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NiCoFe-Based Metal-Organic Framework Nanosheets on Ni Foam for High-Efficiency Electrochemical Water Splitting 镍泡沫上镍铁基金属有机骨架纳米片的高效电化学水分解
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-28 DOI: 10.1007/s10562-025-05023-7
Anlan Hu, Hanbing Li, Shijun Ran, Jie Huang, Muhammad Qasim, Kejian Lu, Kunpeng Ding, Jie Liu, Yupeng Qiao, Maochang Liu
{"title":"NiCoFe-Based Metal-Organic Framework Nanosheets on Ni Foam for High-Efficiency Electrochemical Water Splitting","authors":"Anlan Hu,&nbsp;Hanbing Li,&nbsp;Shijun Ran,&nbsp;Jie Huang,&nbsp;Muhammad Qasim,&nbsp;Kejian Lu,&nbsp;Kunpeng Ding,&nbsp;Jie Liu,&nbsp;Yupeng Qiao,&nbsp;Maochang Liu","doi":"10.1007/s10562-025-05023-7","DOIUrl":"10.1007/s10562-025-05023-7","url":null,"abstract":"<div><p>\u0000 We report the synthesis of a ternary transition metal-based metal-organic framework (MOF) material, NiCoFe-MIL53, using a one-step solvothermal method with nickel foam (NF) as a conductive substrate. The resulting composite, NiCoFe-MIL53/NF, exhibits high activity and excellent stability for electrocatalytic water splitting. It is found that incorporation of cobalt not only enhances the electrical conductivity and intrinsic catalytic activity of the catalyst, but also influences the morphology of the synthesized products. This morphological transformation increases the contact area between the electrocatalyst and the electrolyte solution, leading to an improved electrocatalytic performance. Notably, the optimized composition of NiCoFe-MIL53 with a proper mass ratio of Ni/Co/Fe requires the lowest overpotential of 206 mV at 10 mA cm<sup>− 2</sup> and a Tafel slope of 21.09 mV dec<sup>− 1</sup> for oxygen evolution reaction in alkaline aqueous solution (1 M KOH). Moreover, this composite also shows excellent electrocatalytic performance for both cathodic and anodic reactions during overall water splitting, achieving a current density of 10 mA cm<sup>− 2</sup> at an applied potential of 1.61 V. This work highlights the potential of noble-metal-free MOF-based materials as dual-functional catalysts for highly active and stable electrocatalytic water splitting.</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 6","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143879722","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
Penta-SiAsP Monolayer: A Highly Stable Pentagonal Ternary Material with Photocatalytic Potential for Overall Water Splitting 5 - siasp单层:一种具有光催化全水分解潜力的高度稳定的五边形三元材料
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-28 DOI: 10.1007/s10562-025-05015-7
Chenghao Yang, Yanqing Shen, Kexin Wang, Xiangqian Jiang, Long Pang, E. Peng, Zhongxiang Zhou
{"title":"Penta-SiAsP Monolayer: A Highly Stable Pentagonal Ternary Material with Photocatalytic Potential for Overall Water Splitting","authors":"Chenghao Yang,&nbsp;Yanqing Shen,&nbsp;Kexin Wang,&nbsp;Xiangqian Jiang,&nbsp;Long Pang,&nbsp;E. Peng,&nbsp;Zhongxiang Zhou","doi":"10.1007/s10562-025-05015-7","DOIUrl":"10.1007/s10562-025-05015-7","url":null,"abstract":"<div><p>Currently, photocatalysts that can effectively promote overall water splitting and regulate hydrogen or oxygen release reactions using certain means remain a research hotspot. Based on first principles calculations, we theoretically predict a two-dimensional material called penta-SiAsP with a pentagonal structure. The phonon spectrum, formation energy, binding energy, and ab initio molecular dynamics calculations demonstrate that penta-SiAsP has stability. Under a certain range of electric field applied, the bandgap can still remain unchanged. Even under a certain biaxial strain, penta-SiAsP can still meet the requirements for overall water splitting in different pH ranges with respect to the band edge. Besides, tensile strain can effectively improve the light absorption performance of penta-SiAsP. Under pH 0 and pH 14 conditions, penta-SiAsP can spontaneously undergo photocatalytic water splitting. When pH 7, additional voltages of 0.79 and 0.76 V are required for hydrogen and oxygen evolution reactions. Penta-SiAsP exhibits resistance to photoinduced corrosion. The products of hydrogen and oxygen can be quickly separated from the photocatalyst. This study predicts a novel two-dimensional material with a ternary pentagonal structure and finds that it has potential for application in the field of photocatalysis, further expanding the research field of the pentagonal structured two-dimensional material family.</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 6","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143879723","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
Visible Light Photocatalysis: Efficient S-Scheme γ-Bi2O3/BiOBr Photocatalyst for Phenol Degradation 可见光催化:高效S-Scheme γ-Bi2O3/BiOBr光催化剂降解苯酚
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-24 DOI: 10.1007/s10562-025-05029-1
Zekui Zhou, Yong Li, Fenrong Liu
{"title":"Visible Light Photocatalysis: Efficient S-Scheme γ-Bi2O3/BiOBr Photocatalyst for Phenol Degradation","authors":"Zekui Zhou,&nbsp;Yong Li,&nbsp;Fenrong Liu","doi":"10.1007/s10562-025-05029-1","DOIUrl":"10.1007/s10562-025-05029-1","url":null,"abstract":"<div><p>The development of heterostructures with stabilized heterogeneous structures is crucial for the improvement of photocatalytic activity and practical applications. In this study, a S-type heterojunction of γ-Bi<sub>2</sub>O<sub>3</sub>/BiOBr was synthesized by a simple hydrothermal method. Under simulated sunlight, the degradation ratio of phenol can attain nearly 91.75% for 17%-γ-Bi<sub>2</sub>O<sub>3</sub>/BiOBr heterojunction after 120 min, while only 2.8% and 52.86% for pure γ-Bi<sub>2</sub>O<sub>3</sub> and BiOBr, respectively. Meanwhile, its first-order reaction rate is 3.46 and 22.81 times more than those of pure BiOBr and γ-Bi<sub>2</sub>O<sub>3</sub>, respectively. In addition, the 17%-γ-Bi<sub>2</sub>O<sub>3</sub>/BiOBr heterojunction exhibits the excellent cycle stability, as its phenol degradation ratio can retain nearly 86% after five cycle experiments. The heterojunction was analyzed as an S-type heterojunction based on XPS, EPR and free radical trapping experiments. The performance enhancement of the catalyst is thus due to the formation of an S-type heterojunction, which reduces the recombination rate of photogenerated electrons and photogenerated holes and promotes the formation of active species, thus dramatically increasing the efficiency of photocatalytic degradation of phenol.</p></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 5","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143865413","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
Solid Lewis Acids with Sn Catalyzing Fructose into Methyl Lactate 含锡固体路易斯酸催化果糖生成乳酸甲酯
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-24 DOI: 10.1007/s10562-025-05026-4
An Du, Qingling Zhu, Xue Wu, Runming Hao, Ke Wang, Sijia Liu, Yang Wang
{"title":"Solid Lewis Acids with Sn Catalyzing Fructose into Methyl Lactate","authors":"An Du,&nbsp;Qingling Zhu,&nbsp;Xue Wu,&nbsp;Runming Hao,&nbsp;Ke Wang,&nbsp;Sijia Liu,&nbsp;Yang Wang","doi":"10.1007/s10562-025-05026-4","DOIUrl":"10.1007/s10562-025-05026-4","url":null,"abstract":"<div><p>With the increasing demand of lactic acid (LA), a highly value-added platform chemical, catalytic conversion of biomass to produce LA and its ester is more economical and efficient relative to the fermentative route. We describe here a catalytic process for the formation of methyl lactate (ML) directly from fructose, and ML can be easily hydrolyzed to LA. A series of solid Lewis acids with Sn as active sites were prepared via the pyrolyzing coordinated polymer (PCP) method, converting fructose into ML in methanol. The results of XRD, SEM, ICP-MS, XPS, BET, NH<sub>3</sub>-TPD and Py-IR show that our customized catalysts are microporous-mesoporous materials and their acidities are strong; the Sn<sub>3</sub>-CN catalyst with an optimal Sn loading of 6.39 wt% is rich in Lewis acidic sites and contains almost no Brønsted acidic sites. The catalytic evaluation showed that Sn<sub>3</sub>-CN catalyst completely converted fructose for 20 h at 160 °C, and the yield of ML was 52%. In the repeated use of Sn<sub>3</sub>-CN, ML selectivity remained at about 52% after 6 cycles, and fructose conversion decreased by about 10%, indicating that it had the promising stability.</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 5","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143871435","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
Preparation of Ferric Oxide/Titanium Silicalite Catalyst for Synergistic Adsorption-Persulfate Oxidation Degradation of Tetracycline Hydrochloride 氧化铁/硅酸钛协同吸附-过硫酸盐氧化降解盐酸四环素催化剂的制备
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-24 DOI: 10.1007/s10562-025-05031-7
Dongxue Zhou, Yijie Liu, Boyuan Sun, Jiahui Luo, Haiyuan Jia, Jinlian Li, Jianjun Song
{"title":"Preparation of Ferric Oxide/Titanium Silicalite Catalyst for Synergistic Adsorption-Persulfate Oxidation Degradation of Tetracycline Hydrochloride","authors":"Dongxue Zhou,&nbsp;Yijie Liu,&nbsp;Boyuan Sun,&nbsp;Jiahui Luo,&nbsp;Haiyuan Jia,&nbsp;Jinlian Li,&nbsp;Jianjun Song","doi":"10.1007/s10562-025-05031-7","DOIUrl":"10.1007/s10562-025-05031-7","url":null,"abstract":"<div><p>The development of a sustainable and highly efficient catalyst for advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) activation shows great potential for effectively degrading organic pollutants. This study focused on the development of a ferric oxide/titanium silicalite (Fe<sub>2</sub>O<sub>3</sub>/TS-1) to activate PMS to degrade tetracycline hydrochloride (TC). The optimized 14% Fe<sub>2</sub>O<sub>3</sub>/TS-1 achieves the TC removal efficiency of 99.2% within 1 h. It mainly results from the adsorption-degradation synergy of Fe<sub>2</sub>O<sub>3</sub>/TS-1, where TS-1 has a strong adsorption ability for TC and Fe<sub>2</sub>O<sub>3</sub> provides an abundance of active sites for the generation of free radicals by activating PMS. These techniques indicate the involvement of both radical species (SO<sub>4</sub><sup>⋅−</sup>, ⋅OH and O<sub>2</sub><sup>⋅−</sup>) and non-radical species (<sup>1</sup>O<sub>2</sub>) in the process. Notably, O<sub>2</sub><sup>⋅−</sup> emerged as a pivotal player in the degradation of TC. The effect of coexisting anions (Cl<sup>−</sup>, NO<sub>3</sub><sup>−</sup>, SO<sub>4</sub><sup>2−</sup> and HCO<sub>3</sub><sup>−</sup>) confirms that Fe<sub>2</sub>O<sub>3</sub>/TS-1 is still effective in complex water. Three degradation pathways are confirmed by liquid chromatography-mass spectrometry (LC–MS). Recycling experiments and toxicity evaluation experiments show that the Fe<sub>2</sub>O<sub>3</sub>/TS-1 composite catalyst is stable and efficient, and the leaching concentration of iron is much lower than that in the normal range. This study shows the application prospect of the Fe<sub>2</sub>O<sub>3</sub>/TS-1 + PMS system in the degradation of refractory organic pollutants.</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 5","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143865412","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 Hydrothermal Synthesis of a Dual-Metal-Modified CuMn-ZSM-5/SAPO-34 Zeolite with Excellent MTO Catalytic Performance 具有优异MTO催化性能的双金属改性CuMn-ZSM-5/SAPO-34沸石的一锅水热合成
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-23 DOI: 10.1007/s10562-025-05022-8
Wenjie Yao, Lei Chen, Yinzhong Wang, Gang Yang
{"title":"One-Pot Hydrothermal Synthesis of a Dual-Metal-Modified CuMn-ZSM-5/SAPO-34 Zeolite with Excellent MTO Catalytic Performance","authors":"Wenjie Yao,&nbsp;Lei Chen,&nbsp;Yinzhong Wang,&nbsp;Gang Yang","doi":"10.1007/s10562-025-05022-8","DOIUrl":"10.1007/s10562-025-05022-8","url":null,"abstract":"<div><p>The composite molecular sieve catalysts with long reaction times were successfully synthesized by introducing Cu<sup>2+</sup>/Mn<sup>2+</sup> and ZSM-5 into the initial gel. The catalysts were characterized with XRD, SEM and NH<sub>3</sub>-TPD, and further investigated through the methanol-to-olefin reactions. The results showed that the addition of Cu<sup>2+</sup> caused the crystallinity of ZSM-5/SAPO-34 (Z-S) to increase significantly, but with addition of Mn<sup>2+</sup>, the crystallinity gradually decreased. With the increase of the Mn<sup>2+</sup>/Cu<sup>2+</sup> ratio, the desorption summits of the weak and strong acid sites gradually increased, but the weak acid centres gradually dominated, which is herein thought helped reducing formation of the coke. The designed Cu<sub>0.05</sub>-Mn<sub>0.05</sub>/Z-S samples showed beneficial catalytic performances with a lifetime of 1500 min, a 1.5-fold increase compared with the Cu<sub>0.05</sub>/Z-S, while their selectivities remained exceeding 89%.</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 5","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10562-025-05022-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fabrication of CuSe/ZnO Heterostructure Photocatalyst for Effective Photocatalytic Degradation of Carcinogenic Dye Pollutants CuSe/ZnO异质结构光催化剂的制备及其对致癌染料污染物的有效光催化降解
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-22 DOI: 10.1007/s10562-025-05033-5
Bilal Ahmad Bhat, Nimisha Jadon
{"title":"Fabrication of CuSe/ZnO Heterostructure Photocatalyst for Effective Photocatalytic Degradation of Carcinogenic Dye Pollutants","authors":"Bilal Ahmad Bhat,&nbsp;Nimisha Jadon","doi":"10.1007/s10562-025-05033-5","DOIUrl":"10.1007/s10562-025-05033-5","url":null,"abstract":"<div><p>It is essential to remove harmful carcinogenic dyes from the environment because even minute quantities of these contaminants can have a negative influence on ecosystems. One possible method for removing organic and inorganic contaminants from wastewater is heterogeneous photocatalysis. Hence, in this work, we have successfully synthesized CuSe, ZnO, and their heterostructure nanocomposite by utilizing a simple and cost-effective hydrothermal method. A range of characterization techniques, including XRD, XPS, FT-IR, SEM/EDS and UV-Vis spectroscopy analysis were employed to further understand the structure, morphology, composition and optical characteristics of the synthesized samples. The band gap energy for CuSe, ZnO, and CuSe/ZnO samples were obtained to be 2.14, 2.85, and 2.36 eV, respectively. The synthesized nanocomposite was used to test the photocatalytic degradation of two model dye pollutants Crystal violet and Rose bengal as a function of optimized operational parameters viz., dye concentration (15 mg/L for crystal violet and 10 mg/L for rose bengal), catalyst dose (50 mg), illumination time (125 min) and pH (9 for crystal violet and 6 for rose bengal). The findings of this study demonstrated that CuSe/ZnO heterostructure nanocomposite has shown excellent photocatalytic dye degradation performance. At optimized parameters, the degradation efficiency for crystal violet and rose bengal dyes was achieved to be 94.13% and 90.86%, respectively. The photocatalytic degradation rate was favored by pseudo first order Langmuir-Hinshelwood model with rate constants (k) of 0.018 min<sup>− 1</sup> and 0.017 min<sup>− 1</sup> for crystal violet and rose bengal, respectively.</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 5","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861262","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
Optimization of the Pore Structure of Spherical Alumina by Crosslinking Polymerization Technology 用交联聚合技术优化球形氧化铝的孔隙结构
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-22 DOI: 10.1007/s10562-025-05030-8
Jiale Li, Xingye Lin, Guandong Wu, Xijia Sun, Yufei He, Dianqing Li
{"title":"Optimization of the Pore Structure of Spherical Alumina by Crosslinking Polymerization Technology","authors":"Jiale Li,&nbsp;Xingye Lin,&nbsp;Guandong Wu,&nbsp;Xijia Sun,&nbsp;Yufei He,&nbsp;Dianqing Li","doi":"10.1007/s10562-025-05030-8","DOIUrl":"10.1007/s10562-025-05030-8","url":null,"abstract":"<div><p>It is crucial to enlarge the pore size of spherical alumina while maintaining its high mechanical strength. In this work, acrylamide, maleimide and phenol were introduced as cross-linker into Al sol to prepare spherical alumina supports by the oil-drop method. By conducting crosslinking polymerization reactions using these cross-linkers with formaldehyde, the consumption of formaldehyde reduces its evaporation and thereby minimizes the disruption to the pore structure of the spherical alumina prepared by the oil-drop method. As a result, the pore structure of the spherical alumina is optimized from wedge-shaped pores to interconnected pores, with the proportion of pores in the range of 25–40 nm increasing by ~ 10% while maintaining strength exceed 60 N/P. This pore structure optimization effectively alleviates the reduction in catalytic activity caused by mass transfer limitations, the H<sub>2</sub>O<sub>2</sub> productivity of the Pd/Al<sub>2</sub>O<sub>3</sub>-PH-3% (3% phenol as cross-linker) catalyst increased by 9.3% compared to that of Pd/Al<sub>2</sub>O<sub>3</sub> without cross-linker.</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 5","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861263","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
Dynamic Acid Synergy in Y-Embedded Hβ Zeolite: Structural Tailoring and Acid Cooperativity for Enhanced Friedel-Crafts Acylation Towards 2-Ethylanthraquinone Y 嵌入式 Hβ 沸石中的动态酸协同作用:结构裁剪和酸协同作用可增强对 2-乙基蒽醌的 Friedel-Crafts 酰化反应
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-21 DOI: 10.1007/s10562-025-05027-3
Qingle Zhao, Sai Geng, Jialuo Yin, Dazhuang Gu, Bolin Zhao, Anyang Shi, Jingyi Lao, Zhiping Wang, Hailong Yu, Yue Liu, Huihui Wang, Shiwei Liu
{"title":"Dynamic Acid Synergy in Y-Embedded Hβ Zeolite: Structural Tailoring and Acid Cooperativity for Enhanced Friedel-Crafts Acylation Towards 2-Ethylanthraquinone","authors":"Qingle Zhao,&nbsp;Sai Geng,&nbsp;Jialuo Yin,&nbsp;Dazhuang Gu,&nbsp;Bolin Zhao,&nbsp;Anyang Shi,&nbsp;Jingyi Lao,&nbsp;Zhiping Wang,&nbsp;Hailong Yu,&nbsp;Yue Liu,&nbsp;Huihui Wang,&nbsp;Shiwei Liu","doi":"10.1007/s10562-025-05027-3","DOIUrl":"10.1007/s10562-025-05027-3","url":null,"abstract":"<div><p>To address the bottleneck of insufficient catalytic activity at single acidic sites in traditional Friedel-Crafts acylation reactions, this study innovatively proposes a novel synergistic catalytic strategy combining Lewis and Brønsted acids. A Y-Hβ catalyst with dual-acid functionality and hierarchical pore structure was successfully constructed by precisely introducing yttrium ions (Y<sup>3+</sup>) into the Hβ zeolite framework through an equal-volume impregnation method. Structural characterization confirms that Y<sup>3+</sup> is anchored in the framework as [YO<sub>4</sub>] tetrahedra, establishing strong Lewis acid sites while maintaining the structural integrity of Hβ zeolite. Mechanistic studies reveal that Y<sup>3+</sup> promotes C = O bond cleavage in anhydride molecules through adsorption polarization to generate C<sup>+</sup> intermediates, while simultaneously enhancing the proton acidity of adjacent Brønsted acid sites via electronic induction effects. Under Lewis acid regulation, neighboring Si-OH-Al sites precisely donate protons to the α-position of anthraquinone, forming C<sub>10</sub>H<sub>7</sub><sup>+</sup> intermediates. The synergistic cooperation between dual acids reduces the acylation reaction energy barrier to 32.8 kcal/mol (a 24.1 kcal/mol reduction compared to Hβ zeolite), significantly accelerating reaction kinetics. Under optimized conditions (250 °C, 5 h), the reaction achieves 82.6% conversion and 80.6% selectivity, demonstrating 50.6% improvement in catalytic efficiency over Hβ zeolite. Regeneration tests verify that the Y-Hβ catalyst maintains over 90% initial activity after 5 cycles, attributed to the high stability of Y-O-Si bonds and exceptional anti-coking performance, highlighting its promising industrial application potential.</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 5","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143856663","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
Study on Deep Dechlorination and Reaction Mechanism of Oil on Zn–Al Layered Bimetallic Oxides ZnAl 层状双金属氧化物上石油的深度脱氯及反应机理研究
IF 2.3 4区 化学
Catalysis Letters Pub Date : 2025-04-21 DOI: 10.1007/s10562-025-05019-3
Qing Sun, Bingtian Huang, Liancheng Bing, Dezhi Han, Guangjian Wang, Fang Wang
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