Afdhal Saputra , Averroes Fazlur Rahman Piliang , Dellyansyah , Marpongahtun , Andriayani , Ronn Goei , Risky Ramadhan H.T.S. , Saharman Gea","doi":"10.1016/j.catcom.2024.106914","DOIUrl":"10.1016/j.catcom.2024.106914","url":null,"abstract":"<div><p>This review highlights Carbon Quantum Dots (CQDs) as promising photocatalysts for breaking down organic pollutants, particularly in advancing CQDs-based systems for degrading organic dyes. CQDs, used alone or combined with semiconductors, enhance performance. In scenarios with narrow bandgaps, CQDs assist in separating charges, whereas in wider bandgaps, they enable visible/NIR activity through up-conversion luminescence. When integrated into <em>Z</em>-scheme heterostructures, CQDs reduce recombination by facilitating electron transfer. Synthesis methods—both top-down and bottom-up—are explored along with crucial physicochemical properties. Furthermore, modifying CQDs through doping and integrating functional groups on their surface adjusts their characteristics, promising more effective CQDs-modified photocatalysts in future research.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106914"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000748/pdfft?md5=ea04b775a8257ade3d695dce72d8f813&pid=1-s2.0-S1566736724000748-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140406132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This study presents a straightforward chemical approach to induce cationic surface defects on SrCoO3-δ (SCO) perovskites by selectively etching a-site Sr elements on the surface. The modified SCO-30 catalyst from this method exhibits an optimized thickness of cobalt-rich amorphous layer enriched with oxygen vacancies. This modification enhances the trifunctional catalytic activity for oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and hydrogen evolution reaction (HER) in an alkaline electrolyte. Importantly, the perovskite's structure remains unchanged during the surface engineering process. These findings underscore cationic defect engineering as an effective strategy for the rational design of high-performance electrocatalysts, showcasing potential applications in diverse electrochemical processes.
本研究提出了一种直接的化学方法,通过选择性地蚀刻表面上的 a 位 Sr 元素,诱导 SrCoO (SCO) 包晶石产生阳离子表面缺陷。通过这种方法修饰的 SCO-30 催化剂显示出富含氧空位的富钴无定形层的优化厚度。这种改性提高了碱性电解质中氧进化反应(OER)、氧还原反应(ORR)和氢进化反应(HER)的三重催化活性。重要的是,在表面工程过程中,包晶的结构保持不变。这些发现强调了阳离子缺陷工程是合理设计高性能电催化剂的有效策略,并展示了在各种电化学过程中的潜在应用。
{"title":"Surface regulation of perovskite oxides with cation preference for efficient trifunctional electrocatalysts","authors":"Ruoqi Zong , Xiaobing Wu , Sung Yul Lim , Yusheng Fang , Bareera Raza , Yujuan Lu , Youkun Tao , Jing Shao","doi":"10.1016/j.catcom.2024.106896","DOIUrl":"10.1016/j.catcom.2024.106896","url":null,"abstract":"<div><p>This study presents a straightforward chemical approach to induce cationic surface defects on SrCoO<sub>3-δ</sub> (SCO) perovskites by selectively etching a-site Sr elements on the surface. The modified SCO-30 catalyst from this method exhibits an optimized thickness of cobalt-rich amorphous layer enriched with oxygen vacancies. This modification enhances the trifunctional catalytic activity for oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and hydrogen evolution reaction (HER) in an alkaline electrolyte. Importantly, the perovskite's structure remains unchanged during the surface engineering process. These findings underscore cationic defect engineering as an effective strategy for the rational design of high-performance electrocatalysts, showcasing potential applications in diverse electrochemical processes.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106896"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000566/pdfft?md5=6fbd5729a1e4c4a9ec28c30f7f1f62dd&pid=1-s2.0-S1566736724000566-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140054571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01DOI: 10.1016/j.catcom.2024.106891
Shiyu Wan , Peng Lu , Dongyan Xu , Valentin Valtchev
In the present study, siliceous self-pillared pentasil (SPP) zeolite with regular mesopores was synthesized and used as a support for anchoring bimetallic PdAg clusters through a facile impregnation-reduction method. The as-prepared PdAg/SPP catalysts with different Pd/Ag ratios were demonstrated to catalyze formic acid dehydrogenation for hydrogen production. XRD results confirmed the formation of PdAg alloy on the surface of SPP zeolite. The Pd7Ag3/SPP catalyst showed high activity at 80 °C with an initial turn-over frequency (TOF) of 1263.6 h−1, proving the strategy using hierarchical SPP zeolite as carrier is advantageous over bulky zeolites for making highly active formic acid dehydrogenation catalysts.
{"title":"Bimetallic PdAg clusters loaded on hierarchical self-pillared pentasil zeolite as efficient catalysts for formic acid dehydrogenation","authors":"Shiyu Wan , Peng Lu , Dongyan Xu , Valentin Valtchev","doi":"10.1016/j.catcom.2024.106891","DOIUrl":"10.1016/j.catcom.2024.106891","url":null,"abstract":"<div><p>In the present study, siliceous self-pillared pentasil (SPP) zeolite with regular mesopores was synthesized and used as a support for anchoring bimetallic PdAg clusters through a facile impregnation-reduction method. The as-prepared PdAg/SPP catalysts with different Pd/Ag ratios were demonstrated to catalyze formic acid dehydrogenation for hydrogen production. XRD results confirmed the formation of PdAg alloy on the surface of SPP zeolite. The Pd<sub>7</sub>Ag<sub>3</sub>/SPP catalyst showed high activity at 80 °C with an initial turn-over frequency (TOF) of 1263.6 h<sup>−1</sup>, proving the strategy using hierarchical SPP zeolite as carrier is advantageous over bulky zeolites for making highly active formic acid dehydrogenation catalysts.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106891"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000517/pdfft?md5=9e8f6d15d9b0f9bdaebacb1da6598899&pid=1-s2.0-S1566736724000517-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140054573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01DOI: 10.1016/j.catcom.2024.106900
Yang Zhang , Qizhuang Zou , Ruiqi Fang , Hua Tan , Hongbing Ji , Yingwei Li
Yolk-shell nanoreactors feature numbers of advantages in promoting catalytic performance. This work demonstrates the fabrication of yolk-shell Fe3O4@SiO2/Al2O3-T (T = 500–900 °C) from metal-organic framework. Characterizations indicate the Fe3O4 yolk and SiO2/Al2O3 shell of the obtained nanoreactors. Fe3O4@SiO2/Al2O3–800 showed excellent performance in furfural acetalization to 2-(dimethoxymethyl)furan, achieving a 97% yield at 60 °C, atmospheric pressure within 5 h. Control experiments reveal the high reactivity of Fe3O4 yolks for furfural acetalization, and acidic Al species are favorable for reactivity promotion. Besides, porous SiO2/Al2O3 shells facilitate mass transfer and increase the accessibility of active sites, also contribute to the high performance and stability.
{"title":"MOF-derived Fe3O4@SiO2/Al2O3 yolk-shell nanoreactor for efficient furfural acetalization","authors":"Yang Zhang , Qizhuang Zou , Ruiqi Fang , Hua Tan , Hongbing Ji , Yingwei Li","doi":"10.1016/j.catcom.2024.106900","DOIUrl":"10.1016/j.catcom.2024.106900","url":null,"abstract":"<div><p>Yolk-shell nanoreactors feature numbers of advantages in promoting catalytic performance. This work demonstrates the fabrication of yolk-shell Fe<sub>3</sub>O<sub>4</sub>@SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub>-<em>T</em> (<em>T</em> = 500–900 °C) from metal-organic framework. Characterizations indicate the Fe<sub>3</sub>O<sub>4</sub> yolk and SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> shell of the obtained nanoreactors. Fe<sub>3</sub>O<sub>4</sub>@SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub>–800 showed excellent performance in furfural acetalization to 2-(dimethoxymethyl)furan, achieving a 97% yield at 60 °C, atmospheric pressure within 5 h. Control experiments reveal the high reactivity of Fe<sub>3</sub>O<sub>4</sub> yolks for furfural acetalization, and acidic Al species are favorable for reactivity promotion. Besides, porous SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> shells facilitate mass transfer and increase the accessibility of active sites, also contribute to the high performance and stability.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106900"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000608/pdfft?md5=8f3a0608813be26deef6ff1bbb727283&pid=1-s2.0-S1566736724000608-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140090338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}