Applied Catalysis A: General最新文献_第8页

Metal-Salphen covalent organic polymers for bifunctional electrocatalytic ammonia synthesis and oxygen evolution 用于双功能电催化氨合成和析氧的金属-萨尔芬共价有机聚合物

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-21 DOI: 10.1016/j.apcata.2025.120369

Jiani Zhao , Yuhan Xia , Wenhua Xu, You Lv, Chengbo Li, Jun Li, Ning Wang

{"title":"Metal-Salphen covalent organic polymers for bifunctional electrocatalytic ammonia synthesis and oxygen evolution","authors":"Jiani Zhao , Yuhan Xia , Wenhua Xu, You Lv, Chengbo Li, Jun Li, Ning Wang","doi":"10.1016/j.apcata.2025.120369","DOIUrl":"10.1016/j.apcata.2025.120369","url":null,"abstract":"<div><div>Herein, we report a one-pot synthesis of metal-salphen-based covalent organic polymers (MSalphen-COPs) through Schiff base condensation of 1,3,5-triformylphloroglucinol and o-phenylenediamine in the presence of M(OAc)<sub>2</sub>·nH<sub>2</sub>O (M = Co, Ni, Cu). FTIR spectra confirm the successful formation of COPs via imine condensation while revealing an irreversible enol-keto tautomerization process that drives the structural evolution toward a thermodynamically stabilized framework. XPS analyses reveal that metal ions coordinate with deprotonated amine nitrogen and carbonyl oxygen moieties, deviating from conventional imine nitrogen/phenolate oxygen coordination in Metal-Salphen complexes. The electrocatalytic performance of MSalphen-COPs for nitrate/nitrite reduction (NO<sub>x</sub>RR) and oxygen evolution reaction (OER) exhibits strong metal-dependent trends, with CoSalphen-COP achieving exceptional activity. DFT calculations attribute cobalt’s superiority to its lowest barriers along catalytic cycles. Leveraging its bifunctionality, a CoSalphen-COP-based NO<sub>3</sub>RR||OER system demonstrates efficient NH<sub>3</sub>/O<sub>2</sub> coproduction, validating its potential for sustainable electrochemical applications. This work establishes a paradigm for designing task-specific COPs through tailored metal-ligand coordination environments.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120369"},"PeriodicalIF":4.7,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144124884","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

A comparative study proposing performance benchmarks for convoying industrial CO2-to-formate electroconversion 一项比较研究提出了输送工业二氧化碳到甲酸电转化的性能基准

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-20 DOI: 10.1016/j.apcata.2025.120362

Jie Xiao , Dong-Dong Ma , Xinquan Shen , Shu-Guo Han , Wenbo Wei , Qi-Long Zhu

{"title":"A comparative study proposing performance benchmarks for convoying industrial CO2-to-formate electroconversion","authors":"Jie Xiao , Dong-Dong Ma , Xinquan Shen , Shu-Guo Han , Wenbo Wei , Qi-Long Zhu","doi":"10.1016/j.apcata.2025.120362","DOIUrl":"10.1016/j.apcata.2025.120362","url":null,"abstract":"<div><div>Selecting suitable electrocatalytic benchmarks can greatly enhance electrocatalyst design and better assess their performance and potential applications. However, the absence of standardized electrocatalytic benchmarks bridging laboratory innovation to industrial implementation hinders the development of pH-universal CO<sub>2</sub>-to-formate conversion systems that meet industrial-grade current densities (> 200 mA cm<sup>–2</sup>), Faradaic efficiencies (FE > 90 %), and long-term stability. Herein, through a systematic evaluation of commercial bismuth-based chemicals (metal, oxide, salts) for CO<sub>2</sub> electroreduction, we demonstrated that bismuth salts (e.g., Bi(NO<sub>3</sub>)<sub>3</sub>) as precursors for material development, can emerge as the universal performance benchmarks across all pH conditions (acidic, neutral, and alkaline). Concretely, in various electrolytic environments for formate production, these bismuth salts-coated electrodes generally exhibit exceeding 90 % FE, large current densities, low onset potentials and potential operational stability. Moreover, a comparative analysis with In/Sn/Pb analogues profoundly elucidates the general benchmarking feasibility of bismuth salts in facilitating CO<sub>2</sub>-to-formate electroconversion. This work establishes a screening paradigm of formate-targeted electrocatalytic materials, which can assess and guide the design of practical CO<sub>2</sub> electrocatalysts for sustainable formate production at industrial scales.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120362"},"PeriodicalIF":4.7,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105319","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

The two-stage formation process of coke species on ferrierite zeolite during 1-butene skeletal isomerization revealed by surface-enhanced Raman scattering technique 利用表面增强拉曼散射技术揭示了1-丁烯骨架异构化过程中铁素体沸石上焦炭的两阶段形成过程

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-20 DOI: 10.1016/j.apcata.2025.120355

Guoliang Wu, Qiang Bao, Jian Zhang, Mingjian Luo, Zhirui Chen, Xue Qiao, Yi Hu, Wenlin Wang, Yunfeng Hu

{"title":"The two-stage formation process of coke species on ferrierite zeolite during 1-butene skeletal isomerization revealed by surface-enhanced Raman scattering technique","authors":"Guoliang Wu, Qiang Bao, Jian Zhang, Mingjian Luo, Zhirui Chen, Xue Qiao, Yi Hu, Wenlin Wang, Yunfeng Hu","doi":"10.1016/j.apcata.2025.120355","DOIUrl":"10.1016/j.apcata.2025.120355","url":null,"abstract":"<div><div>In this paper, a series of ferrierite (FER) zeolites with different acidities were successfully synthesized using silica sol with different concentrations as the silica sources. With the assistance of TG-MS/TPO measurement, the formation process of coke species on FER zeolite during 1-butene skeletal isomerization was investigated using surface-enhanced Raman scattering (SERS) technique with iodide-modified Ag NPs as the substrate. The results revealed that in the early reaction stage, polyaromatics and polyolefins are formed in the first stage due to strong acid sites. Later, polyolefin and olefin components from the second stage can potentially transform into polyaromatics, causing the deactivation of FER zeolite. This potential is controlled by the quantity of weak acid sites. In other words, the stability of FER zeolite in the skeletal isomerization of 1-butene exhibits a negative correlation with the abundance of its weak acid sites. These findings indirectly demonstrate the significant advantages of SERS-based coke detection method.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120355"},"PeriodicalIF":4.7,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105320","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

Developing a supported metal oxide catalyst for direct dehydrogenation of propane to propene 丙烷直接脱氢制丙烯负载型金属氧化物催化剂的研制

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-20 DOI: 10.1016/j.apcata.2025.120354

Rajvikram Singh, Raghvendra Singh, Goutam Deo

{"title":"Developing a supported metal oxide catalyst for direct dehydrogenation of propane to propene","authors":"Rajvikram Singh, Raghvendra Singh, Goutam Deo","doi":"10.1016/j.apcata.2025.120354","DOIUrl":"10.1016/j.apcata.2025.120354","url":null,"abstract":"<div><div>Propene is an important building block in the petrochemical industry and its demand is rapidly increasing. However, the production through conventional processes is limited, and there is a dire need to develop a suitable catalyst for the direct dehydrogenation of propane. Multiple set of catalysts are synthesized via incipient wetness impregnation method and characterized by various techniques. These catalysts are also tested for the direct dehydrogenation reaction, to examine the effect of active metal oxide species, support material, metal oxide loading and potassium (K) loading. Subsequently, the reaction temperature and contact time are optimized for the reaction. A near-monolayer loading chromium oxide supported on ZrO<sub>2</sub> is the most active. At this loading incipient amounts of Cr<sub>2</sub>O<sub>3</sub> crystallites are detected, which became larger at higher coverages. The monolayer coverage appears to be between 5.2 and 6.6 <span><math><mrow><mi>ato</mi><msub><mrow><mi>m</mi></mrow><mrow><mi>Cr</mi></mrow></msub><mo>/</mo><mi>n</mi><msup><mrow><mi>m</mi></mrow><mrow><mn>2</mn></mrow></msup></mrow></math></span>. Furthermore, at this coverage the amount of reducible Cr<sup>+6</sup> species was maximum. The activity of this near-monolayer catalyst is further improved by co-impregnating K. A Cr to K molar ratio of 1:0.05 is found to increase the amount of reducible Cr<sup>+6</sup> and the catalyst activity and selectivity. Increasing the K amount further leads to a decrease in activity. Activity is increased by increasing the reaction temperature till 550 ℃; however, above 550 ℃ the catalyst deactivates due to coke formation. Further improvement in activity is achieved by increasing the contact time and a conversion of ∼30 % and yield of ∼27 % is achieved for the K-promoted supported chromia catalyst at 550 °C and a contact time of 37.33 <span><math><mrow><msub><mrow><mi>g</mi></mrow><mrow><mi>cat</mi></mrow></msub><mo>.</mo><mi>h</mi><mo>/</mo><mi>mol</mi></mrow></math></span>.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120354"},"PeriodicalIF":4.7,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144134415","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

Promotional effect of CeO2 and Fe2O3 species on mesoporous silica as efficient catalysts for the vapor-phase dehydration of iso-butyl alcohol to isobutylene CeO2和Fe2O3对介孔二氧化硅气相脱水异丁醇制异丁烯的促进作用

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-17 DOI: 10.1016/j.apcata.2025.120352

Walaa A. Elhamdy , Abd El-Aziz A. Said , Mohamed N. Goda , Kamal M.S. Khalil

{"title":"Promotional effect of CeO2 and Fe2O3 species on mesoporous silica as efficient catalysts for the vapor-phase dehydration of iso-butyl alcohol to isobutylene","authors":"Walaa A. Elhamdy , Abd El-Aziz A. Said , Mohamed N. Goda , Kamal M.S. Khalil","doi":"10.1016/j.apcata.2025.120352","DOIUrl":"10.1016/j.apcata.2025.120352","url":null,"abstract":"<div><div>CeO₂–Fe₂O₃ binary oxides were effectively incorporated into mesoporous spherical silica (MCM-41) via a sol–gel technique. The resultant CFO/MCM-41 nanocomposites, with metal loadings ranging from 3 to 30 wt%, were subsequently calcined at 550 °C and assessed as catalysts for the gas-phase dehydration of isobutyl alcohol. Structural and surface analyses using XRD, TG-DTA, ATR-FTIR, BET, TEM, EDX, XPS, and pyridine-adsorbed FTIR confirmed the formation of thermally stable, well-dispersed active phases, as well as the presence of both Lewis and Brønsted acid sites. The differences in catalytic activity among these nanocomposites were closely linked to variations in their acidity. Among all the catalysts, the 10 wt% CeFeO₃/MCM-41 sample demonstrated the best performance at 350 °C, achieving approximately 92 % isobutanol conversion, 100 % selectivity toward isobutylene, and a butene production rate of 45.10 mmol g⁻¹ h⁻¹ . The catalyst also showed excellent stability across five reuse cycles. The outstanding catalytic performance and stability were directly correlated with the material's enhanced structural integrity and optimized textural properties. Furthermore, XPS analysis revealed that the Ce<sup>3 +</sup>/Ce<sup>4+</sup> and Fe<sup>2+</sup>/Fe<sup>3+</sup> redox states, modulated by Ce–Fe interactions, played a crucial role in tuning the catalyst’s acidity and catalytic performance.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"702 ","pages":"Article 120352"},"PeriodicalIF":4.7,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071720","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

Phenolic resin/cadmium selenide heterojunctions for efficient hydrogen peroxide production with broad-spectrum light utilization 酚醛树脂/硒化镉异质结用于广谱光高效过氧化氢生产

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-16 DOI: 10.1016/j.apcata.2025.120353

Zhixiong Zheng , Yazhou Zhou

{"title":"Phenolic resin/cadmium selenide heterojunctions for efficient hydrogen peroxide production with broad-spectrum light utilization","authors":"Zhixiong Zheng , Yazhou Zhou","doi":"10.1016/j.apcata.2025.120353","DOIUrl":"10.1016/j.apcata.2025.120353","url":null,"abstract":"<div><div>The efficient and sustainable production of hydrogen peroxide (H₂O₂) via solar-driven photocatalysis is hindered by poor charge separation and limited light absorption. To address these challenges, we present a novel S-scheme heterojunction photocatalyst composed of cadmium selenide (CdSe) nanoparticles and phenolic resin (RF523). The integration of RF523 with CdSe promotes efficient charge separation by generating a built-in electric field, reducing electron-hole recombination. This design enhances both the oxidation and reduction capabilities of the materials and expands spectral absorption to the near-infrared region (800 nm), which is underutilized in conventional systems. The RF/CdSe-100 composite demonstrated a remarkable H₂O₂ production rate of 888.9 μmol·h⁻¹ under full-spectrum light, outperforming mechanically mixed samples by a factor of 2.0. Additionally, the composite exhibited broad-spectrum light absorption, with an apparent quantum yield of 19.0 % under 365 nm light and 1.7 % under 800 nm light, highlighting its ability to efficiently utilize a wide range of solar energy. The photocatalytic mechanism is driven by the S-scheme charge transfer process, enhancing redox efficiency and promoting the generation of reactive oxygen species (ROS) for H₂O₂ production. This work offers an efficient strategy for solar-driven H₂O₂ synthesis, advancing the design of photocatalysts for renewable energy and environmental applications.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120353"},"PeriodicalIF":4.7,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088990","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

Engineering hybrid plasmonic nanomaterials for solar energy conversion: Insight into the structure-function relations 用于太阳能转换的工程杂化等离子体纳米材料：结构-功能关系的洞察

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-15 DOI: 10.1016/j.apcata.2025.120351

Fengxia Tong , Leitao Zhu , Xiaolei Bao , Xizhuang Liang , Zhaoke Zheng

{"title":"Engineering hybrid plasmonic nanomaterials for solar energy conversion: Insight into the structure-function relations","authors":"Fengxia Tong , Leitao Zhu , Xiaolei Bao , Xizhuang Liang , Zhaoke Zheng","doi":"10.1016/j.apcata.2025.120351","DOIUrl":"10.1016/j.apcata.2025.120351","url":null,"abstract":"<div><div>Plasmonic nanomaterials, endowed with the unique surface plasmon resonance (SPR) effect, offer a promising route to convert low-intensity solar energy into chemical energy with a higher efficiency. However, the significant mismatch in timescales between rapid SPR relaxation (∼100 picoseconds) and slow chemical reaction kinetics (milliseconds or seconds) poses a major obstacle to their widespread application. To overcome these challenges, it is crucial to design multicomponent plasmonic nanostructures and establish efficient charge carrier channels. This review focuses on the effect of unique structures of plasmonic nanomaterials with precise geometries on catalytic performance. The key design strategies for hybrid plasmonic nanostructures and the deep physical and chemical mechanism have been summarized to effectively promote charge carrier excitation and migration. These strategies involve the shape, size and electronic structures tailoring of plasmonic components, an atomistic control over their coupling with other plasmonic components, doped semiconductors or non-plasmonic components, single-atom doping, crystal phase engineering as well as external field coupling. Finally, we discuss the future challenges and prospects in this field. This review aims to offer valuable insights in the design of plasmonic photocatalytic materials, ultimately accelerating the development of high-performance plasmonic photocatalysts.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"702 ","pages":"Article 120351"},"PeriodicalIF":4.7,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144068475","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

Porous organic polymers based on benzothiazole or benzimidazole for photocatalytic synthesis of hydrogen peroxide in pure water 基于苯并噻唑或苯并咪唑的多孔有机聚合物在纯水中光催化合成过氧化氢

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-15 DOI: 10.1016/j.apcata.2025.120338

Tongtong Li , Yue Wang , Huawei Shen , Hongqi Zhu , Run Wang , Shibing Wu , Chenyang Jin , Ligong Chen , Yang Li , Xilong Yan , Bowei Wang

{"title":"Porous organic polymers based on benzothiazole or benzimidazole for photocatalytic synthesis of hydrogen peroxide in pure water","authors":"Tongtong Li , Yue Wang , Huawei Shen , Hongqi Zhu , Run Wang , Shibing Wu , Chenyang Jin , Ligong Chen , Yang Li , Xilong Yan , Bowei Wang","doi":"10.1016/j.apcata.2025.120338","DOIUrl":"10.1016/j.apcata.2025.120338","url":null,"abstract":"<div><div>Developing photocatalysts featuring appropriate active sites and bandgaps for sustainable photocatalytic production of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) remains a major challenge. Herein, novel porous organic polymers (denoted as SZ and MZ) based on benzothiazole and benzimidazole were constructed and utilized for photocatalytic production of H<sub>2</sub>O<sub>2</sub> by virtue of their excellent photovoltaic properties and chemical stability. Under simulated sunlight, SZ exhibited noteworthy photocatalytic performance with a H<sub>2</sub>O<sub>2</sub> production rate of 3109 μmol g<sup>−1</sup> h<sup>−1</sup> in water without sacrificial agent, and maintained high catalytic efficiency after six consecutive reactions. Similarly, MZ demonstrated an H<sub>2</sub>O<sub>2</sub> production rate of 2700 μmol g<sup>−1</sup> h<sup>−1</sup>. Furthermore, the mechanism of photocatalytic production of H<sub>2</sub>O<sub>2</sub> by benzothiazole porous organic polymers (POPs) was further investigated, and the superiority of photocatalytic production of H<sub>2</sub>O<sub>2</sub> by one-step two-electron oxygen reduction process was verified.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120338"},"PeriodicalIF":4.7,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088991","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

Catalytic acetalization of glycerol to solketal using mesoporous silica, Cu-FSM-16 介孔二氧化硅Cu-FSM-16催化甘油缩醛制溶胶

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-13 DOI: 10.1016/j.apcata.2025.120350

Rupak Kumar Singh, Vijayalakshmi Gosu

引用次数: 0

FeOx clusters confined in ZSM-5 as a high-performance catalyst for Fischer-Tropsch synthesis of lower hydrocarbons 限定在ZSM-5中的FeOx簇作为费托合成低碳氢化合物的高性能催化剂

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-05-13 DOI: 10.1016/j.apcata.2025.120335

Qichao Lu, Jie Li, Chen Liang, Lei Liu, Jinxiang Dong

{"title":"FeOx clusters confined in ZSM-5 as a high-performance catalyst for Fischer-Tropsch synthesis of lower hydrocarbons","authors":"Qichao Lu, Jie Li, Chen Liang, Lei Liu, Jinxiang Dong","doi":"10.1016/j.apcata.2025.120335","DOIUrl":"10.1016/j.apcata.2025.120335","url":null,"abstract":"<div><div>Under the dual pressures of oil depletion and low-carbon transition, Fischer-Tropsch synthesis (FTS) technology offers a viable option for producing high value-added lower (C<sub>2</sub>-C<sub>4</sub>) hydrocarbons from non-oil sources. However, conventional Fe-based catalysts often suffer from deactivation due to carbon deposition and sintering. Here, we report a unique Fe-ZSM-5 catalyst synthesized by doping Fe into ZSM-5, which demonstrates excellent FTS catalytic performance. During high-temperature template removal, Fe species migrated from the zeolite framework to form highly dispersed FeO<sub>x</sub> clusters (∼2 nm). Upon treatment by syngas, these FeO<sub>x</sub> clusters aggregate to form uniformly small-sized Fe<sub>5</sub>C<sub>2</sub>@C core-shell particles distributed on ZSM-5 support. The confinement effect of the inter-crystalline structure effectively prevents the sintering of Fe<sub>5</sub>C<sub>2</sub>. The smaller Fe<sub>5</sub>C<sub>2</sub> particles exhibit controlled CO dissociation, reducing the concentration of activated carbon species (C*), and the carbon shells (∼6.5 nm) limit the departure of C*, effectively suppressing carbon deposition. This unique structure enables stable catalytic activity for over 100 hours with maintained product selectivity. The Fe-ZSM-5 catalyst achieved a C<sub>2</sub>-C<sub>4</sub> hydrocarbons selectivity of 54.52 %, nearing the 56 % theoretical limit of the Anderson-Schulz-Flory (ASF) distribution. Additionally, the hydrophobic carbon shell prevents excessive oxidation of Fe<sub>5</sub>C<sub>2</sub>, reducing CO<sub>2</sub> selectivity by ∼56 % compared to conventional Fe/ZSM-5 catalysts, significantly enhancing atomic utilization efficiency and aligning with the principles of green development.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"702 ","pages":"Article 120335"},"PeriodicalIF":4.7,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144068448","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