Applied Catalysis A: General最新文献

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Influence of pretreatment condition of amorphous-type Cu-ZrO2 catalyst on direct ethyl acetate synthesis from ethanol 非晶型Cu-ZrO2催化剂预处理条件对乙醇直接合成乙酸乙酯的影响
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-25 DOI: 10.1016/j.apcata.2025.120598
Takashi Yamamoto, Taketo Tone, Hirotaka Mine
{"title":"Influence of pretreatment condition of amorphous-type Cu-ZrO2 catalyst on direct ethyl acetate synthesis from ethanol","authors":"Takashi Yamamoto,&nbsp;Taketo Tone,&nbsp;Hirotaka Mine","doi":"10.1016/j.apcata.2025.120598","DOIUrl":"10.1016/j.apcata.2025.120598","url":null,"abstract":"<div><div>Amorphous ZrO<sub>2</sub>-supported copper catalysts promote direct ethanol conversion into ethyl acetate with high yield and high selectivity. Regarding the pretreatment procedure prior to conducting activity tests, effects of reduction treatment with hydrogen, treatment temperature, and hydrogen-exposure procedure on catalyst performance were investigated. The local and/or bulk structural characterization of each catalyst were also carried out by XRD, XANES/EXAFS, XPS and STEM techniques. The optimal pretreatment conditions were heating from room temperature to 573 K under hydrogen gas flow, which resulted in an ethyl acetate/by-products ratio more than twice that previously reported by us. Appropriate pretreatment is the reduction treatment under mild conditions, which increases the amount of small metallic copper species. Crystallization of the amorphous ZrO₂ phase by inappropriate pretreatment procedures decreased the selectivity for ethyl acetate formation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120598"},"PeriodicalIF":4.8,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156023","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Synergistic dehydrogenation-acid site interactions in CoOx@HZSM-5 for efficient n-butane catalytic cracking CoOx@HZSM-5中协同脱氢-酸位点相互作用对高效正丁烷催化裂化的影响
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-25 DOI: 10.1016/j.apcata.2025.120602
Yangping Lv , Shanlei Han , Zhaoshuo Ge , Yi Dai , Lixia Bao , Daxin Shi , Qi Liu , Qin Wu , Kangcheng Chen , Guiyuan Jiang , Hansheng Li , Yaoyuan Zhang
{"title":"Synergistic dehydrogenation-acid site interactions in CoOx@HZSM-5 for efficient n-butane catalytic cracking","authors":"Yangping Lv ,&nbsp;Shanlei Han ,&nbsp;Zhaoshuo Ge ,&nbsp;Yi Dai ,&nbsp;Lixia Bao ,&nbsp;Daxin Shi ,&nbsp;Qi Liu ,&nbsp;Qin Wu ,&nbsp;Kangcheng Chen ,&nbsp;Guiyuan Jiang ,&nbsp;Hansheng Li ,&nbsp;Yaoyuan Zhang","doi":"10.1016/j.apcata.2025.120602","DOIUrl":"10.1016/j.apcata.2025.120602","url":null,"abstract":"<div><div>The efficient conversion of light alkanes into high-value-added products is crucial for achieving a carbon-neutral society. Catalytic cracking of light alkanes has emerged as a promising alternative to conventional steam cracking for light olefins production and has garnered significant attention. Herein, we designed bifunctional CoO<sub>x</sub>@HZSM-5 catalysts integrating dehydrogenation and cracking active sites. The effects of cobalt loading and Si/Al ratio on the catalytic performance of n-butane catalytic cracking were systematically investigated over CoO<sub>x</sub>@HZSM-5, and the structure-activity relationship and reaction pathway were carefully established. A clear volcano-type relationship between the n-butane conversion/yield of ethene and propene and Co content was identified, and 1 %CoO<sub>x</sub>@HZSM-5(Si/Al=91) exhibits the highest catalytic performance, while the catalytic activity increases with the decrease of Si/Al ratio. It is demonstrated the introduction of cobalt species into HZSM-5 contributes to increasing the dehydrogenation rate of n-butane and facilitating the formation of butene, a more reactive intermediate, thereby improving the catalytic activity. Structure-activity analysis indicates that the increased density of Lewis and Brønsted acid sites enhances the yield of ethene and propene, primarily owing to the improved conversion of n-butane, while the ratio of B/L governs the dehydrogenation-to-cracking rate. Furthermore, butene was identified as a primary coke precursor in the course of n-butane catalytic cracking. The obtained knowledge of tuning the catalytic performance and coke formation facilitates the development of efficient bifunctional catalysts, and advances the understanding of synergetic effects in heterogeneous catalysis.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120602"},"PeriodicalIF":4.8,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217381","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
In situ Raman spectroscopy studies of single-atom catalysis 单原子催化的原位拉曼光谱研究
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-24 DOI: 10.1016/j.apcata.2025.120600
Mulin Li , Yifei Wang , Hua Zhang , Zechao Zhuang , Jian-Feng Li
{"title":"In situ Raman spectroscopy studies of single-atom catalysis","authors":"Mulin Li ,&nbsp;Yifei Wang ,&nbsp;Hua Zhang ,&nbsp;Zechao Zhuang ,&nbsp;Jian-Feng Li","doi":"10.1016/j.apcata.2025.120600","DOIUrl":"10.1016/j.apcata.2025.120600","url":null,"abstract":"<div><div><em>In situ</em> Raman spectroscopy enables real-time identification of key reaction intermediates and pathways in single-atom catalysis. This Perspective highlights recent methodological advances and mechanistic insights achieved through its application in electrocatalysis and organocatalysis over single-atom catalysts (SACs). We discuss the strengths and limitations of conventional and surface-enhanced Raman approaches in SACs’ mechanistic studies, and outline emerging opportunities for probing catalytic processes at the single-atom limit. We hope this summary will advance insights into single-atom catalysis and promote the rational design of SACs for real-world applications.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120600"},"PeriodicalIF":4.8,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156008","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
CO2 capture and selective hydrogenation to CO over Ag-K co-loaded Al2O3 under simulated realistic conditions 模拟真实条件下Ag-K共载Al2O3上CO2捕集和选择性加氢成CO
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-24 DOI: 10.1016/j.apcata.2025.120599
Soma Shukuya , Norikazu Namiki , Zen Maeno
{"title":"CO2 capture and selective hydrogenation to CO over Ag-K co-loaded Al2O3 under simulated realistic conditions","authors":"Soma Shukuya ,&nbsp;Norikazu Namiki ,&nbsp;Zen Maeno","doi":"10.1016/j.apcata.2025.120599","DOIUrl":"10.1016/j.apcata.2025.120599","url":null,"abstract":"<div><div>CO<sub>2</sub> capture and reduction with H<sub>2</sub> (CCR) to CO over dual-functional materials (DFMs) with CO<sub>2</sub> chemisorption and hydrogenation abilities have attracted attention as a promising approach to utilize low-concentration CO<sub>2</sub> in exhaust gases. However, the reported DFMs suffer from the requirement of high reaction temperatures, deactivation by O<sub>2</sub> in simulated exhaust gases, and the use of platinum group metal elements. Recently, we found that Ag-K-based DFMs exhibited low-temperature activity in the CCR for selective CO formation and good compatibility with O<sub>2</sub> in the CO<sub>2</sub> capture step. In this study, the screening of metal oxide supports and metal loading amounts of Ag-K-based DFMs were investigated during CCR in the presence of O<sub>2</sub> at 350 °C. The Al<sub>2</sub>O<sub>3</sub>-supported Ag-K DFMs with 1 and 8 wt% loading of Ag and K (Ag(1)K(8)/Al<sub>2</sub>O<sub>3</sub>), respectively, were the best among the tested DFMs. Using the optimized Ag-K/Al<sub>2</sub>O<sub>3</sub>, CCR operation under scaled-up conditions was also performed. Notably, the amount of CO formed was maintained even in the presence of water vapor, which is advantageous for practical applications under realistic conditions. The effect of the co-loaded K species on the CO<sub>2</sub> hydrogenation catalysis is also discussed.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120599"},"PeriodicalIF":4.8,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217429","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Core@shell catalysts based on nickel phyllosilicates for dry reforming of methane: Effects of aging under hydrolysis conditions Core@shell层状硅酸盐镍基甲烷干重整催化剂:水解条件下老化的影响
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-23 DOI: 10.1016/j.apcata.2025.120593
Breno C. da Silva , Igor R. Neves , Pedro H.C. Bastos , Vitor S. Queiroz , Noemi R.C. Huaman , Maria L.A. da Silva , Roger Frety , Soraia T. Brandao
{"title":"Core@shell catalysts based on nickel phyllosilicates for dry reforming of methane: Effects of aging under hydrolysis conditions","authors":"Breno C. da Silva ,&nbsp;Igor R. Neves ,&nbsp;Pedro H.C. Bastos ,&nbsp;Vitor S. Queiroz ,&nbsp;Noemi R.C. Huaman ,&nbsp;Maria L.A. da Silva ,&nbsp;Roger Frety ,&nbsp;Soraia T. Brandao","doi":"10.1016/j.apcata.2025.120593","DOIUrl":"10.1016/j.apcata.2025.120593","url":null,"abstract":"<div><div>A new method for synthesis of catalysts with core@shell architecture has been developed for syngas production via dry reforming of methane (DRM). This route is based on the confinement of Stöber particles (silica nanospheres) by nickel phyllosilicates and a layer-analogous decoration made of SiO<sub>2</sub> (shell). Dry reforming catalysts based on non-noble metals suffer from deactivation via sintering and coke formation. Core@shell structures offer a strategy to enhance stability and control metal dispersion. In this work, the Stöber particles were obtained and then nickel phyllosilicate was synthetized over them (NiPS); silica was deposited on the resulting material producing a decorated material (S0@NiPS) and the effect of its aging under hydrolysis conditions for 12, 24, 36 and 48 h was evaluated (S12, S24, S36 and S48@NiPS). It was possible to demonstrate the efficiency of the proposed structures, with reagent conversion above 90 %, good yield to syngas and no signs of deactivation in the catalytic test at 700°C (coking condition), for the S24@NiPS sample (reducible nickel content 8 % w/w). The superior activity of S24@NiPS is attributed to optimal Ni dispersion and shell structure, balancing accessibility and confinement. The order of activity obtained was: S24@NiPS &gt; S12@NiPS &gt; NiPS &gt; S36@NiPS &gt; S48@NiPS &gt; S0@NiPS. The materials were characterized by XRD, TPR-H2, TPO-O2, TEM, EDS and TPSR-DRM. The modification of the hydrolysis time changed the properties of the catalysts: the shortest and longest times generated the less active catalysts. These findings offer a route to a coke-resistant catalysts for CO₂ valorization and methane upgrading.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120593"},"PeriodicalIF":4.8,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217431","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Sulfated SnO2 promoted FeVO4/CeO2-nanosheet catalyst for enhanced SCR deNOx performance with superior SO2 and H2O tolerance: Effect of various sulfated supports 硫酸化SnO2促进FeVO4/ ceo2纳米片催化剂增强SCR脱氧性能,具有优异的SO2和H2O耐受性:不同硫酸化载体的影响
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-23 DOI: 10.1016/j.apcata.2025.120597
Yuqiu Liu , Xuan Jia , Hongyu Zhao , Jianyi Zhang , Yanting Chen , Jinsheng Chen , Jinxiu Wang
{"title":"Sulfated SnO2 promoted FeVO4/CeO2-nanosheet catalyst for enhanced SCR deNOx performance with superior SO2 and H2O tolerance: Effect of various sulfated supports","authors":"Yuqiu Liu ,&nbsp;Xuan Jia ,&nbsp;Hongyu Zhao ,&nbsp;Jianyi Zhang ,&nbsp;Yanting Chen ,&nbsp;Jinsheng Chen ,&nbsp;Jinxiu Wang","doi":"10.1016/j.apcata.2025.120597","DOIUrl":"10.1016/j.apcata.2025.120597","url":null,"abstract":"<div><div>The support effect of sulfated SnO<sub>2</sub>, TiO<sub>2</sub>, ZrO<sub>2</sub>, and SiO<sub>2</sub> on FeVO<sub>4</sub>/CeO<sub>2</sub>-nanosheet was systematically investigated in this work. Among them, FeVO<sub>4</sub>/CeO<sub>2</sub>-nanosheet/sulfated-SnO<sub>2</sub> (FeVCe/SSn) catalyst exhibited the widest operating temperature window (227–422 °C) with efficient NO<sub><em>x</em></sub> conversion beyond 90 % and N<sub>2</sub> selectivity exceeding 97 %, as well as superior resistance to SO<sub>2</sub> and H<sub>2</sub>O (above 90 % activity retention for 24 h). The catalytic performance followed the order: FeVCe/SSn &gt; FeVCe/STi &gt; FeVCe/SZr &gt; FeVCe/SSi, which aligns well with their redox properties. FeVCe/SSn presents the best redox ability and the second highest surface acidity. Owing to the most pronounced interaction of sulfated SnO<sub>2</sub> with FeVO<sub>4</sub> and CeO<sub>2</sub> nanosheet, surface oxygen vacancies were significantly increased; simultaneously, sulfated SnO<sub>2</sub> provided abundant superacidic Brønsted acid sites and Lewis acid sites inherent to SnO<sub>2</sub>. This synergistic effect enhanced NH<sub>3</sub> adsorption/activation and suppressed SO<sub>2</sub> adsorption, thereby improving SCR activity and SO<sub>2</sub>/H<sub>2</sub>O resistance. The plausible mechanistic studies reveal that the SCR reaction over FeVCe/SSn is governed by a synergistic Eley–Rideal and Langmuir–Hinshelwood pathway. This study demonstrates that the rational design of acid-site density and the interfacial synergy between support and active phase constitute a feasible design principle for SCR catalysts that simultaneously afford a broad temperature window and high SO<sub>2</sub>/H<sub>2</sub>O durability.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120597"},"PeriodicalIF":4.8,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156020","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
High-entropy layered double hydroxide for the coupling cyclohexanol dehydrogenation with phenol hydrogenation 高熵层状双氢氧化物耦合环己醇脱氢与苯酚加氢
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-22 DOI: 10.1016/j.apcata.2025.120596
Rui Li , Yibin Zhang , Fang Chen , Huaiyuan Zhao , Weichen Du , Zhaoyin Hou
{"title":"High-entropy layered double hydroxide for the coupling cyclohexanol dehydrogenation with phenol hydrogenation","authors":"Rui Li ,&nbsp;Yibin Zhang ,&nbsp;Fang Chen ,&nbsp;Huaiyuan Zhao ,&nbsp;Weichen Du ,&nbsp;Zhaoyin Hou","doi":"10.1016/j.apcata.2025.120596","DOIUrl":"10.1016/j.apcata.2025.120596","url":null,"abstract":"<div><div>Coupling dehydrogenation of cyclohexanol (CHOL) and hydrogenation of phenol (PhOH) for the production of cyclohexanone (CHON) was seldom reported as the separated dehydrogenation of CHOL and hydrogenation of PhOH require different active sites, varied surface acidity and opposite conditions. High-entropy layered double hydroxides (HE-LDHs) might be a promising candidate for this coupling reaction via the synergistic effect of all components and modulated acidity/basicity. In this work, a series of well-structured Ru-containing HE-LDHs were synthesized and utilized in the coupling dehydrogenation of CHOL with hydrogenation of PhOH for the first time. Characterizations revealed that the hexa-metallic Cu<sub>1</sub>Co<sub>1</sub>Mg<sub>4</sub>Ru<sub>0.2</sub>Al<sub>0.9</sub>Sc<sub>0.9</sub>(OH)<sub>16</sub>CO<sub>3</sub>·4.8 H<sub>2</sub>O catalyst possesses large surface area (231 m<sup>2</sup>/g), enhanced acidity/basicity (254 µmol/g acid sites and 674 µmol/g basic sites), improved hydrogen adsorption capacity than those catalysts composed of two-, three-, four-, and five-metal components. It showed excellent activity under optimized reaction conditions (100 mmol CHOL + 5 mmol PhOH, 230 °C, 15 min), and the apparent conversion of PhOH reached 93.1 % with a formation rate of CHON as high as 661.5 g-CHON/g-Ru/h. Additionally, it was found that the dehydrogenation of CHOL could be accelerated when PhOH was added as a hydrogen acceptor, and hydrogen dehydrogenated from CHOL was utilized by PhOH which increased formation rate of CHON. The best hydrogen utilization achieved 86 %.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120596"},"PeriodicalIF":4.8,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156022","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Elucidating Keggin site-specific activity of NH4PM catalysts associated with dolomite-added H-MMT in gas-phase glycerol valorisation reactions 在气相甘油活化反应中,添加白云石H-MMT的NH4PM催化剂的Keggin位点特异性活性研究
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-22 DOI: 10.1016/j.apcata.2025.120595
Tania Roy , Jin Wang , Rongzhen Mu , Alfin Kurniawan , Xiaolan Chen , Chenglan Liu , Guoya Wang , Chun Hui Zhou
{"title":"Elucidating Keggin site-specific activity of NH4PM catalysts associated with dolomite-added H-MMT in gas-phase glycerol valorisation reactions","authors":"Tania Roy ,&nbsp;Jin Wang ,&nbsp;Rongzhen Mu ,&nbsp;Alfin Kurniawan ,&nbsp;Xiaolan Chen ,&nbsp;Chenglan Liu ,&nbsp;Guoya Wang ,&nbsp;Chun Hui Zhou","doi":"10.1016/j.apcata.2025.120595","DOIUrl":"10.1016/j.apcata.2025.120595","url":null,"abstract":"<div><div>Transforming glycerol into value-added chemicals like acrylic acid and allyl alcohol enhances biorefinery sustainability. We report a one-pot gas-phase process using a dual-bed catalytic system: acidified montmorillonite (H-MMT, upper bed) and vanadium-doped ammonium phosphomolybdate (V-doped NH<sub>4</sub>PM, lower bed). The combination of H-MMT and primary V-doped NH<sub>4</sub>PM (NH<sub>4</sub>PMV) catalyst favoured the oxydehydration reaction and was susceptible to the selective conversion of glycerol to acrylic acid (Sel.- 63 %). On the other hand, H-MMT and secondary VO<sub>x</sub>-doped NH<sub>4</sub>PM ((VO)<sub>x</sub>-NH<sub>4</sub>PM) catalysts preferred the selective production of allyl alcohol via deoxydehydration reaction. Maximum allyl alcohol selectivity of 61 % was achieved by 1:2 wt. ratio of HMMT and (VO)<sub>0.2</sub>-NH<sub>4</sub>PM dual bed catalytic system. O<sub>2</sub>-TPD and XPS analyses revealed that V doping at the primary Keggin site of NH<sub>4</sub>PM increased surface oxygen defects and enhanced Mo<sup>6 +</sup> /Mo<sup>5+</sup> charge transfer, promoting acrolein oxidation to acrylic acid. In contrast, secondary V-doped catalysts had fewer oxygen vacancies and were less effective for oxidation but showed high efficiency in hydrogen transfer from formic acid, methanol, or water, favoring allyl alcohol formation. Additionally, the following thermo-kinetic factors were evaluated for the best-performing catalysts, providing insights into the factors contributing to their high catalytic activity. Furthermore, incorporating 15 wt% dolomite into H-MMT reduced coke formation from 34.1 % to 2.54 % post-regeneration and extended catalyst life to 8 h of TOS while maintaining &gt; 40 % product selectivity, offering a practical strategy for coking resistance.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120595"},"PeriodicalIF":4.8,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145264272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Synergistic N-P coordination enables low-melting, high-crystallinity syndiotactic 1,2-polybutadiene via iron-based catalyst 协同N-P配位通过铁基催化剂实现了低熔点、高结晶度的间二聚1,2-聚丁二烯
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-21 DOI: 10.1016/j.apcata.2025.120594
Lihua Na , Yunqing Fan , Liang Fang, Xiaohua Wang, Heng Liu, Chunyu Zhang, Xuequan Zhang, Qi Yang
{"title":"Synergistic N-P coordination enables low-melting, high-crystallinity syndiotactic 1,2-polybutadiene via iron-based catalyst","authors":"Lihua Na ,&nbsp;Yunqing Fan ,&nbsp;Liang Fang,&nbsp;Xiaohua Wang,&nbsp;Heng Liu,&nbsp;Chunyu Zhang,&nbsp;Xuequan Zhang,&nbsp;Qi Yang","doi":"10.1016/j.apcata.2025.120594","DOIUrl":"10.1016/j.apcata.2025.120594","url":null,"abstract":"<div><div>Syndiotactic 1,2-polybutadiene (SPB) is promising crystalline material with high wear resistance, yet its practical applications remain limited due to excessively high melting temperature (<em>T</em>ₘ), which hinder melt processing. In this study, we report a novel iron-based catalyst system, Fe(acac)<sub>3</sub>/AIBN/PPh<sub>3</sub>/AlR<sub>3</sub>, that enables the synthesis of SPB with low melting temperature (<em>T</em><sub>m</sub>) (&lt; 120 °C) and relatively high crystallinity (up to 18 %), thereby addressing a long-standing challenge. The catalyst design features a synergistic <strong>N-P</strong> coordination strategy: AIBN serves as the primary ligand, coordinating to the Fe center via cyano groups to modulate its electronic and steric environment, effectively lowering <em>T</em>ₘ while promoting syndiotactic monomer insertion. Meanwhile, PPh<sub>3</sub> functions as an auxiliary ligand, enhancing stereoselectivity by fine-tuning the coordination geometry through its strong σ-donating character. Comparative studies reveal that the presence of PPh<sub>3</sub> significantly improves the syndiotacticity and crystallinity of the resulting polymers without compromising catalytic activity. This work not only provides a simple and scalable catalyst platform for producing processable crystalline polybutadiene, but also offers new mechanistic insights into ligand field modulation for stereocontrol in Fe-catalyzed diene polymerizations, paving the way for future advances in tunable diene synthesis.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120594"},"PeriodicalIF":4.8,"publicationDate":"2025-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156009","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Ni-loaded AFeO3 (Ca, Ce, and Sr) perovskite catalysts for efficient hydrogen-rich syngas production via steam gasification of wood–plastic composites 载ni的AFeO3 (Ca, Ce, Sr)钙钛矿催化剂用于木塑复合材料蒸汽气化高效富氢合成气生产
IF 4.8 2区 化学
Applied Catalysis A: General Pub Date : 2025-09-20 DOI: 10.1016/j.apcata.2025.120588
Jihyeon Seo , Yasin Khani , Kanghee Cho , Myung Won Seo , Jaewook Myung , Young-Kwon Park
{"title":"Ni-loaded AFeO3 (Ca, Ce, and Sr) perovskite catalysts for efficient hydrogen-rich syngas production via steam gasification of wood–plastic composites","authors":"Jihyeon Seo ,&nbsp;Yasin Khani ,&nbsp;Kanghee Cho ,&nbsp;Myung Won Seo ,&nbsp;Jaewook Myung ,&nbsp;Young-Kwon Park","doi":"10.1016/j.apcata.2025.120588","DOIUrl":"10.1016/j.apcata.2025.120588","url":null,"abstract":"<div><div>In this study, nickel (Ni)-loaded AFeO<sub>3</sub> perovskite catalysts were synthesized with various A-site species (Ca, Ce, and Sr) and utilized them for the hydrogen(H<sub>2</sub>)-rich syngas production via steam gasification of wood-plastic composites (WPC). To investigate the effect of A-site species (Ca, Ce, and Sr) composition on catalytic properties, the catalysts were tested under reaction conditions of 800 °C and a catalyst-to-feedstock (C/F) ratio of 0.1. 10 wt% Ni/CeFeO<sub>3</sub> indicated the highest gas yield (68.32 wt%) and H<sub>2</sub> selectivity (53.91 vol%). These results are attributed to its excellent oxygen storage capacity (OSC) associated with the Ce<sup>4 + /</sup>Ce<sup>3+</sup> redox pair, high lattice oxygen mobility, and strong metal–support interaction. These properties effectively promoted tar cracking and H<sub>2</sub> production through reforming and surface redox reactions. In addition, 10 wt% Ni/CeFeO<sub>3</sub> was tested at various temperatures (700, 750, and 800 °C), C/Fs (0.05, 0.1, and 0.2) and catalyst conditions (fresh and regenerated). An increase in the gasification temperature from 700 °C to 800 °C improved both gas yield and H<sub>2</sub> selectivity. Furthermore, at a C/F ratio of 0.2, the maximum gas yield (74.99 wt%) and H<sub>2</sub> selectivity (57.94 vol%) were achieved. The findings of this study demonstrate that 10 wt% Ni/AFeO<sub>3</sub> (A = Ca, Ce, and Sr) catalysts possess considerable potential for efficient H<sub>2</sub> production and stable performance in the steam gasification of WPC.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"708 ","pages":"Article 120588"},"PeriodicalIF":4.8,"publicationDate":"2025-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145109593","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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