Pub Date : 2024-07-08DOI: 10.1007/s10562-024-04765-0
Simanye Sam, Babatope O. Ojo, Soraya P. Malinga, Nonhlangabezo Mabuba
Organic compounds of various classes have been identified as major pollutants commonly detected in several environmental freshwaters. As a potential solution, electrospun mat-like nanofibers comprising polyvinylidene fluoride (PVDF) nanofibers and kaolin clay composite were synthesized for the degradation of methylene blue dye in wastewater using piezocatalytic technique. The kaolin/PVDF composites were characterized with SEM, XRD, FTIR, Chronoamperometry and electrochemical impedance spectroscopy. The poling of the piezoelectric charges of the electrospun mat-like nanofibers, enhanced by the presence of the crystalline nature of the kaolin clay occasioned the generation of reactive species upon exposure to ultrasonic vibration. Moreover, ultrasound waves in the system prevented passivation of the mat’s active surface during piezocatalysis through continuous cleaning action. A degradation efficiency of 100% was obtained from the degradation of methylene blue dye using the synthesized kaolin/PVDF composites during piezocatalysis. This result positions the nanofiber as an effective catalyst in wastewater treatment applications.
{"title":"A Piezoelectric Electrospun Nanofiber mat (Kaolin/PVDF) for the Degradation of Methylene Blue in Water","authors":"Simanye Sam, Babatope O. Ojo, Soraya P. Malinga, Nonhlangabezo Mabuba","doi":"10.1007/s10562-024-04765-0","DOIUrl":"10.1007/s10562-024-04765-0","url":null,"abstract":"<div><p>Organic compounds of various classes have been identified as major pollutants commonly detected in several environmental freshwaters. As a potential solution, electrospun mat-like nanofibers comprising polyvinylidene fluoride (PVDF) nanofibers and kaolin clay composite were synthesized for the degradation of methylene blue dye in wastewater using piezocatalytic technique. The kaolin/PVDF composites were characterized with SEM, XRD, FTIR, Chronoamperometry and electrochemical impedance spectroscopy. The poling of the piezoelectric charges of the electrospun mat-like nanofibers, enhanced by the presence of the crystalline nature of the kaolin clay occasioned the generation of reactive species upon exposure to ultrasonic vibration. Moreover, ultrasound waves in the system prevented passivation of the mat’s active surface during piezocatalysis through continuous cleaning action. A degradation efficiency of 100% was obtained from the degradation of methylene blue dye using the synthesized kaolin/PVDF composites during piezocatalysis. This result positions the nanofiber as an effective catalyst in wastewater treatment applications.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10562-024-04765-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141573037","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}
Ammonia (NH3) synthesis via nitrogen reduction reaction under mild conditions is challenging due to the difficulty of activating nitrogen. Herein, Mn-doped g-C3N4 (x-Mn-CN, x = 5, 10, and 15) catalysts with efficiency NRR performance were synthesized. The resulting 5-Mn-CN exhibits higher NRR performance (NH3 yield rate: 15.2 μg h−1 mgcat−1, Faradaic efficiency: 7.1%) at -0.4 V (vs. RHE) than others. It is found that the active sites of Mn3+ are generated by electron transfer from Mn2+ to the N of g-C3N4, and active N2 through the π back-donation process. This is evidenced by the experimental result that the NH3 yield rate of 5-Mn-CN significantly decreases from 15.2 μg h−1 mgcat−1 to 2.6 μg h−1 mgcat−1 after lowering the concentration of Mn3+. The concentration of Mn3+ is reduced by treating the catalyst in the ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) solution. This study enhances the understanding of N2 activation and provides insights into the transition metal-doped g-C3N4 as NRR catalysts.
{"title":"Effective Electrochemical Nitrogen Reduction through π Back-donation Process in Mn3+ of Mn-doped g-C3N4","authors":"Yijin Ma, Yinpeng Lu, Chang Li, Liangqing Hu, Hexin Zhang, Jing Feng","doi":"10.1007/s10562-024-04772-1","DOIUrl":"10.1007/s10562-024-04772-1","url":null,"abstract":"<div><p>Ammonia (NH<sub>3</sub>) synthesis via nitrogen reduction reaction under mild conditions is challenging due to the difficulty of activating nitrogen. Herein, Mn-doped g-C<sub>3</sub>N<sub>4</sub> (x-Mn-CN, x = 5, 10, and 15) catalysts with efficiency NRR performance were synthesized. The resulting 5-Mn-CN exhibits higher NRR performance (NH<sub>3</sub> yield rate: 15.2 μg h<sup>−1</sup> mg<sub>cat</sub><sup>−1</sup>, Faradaic efficiency: 7.1%) at -0.4 V (<i>vs. RHE</i>) than others. It is found that the active sites of Mn<sup>3+</sup> are generated by electron transfer from Mn<sup>2+</sup> to the N of g-C<sub>3</sub>N<sub>4,</sub> and active N<sub>2</sub> through the π back-donation process. This is evidenced by the experimental result that the NH<sub>3</sub> yield rate of 5-Mn-CN significantly decreases from 15.2 μg h<sup>−1</sup> mg<sub>cat</sub><sup>−1</sup> to 2.6 μg h<sup>−1</sup> mg<sub>cat</sub><sup>−1</sup> after lowering the concentration of Mn<sup>3+</sup>. The concentration of Mn<sup>3+</sup> is reduced by treating the catalyst in the ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) solution. This study enhances the understanding of N<sub>2</sub> activation and provides insights into the transition metal-doped g-C<sub>3</sub>N<sub>4</sub> as NRR catalysts.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141573036","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}
Pub Date : 2024-07-05DOI: 10.1007/s10562-024-04769-w
María A. Vicerich, María A. Sánchez, Cristhian Fonseca Benítez, Vanina A. Mazzieri
The selection of an appropriate preparation method is crucial to enhance catalytic performance and optimize the resources used in catalyst synthesis. Achieving improvements in conversion rates, desired product yields are essential for increasing interest and competitiveness in the industrial sector. This study aims to analyze the influence of the preparation method of Rh(1%)-Sn(4%)/γ-Al2O3 catalysts on the selective hydrogenation of oleic acid to oleyl alcohol. Results from temperature-programmed reduction (TPR), cyclohexane dehydrogenation (DHC), and X-ray photoelectron spectroscopy (XPS) clearly demonstrate that incorporating sodium borohydride in the preparation process results in a stronger interaction between Rh and Sn. The degree of interaction between Rh and Sn is significantly influenced by the catalyst preparation and activation method, with a strong interaction promoting selectivity towards the formation of oleyl alcohol.
Graphical Abstract
选择合适的制备方法对于提高催化性能和优化催化剂合成过程中的资源使用至关重要。提高转化率和理想的产品收率对于增强工业领域的兴趣和竞争力至关重要。本研究旨在分析 Rh(1%)-Sn(4%)/γ-Al2O3 催化剂的制备方法对油酸选择性加氢制取油醇的影响。温度编程还原 (TPR)、环己烷脱氢 (DHC) 和 X 射线光电子能谱 (XPS) 的研究结果清楚地表明，在制备过程中加入硼氢化钠会增强 Rh 和 Sn 之间的相互作用。催化剂的制备和活化方法对 Rh 和 Sn 之间的相互作用程度有显著影响，强相互作用会提高生成油醇的选择性。
{"title":"Influence of the Activation Method of Rh-Sn-B/γ-Al2O3 Catalysts on the Selective Hydrogenation of Oleic Acid to Oleyl Alcohol","authors":"María A. Vicerich, María A. Sánchez, Cristhian Fonseca Benítez, Vanina A. Mazzieri","doi":"10.1007/s10562-024-04769-w","DOIUrl":"10.1007/s10562-024-04769-w","url":null,"abstract":"<div><p>The selection of an appropriate preparation method is crucial to enhance catalytic performance and optimize the resources used in catalyst synthesis. Achieving improvements in conversion rates, desired product yields are essential for increasing interest and competitiveness in the industrial sector. This study aims to analyze the influence of the preparation method of Rh(1%)-Sn(4%)/γ-Al<sub>2</sub>O<sub>3</sub> catalysts on the selective hydrogenation of oleic acid to oleyl alcohol. Results from temperature-programmed reduction (TPR), cyclohexane dehydrogenation (DHC), and X-ray photoelectron spectroscopy (XPS) clearly demonstrate that incorporating sodium borohydride in the preparation process results in a stronger interaction between Rh and Sn. The degree of interaction between Rh and Sn is significantly influenced by the catalyst preparation and activation method, with a strong interaction promoting selectivity towards the formation of oleyl alcohol.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141573040","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}
Pub Date : 2024-07-05DOI: 10.1007/s10562-024-04767-y
Malihe Hadadi, Alireza Habibi
Saccharification of cellulosic material is crucial before utilizing it as the feedstock of fermentation processes. This study focuses on developing of robust catalysts for enzymatic hydrolysis of paper waste. Cellulase enzyme was immobilized on Fe3O4 magnetic nanoparticles (MNPs) via multi-covalent bonds. Therefore, the attachments of MNPs were performed by three approaches (3-aminopropyl)triethoxysilane (APTES) (Method I), polyethyleneimine (PEI) (Method II), and both monolayer molybdenum disulfide and PEI (MoS2-PEI) (Method III). The biocatalysts were characterized using Fourier transform infrared (FTIR) and thermogravimetric analysis (TGA). The immobilization yield and loading efficiency of cellulase were determined at 38.65% and 162 mg g−1 in Method I, 13.33% and 31 mg g−1 in Method II, and 14.38% and 33 mg g−1 in Method III. The specification of the biocatalysts was determined for the hydrolysis of filter paper, carboxymethylcellulose (CMC), microcrystalline cellulose, and cellobiose. The total cellulase activity was 2.77, 0.943, 1.38, and 2.02 µmolGlucose mgEnzyme−1 h−1for free-cellulase and the immobilized biocatalysts prepared by Method I, II, and III, respectively. The prepared biocatalyst in Method I maintained 54.54% of its original activity after five cycles, which was more robust than Method II (20.25%) and Method III (12.33%). Further studies were performed on the saccharification of paper waste. The results showed the biocatalyst obtained by Method II resulted in 5.8 folds of higher glucose than the free-cellulase. The highest glucose recovery of about 72.47% was achieved after 48 h using the immobilized biocatalyst prepared by Method II.
Graphical Abstract
在将纤维素材料用作发酵工艺的原料之前，对其进行糖化处理至关重要。本研究的重点是开发用于酶水解废纸的强效催化剂。纤维素酶通过多共价键固定在 Fe3O4 磁性纳米粒子（MNPs）上。因此，通过三种方法（3-氨丙基三乙氧基硅烷（APTES）（方法 I）、聚乙烯亚胺（PEI）（方法 II）以及单层二硫化钼和 PEI（MoS2-PEI）（方法 III））对 MNPs 进行了附着。利用傅立叶变换红外（FTIR）和热重分析（TGA）对生物催化剂进行了表征。经测定，方法 I 中纤维素酶的固定化产率和负载效率分别为 38.65% 和 162 mg g-1，方法 II 中分别为 13.33% 和 31 mg g-1，方法 III 中分别为 14.38% 和 33 mg g-1。测定了生物催化剂水解滤纸、羧甲基纤维素（CMC）、微晶纤维素和纤维生物糖的规格。用方法 I、II 和 III 制备的游离纤维素酶和固定化生物催化剂的总纤维素酶活性分别为 2.77、0.943、1.38 和 2.02 µmolGlucose mgEnzyme-1 h-1。方法 I 中制备的生物催化剂在五个周期后保持了 54.54% 的原始活性，比方法 II（20.25%）和方法 III（12.33%）更强。对废纸糖化进行了进一步研究。结果表明，用方法 II 获得的生物催化剂比游离纤维素酶产生的葡萄糖高 5.8 倍。采用方法 II 制备的固定化生物催化剂在 48 小时后的葡萄糖回收率最高，约为 72.47%。
{"title":"Development of Magnetic Immobilized Cellulase Biocatalysts for Saccharification of Paper Waste","authors":"Malihe Hadadi, Alireza Habibi","doi":"10.1007/s10562-024-04767-y","DOIUrl":"10.1007/s10562-024-04767-y","url":null,"abstract":"<div><p>Saccharification of cellulosic material is crucial before utilizing it as the feedstock of fermentation processes. This study focuses on developing of robust catalysts for enzymatic hydrolysis of paper waste. Cellulase enzyme was immobilized on Fe<sub>3</sub>O<sub>4</sub> magnetic nanoparticles (MNPs) via multi-covalent bonds. Therefore, the attachments of MNPs were performed by three approaches (3-aminopropyl)triethoxysilane (APTES) (Method I), polyethyleneimine (PEI) (Method II), and both monolayer molybdenum disulfide and PEI (MoS<sub>2</sub>-PEI) (Method III). The biocatalysts were characterized using Fourier transform infrared (FTIR) and thermogravimetric analysis (TGA). The immobilization yield and loading efficiency of cellulase were determined at 38.65% and 162 mg g<sup>−1</sup> in Method I, 13.33% and 31 mg g<sup>−1</sup> in Method II, and 14.38% and 33 mg g<sup>−1</sup> in Method III. The specification of the biocatalysts was determined for the hydrolysis of filter paper, carboxymethylcellulose (CMC), microcrystalline cellulose, and cellobiose. The total cellulase activity was 2.77, 0.943, 1.38, and 2.02 µmol<sub>Glucose</sub> mg<sub>Enzyme</sub><sup>−1</sup> h<sup>−1</sup>for free-cellulase and the immobilized biocatalysts prepared by Method I, II, and III, respectively. The prepared biocatalyst in Method I maintained 54.54% of its original activity after five cycles, which was more robust than Method II (20.25%) and Method III (12.33%). Further studies were performed on the saccharification of paper waste. The results showed the biocatalyst obtained by Method II resulted in 5.8 folds of higher glucose than the free-cellulase. The highest glucose recovery of about 72.47% was achieved after 48 h using the immobilized biocatalyst prepared by Method II.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141547520","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}
The modification of petroleum resin (PR) by catalytic hydrogenation is an upgrading technology for producing high-value-added hydrogenated petroleum resin (HPR) from of pyrolysis petroleum by-product. This research employed alumina supports with different pore size distributions to prepare supported Mo-Ni type catalysts and investigated their catalytic hydrogenation performance on C9 petroleum resin. Catalysts prepared with bimodal pore alumina (BPA) supports effectively overcome the limitations of internal diffusion and increase the quantity of active sites, thus increasing the catalytic activity for hydrogenation. The experimental results demonstrated that MoNi/BPA achieved a hydrogenation degree of 99.94% for HC9PR, with the hydrogenated product having a Pt–Co colour of 2.37 Hazen. After 140 h of reaction, the hydrogenation degree of HC9PR remained at 96.51%, and the Pt–Co colour value was lower than 40 Hazen. This investigation confirms that solving the mass transfer issues of petroleum resin molecules in the pores of supported catalysts is key to designing efficient hydrogenation catalysts for petroleum resin.
{"title":"Effect of Pore Structure on the Performance of Mo-Ni Catalysts for Petroleum Resin Hydrogenation","authors":"Tong Niu, Zhengyang Shi, Jinchang Sun, Qianwen Zhang","doi":"10.1007/s10562-024-04768-x","DOIUrl":"10.1007/s10562-024-04768-x","url":null,"abstract":"<div><p>The modification of petroleum resin (PR) by catalytic hydrogenation is an upgrading technology for producing high-value-added hydrogenated petroleum resin (HPR) from of pyrolysis petroleum by-product. This research employed alumina supports with different pore size distributions to prepare supported Mo-Ni type catalysts and investigated their catalytic hydrogenation performance on C<sub>9</sub> petroleum resin. Catalysts prepared with bimodal pore alumina (BPA) supports effectively overcome the limitations of internal diffusion and increase the quantity of active sites, thus increasing the catalytic activity for hydrogenation. The experimental results demonstrated that MoNi/BPA achieved a hydrogenation degree of 99.94% for HC<sub>9</sub>PR, with the hydrogenated product having a Pt–Co colour of 2.37 Hazen. After 140 h of reaction, the hydrogenation degree of HC<sub>9</sub>PR remained at 96.51%, and the Pt–Co colour value was lower than 40 Hazen. This investigation confirms that solving the mass transfer issues of petroleum resin molecules in the pores of supported catalysts is key to designing efficient hydrogenation catalysts for petroleum resin.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141547519","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}
Pub Date : 2024-07-03DOI: 10.1007/s10562-024-04747-2
Daomei Chen, Guo Xiao, Jian Tang, Lixia zhao, Sicong Li, Lingli Li, Bin Li, Tao Lei, Jiaqiang Wang
Developing efficient artificial proteases still remains a great challenge due to the high stability of peptide bonds. Nanozymes have attracted great attention for their high stability, low cost and inherent physicochemical properties, providing new opportunities to break through natural enzyme inherent limitations, but the intrinsic mimic proteases properties of nanomaterials were seldom explored. Herein, we describe for the first time that SBA-3 supported Cu2O (Cu2O/SBA-3) exhibited excellent protease-like activity to hydrolysis of bovine serum albumin (BSA) and casein under neutral conditions, which is even superior to natural proteases (trypsin) and most of the other protease mimics under identical conditions. It exhibited surprisingly high catalytic activity and possessed good stability. As the first example of protease mimics consist of metallic compounds and mesoporous materials, Cu2O/SBA-3 has many advantages, such as easy preparation and separation, high activity and stability, mild reaction conditions, which makes this catalytic system have multiple of potential applications in biological systems.
{"title":"Cu2O/SBA-3 Possess Intrinsic High Protease-Like Activity for Efficient Hydrolysis of Protein Under Physiological Conditions","authors":"Daomei Chen, Guo Xiao, Jian Tang, Lixia zhao, Sicong Li, Lingli Li, Bin Li, Tao Lei, Jiaqiang Wang","doi":"10.1007/s10562-024-04747-2","DOIUrl":"10.1007/s10562-024-04747-2","url":null,"abstract":"<div><p>Developing efficient artificial proteases still remains a great challenge due to the high stability of peptide bonds. Nanozymes have attracted great attention for their high stability, low cost and inherent physicochemical properties, providing new opportunities to break through natural enzyme inherent limitations, but the intrinsic mimic proteases properties of nanomaterials were seldom explored. Herein, we describe for the first time that SBA-3 supported Cu2O (Cu2O/SBA-3) exhibited excellent protease-like activity to hydrolysis of bovine serum albumin (BSA) and casein under neutral conditions, which is even superior to natural proteases (trypsin) and most of the other protease mimics under identical conditions. It exhibited surprisingly high catalytic activity and possessed good stability. As the first example of protease mimics consist of metallic compounds and mesoporous materials, Cu2O/SBA-3 has many advantages, such as easy preparation and separation, high activity and stability, mild reaction conditions, which makes this catalytic system have multiple of potential applications in biological systems.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511516","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}
Pub Date : 2024-07-03DOI: 10.1007/s10562-024-04770-3
M. Sadegh Ramezani, Sadegh Safaei, Zahra Goodarzi, Mahsa Moradi
Herein, a modified synthesis method was presented and the effect of using an aqueous acetic acid solution in the process of synthesizing SQCOF was investigated. Adding a catalytic amount of aqueous solution of acetic acid as a co-catalyst has contributed to improving the quality of crystallinity. Effective parameters in the synthesis of SQCOF, including the concentration and volume of the co-catalyst and reaction solvent, were optimized. Then, the prepared SQCOF was used as a metal-free catalyst with Brønsted acid groups in the condensation reaction between 1,3-dicarbonyl compounds and primary amines. SQCOF was used under solvent-free conditions for the synthesis of enaminones at ambient temperature by mild manual grinding with a mortar and pestle and showed excellent catalytic performance in the above reaction. High performance and efficiency (62 to 96%), high TOF (833 to 1283 h−1), short reaction time, easy operation, minimizing the consumption of toxic organic solvents, absence of heavy metals in the framework and green conditions are the main advantages of this study. Also, SQCOF shows good chemical stability and recyclability (7 runs) and acts as an efficient catalyst in the synthesis of β-enaminones.
{"title":"Synthesis and Improving the Crystallinity of a Squaranine Covalent Organic Framework by Modifying the Preparation Method and Using it as a Green and Metal-Free Catalyst for the Synthesis of Enaminone","authors":"M. Sadegh Ramezani, Sadegh Safaei, Zahra Goodarzi, Mahsa Moradi","doi":"10.1007/s10562-024-04770-3","DOIUrl":"10.1007/s10562-024-04770-3","url":null,"abstract":"<div><p>Herein, a modified synthesis method was presented and the effect of using an aqueous acetic acid solution in the process of synthesizing SQCOF was investigated. Adding a catalytic amount of aqueous solution of acetic acid as a co-catalyst has contributed to improving the quality of crystallinity. Effective parameters in the synthesis of SQCOF, including the concentration and volume of the co-catalyst and reaction solvent, were optimized. Then, the prepared SQCOF was used as a metal-free catalyst with Brønsted acid groups in the condensation reaction between 1,3-dicarbonyl compounds and primary amines. SQCOF was used under solvent-free conditions for the synthesis of enaminones at ambient temperature by mild manual grinding with a mortar and pestle and showed excellent catalytic performance in the above reaction. High performance and efficiency (62 to 96%), high TOF (833 to 1283 h<sup>−1</sup>), short reaction time, easy operation, minimizing the consumption of toxic organic solvents, absence of heavy metals in the framework and green conditions are the main advantages of this study. Also, SQCOF shows good chemical stability and recyclability (7 runs) and acts as an efficient catalyst in the synthesis of <i>β</i>-enaminones.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511551","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}
Pub Date : 2024-07-02DOI: 10.1007/s10562-024-04771-2
Yongjia Liang, Jianliang Zuo, Zhaohao Cai, Jing Lin, Zili Liu
The direct conversion of furfural (FA) from biomass to pentanediols (PeDs), including 1,2-PeD and 1,5-PeD, is important for replacing fossil resources and developing bio-based polyesters from renewable sources. However, achieving high selectivity for the C–O hydrogenation of the furan ring remains a significant challenge. In this study, we synthesized a series of trimetallic CuCoLa catalysts, using a coprecipitation method with various metal ratios. The reduced CuCoLa catalyst with a metal ratio of 1/3/1, exhibited the highest activity for the selective hydrogenolysis of FA to PeDs. Under optimal reaction conditions (160 °C, 4 MPa H2 for 9 h), CuCoLa(1/3/1)-R achieved yields of 21.7% for 1,2-PeD and 50.1% for 1,5-PeD. Furthermore, the catalyst remained stable after five cycles of FA conversion to PeDs. The high selectivity for PeDs is attributed to the synergistic interaction between Cu and Co and the appropriate number of basic surface sites.
{"title":"Highly Efficient CuCoLa Catalyst for the Direct Hydrogenation of Furfural to Pentanediols","authors":"Yongjia Liang, Jianliang Zuo, Zhaohao Cai, Jing Lin, Zili Liu","doi":"10.1007/s10562-024-04771-2","DOIUrl":"10.1007/s10562-024-04771-2","url":null,"abstract":"<div><p>The direct conversion of furfural (FA) from biomass to pentanediols (PeDs), including 1,2-PeD and 1,5-PeD, is important for replacing fossil resources and developing bio-based polyesters from renewable sources. However, achieving high selectivity for the C–O hydrogenation of the furan ring remains a significant challenge. In this study, we synthesized a series of trimetallic CuCoLa catalysts, using a coprecipitation method with various metal ratios. The reduced CuCoLa catalyst with a metal ratio of 1/3/1, exhibited the highest activity for the selective hydrogenolysis of FA to PeDs. Under optimal reaction conditions (160 °C, 4 MPa H<sub>2</sub> for 9 h), CuCoLa(1/3/1)-R achieved yields of 21.7% for 1,2-PeD and 50.1% for 1,5-PeD. Furthermore, the catalyst remained stable after five cycles of FA conversion to PeDs. The high selectivity for PeDs is attributed to the synergistic interaction between Cu and Co and the appropriate number of basic surface sites.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511514","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}
Reduction of nitric acid reaction (2NO + HNO3 + 3CH3OH → 3CH3ONO + 2H2O) can convert by-product nitric acid into raw material methyl nitrite in the coal to ethylene glycol (CTEG) technology. This not only realizes the efficient recycling of nitrogen resources but also plays a crucial role in mitigating environmental pollution. Despite being a promising catalyst, the Pd/C catalyst face challenges due to its high metal loading, substantial loss rate, and consequent issues of poor stability, presenting obstacles in meeting industrial requirements. To address this issue, a defect strategy has been employed to develop a low-loaded 0.3% Pd/NC catalyst with robust metal-support interaction, resulting in a significant enhancement of catalyst stability. Remarkably, even after undergoing five cycles, the catalyst maintains a high nitric acid conversion rate of 90%. This improved performance can be attributed to the strong metal-support interaction driven by electron transfer from the nitrogen-doped carbon (NC) substrate to the Pd nanoparticles evident in the Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma (ICP) results. This interaction effectively suppresses the leaching of the active Pd nanoparticles, leading to significantly enhanced stability and a noticeable reduction in the loss rate. Raman spectrum and electron paramagnetic resonance (EPR) results can further reveal that the increase in the defect density lead to the strong metal-support interaction after nitrogen doping (pyridinic-N-dominated). These findings highlight the significant potential of the Pd/NC catalyst and its applicability in expediting the industrialization process of catalyst.
{"title":"Boosting Stability and Efficiency: Defect-Rich Pd/NC Catalysts for Nitric Acid Reduction to Methyl Nitrite","authors":"Jia-Kai Li, Xiang-Yu Li, Zhong-Ning Xu, Jing Sun, Shu-Juan Lin, Qiu-Pei Qin, Bin-Wen Liu, Ming-Sheng Wang, Guo-Cong Guo","doi":"10.1007/s10562-024-04741-8","DOIUrl":"10.1007/s10562-024-04741-8","url":null,"abstract":"<div><p>Reduction of nitric acid reaction (2NO + HNO<sub>3</sub> + 3CH<sub>3</sub>OH → 3CH<sub>3</sub>ONO + 2H<sub>2</sub>O) can convert by-product nitric acid into raw material methyl nitrite in the coal to ethylene glycol (CTEG) technology. This not only realizes the efficient recycling of nitrogen resources but also plays a crucial role in mitigating environmental pollution. Despite being a promising catalyst, the Pd/C catalyst face challenges due to its high metal loading, substantial loss rate, and consequent issues of poor stability, presenting obstacles in meeting industrial requirements. To address this issue, a defect strategy has been employed to develop a low-loaded 0.3% Pd/NC catalyst with robust metal-support interaction, resulting in a significant enhancement of catalyst stability. Remarkably, even after undergoing five cycles, the catalyst maintains a high nitric acid conversion rate of 90%. This improved performance can be attributed to the strong metal-support interaction driven by electron transfer from the nitrogen-doped carbon (NC) substrate to the Pd nanoparticles evident in the Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma (ICP) results. This interaction effectively suppresses the leaching of the active Pd nanoparticles, leading to significantly enhanced stability and a noticeable reduction in the loss rate. Raman spectrum and electron paramagnetic resonance (EPR) results can further reveal that the increase in the defect density lead to the strong metal-support interaction after nitrogen doping (pyridinic-N-dominated). These findings highlight the significant potential of the Pd/NC catalyst and its applicability in expediting the industrialization process of catalyst.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511553","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}
Pub Date : 2024-07-02DOI: 10.1007/s10562-024-04755-2
Lishan Zheng, Sitan Wang, Shifeng Lou, Kande Liu, Xuan Meng, Naiwang Liu, Li Shi
A series of Ni-W bimetallic catalysts were prepared by Ni2O3 and WO3 on porous materials and used in a fixed bed reactor for the hydrogenation of poly alpha-olefin base oil synthesis. The catalysts were characterized by N2 adsorption–desorption, XRD, H2-TPR, H2-TPD, XPS, TEM and ICP-OES to investigate the catalytic activity and explore the possible deactivation mechanism. Under the optimal reaction conditions of 250℃, 4 MPa, LHSV = 3 h−1 and H2: PAO = 200, the Ni5W1/Clay catalyst with 5% nickel and 1% tungsten loading can make the hydrogenation conversion rate as high as 100%, and the catalyst deactivation is not obvious within 8 h. The addition of W led to the reduction of the metal particle size as well as the formation of more dispersed active sites, thus improve its catalytic activity.
{"title":"Supported Ni-W Bimetallic Catalysts for Hydrogenation of Poly-Alpha-Olefins Synthetic Base Oil","authors":"Lishan Zheng, Sitan Wang, Shifeng Lou, Kande Liu, Xuan Meng, Naiwang Liu, Li Shi","doi":"10.1007/s10562-024-04755-2","DOIUrl":"10.1007/s10562-024-04755-2","url":null,"abstract":"<div><p>A series of Ni-W bimetallic catalysts were prepared by Ni<sub>2</sub>O<sub>3</sub> and WO<sub>3</sub> on porous materials and used in a fixed bed reactor for the hydrogenation of poly alpha-olefin base oil synthesis. The catalysts were characterized by N<sub>2</sub> adsorption–desorption, XRD, H<sub>2</sub>-TPR, H<sub>2</sub>-TPD, XPS, TEM and ICP-OES to investigate the catalytic activity and explore the possible deactivation mechanism. Under the optimal reaction conditions of 250℃, 4 MPa, LHSV = 3 h<sup>−1</sup> and H<sub>2</sub>: PAO = 200, the Ni5W1/Clay catalyst with 5% nickel and 1% tungsten loading can make the hydrogenation conversion rate as high as 100%, and the catalyst deactivation is not obvious within 8 h. The addition of W led to the reduction of the metal particle size as well as the formation of more dispersed active sites, thus improve its catalytic activity.</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":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511554","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}
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