Pub Date : 2025-10-27DOI: 10.1016/j.apcata.2025.120662
Xiaodan Zhang , Yongjun Zhang , Hongjing Han , Yanan Zhang , Haiying Wang , Jiayu Zhang , Yanguang Chen
In recent years, there has been a significant increase in the focus on composite catalysts with a core-shell structure, owing to their unique porous structure and adaptable functionality in the catalytic cracking of shale oil to light olefins. However, the precise mechanism of the synergistic catalytic effect between the shell and core layers on the reactants remains to be elucidated. In this study, a series of Z5@Fe-La-Z35 core-shell catalysts with tunable shell thickness were synthesized, wherein ZSM-5 as the shell and Fe-La-ZSM-35 as the core. The catalytic cracking performance was investigated for different alkanes and shale oil. It has been demonstrated that long-chain alkanes undergo primary cracking in the shell layer to form larger olefin molecules, and then proceed to the Fe-La-Z35 core layer for secondary cracking to form smaller molecules such as methane, ethane, ethylene, and propylene. This “tandem catalysis” strategy has been shown to be capable of significantly increasing the yields of ethylene and propylene during the reaction process. In the catalytic cracking of shale oil, the total yields of ethylene and propylene were as high as 52.32 % for 3-Z5@Fe-La-Z35 catalyst, which was an improvement of 16.51 % compared to Z5/Fe-La-Z35 catalyst (43.68 %). The present study elucidated the design and construction strategies of novel core-shell composite catalysts, providing a theoretical basis for further innovation and development in the field of catalytic cracking of oil to olefins.
{"title":"Tailoring molecular diffusion in the cracking process of alkanes and shale oil over core-shell structured Z5@Fe-La-Z35 zeolites with tunable shell thickness","authors":"Xiaodan Zhang , Yongjun Zhang , Hongjing Han , Yanan Zhang , Haiying Wang , Jiayu Zhang , Yanguang Chen","doi":"10.1016/j.apcata.2025.120662","DOIUrl":"10.1016/j.apcata.2025.120662","url":null,"abstract":"<div><div>In recent years, there has been a significant increase in the focus on composite catalysts with a core-shell structure, owing to their unique porous structure and adaptable functionality in the catalytic cracking of shale oil to light olefins. However, the precise mechanism of the synergistic catalytic effect between the shell and core layers on the reactants remains to be elucidated. In this study, a series of Z5@Fe-La-Z35 core-shell catalysts with tunable shell thickness were synthesized, wherein ZSM-5 as the shell and Fe-La-ZSM-35 as the core. The catalytic cracking performance was investigated for different alkanes and shale oil. It has been demonstrated that long-chain alkanes undergo primary cracking in the shell layer to form larger olefin molecules, and then proceed to the Fe-La-Z35 core layer for secondary cracking to form smaller molecules such as methane, ethane, ethylene, and propylene. This “tandem catalysis” strategy has been shown to be capable of significantly increasing the yields of ethylene and propylene during the reaction process. In the catalytic cracking of shale oil, the total yields of ethylene and propylene were as high as 52.32 % for 3-Z5@Fe-La-Z35 catalyst, which was an improvement of 16.51 % compared to Z5/Fe-La-Z35 catalyst (43.68 %). The present study elucidated the design and construction strategies of novel core-shell composite catalysts, providing a theoretical basis for further innovation and development in the field of catalytic cracking of oil to olefins.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120662"},"PeriodicalIF":4.8,"publicationDate":"2025-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145413383","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}
Pub Date : 2025-10-27DOI: 10.1016/j.apcata.2025.120663
Zhenhua Ji , Shijing Xie , Hao Chen , Peng Zhang , Ding Luo , Yixuan Chai , Zhuo Wang
Aiming at the key issues of current vehicle Ammonia Slip Catalyst (ASC) catalysts, such as poor low-temperature activity, high noble metal content, and narrow operating window, this study aims to construct multi-scale pore structures in Al2O3 supports of supported catalysts to regulate selective catalytic oxidation of NH3 (NH3-SCO) across broad temperature ranges and space velocities by improving convective diffusion, conduction, migration, and adsorption processes within catalyst voids. Characterization results show that a series of catalyst supports with different pore structures was successfully prepared using different templates. Pt was loaded using an optimized supported catalyst preparation method. Meanwhile, the coating amount of the prepared catalyst on cordierite monolith substrates was significantly reduced, and NH3-SCO performance tests were conducted. The results indicate that single mesoporous structures have limited regulation on the intrinsic activity of catalysts, while macroporous structures enhance the influence of desorption and void diffusion of gas-phase reactants and products on catalytic reactions. In the presence of macroporous structures, the promotional effect of mesopores on NH3-SCO reactions is enhanced. Among all catalysts, hierarchical porous catalysts with larger pore diameters and better interconnected pore structures exhibit NH₃ conversion rates exceeding 99 % across the full temperature range of 200℃ - 500℃, with NH3 concentrations below the regulatory limit of 10 ppm throughout the operating window. Macroporous structures and their pore diameters play a dominant role in regulating NH3-SCO reactions, particularly with stronger regulation at low temperatures. Increasing space velocity enhances the diffusion rate of NH3 gas molecules while amplifying the influence of pore structure regulation on catalysts. Notably, compared with traditional Pt/Al2O3, pore structure regulation does not significantly increase the generation of N2O while effectively enhancing the catalytic activity of the ASC catalyst.
{"title":"Study on improving NH3 oxidation reaction performance of Pt/Al2O3 supported catalysts through optimization of porous structures","authors":"Zhenhua Ji , Shijing Xie , Hao Chen , Peng Zhang , Ding Luo , Yixuan Chai , Zhuo Wang","doi":"10.1016/j.apcata.2025.120663","DOIUrl":"10.1016/j.apcata.2025.120663","url":null,"abstract":"<div><div>Aiming at the key issues of current vehicle Ammonia Slip Catalyst (ASC) catalysts, such as poor low-temperature activity, high noble metal content, and narrow operating window, this study aims to construct multi-scale pore structures in Al<sub>2</sub>O<sub>3</sub> supports of supported catalysts to regulate selective catalytic oxidation of NH<sub>3</sub> (NH<sub>3</sub>-SCO) across broad temperature ranges and space velocities by improving convective diffusion, conduction, migration, and adsorption processes within catalyst voids. Characterization results show that a series of catalyst supports with different pore structures was successfully prepared using different templates. Pt was loaded using an optimized supported catalyst preparation method. Meanwhile, the coating amount of the prepared catalyst on cordierite monolith substrates was significantly reduced, and NH<sub>3</sub>-SCO performance tests were conducted. The results indicate that single mesoporous structures have limited regulation on the intrinsic activity of catalysts, while macroporous structures enhance the influence of desorption and void diffusion of gas-phase reactants and products on catalytic reactions. In the presence of macroporous structures, the promotional effect of mesopores on NH<sub>3</sub>-SCO reactions is enhanced. Among all catalysts, hierarchical porous catalysts with larger pore diameters and better interconnected pore structures exhibit NH₃ conversion rates exceeding 99 % across the full temperature range of 200℃ - 500℃, with NH<sub>3</sub> concentrations below the regulatory limit of 10 ppm throughout the operating window. Macroporous structures and their pore diameters play a dominant role in regulating NH<sub>3</sub>-SCO reactions, particularly with stronger regulation at low temperatures. Increasing space velocity enhances the diffusion rate of NH<sub>3</sub> gas molecules while amplifying the influence of pore structure regulation on catalysts. Notably, compared with traditional Pt/Al<sub>2</sub>O<sub>3</sub>, pore structure regulation does not significantly increase the generation of N<sub>2</sub>O while effectively enhancing the catalytic activity of the ASC catalyst.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120663"},"PeriodicalIF":4.8,"publicationDate":"2025-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145413505","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}
Pub Date : 2025-10-27DOI: 10.1016/j.apcata.2025.120661
David Aroustamyan , Amélie D’Ascia , Marta Marinelli , Hélène Provendier , Yves Schuurman , Valentin L'hospital , Marilena Radoiu , Bhupinder Singh , Georgios Dimitrakis , Frederic C. Meunier
The oxidation of N2 by O2 in a quartz flow reactor operated at atmospheric pressure using 2.45 GHz microwave (MW) heating of La0.65Sr0.35MnO3 and LaMnO3 perovskites was investigated here. The perovskites were activated by a brief exposure to 600 W irradiation to facilitate MW absorption, resulting in more crystalline materials. La0.65Sr0.35MnO3 exhibited an increased permittivity constant and loss factor at low temperatures. MW in combination with perovskites enabled triggering plasmas leading to NO and NO2 as sole reaction products. The plasma temperature was in excess of 1800 °C. The maximal concentration of NOx obtained was ca. 2.2 vol% for an energy cost of about 86 MJ/molNOx. This high value is typical of small-scale systems for which MW power coupling and heat losses were not optimised. The plasma could be maintained down to 30 W of MW incident power on La0.65Sr0.35MnO3. The direction of the gas had no significant effect on the NOx output, but influenced the stability of the plasma at low MW incident powers. The role of perovskites in the process, other than acting as an MW susceptor and favoring plasma formation, should be further investigated, but the present data suggest no catalytic role. Quartz appeared as the best reactor material, given that alumina and modified zirconias led to reactor breakage. This work shows that varied perovskite formulations are able to trigger stable plasma under MW at atmospheric pressure, in particular the simple stoichiometry LaMnO3 and a commercially-available La0.65Sr0.35MnO3.
{"title":"Microwave-assisted oxidation of N2 to NOx over perovskites","authors":"David Aroustamyan , Amélie D’Ascia , Marta Marinelli , Hélène Provendier , Yves Schuurman , Valentin L'hospital , Marilena Radoiu , Bhupinder Singh , Georgios Dimitrakis , Frederic C. Meunier","doi":"10.1016/j.apcata.2025.120661","DOIUrl":"10.1016/j.apcata.2025.120661","url":null,"abstract":"<div><div>The oxidation of N<sub>2</sub> by O<sub>2</sub> in a quartz flow reactor operated at atmospheric pressure using 2.45 GHz microwave (MW) heating of La<sub>0.65</sub>Sr<sub>0.35</sub>MnO<sub>3</sub> and LaMnO<sub>3</sub> perovskites was investigated here. The perovskites were activated by a brief exposure to 600 W irradiation to facilitate MW absorption, resulting in more crystalline materials. La<sub>0.65</sub>Sr<sub>0.35</sub>MnO<sub>3</sub> exhibited an increased permittivity constant and loss factor at low temperatures. MW in combination with perovskites enabled triggering plasmas leading to NO and NO<sub>2</sub> as sole reaction products. The plasma temperature was in excess of 1800 °C. The maximal concentration of NO<sub><em>x</em></sub> obtained was ca. 2.2 vol% for an energy cost of about 86 MJ/mol<sub>NOx</sub>. This high value is typical of small-scale systems for which MW power coupling and heat losses were not optimised. The plasma could be maintained down to 30 W of MW incident power on La<sub>0.65</sub>Sr<sub>0.35</sub>MnO<sub>3</sub>. The direction of the gas had no significant effect on the NOx output, but influenced the stability of the plasma at low MW incident powers. The role of perovskites in the process, other than acting as an MW susceptor and favoring plasma formation, should be further investigated, but the present data suggest no catalytic role. Quartz appeared as the best reactor material, given that alumina and modified zirconias led to reactor breakage. This work shows that varied perovskite formulations are able to trigger stable plasma under MW at atmospheric pressure, in particular the simple stoichiometry LaMnO<sub>3</sub> and a commercially-available La<sub>0.65</sub>Sr<sub>0.35</sub>MnO<sub>3</sub>.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120661"},"PeriodicalIF":4.8,"publicationDate":"2025-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145413507","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}
Pub Date : 2025-10-27DOI: 10.1016/j.apcata.2025.120659
Xiao Lin, Soosan Kim, Monica Abdallah , Robert J. Farrauto
This study is focused on moisture enhancement of CO2 adsorption by Na-based dual function materials (DFMs) for direct air capture at elevated moisture levels (2–5 mol%), which includes typical humidity from temperate spring to tropical summer. Multi-cycle adsorption/methanation tests conducted under different moisture levels in ambient air demonstrate enhanced adsorption. It was found that moisture levels above about 4 mol% (>40 °C) lead to unstable performance. An extreme moisture level (5 %), which simulates a tropical climate, can lead to partial deactivation of adsorption and therefore lower CH4 formation. To fully utilize the potential of the moisture enhancement effect for this DFM sorbent, it is recommended to avoid deployment in regions with freezing temperatures (moisture-free) or extremely hot and humid tropical areas.
{"title":"Enhancement of CO2 adsorption on dual functional materials/catalytic methanation with varying moisture contents present in atmospheric ambient air","authors":"Xiao Lin, Soosan Kim, Monica Abdallah , Robert J. Farrauto","doi":"10.1016/j.apcata.2025.120659","DOIUrl":"10.1016/j.apcata.2025.120659","url":null,"abstract":"<div><div>This study is focused on moisture enhancement of CO<sub>2</sub> adsorption by Na-based dual function materials (DFMs) for direct air capture at elevated moisture levels (2–5 mol%), which includes typical humidity from temperate spring to tropical summer. Multi-cycle adsorption/methanation tests conducted under different moisture levels in ambient air demonstrate enhanced adsorption. It was found that moisture levels above about 4 mol% (>40 °C) lead to unstable performance. An extreme moisture level (5 %), which simulates a tropical climate, can lead to partial deactivation of adsorption and therefore lower CH<sub>4</sub> formation. To fully utilize the potential of the moisture enhancement effect for this DFM sorbent, it is recommended to avoid deployment in regions with freezing temperatures (moisture-free) or extremely hot and humid tropical areas.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120659"},"PeriodicalIF":4.8,"publicationDate":"2025-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145517018","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}
Pub Date : 2025-10-27DOI: 10.1016/j.apcata.2025.120660
Laura Fratalocchi, Stefano Rossini
The CCUS chain is an essential part of the global effort to reduce carbon emissions. It not only provides a means of mitigating climate change but also offers potential economic opportunities in various industries. The development and scaling of all the technologies covering the CCUS chain, alongside supportive policies, plays a crucial role in achieving global emissions reduction goals. In this review, a general overview of the CCUS process status and way forward from an industrial point of view is reported. A focus on the evaluation of the techno-economical potential of both the carbon capture to carbon storage pathway and carbon capture to utilization strategy is also given.
{"title":"A review on the role of carbon capture, utilization and storage (CCUS) in energy transition: An industrial perspective","authors":"Laura Fratalocchi, Stefano Rossini","doi":"10.1016/j.apcata.2025.120660","DOIUrl":"10.1016/j.apcata.2025.120660","url":null,"abstract":"<div><div>The CCUS chain is an essential part of the global effort to reduce carbon emissions. It not only provides a means of mitigating climate change but also offers potential economic opportunities in various industries. The development and scaling of all the technologies covering the CCUS chain, alongside supportive policies, plays a crucial role in achieving global emissions reduction goals. In this review, a general overview of the CCUS process status and way forward from an industrial point of view is reported. A focus on the evaluation of the techno-economical potential of both the carbon capture to carbon storage pathway and carbon capture to utilization strategy is also given.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120660"},"PeriodicalIF":4.8,"publicationDate":"2025-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145413382","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}
Pub Date : 2025-10-25DOI: 10.1016/j.apcata.2025.120657
Hao Luo , Xudong Zhang , Pu Guo , Haiyang Wang , Qian Zhang , Dongfan Li , Lei Lin , Fan Qu , Yuzhen Zhao , Zeming He , Zongcheng Miao
A self-supported Se-CoP@NG heterostructure featuring selenium-doped CoP nanoparticles encapsulated within N-doped carbon nanotubes (NCNTs) on carbon fiber paper is rationally designed to overcome persistent challenges in cobalt phosphide electrocatalysts, including poor intrinsic activity, ambiguous active sites, and structural instability. The peapod-inspired architecture, synthesized via in situ morphological and interfacial engineering, ensures structural integrity through dual-confinement against particle detachment. This catalyst delivers exceptional hydrogen evolution reaction (HER) performance, achieving remarkably low overpotentials of 105 mV in 1.0 M KOH and 121 mV in 0.5 M H₂SO₄ at 10 mA cm⁻². Integrated experimental and theoretical studies demonstrate that NCNT encapsulation redirects active sites from CoP to N-doped carbon layers, while Se doping optimizes interfacial charge polarization and electronic structure. Density functional theory calculations confirm a near-thermoneutral hydrogen adsorption free energy (ΔGH*= −0.18 eV) at N sites, synergistically boosting intrinsic HER activity.
合理设计了一种自支撑Se-CoP@NG异质结构，将硒掺杂的CoP纳米颗粒包裹在碳纤维纸上的n掺杂碳纳米管（NCNTs）中，以克服磷化钴电催化剂存在的固有活性差、活性位点不明确和结构不稳定等挑战。豆荚启发的建筑，通过原位形态学和界面工程合成，通过双重约束防止颗粒脱离，确保结构完整性。该催化剂具有优异的出氢反应（HER）性能，在1.0 M KOH中达到105 mV，在0.5 M H₂SO₄中达到121 mV，在10 mA cm⁻²。综合实验和理论研究表明，NCNT封装将活性位点从CoP重定向到n掺杂碳层，而Se掺杂优化了界面电荷极化和电子结构。密度泛函理论计算证实了N个位点的近热中性氢吸附自由能（ΔGH*= - 0.18 eV），协同提高了内在HER活性。
{"title":"Redirecting active sites to N-doped carbon layers via electronic coupling in Se-CoP@NG for efficient hydrogen evolution","authors":"Hao Luo , Xudong Zhang , Pu Guo , Haiyang Wang , Qian Zhang , Dongfan Li , Lei Lin , Fan Qu , Yuzhen Zhao , Zeming He , Zongcheng Miao","doi":"10.1016/j.apcata.2025.120657","DOIUrl":"10.1016/j.apcata.2025.120657","url":null,"abstract":"<div><div>A self-supported Se-CoP@NG heterostructure featuring selenium-doped CoP nanoparticles encapsulated within N-doped carbon nanotubes (NCNTs) on carbon fiber paper is rationally designed to overcome persistent challenges in cobalt phosphide electrocatalysts, including poor intrinsic activity, ambiguous active sites, and structural instability. The peapod-inspired architecture, synthesized via in situ morphological and interfacial engineering, ensures structural integrity through dual-confinement against particle detachment. This catalyst delivers exceptional hydrogen evolution reaction (HER) performance, achieving remarkably low overpotentials of 105 mV in 1.0 M KOH and 121 mV in 0.5 M H₂SO₄ at 10 mA cm⁻². Integrated experimental and theoretical studies demonstrate that NCNT encapsulation redirects active sites from CoP to N-doped carbon layers, while Se doping optimizes interfacial charge polarization and electronic structure. Density functional theory calculations confirm a near-thermoneutral hydrogen adsorption free energy (ΔG<sub>H*</sub>= −0.18 eV) at N sites, synergistically boosting intrinsic HER activity.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120657"},"PeriodicalIF":4.8,"publicationDate":"2025-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145359564","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}
Pub Date : 2025-10-25DOI: 10.1016/j.apcata.2025.120652
Aimin Gu, Zhaodong Nan
Iron-based catalysts are widely used in Fenton-like reactions. However, the leaching of Fe ions from the catalyst not only leads to secondary pollution but also results in the loss of active sites, thereby compromising the stability and long-term activity of the catalyst. Simultaneously, the selective degradation of organic contaminants still faces a challenge. Fe(OH)3@HNT was synthesized by selecting inexpensive halloysite nanotubes (HNT) as the carrier, which amorphous iron hydroxide nanoparticles (less than 5 nm) were encapsulated in the HNT’s cavity via oil-water biphasic system. Tetracycline (TC) was selected as the target pollutant to test the Fenton-like catalytic performance of Fe(OH)3@HNT. Fe(OH)3@HNT displays excellent catalytic activity than that of Fe(OH)3 and HNT. The nanoconfinement effect can improve the TC degradation. Moreover, Fe(OH)3@HNT shows selective adsorption and degradation of tetracycline pollutants contained rich hydroxyl groups through hydrogen bonding interaction between the catalyst and the contaminant. After five cycles, the TC removal ratio is still 90 % without Fe ions leached in the solution.
{"title":"Selective adsorption and degradation of tetracycline-based pollutants via Fenton-like reaction catalyzed by outstanding stable nanoreactor Fe(OH)3@HNT","authors":"Aimin Gu, Zhaodong Nan","doi":"10.1016/j.apcata.2025.120652","DOIUrl":"10.1016/j.apcata.2025.120652","url":null,"abstract":"<div><div>Iron-based catalysts are widely used in Fenton-like reactions. However, the leaching of Fe ions from the catalyst not only leads to secondary pollution but also results in the loss of active sites, thereby compromising the stability and long-term activity of the catalyst. Simultaneously, the selective degradation of organic contaminants still faces a challenge. Fe(OH)<sub>3</sub>@HNT was synthesized by selecting inexpensive halloysite nanotubes (HNT) as the carrier, which amorphous iron hydroxide nanoparticles (less than 5 nm) were encapsulated in the HNT’s cavity via oil-water biphasic system. Tetracycline (TC) was selected as the target pollutant to test the Fenton-like catalytic performance of Fe(OH)<sub>3</sub>@HNT. Fe(OH)<sub>3</sub>@HNT displays excellent catalytic activity than that of Fe(OH)<sub>3</sub> and HNT. The nanoconfinement effect can improve the TC degradation. Moreover, Fe(OH)<sub>3</sub>@HNT shows selective adsorption and degradation of tetracycline pollutants contained rich hydroxyl groups through hydrogen bonding interaction between the catalyst and the contaminant. After five cycles, the TC removal ratio is still 90 % without Fe ions leached in the solution.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120652"},"PeriodicalIF":4.8,"publicationDate":"2025-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145413433","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}
Pub Date : 2025-10-24DOI: 10.1016/j.apcata.2025.120654
Giuseppe Nava, Alessandro Porta, Carlo Giorgio Visconti, Roberto Matarrese
Dual Function Materials (DFMs) for integrated CO2 capture and methanation were investigated to assess the role of the spatial configuration between a Ru-based methanation catalyst and a K-based CO2 sorbent by combining microreactor experiments and in situ FT-IR spectroscopy. The presence of Ru and K over the same support (i.e., Ru-K/Al2O3), as in conventional DFMs, resulted in a significantly higher utilization of the adsorbed CO2 compared to a physical mixture of segregated Ru/Al2O3 and K/Al2O3. However, the physical mixture still enabled cyclic operations, achieving complete CH4 selectivity, unlike Ru-K/Al2O3. Indeed, the proximity of Ru and K introduced a trade-off between a reduced methanation rate and increased utilization of the captured CO2 during the cycle. These findings pave the way for the separate optimization of catalyst and sorbent components in integrated CO₂ capture and conversion systems, since the physical mixture outperforms conventional DFMs in some respects.
{"title":"Impact of sorbent-catalyst layouts on Ru/K-based DFMs for integrated CO2 capture and methanation","authors":"Giuseppe Nava, Alessandro Porta, Carlo Giorgio Visconti, Roberto Matarrese","doi":"10.1016/j.apcata.2025.120654","DOIUrl":"10.1016/j.apcata.2025.120654","url":null,"abstract":"<div><div>Dual Function Materials (DFMs) for integrated CO<sub>2</sub> capture and methanation were investigated to assess the role of the spatial configuration between a Ru-based methanation catalyst and a K-based CO<sub>2</sub> sorbent by combining microreactor experiments and <em>in situ</em> FT-IR spectroscopy. The presence of Ru and K over the same support (i.e., Ru-K/Al<sub>2</sub>O<sub>3</sub>), as in conventional DFMs, resulted in a significantly higher utilization of the adsorbed CO<sub>2</sub> compared to a physical mixture of segregated Ru/Al<sub>2</sub>O<sub>3</sub> and K/Al<sub>2</sub>O<sub>3</sub>. However, the physical mixture still enabled cyclic operations, achieving complete CH<sub>4</sub> selectivity, unlike Ru-K/Al<sub>2</sub>O<sub>3</sub>. Indeed, the proximity of Ru and K introduced a trade-off between a reduced methanation rate and increased utilization of the captured CO<sub>2</sub> during the cycle. These findings pave the way for the separate optimization of catalyst and sorbent components in integrated CO₂ capture and conversion systems, since the physical mixture outperforms conventional DFMs in some respects.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120654"},"PeriodicalIF":4.8,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145413436","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}
Using a simple reverse-phase microemulsion method, a higher content of two kinds of organic alkylamino groups including aminopropyl groups (AP, 50 mol%) and N,N-diethyl-3-aminopropyl groups (DEAP, 15 mol%) were simultaneously introduced on the surface of SiO2. The former organic group of AP acted as the catalytic active sites for the aldol condensation reaction, and the latter organic group of DEAP acted as the mesopore structure-generated agent to realize a high surface area of 102 m2/g. In a very short time of 5 min, high conversion of 99 % was successfully obtained for the aldol condensation of benzaldehyde and n-heptanal, together with a high selectivity of 81 % to (2Z)-2-benzylideneheptanal heptanal at a lower reaction temperature of 90 ℃. Specific surface groups and porous property facilitated to realize this excellent catalytic performance. Furthermore, prewetting treatment was found to be able to obviously accelerate the reaction through the generation of more silanol on its surface. Under the same reaction conditions, the reaction rate improved apparently by 60 %, and conversion of 95 % and selectivity of 81 % could be realized in an even shorter time of 3 min.
{"title":"Fast aldol condensation of benzaldehyde and n-heptanal catalyzed by high-content aminopropyl- and N, N-diethyl-3-aminopropyl-doped mesoporous silica","authors":"Meifang Zhang , Zhenyun Wang , Zhijiao Pan, Qiaohong Zhang, Chen Chen","doi":"10.1016/j.apcata.2025.120656","DOIUrl":"10.1016/j.apcata.2025.120656","url":null,"abstract":"<div><div>Using a simple reverse-phase microemulsion method, a higher content of two kinds of organic alkylamino groups including aminopropyl groups (AP, 50 mol%) and <em>N,N</em>-diethyl-3-aminopropyl groups (DEAP, 15 mol%) were simultaneously introduced on the surface of SiO<sub>2</sub>. The former organic group of AP acted as the catalytic active sites for the aldol condensation reaction, and the latter organic group of DEAP acted as the mesopore structure-generated agent to realize a high surface area of 102 m<sup>2</sup>/g. In a very short time of 5 min, high conversion of 99 % was successfully obtained for the aldol condensation of benzaldehyde and <em>n</em>-heptanal, together with a high selectivity of 81 % to (2<em>Z</em>)-2-benzylideneheptanal heptanal at a lower reaction temperature of 90 ℃. Specific surface groups and porous property facilitated to realize this excellent catalytic performance. Furthermore, prewetting treatment was found to be able to obviously accelerate the reaction through the generation of more silanol on its surface. Under the same reaction conditions, the reaction rate improved apparently by 60 %, and conversion of 95 % and selectivity of 81 % could be realized in an even shorter time of 3 min.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120656"},"PeriodicalIF":4.8,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145413434","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}
Pub Date : 2025-10-24DOI: 10.1016/j.apcata.2025.120655
Meng Lian , Yao-Mei Fu , Teng Liu , Xing Meng , Hai-Ning Wang , Zhong-Min Su
Converting carbon dioxide (CO2) into valuable chemical raw materials through photocatalysis is an environmentally friendly and efficient way to recycle carbon resources. Metal-organic polyhedra (MOPs) have received extensive attention as promising photocatalysts due to their tunable chemical structure and versatility. In this work, a series of covalently modified Cu@MOP-COF are prepared at room temperature. Among them, the CO generation rate of Cu@MOP-COF-2 can reach up to 162.46 μmol g−1·h−1, which is about 8 times that of MOP-NH2. In the photocatalytic process, in addition to generating hot electrons through the surface plasmon resonance (SPR) effect, Cu nanoclusters (Cu NCs) may also act as a co-catalyst, effectively capturing photoexcited electrons in MOP-COF. And the covalent bonds formed during the post-modification (PSM) process can significantly improves the charge carrier transfer performance and effectively reduces the charge recombination. Due to the existence of the above two synergistic effects, the photocatalytic performance of Cu@MOP-COF was significantly improved. In this work, a novel composite photocatalyst based on MOP-NH2 was proposed, which provided an innovative solution for the development of efficient photocatalytic systems.
{"title":"Construction of covalent cross-linked Zr-based metal organic polyhedra for efficient photocatalytic reduction of CO2 to CO","authors":"Meng Lian , Yao-Mei Fu , Teng Liu , Xing Meng , Hai-Ning Wang , Zhong-Min Su","doi":"10.1016/j.apcata.2025.120655","DOIUrl":"10.1016/j.apcata.2025.120655","url":null,"abstract":"<div><div>Converting carbon dioxide (CO<sub>2</sub>) into valuable chemical raw materials through photocatalysis is an environmentally friendly and efficient way to recycle carbon resources. Metal-organic polyhedra (MOPs) have received extensive attention as promising photocatalysts due to their tunable chemical structure and versatility. In this work, a series of covalently modified Cu@MOP-COF are prepared at room temperature. Among them, the CO generation rate of Cu@MOP-COF-2 can reach up to 162.46 μmol g<sup>−1</sup>·h<sup>−1</sup>, which is about 8 times that of MOP-NH<sub>2</sub>. In the photocatalytic process, in addition to generating hot electrons through the surface plasmon resonance (SPR) effect, Cu nanoclusters (Cu NCs) may also act as a co-catalyst, effectively capturing photoexcited electrons in MOP-COF. And the covalent bonds formed during the post-modification (PSM) process can significantly improves the charge carrier transfer performance and effectively reduces the charge recombination. Due to the existence of the above two synergistic effects, the photocatalytic performance of Cu@MOP-COF was significantly improved. In this work, a novel composite photocatalyst based on MOP-NH<sub>2</sub> was proposed, which provided an innovative solution for the development of efficient photocatalytic systems.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"709 ","pages":"Article 120655"},"PeriodicalIF":4.8,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145413506","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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