首页 > 最新文献

Catalysis Letters最新文献

英文 中文
Enhancement the Photo-Quantum Efficiency in Photocatalytic Reactions via Well-Designed Rutile/Anatase TiO2 Growth on 2D Ti3C2Tx 设计金红石/锐钛矿型TiO2在二维Ti3C2Tx上生长提高光催化反应的光量子效率
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-17 DOI: 10.1007/s10562-025-04934-9
Wei Gan, Yan Guo, Dan Zhu, Min Ling, Can Jiang, Shengfu Zhang

With the increasing problems caused by water pollution, the use of photocatalytic oxidation to remove pollutants from wastewater is a sustainable strategy. However, it is challenging to develop well-designed photocatalysts with high photo-quantum efficiency and the comprehension of their photocatalytic reaction mechanisms. Herein, a R/A-TiO2/Ti3C2Tx (R: rutile; A: anatase) photocatalyst with different ratios of rutile and anatase phases was prepared by a facile hydrothermal method. The results showed that the number of rutile and anatase phases could be readily regulated by adjusting the dosage of titanium isopropoxide (TTIP) and Ti3C2Tx. The prepared R/A-TiO2/Ti3C2Tx-0.2 contained a mass fraction of 42% rutile phase and 58% anatase phase, with the interface between the two phases exhibited a tightly bonded structure. Meanwhile, the heterojunction between the heterophase TiO2 and Ti3C2Tx interfaces improved the photo-quantum efficiency of R/A-TiO2/Ti3C2Tx, and the degradation efficiency of Rhodamine B (RhB) by R/A-TiO2/Ti3C2Tx-0.2 was 77.82% in 2 h under ultraviolet light illumination. Ultimately, the active species capture experiments verified that the primary active species in the photocatalytic reaction was h+, ·OH, and·O2. This work could shed light on the new approach to the rational design of high-efficiency heterophase TiO2-based photocatalysts.

Graphical Abstract

R/A-TiO2/Ti3C2Tx photocatalysts with heterojunctions were controllably synthesized by an EDTA-2Na-assisted hydrothermal method.

随着水污染问题的日益严重,利用光催化氧化技术去除废水中的污染物是一种可持续发展的策略。然而,开发设计良好、光量子效率高的光催化剂及其光催化反应机理是一个挑战。其中,R/ a - tio2 /Ti3C2Tx (R:金红石;采用水热法制备了金红石与锐钛矿不同配比的光催化剂。结果表明,通过调节异丙醇钛(TTIP)和Ti3C2Tx的用量,可以很容易地调节金红石相和锐钛矿相的数量。制备的R/ a - tio2 /Ti3C2Tx-0.2的金红石相质量分数为42%,锐钛矿相质量分数为58%,两相界面呈紧密结合结构。同时,异相TiO2与Ti3C2Tx界面的异质结提高了R/A-TiO2/Ti3C2Tx的光量子效率,在紫外光照射下,R/A-TiO2/Ti3C2Tx-0.2在2 h内对Rhodamine B (RhB)的降解效率为77.82%。最终,活性物质捕获实验验证了光催化反应中的主要活性物质是h+、·OH和·O2−。本研究为合理设计高效异相tio2基光催化剂提供了新思路。采用edta - 2na辅助水热法合成了具有异质结的r /A-TiO2/Ti3C2Tx光催化剂。
{"title":"Enhancement the Photo-Quantum Efficiency in Photocatalytic Reactions via Well-Designed Rutile/Anatase TiO2 Growth on 2D Ti3C2Tx","authors":"Wei Gan,&nbsp;Yan Guo,&nbsp;Dan Zhu,&nbsp;Min Ling,&nbsp;Can Jiang,&nbsp;Shengfu Zhang","doi":"10.1007/s10562-025-04934-9","DOIUrl":"10.1007/s10562-025-04934-9","url":null,"abstract":"<div><p>With the increasing problems caused by water pollution, the use of photocatalytic oxidation to remove pollutants from wastewater is a sustainable strategy. However, it is challenging to develop well-designed photocatalysts with high photo-quantum efficiency and the comprehension of their photocatalytic reaction mechanisms. Herein, a R/A-TiO<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> (R: rutile; A: anatase) photocatalyst with different ratios of rutile and anatase phases was prepared by a facile hydrothermal method. The results showed that the number of rutile and anatase phases could be readily regulated by adjusting the dosage of titanium isopropoxide (TTIP) and Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>. The prepared R/A-TiO<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>-0.2 contained a mass fraction of 42% rutile phase and 58% anatase phase, with the interface between the two phases exhibited a tightly bonded structure. Meanwhile, the heterojunction between the heterophase TiO<sub>2</sub> and Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> interfaces improved the photo-quantum efficiency of R/A-TiO<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>, and the degradation efficiency of Rhodamine B (RhB) by R/A-TiO<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>-0.2 was 77.82% in 2 h under ultraviolet light illumination. Ultimately, the active species capture experiments verified that the primary active species in the photocatalytic reaction was h<sup>+</sup>, ·OH, and·O<sub>2</sub><sup>−</sup>. This work could shed light on the new approach to the rational design of high-efficiency heterophase TiO<sub>2</sub>-based photocatalysts.</p><h3>Graphical Abstract</h3><p>R/A-TiO<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> photocatalysts with heterojunctions were controllably synthesized by an EDTA-2Na-assisted hydrothermal method.</p>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994964","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
Efficient Catalytic Dehalogenation of Aryl Halides Under Mild Conditions Using Reusable Reduced Graphene Oxide Loaded Simple Transition Metal–Organic Framework 使用可重复使用的还原氧化石墨烯负载简单过渡金属-有机框架在温和条件下催化芳基卤化物的高效脱卤
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04911-8
Ilavarasan Lavanya, Muthumuniyandi Nishanthan, Rajendran Lakshmi Priya, Boopathi Shagunthala Hariprasad, Chettipalayam Arunasalam Dhayanithi, Sundaram Ganesh Babu

Transition metal-based Metal–Organic Frameworks (MOFs) (M-BDC (M – Ni, Cu, Zn)) are prepared by solvothermal method. The loading of MOF on the support material, rGO, is done through the simple ultrasonication technique. The MOF materials are characterized using powder X-ray diffraction, Fourier-transform infrared spectroscopy, Scanning electron microscopy, and Thermogravimetric analysis. The catalytic activity of the synthesized MOFs is tested towards the dehalogenation of aryl halides reaction. The reaction conditions are optimized, in which the Ni-BDC MOF shows high catalytic activity. Hence, Ni-BDC MOF is loaded with different weight percentages (10wt%, 20wt%, 30wt%, and 40wt%) of rGO. Subsequently, 10 wt% Ni-BDC MOF/rGO is found to be the best catalyst among the other weight percentages of rGO-loaded catalysts. Moreover, the catalyst is easily recoverable and can be used for many cycles without leaching of active species, structural changes, and loss in activity.

Graphical Abstract

采用溶剂热法制备了过渡金属基金属有机骨架(M- bdc (M- Ni, Cu, Zn))。MOF对支撑材料rGO的加载是通过简单的超声技术完成的。利用粉末x射线衍射、傅里叶变换红外光谱、扫描电镜和热重分析对MOF材料进行了表征。测试了所合成的MOFs对芳基卤化物脱卤反应的催化活性。对反应条件进行了优化,得到的Ni-BDC MOF具有较高的催化活性。因此,Ni-BDC MOF装载了不同重量百分比(10wt%、20wt%、30wt%和40wt%)的氧化石墨烯。结果表明,10 wt% Ni-BDC MOF/rGO是其他重量百分比rGO负载催化剂中最好的催化剂。此外,该催化剂易于回收,可以多次循环使用,而不会导致活性物质的浸出、结构变化和活性损失。图形抽象
{"title":"Efficient Catalytic Dehalogenation of Aryl Halides Under Mild Conditions Using Reusable Reduced Graphene Oxide Loaded Simple Transition Metal–Organic Framework","authors":"Ilavarasan Lavanya,&nbsp;Muthumuniyandi Nishanthan,&nbsp;Rajendran Lakshmi Priya,&nbsp;Boopathi Shagunthala Hariprasad,&nbsp;Chettipalayam Arunasalam Dhayanithi,&nbsp;Sundaram Ganesh Babu","doi":"10.1007/s10562-024-04911-8","DOIUrl":"10.1007/s10562-024-04911-8","url":null,"abstract":"<div><p>Transition metal-based Metal–Organic Frameworks (MOFs) (M-BDC (M – Ni, Cu, Zn)) are prepared by solvothermal method. The loading of MOF on the support material, rGO, is done through the simple ultrasonication technique. The MOF materials are characterized using powder X-ray diffraction, Fourier-transform infrared spectroscopy, Scanning electron microscopy, and Thermogravimetric analysis. The catalytic activity of the synthesized MOFs is tested towards the dehalogenation of aryl halides reaction. The reaction conditions are optimized, in which the Ni-BDC MOF shows high catalytic activity. Hence, Ni-BDC MOF is loaded with different weight percentages (10wt%, 20wt%, 30wt%, and 40wt%) of rGO. Subsequently, 10 wt% Ni-BDC MOF/rGO is found to be the best catalyst among the other weight percentages of rGO-loaded catalysts. Moreover, the catalyst is easily recoverable and can be used for many cycles without leaching of active species, structural changes, and loss in 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":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142913014","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
Comparative Study of Catalytic Performance of Post Treated H-BEA Zeolites for n-Hexyl Levulinate Synthesis from Renewable Feedstock 后处理H-BEA沸石催化再生原料合成乙酰丙酸正己酯性能比较研究
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04903-8
Ayushikumari R. Patel, Aayushi Lodhi, Hemant Parmar, Ajay Dalai, Kalpana Maheria

In the present study, zeolite H-BEA catalyst has been modified by controlled desilication post modification route using first with cationic surfactant, (6-Bromohexyl)trimethylammonium Bromide (6-Br-TMA) designated as MBB catalyst and then the other with 6-Br-TMA and yeast, designated as MBBY catalyst. These newly synthesized catalytic materials have been characterized by several techniques such as, Fourier-transform infrared spectroscopy (FT-IR), X-ray diffraction, scanning electron microscopy, solid state NMR (29Si, 27Al, 1H) N2 sorption isotherm analysis, thermogravimetric analysis, ammonia temperature program desorption (NH3-TPD) analysis, etc. These mesozeolites were found to exhibit enhanced physicochemical (BET surface area, surface acidity, pore volume, mesoporosity, etc.) characteristics as compared to their parent zeolite H-BEA. Catalytic assessement studies of the synthesized zeolites has been demonstrated via conducting experiments involving esterification of levulinic acid (LA) and n-hexanol. Parametric studies has been undertaken in order to get maximum LA conversion by varying several reaction parameters such as molar ratio (acid to n-hexanol), catalyst concentration, reaction time, etc. Further catalysts’ reusability studies has been carried out to assess their potential for reusability. The results indicated better catalytic performance of the zeolite H-BEA which is modified with the use of yeast (MBBY) as compared to microporous zeolite H-BEA and MBB catalyst which may be due to its enhanced surface area and surface acidity.

Graphical Abstract

本研究采用阳离子表面活性剂(6-溴己基)三甲基溴化铵(6-Br-TMA)为MBB催化剂,再以6-Br-TMA和酵母为MBBY催化剂,采用可控脱硅后改性路线对沸石H-BEA催化剂进行改性。利用傅里叶变换红外光谱(FT-IR)、x射线衍射、扫描电镜、固体核磁共振(29Si, 27Al, 1H) N2吸附等温线分析、热重分析、氨温度程序解吸(NH3-TPD)分析等技术对新合成的催化材料进行了表征。研究发现,这些介孔沸石的物理化学特征(BET表面积、表面酸度、孔隙体积、介孔率等)都比它们的母体沸石H-BEA要好。通过乙酰丙酸(LA)和正己醇的酯化实验,证明了所合成的沸石的催化评价研究。为了获得最大的LA转化率,通过改变几个反应参数,如摩尔比(酸与正己醇)、催化剂浓度、反应时间等,进行了参数化研究。进一步开展了催化剂的可重复使用性研究,以评估其可重复使用的潜力。结果表明,与微孔沸石H-BEA和MBB催化剂相比,经酵母修饰的H-BEA分子筛具有更好的催化性能,这可能是由于其表面积和表面酸性增强所致。图形抽象
{"title":"Comparative Study of Catalytic Performance of Post Treated H-BEA Zeolites for n-Hexyl Levulinate Synthesis from Renewable Feedstock","authors":"Ayushikumari R. Patel,&nbsp;Aayushi Lodhi,&nbsp;Hemant Parmar,&nbsp;Ajay Dalai,&nbsp;Kalpana Maheria","doi":"10.1007/s10562-024-04903-8","DOIUrl":"10.1007/s10562-024-04903-8","url":null,"abstract":"<div><p>In the present study, zeolite H-BEA catalyst has been modified by controlled desilication post modification route using first with cationic surfactant, (6-Bromohexyl)trimethylammonium Bromide (6-Br-TMA) designated as MBB catalyst and then the other with 6-Br-TMA and yeast, designated as MBBY catalyst. These newly synthesized catalytic materials have been characterized by several techniques such as, Fourier-transform infrared spectroscopy (FT-IR), X-ray diffraction, scanning electron microscopy, solid state NMR (<sup>29</sup>Si, <sup>27</sup>Al, <sup>1</sup>H) N<sub>2</sub> sorption isotherm analysis, thermogravimetric analysis, ammonia temperature program desorption (NH<sub>3</sub>-TPD) analysis, etc. These mesozeolites were found to exhibit enhanced physicochemical (BET surface area, surface acidity, pore volume, mesoporosity, etc.) characteristics as compared to their parent zeolite H-BEA. Catalytic assessement studies of the synthesized zeolites has been demonstrated via conducting experiments involving esterification of levulinic acid (LA) and <i>n</i>-hexanol. Parametric studies has been undertaken in order to get maximum LA conversion by varying several reaction parameters such as molar ratio (acid to <i>n</i>-hexanol), catalyst concentration, reaction time, etc. Further catalysts’ reusability studies has been carried out to assess their potential for reusability. The results indicated better catalytic performance of the zeolite H-BEA which is modified with the use of yeast (MBBY) as compared to microporous zeolite H-BEA and MBB catalyst which may be due to its enhanced surface area and surface acidity.</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":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142912953","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
Ultrasound-Assisted Dual-Enzyme System for the Preparation of Fatty Acid Ethyl Esters 超声辅助双酶体系制备脂肪酸乙酯
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04908-3
Yan Wang, Xiaohong Hao, Xiongzhi Da, Xiangsheng Zheng

This study focuses on the preparation of fatty acid ethyl esters (FAEE) in a solvent-free system using high-acid-value waste oil as the raw material. The research involves the addition of two enzymes with different substrate specificities, accompanied by ultrasonic assistance. The investigation explores the impact of enzyme addition (3–7 wt%), enzyme ratio (3:1–1:3), alcohol–oil ratio (5:1–25:1 mmol/g), reaction temperature (30–70 °C), reaction time (30–210 min), and ultrasonic power (0–150 W) on the experimental outcomes. Reaction conditions were optimized by analyzing regression models. The predicted optimal process parameters for FAEE conversion are as follows: enzyme addition of 5.46 wt%, enzyme ratio of 1:2.23, alcohol–oil ratio of 13.79:1 mmol/g, reaction temperature of 60 °C, reaction time of 160 min, and ultrasonic power of 120 W. Under these optimized conditions, three validation experiments were carried out to take the average value, and the conversion rate of FAEE was 93.57 ± 1.17%, which was in good agreement with the predicted value. These results showed that the synergistic effect of the two enzymes accelerated the migration of acyl groups, verified the advantages of the dual enzyme as a catalyst, and provided theoretical support for the preparation of biodiesel by the dual enzyme system.

Graphical Abstract

本研究以高酸值废油为原料,在无溶剂体系中制备脂肪酸乙酯(FAEE)。该研究涉及添加两种具有不同底物特异性的酶,并伴有超声波辅助。考察了酶添加量(3-7 wt%)、酶比(3:1-1:3)、醇油比(5:1-25:1 mmol/g)、反应温度(30-70℃)、反应时间(30-210 min)、超声功率(0-150 W)对实验结果的影响。通过分析回归模型对反应条件进行优化。预测FAEE转化的最佳工艺参数为:酶添加量5.46 wt%,酶比1:2.23,醇油比13.79:1 mmol/g,反应温度60℃,反应时间160 min,超声功率120 W。在此优化条件下,进行3次验证实验取平均值,FAEE转化率为93.57±1.17%,与预测值吻合较好。这些结果表明,两种酶的协同作用加速了酰基的迁移,验证了双酶作为催化剂的优势,为双酶体系制备生物柴油提供了理论支持。图形抽象
{"title":"Ultrasound-Assisted Dual-Enzyme System for the Preparation of Fatty Acid Ethyl Esters","authors":"Yan Wang,&nbsp;Xiaohong Hao,&nbsp;Xiongzhi Da,&nbsp;Xiangsheng Zheng","doi":"10.1007/s10562-024-04908-3","DOIUrl":"10.1007/s10562-024-04908-3","url":null,"abstract":"<div><p>This study focuses on the preparation of fatty acid ethyl esters (FAEE) in a solvent-free system using high-acid-value waste oil as the raw material. The research involves the addition of two enzymes with different substrate specificities, accompanied by ultrasonic assistance. The investigation explores the impact of enzyme addition (3–7 wt%), enzyme ratio (3:1–1:3), alcohol–oil ratio (5:1–25:1 mmol/g), reaction temperature (30–70 °C), reaction time (30–210 min), and ultrasonic power (0–150 W) on the experimental outcomes. Reaction conditions were optimized by analyzing regression models. The predicted optimal process parameters for FAEE conversion are as follows: enzyme addition of 5.46 wt%, enzyme ratio of 1:2.23, alcohol–oil ratio of 13.79:1 mmol/g, reaction temperature of 60 °C, reaction time of 160 min, and ultrasonic power of 120 W. Under these optimized conditions, three validation experiments were carried out to take the average value, and the conversion rate of FAEE was 93.57 ± 1.17%, which was in good agreement with the predicted value. These results showed that the synergistic effect of the two enzymes accelerated the migration of acyl groups, verified the advantages of the dual enzyme as a catalyst, and provided theoretical support for the preparation of biodiesel by the dual enzyme system.</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":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142912962","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
Photocatalytic Applications of Cardanol-Derived meso-Metalloporphyrins Based g-C3N4 Nanocomposites 腰果酚类介金属卟啉基g-C3N4纳米复合材料的光催化应用
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04916-3
Malena Gomes Martins, Fernando Lima de Menezes, Tiago Melo Freire, Rafaelly Nascimento Araújo, Vitória de Paula Santos, Vivian Stephanie Ferreira Rodrigues, Leonardo Mapurunga de Menezes, Claudenilson da Silva Clemente, Giuseppe Mele, Diego Lomonaco, Pierre Basílio Almeida Fechine, Selma Elaine Mazzetto

Graphitic carbon nitride (g-C3N4) is a polymer conjugated composed of carbon and nitrogen atoms in a graphite-like structure. Despite its structure, its catalytic potential is limited due to its small surface area, abundance of electron pairs, and low UV absorption. Recent research has focused on synthesizing nanocomposites from g-C3N4 and meso-metalloporphyrins, which exhibit synergistic properties for photocatalysis through π-π interactions. This study aims to synthesize zinc (ZnP) and palladium (PdP) meso-metalloporphyrins from cardanol, a major constituent of cashew nut shell liquid (CNSL), to create g-C3N4 nanocomposites. These systems were characterized using UV-vis, FT-IR, NMR, TGA, and SEM, and applied to reduce 4-nitrophenol (4-NP) in wastewater to the less toxic 4-aminophenol (4-AP). The synthesis of g-C3N4 with PdP and ZnP produced new nanocomposites, g-C3N4/PdP and g-C3N4/ZnP, with yields of 43% and 16%, respectively. These materials demonstrated significant success in the photocatalytic reduction of 4-NP, highlighting the potential of renewable catalysts and promoting cleaner chemical processes, thereby reducing environmental impact.

Graphical abstract

石墨化氮化碳(g-C3N4)是一种由碳原子和氮原子组成的共轭聚合物,具有石墨状结构。尽管它的结构,它的催化潜力是有限的,由于它的小表面积,丰富的电子对,和低紫外线吸收。近年来的研究主要集中在以g-C3N4和介金属卟啉为原料合成纳米复合材料,通过π-π相互作用表现出光催化的协同特性。以腰果壳液(CNSL)的主要成分腰果酚为原料,合成锌(ZnP)和钯(PdP)介金属卟啉,制备g-C3N4纳米复合材料。这些体系通过UV-vis、FT-IR、NMR、TGA和SEM进行了表征,并应用于将废水中的4-硝基酚(4-NP)还原为毒性较小的4-氨基酚(4-AP)。用PdP和ZnP合成g-C3N4制备了g-C3N4/PdP和g-C3N4/ZnP纳米复合材料,产率分别为43%和16%。这些材料在光催化还原4-NP方面取得了重大成功,突出了可再生催化剂的潜力,促进了更清洁的化学过程,从而减少了对环境的影响。图形抽象
{"title":"Photocatalytic Applications of Cardanol-Derived meso-Metalloporphyrins Based g-C3N4 Nanocomposites","authors":"Malena Gomes Martins,&nbsp;Fernando Lima de Menezes,&nbsp;Tiago Melo Freire,&nbsp;Rafaelly Nascimento Araújo,&nbsp;Vitória de Paula Santos,&nbsp;Vivian Stephanie Ferreira Rodrigues,&nbsp;Leonardo Mapurunga de Menezes,&nbsp;Claudenilson da Silva Clemente,&nbsp;Giuseppe Mele,&nbsp;Diego Lomonaco,&nbsp;Pierre Basílio Almeida Fechine,&nbsp;Selma Elaine Mazzetto","doi":"10.1007/s10562-024-04916-3","DOIUrl":"10.1007/s10562-024-04916-3","url":null,"abstract":"<div><p>Graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) is a polymer conjugated composed of carbon and nitrogen atoms in a graphite-like structure. Despite its structure, its catalytic potential is limited due to its small surface area, abundance of electron pairs, and low UV absorption. Recent research has focused on synthesizing nanocomposites from g-C<sub>3</sub>N<sub>4</sub> and <i>meso</i>-metalloporphyrins, which exhibit synergistic properties for photocatalysis through π-π interactions. This study aims to synthesize zinc (ZnP) and palladium (PdP) <i>meso</i>-metalloporphyrins from cardanol, a major constituent of cashew nut shell liquid (CNSL), to create g-C<sub>3</sub>N<sub>4</sub> nanocomposites. These systems were characterized using UV-vis, FT-IR, NMR, TGA, and SEM, and applied to reduce 4-nitrophenol (4-NP) in wastewater to the less toxic 4-aminophenol (4-AP). The synthesis of g-C<sub>3</sub>N<sub>4</sub> with PdP and ZnP produced new nanocomposites, g-C<sub>3</sub>N<sub>4</sub>/PdP and g-C<sub>3</sub>N<sub>4</sub>/ZnP, with yields of 43% and 16%, respectively. These materials demonstrated significant success in the photocatalytic reduction of 4-NP, highlighting the potential of renewable catalysts and promoting cleaner chemical processes, thereby reducing environmental impact.</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":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142912964","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
Investigation of Catalytic Performance of γ-Bi2MoO6 Material on the Epoxidation of the Cyclohexene γ-Bi2MoO6材料对环己烯环氧化反应的催化性能研究
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04909-2
Lei Zhang, Zhihao Shu, Ji’E Tang, Xinmiao Wang, Bin Xie, Tiandi Tang

The development of efficient catalyst for the epoxidation of alkenes is crucial in industrial application. Herein, bismuth molybdate samples with different surface properties (BMO-x, x = A, B, and C) were synthesized via a hydrothermal method and tested in cyclohexene epoxidation. The BMO-A catalyst exhibited superior catalytic activity, achieving a 67.3% cyclohexene conversion with 83.6% epoxide selectivity, outperforming the BMO-B (17.4% conversion, 40.2% selectivity) and BMO-C (27.0% conversion, 59.1% selectivity) catalysts. This enhanced activity is attributed to BMO-A’s higher percentage of surface exchangeable oxygen, high surface Mo/Bi ratio, and optimal surface wettability. The high epoxidation performance of the BMO-A catalyst was attributed to its larger percentage of surface exchangeable oxygen, high surface Mo/Bi ratio, and suitable surface wettability. Specifically, the BMO-A with more exchangeable oxygen facilitated the adsorption of H2O2 molecules, and subsequent reaction with cyclohexene to yield epoxy-cyclohexane. The hydrophilic surface of BMO-A further enhanced H2O2 enrichment at the reaction interface. This work provides a new strategy for preparing highly active catalyst for the epoxidation of alkenes.

Graphical Abstract

开发高效的烯烃环氧化催化剂是烯烃环氧化工业应用的关键。本文通过水热法合成了具有不同表面性质(BMO-x, x = A, B, C)的钼酸铋样品,并在环己烯环氧化反应中进行了测试。BMO-A催化剂表现出优异的催化活性,环己烯转化率为67.3%,环氧化物选择性为83.6%,优于BMO-B(转化率17.4%,选择性40.2%)和BMO-C(转化率27.0%,选择性59.1%)催化剂。这种增强的活性归因于BMO-A具有较高的表面交换氧百分比、较高的表面Mo/Bi比和最佳的表面润湿性。BMO-A催化剂具有较高的表面交换氧率、较高的表面Mo/Bi比和适宜的表面润湿性,具有较高的环氧化性能。具体来说,BMO-A具有更多的交换氧,有利于H2O2分子的吸附,随后与环己烯反应生成环氧环己烷。BMO-A的亲水表面进一步增强了反应界面处H2O2的富集。本研究为烯烃环氧化反应制备高活性催化剂提供了新的思路。图形抽象
{"title":"Investigation of Catalytic Performance of γ-Bi2MoO6 Material on the Epoxidation of the Cyclohexene","authors":"Lei Zhang,&nbsp;Zhihao Shu,&nbsp;Ji’E Tang,&nbsp;Xinmiao Wang,&nbsp;Bin Xie,&nbsp;Tiandi Tang","doi":"10.1007/s10562-024-04909-2","DOIUrl":"10.1007/s10562-024-04909-2","url":null,"abstract":"<div><p>The development of efficient catalyst for the epoxidation of alkenes is crucial in industrial application. Herein, bismuth molybdate samples with different surface properties (BMO-<i>x</i>, <i>x</i> = A, B, and C) were synthesized <i>via</i> a hydrothermal method and tested in cyclohexene epoxidation. The BMO-A catalyst exhibited superior catalytic activity, achieving a 67.3% cyclohexene conversion with 83.6% epoxide selectivity, outperforming the BMO-B (17.4% conversion, 40.2% selectivity) and BMO-C (27.0% conversion, 59.1% selectivity) catalysts. This enhanced activity is attributed to BMO-A’s higher percentage of surface exchangeable oxygen, high surface Mo/Bi ratio, and optimal surface wettability. The high epoxidation performance of the BMO-A catalyst was attributed to its larger percentage of surface exchangeable oxygen, high surface Mo/Bi ratio, and suitable surface wettability. Specifically, the BMO-A with more exchangeable oxygen facilitated the adsorption of H<sub>2</sub>O<sub>2</sub> molecules, and subsequent reaction with cyclohexene to yield epoxy-cyclohexane. The hydrophilic surface of BMO-A further enhanced H<sub>2</sub>O<sub>2</sub> enrichment at the reaction interface. This work provides a new strategy for preparing highly active catalyst for the epoxidation of alkenes.</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":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142912934","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
Electrospun Fiber Membranes of Fe2O3/ZnO with High Photocatalytic Activity for Wastewater Treatment Application under Visible Light Irradiation 具有高光催化活性的Fe2O3/ZnO静电纺丝膜在可见光下处理废水中的应用
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04905-6
Qing Lin, Rui Zhang, Xiujuan Zhang, Shuang Li, Junhao Dai, Shuiping Li, Zhao Wang, Dong Liang, Hailuo Fu, Xiaojuan Zhang

Fe2O3/ZnO fiber membranes, characterized by their high specific surface area and expanded UV–Vis absorption spectrum, were successfully synthesized through a process of electrospinning followed by calcination. The diameters of Fe2O3/ZnO fibers are approximately 150 nm, and the specific surface areas of Fe2O3/ZnO fiber membranes are around 29 m2/g. XRD, SEM, and XPS results confirm the formation of a heterojunction between ZnO and α-Fe2O3. Compared with pure ZnO fiber membrane, the UV–Vis absorptions of the Fe2O3/ZnO fiber membranes are extended, and transient photocurrent intensities are significantly increased from 0.65 mA/cm2 to 0.86 mA/cm2. Free radical capture experiments further reveal the generation of abundant •OH radicals, which play a crucial role in enhancing the photocatalytic performance of these Fe2O3/ZnO fiber membranes. Optimization studies have determined that the optimal molar ratio of Fe to Zn is 8 mol% in the Fe2O3/ZnO heterojunction, which corresponds to a 45% improvement in photocatalytic degradation efficiency for MB. Furthermore, the remarkable cycling stability of the Fe2O3/ZnO fiber membranes demonstrate their substantial potential for photocatalytic dye wastewater treatment.

采用静电纺丝-煅烧法制备了Fe2O3/ZnO纤维膜,具有高比表面积和扩大紫外可见吸收光谱的特点。Fe2O3/ZnO纤维的直径约为150 nm, Fe2O3/ZnO纤维膜的比表面积约为29 m2/g。XRD、SEM和XPS结果证实ZnO与α-Fe2O3之间形成了异质结。与纯ZnO纤维膜相比,Fe2O3/ZnO纤维膜的UV-Vis吸收增强,瞬态光电流强度从0.65 mA/cm2显著提高到0.86 mA/cm2。自由基捕获实验进一步揭示了丰富的•OH自由基的产生,这对提高这些Fe2O3/ZnO纤维膜的光催化性能起着至关重要的作用。优化研究确定Fe2O3/ZnO异质结中Fe与Zn的最佳摩尔比为8 mol%,这相当于将MB的光催化降解效率提高45%。此外,Fe2O3/ZnO纤维膜具有显着的循环稳定性,表明其在光催化染料废水处理方面具有巨大的潜力。
{"title":"Electrospun Fiber Membranes of Fe2O3/ZnO with High Photocatalytic Activity for Wastewater Treatment Application under Visible Light Irradiation","authors":"Qing Lin,&nbsp;Rui Zhang,&nbsp;Xiujuan Zhang,&nbsp;Shuang Li,&nbsp;Junhao Dai,&nbsp;Shuiping Li,&nbsp;Zhao Wang,&nbsp;Dong Liang,&nbsp;Hailuo Fu,&nbsp;Xiaojuan Zhang","doi":"10.1007/s10562-024-04905-6","DOIUrl":"10.1007/s10562-024-04905-6","url":null,"abstract":"<div><p>Fe<sub>2</sub>O<sub>3</sub>/ZnO fiber membranes, characterized by their high specific surface area and expanded UV–Vis absorption spectrum, were successfully synthesized through a process of electrospinning followed by calcination. The diameters of Fe<sub>2</sub>O<sub>3</sub>/ZnO fibers are approximately 150 nm, and the specific surface areas of Fe<sub>2</sub>O<sub>3</sub>/ZnO fiber membranes are around 29 m<sup>2</sup>/g. XRD, SEM, and XPS results confirm the formation of a heterojunction between ZnO and α-Fe<sub>2</sub>O<sub>3</sub>. Compared with pure ZnO fiber membrane, the UV–Vis absorptions of the Fe<sub>2</sub>O<sub>3</sub>/ZnO fiber membranes are extended, and transient photocurrent intensities are significantly increased from 0.65 mA/cm<sup>2</sup> to 0.86 mA/cm<sup>2</sup>. Free radical capture experiments further reveal the generation of abundant •OH radicals, which play a crucial role in enhancing the photocatalytic performance of these Fe<sub>2</sub>O<sub>3</sub>/ZnO fiber membranes. Optimization studies have determined that the optimal molar ratio of Fe to Zn is 8 mol% in the Fe<sub>2</sub>O<sub>3</sub>/ZnO heterojunction, which corresponds to a 45% improvement in photocatalytic degradation efficiency for MB. Furthermore, the remarkable cycling stability of the Fe<sub>2</sub>O<sub>3</sub>/ZnO fiber membranes demonstrate their substantial potential for photocatalytic dye wastewater treatment.</p></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142912976","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
Photoreduction of Carbon Dioxide to Methane Employing Benzimidazole-Linked Microporous Conjugated Polymers Anchored on Dendritic Fibrous Nanosilic 利用树枝状纳米硅纤维锚定的苯并咪唑连接的微孔共轭聚合物将二氧化碳光还原为甲烷
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04918-1
Ruijie Xiao, Guirong Cao, Rui Qi

Capturing and transforming diluted CO2 into energy-rich fuels is a notable and increasingly interesting challenge in renewable energy research. This study successfully developed an enhanced form of silicon oxide with a unique exterior level and a SiO2/anatase phase interface. A base complex of Pd (II) and Cu (II) was created using a simple synthetic method, along with 3-chloropropyltriethoxysilane loaded on dendritic fibrous nanosilica (Cu-IL/DFNS and Pd-IL/DFNS). The use of DFNS provided numerous hydroxyl groups for the stable loading of Cu-IL and Pd-IL through chemical bonding interaction. Moreover, Cu-IL and Pd-IL were able to control the appropriate strand dimensions and offer active adsorption locations of metal groups, aiding in the chemical absorption of carbon dioxide. The DFNS composite’s topography and mesoporous structure remained consistent upon Cu-IL and Pd-IL loading, indicating the maintained crystalline form. The use of light-driven biomass valorisation has become a leading field for CO2 to CH4 photoreduction due to its sustainable characteristics. Photocatalytic CO2 reduction is a highly beneficial method to counteract the negative impacts of greenhouse gases and achieve carbon neutrality. The construction of active sites with specific designs that exhibit increased activity and selectivity for photoreduction is a significant challenge. The reduction of carbon dioxide is crucial in today’s era of petroleum refineries. The present paper showcases the initial application of a reusable nanocatalyst with outer magnetism for the efficient and specific light reduction of CO2 to CH4 under eco-friendly circumstances that employ earth-friendly reduction, ambient pressure, cool thermal condition, and sustainable dehydration reactants in a shorter duration. This method extends substantial advantages, incorporating substantial financial return and acceptance of functional groups. This investigation emphasizes the possibility of integrating 3D nanoparticle architecture with eco-friendly chemical processes to create highly efficient catalytic reactions for the targeted light reduction of CO2 to CH4.

Graphical Abstract

在可再生能源研究中,捕获并将稀释后的二氧化碳转化为富含能量的燃料是一项引人注目且日益有趣的挑战。该研究成功地开发了一种具有独特外部水平和SiO2/锐钛矿相界面的增强型氧化硅。用简单的方法合成了Pd (II)和Cu (II)的碱配合物,并将3-氯丙基三乙氧基硅烷负载在树枝状纤维纳米二氧化硅上(Cu- il /DFNS和Pd- il /DFNS)。DFNS的使用为Cu-IL和Pd-IL通过化学键相互作用的稳定负载提供了大量的羟基。此外,Cu-IL和Pd-IL能够控制适当的链尺寸,并提供金属基团的活性吸附位置,有助于二氧化碳的化学吸收。负载Cu-IL和Pd-IL后,DFNS复合材料的形貌和介孔结构保持一致,表明其晶体形态保持不变。由于其可持续的特性,使用光驱动生物质增值已成为CO2光还原为CH4的领先领域。光催化CO2还原是一种非常有益的方法,可以抵消温室气体的负面影响,实现碳中和。构建具有特定设计的活性位点,以增加光还原的活性和选择性是一个重大挑战。在今天的炼油厂时代,二氧化碳的减少是至关重要的。本论文展示了一种可重复使用的外磁纳米催化剂的初步应用,在环境友好的环境下,利用环境压力、低温条件和可持续的脱水反应物,在较短的时间内,将二氧化碳高效、特异地光还原为CH4。这种方法扩展了大量的优势,包括大量的财务回报和功能组的接受。这项研究强调了将3D纳米颗粒结构与环保化学工艺相结合的可能性,以创造高效的催化反应,将二氧化碳定向光还原为CH4。图形抽象
{"title":"Photoreduction of Carbon Dioxide to Methane Employing Benzimidazole-Linked Microporous Conjugated Polymers Anchored on Dendritic Fibrous Nanosilic","authors":"Ruijie Xiao,&nbsp;Guirong Cao,&nbsp;Rui Qi","doi":"10.1007/s10562-024-04918-1","DOIUrl":"10.1007/s10562-024-04918-1","url":null,"abstract":"<div><p>Capturing and transforming diluted CO<sub>2</sub> into energy-rich fuels is a notable and increasingly interesting challenge in renewable energy research. This study successfully developed an enhanced form of silicon oxide with a unique exterior level and a SiO<sub>2</sub>/anatase phase interface. A base complex of Pd (II) and Cu (II) was created using a simple synthetic method, along with 3-chloropropyltriethoxysilane loaded on dendritic fibrous nanosilica (Cu-IL/DFNS and Pd-IL/DFNS). The use of DFNS provided numerous hydroxyl groups for the stable loading of Cu-IL and Pd-IL through chemical bonding interaction. Moreover, Cu-IL and Pd-IL were able to control the appropriate strand dimensions and offer active adsorption locations of metal groups, aiding in the chemical absorption of carbon dioxide. The DFNS composite’s topography and mesoporous structure remained consistent upon Cu-IL and Pd-IL loading, indicating the maintained crystalline form. The use of light-driven biomass valorisation has become a leading field for CO<sub>2</sub> to CH<sub>4</sub> photoreduction due to its sustainable characteristics. Photocatalytic CO<sub>2</sub> reduction is a highly beneficial method to counteract the negative impacts of greenhouse gases and achieve carbon neutrality. The construction of active sites with specific designs that exhibit increased activity and selectivity for photoreduction is a significant challenge. The reduction of carbon dioxide is crucial in today’s era of petroleum refineries. The present paper showcases the initial application of a reusable nanocatalyst with outer magnetism for the efficient and specific light reduction of CO<sub>2</sub> to CH<sub>4</sub> under eco-friendly circumstances that employ earth-friendly reduction, ambient pressure, cool thermal condition, and sustainable dehydration reactants in a shorter duration. This method extends substantial advantages, incorporating substantial financial return and acceptance of functional groups. This investigation emphasizes the possibility of integrating 3D nanoparticle architecture with eco-friendly chemical processes to create highly efficient catalytic reactions for the targeted light reduction of CO<sub>2</sub> to CH<sub>4</sub>.</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":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142912965","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
Mo132-Ionic Liquid As An Effective Hybrid Catalyst For Selective Epoxidation of Different Alkenes with H2O2 mo132 -离子液体作为H2O2选择性环氧化烯烃的有效杂化催化剂
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04902-9
Mostafa Riahi Farsani, Bahram Yadollahi, Hamid Taghiyar, Ahmad Jamali Moghadam

A hybrid catalyst based on Mo132 as a Keplerate type polyoxometalate and MimAm as an ionic liquid was used as an effective catalyst for selective epoxidation of different alkenes with H2O2 as a green and safe oxidant. The effects of various parameters such as catalyst, oxidant amounts, reaction time, and temperature were also studied in selective epoxidation of cyclooctene. Moreover, under the optimal reaction conditions, the epoxidation of different alkenes was performed with 54–100% yields. Interestingly, this catalyst complies with the benefits of easy preparation, recovery, recycle, high catalytic activity, simplified workup, and flexible composition.

Graphical Abstract

以Mo132为Keplerate型多金属氧酸盐,MimAm为离子液体,以H2O2为绿色安全氧化剂,制备了一种高效的杂化催化剂,用于不同烯烃的选择性环氧化反应。考察了催化剂、氧化剂用量、反应时间、温度等参数对环烯选择性环氧化反应的影响。在最佳反应条件下,不同烯烃的环氧化反应收率为54% ~ 100%。有趣的是,该催化剂具有易于制备、回收、再循环、高催化活性、简化处理和灵活组成等优点。图形抽象
{"title":"Mo132-Ionic Liquid As An Effective Hybrid Catalyst For Selective Epoxidation of Different Alkenes with H2O2","authors":"Mostafa Riahi Farsani,&nbsp;Bahram Yadollahi,&nbsp;Hamid Taghiyar,&nbsp;Ahmad Jamali Moghadam","doi":"10.1007/s10562-024-04902-9","DOIUrl":"10.1007/s10562-024-04902-9","url":null,"abstract":"<div><p>A hybrid catalyst based on Mo132 as a Keplerate type polyoxometalate and MimAm as an ionic liquid was used as an effective catalyst for selective epoxidation of different alkenes with H<sub>2</sub>O<sub>2</sub> as a green and safe oxidant. The effects of various parameters such as catalyst, oxidant amounts, reaction time, and temperature were also studied in selective epoxidation of cyclooctene. Moreover, under the optimal reaction conditions, the epoxidation of different alkenes was performed with 54–100% yields. Interestingly, this catalyst complies with the benefits of easy preparation, recovery, recycle, high catalytic activity, simplified workup, and flexible composition.</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":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142913011","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
One-Pot Alkaline Earth and Alkali Metal Salts Assisted Conversion of Glucose to 5-Hydroxymethylfurfural Over Bifunctional SAPO_34 Molecular Sieve Using γ-Valerolactone/Water Solvent System 用γ-戊内酯/水溶剂体系在双功能SAPO_34分子筛上,碱土和碱金属盐辅助葡萄糖转化为5-羟甲基糠醛
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-01-03 DOI: 10.1007/s10562-024-04904-7
Farshad Bagherian Rostami, Reza Bagherian Rostami, Mohsen Abbasi Rostami, Aboozar Sadeghi, Mohammad Ranjkesh

5-Hydroxymethylfurfural known as a biomass-derived pivotal platform chemical is an important alternative for petroleum-based chemicals. However, its large-scale production faces serious barriers and limitation in terms of 5-Hydroxymethylfurfural yield and production cost. In the present work, dual structure directing agent SAPO_34 molecular sieve was prepared by hydrothermal method and XRD, SEM, XRF, BET and pyridine FTIR spectroscopy techniques were employed to characterize the synthesized catalyst. The Lewis/Bronsted SAPO_34 molecular sieve performance was evaluated in the conversion of glucose into 5-Hydroxymethylfurfural in γ-Valerolactone/water solvent system. The effects of alkaline earth and alkali metal salts were also studied. Promising results were obtained which could optimize the 5-Hydroxymethylfurfural yield up to 92%. The ascending overall 5-Hydroxymethylfurfural selectivity trend suggests that the formation of 5-hydroxymethylfurfural is in dominant position at the expense of glucose until 5-HMF yield peak values are obtained. The introduction of metal salts to the reaction medium was beneficial to the reaction efficiency and it was shown that the cations rather than the anions play the main role in the promotion of the conversion. Furthermore, salts containing cations of smaller ionic radius and higher charge density demonstrating superior performance. The analysis of reaction kinetic revealed that glucose conversion activation energy decreased by 5.8 kJ/mole with the addition of MgCl2 to the reaction medium. Finally, the tests to evaluate the catalyst’s recyclability were conducted both with and without the addition of salt.

Graphical Abstract

5-羟甲基糠醛是一种生物质衍生的关键平台化学品,是石油基化学品的重要替代品。但其规模化生产在5-羟甲基糠醛收率和生产成本方面存在严重的障碍和限制。本文采用水热法制备了双结构定向剂SAPO_34分子筛,并采用XRD、SEM、XRF、BET和吡啶FTIR等技术对合成的催化剂进行了表征。研究了γ-戊内酯/水溶剂体系中葡萄糖转化为5-羟甲基糠醛的Lewis/Bronsted SAPO_34分子筛性能。还研究了碱土和碱金属盐的作用。结果表明,5-羟甲基糠醛的收率可达92%。5-羟甲基糠醛选择性总体呈上升趋势,表明在5-HMF产率达到峰值之前,5-羟甲基糠醛的形成以葡萄糖为代价处于主导地位。在反应介质中引入金属盐有利于提高反应效率,表明促进转化的主要是阳离子而不是阴离子。此外,含有离子半径小、电荷密度高的阳离子的盐表现出优异的性能。反应动力学分析表明,在反应介质中加入MgCl2使葡萄糖转化活化能降低了5.8 kJ/mol。最后,在加盐和不加盐的情况下,对催化剂的可回收性进行了评价。图形抽象
{"title":"One-Pot Alkaline Earth and Alkali Metal Salts Assisted Conversion of Glucose to 5-Hydroxymethylfurfural Over Bifunctional SAPO_34 Molecular Sieve Using γ-Valerolactone/Water Solvent System","authors":"Farshad Bagherian Rostami,&nbsp;Reza Bagherian Rostami,&nbsp;Mohsen Abbasi Rostami,&nbsp;Aboozar Sadeghi,&nbsp;Mohammad Ranjkesh","doi":"10.1007/s10562-024-04904-7","DOIUrl":"10.1007/s10562-024-04904-7","url":null,"abstract":"<div><p>5-Hydroxymethylfurfural known as a biomass-derived pivotal platform chemical is an important alternative for petroleum-based chemicals. However, its large-scale production faces serious barriers and limitation in terms of 5-Hydroxymethylfurfural yield and production cost. In the present work, dual structure directing agent SAPO_34 molecular sieve was prepared by hydrothermal method and XRD, SEM, XRF, BET and pyridine FTIR spectroscopy techniques were employed to characterize the synthesized catalyst. The Lewis/Bronsted SAPO_34 molecular sieve performance was evaluated in the conversion of glucose into 5-Hydroxymethylfurfural in γ-Valerolactone/water solvent system. The effects of alkaline earth and alkali metal salts were also studied. Promising results were obtained which could optimize the 5-Hydroxymethylfurfural yield up to 92%. The ascending overall 5-Hydroxymethylfurfural selectivity trend suggests that the formation of 5-hydroxymethylfurfural is in dominant position at the expense of glucose until 5-HMF yield peak values are obtained. The introduction of metal salts to the reaction medium was beneficial to the reaction efficiency and it was shown that the cations rather than the anions play the main role in the promotion of the conversion. Furthermore, salts containing cations of smaller ionic radius and higher charge density demonstrating superior performance. The analysis of reaction kinetic revealed that glucose conversion activation energy decreased by 5.8 kJ/mole with the addition of MgCl<sub>2</sub> to the reaction medium. Finally, the tests to evaluate the catalyst’s recyclability were conducted both with and without the addition of salt.</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":"155 2","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142912932","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
期刊
Catalysis Letters
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1