Applied Catalysis A: General最新文献

筛选
英文 中文
Recent advances of CO2 electroreduction towards ethanol over Cu-based catalysts cu基催化剂上CO2电还原乙醇的研究进展
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-06-10 DOI: 10.1016/j.apcata.2025.120404
Huan Zhang , Jiahui Li , Zhe Shen , Haijie Hu , Wenbo Jin , Chengtun Qu
{"title":"Recent advances of CO2 electroreduction towards ethanol over Cu-based catalysts","authors":"Huan Zhang ,&nbsp;Jiahui Li ,&nbsp;Zhe Shen ,&nbsp;Haijie Hu ,&nbsp;Wenbo Jin ,&nbsp;Chengtun Qu","doi":"10.1016/j.apcata.2025.120404","DOIUrl":"10.1016/j.apcata.2025.120404","url":null,"abstract":"<div><div>Electrochemical reduction of CO<sub>2</sub> (ERCO<sub>2</sub>) represents a promising strategy for atmospheric CO<sub>2</sub> mitigation by converting this greenhouse gas into value-added chemical feed stocks. Among various catalytic materials, copper-based electrocatalysts have emerged as frontier candidates due to their distinctive capability in promoting C-C coupling reactions, which selectively steer the reaction pathway toward multi-carbon products. Notably, these catalysts exhibit superior performance in producing industrially important C<sub>2</sub> compounds such as ethylene and ethanol through precise modulation of reaction intermediates, thereby demonstrating significant potential for establishing a circular carbon economy. This paper provides a review of the reaction mechanism involved in the electrocatalytic reduction of CO<sub>2</sub> to ethanol. It also discusses the research progress made in the development of Cu-based catalysts for this reaction, including Cu monomers, Cu-based bimetallic catalysts, CuO-based catalysts and non-metallic modified Cu-based catalysts. Additionally, the paper introduces various strategies that have been employed to enhance the selectivity of ethanol products, such as the confinement strategy、local environment modulation and electronic structure modulation. Finally, the paper discusses the challenges and future development directions of Cu-based catalysts in the electrocatalytic reduction of CO<sub>2</sub> to ethanol.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120404"},"PeriodicalIF":4.7,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144271606","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
Carbon film-modified Bi5O7I composites for highly efficient simultaneous photocatalytic removal of bisphenol-A and Cr(VI) under visible light irradiation 碳膜改性Bi5O7I复合材料在可见光照射下高效同时光催化去除双酚a和Cr(VI)
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-06-09 DOI: 10.1016/j.apcata.2025.120403
Xiaomeng Yang , Jinghao Huo , Hanjun Zhu , Xin Nie , Quan Wan , Jukun Xiong , Huixian Shi
{"title":"Carbon film-modified Bi5O7I composites for highly efficient simultaneous photocatalytic removal of bisphenol-A and Cr(VI) under visible light irradiation","authors":"Xiaomeng Yang ,&nbsp;Jinghao Huo ,&nbsp;Hanjun Zhu ,&nbsp;Xin Nie ,&nbsp;Quan Wan ,&nbsp;Jukun Xiong ,&nbsp;Huixian Shi","doi":"10.1016/j.apcata.2025.120403","DOIUrl":"10.1016/j.apcata.2025.120403","url":null,"abstract":"<div><div>The coexistence of heavy metals and organic pollutants in aquatic ecosystems poses significant threats to environmental and human health. To address this issue, a novel carbon film-modified Bi<sub>5</sub>O<sub>7</sub>I photocatalyst (C/Bi<sub>5</sub>O<sub>7</sub>I) was developed for the simultaneous removal of bisphenol-A (BPA) and Cr(VI) under visible light. The C/Bi<sub>5</sub>O<sub>7</sub>I composite exploited the synergistic effect between the carbon film and Bi<sub>5</sub>O<sub>7</sub>I, enhancing light absorption and facilitating efficient electron transfer, which promoted the separation of electron-hole pairs. This mechanism enabled holes to degrade BPA and electrons to reduce Cr(VI), with each process mutually accelerating the other. The composite exhibited high photocatalytic activity across a wide pH range (3.0–11.0) and was minimally inhibited by typical water matrix components. Characterization techniques and theoretical calculations were employed to elucidate the degradation pathways, confirming the stability and efficiency of C/Bi<sub>5</sub>O<sub>7</sub>I over multiple cycles. This makes C/Bi<sub>5</sub>O<sub>7</sub>I a promising material for treating wastewater contaminated with coexisting heavy metals and organic pollutants.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120403"},"PeriodicalIF":4.7,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144261779","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
Investigation of oxygen mobility on LaNi-Zn perovskite catalyst for carbon inhibition in dry reforming of methane 甲烷干重整碳抑制用镧锌钙钛矿催化剂氧迁移率研究
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-06-08 DOI: 10.1016/j.apcata.2025.120400
Juliana Bertoldi , Camila E. Kozonoe , Éder V. Oliveira , Morgana Rosset , Larissa Otubo , Elisabete M. Assaf , Martin Schmal
{"title":"Investigation of oxygen mobility on LaNi-Zn perovskite catalyst for carbon inhibition in dry reforming of methane","authors":"Juliana Bertoldi ,&nbsp;Camila E. Kozonoe ,&nbsp;Éder V. Oliveira ,&nbsp;Morgana Rosset ,&nbsp;Larissa Otubo ,&nbsp;Elisabete M. Assaf ,&nbsp;Martin Schmal","doi":"10.1016/j.apcata.2025.120400","DOIUrl":"10.1016/j.apcata.2025.120400","url":null,"abstract":"<div><div>Carbon formation is one of the major problems in methane reforming reactions, mainly in dry reforming of methane (DRM), limiting its industrial competitiveness. Thus, in this work, we investigate the oxygen mobility and carbon resistance of the LaNi-Zn perovskite in the DRM reaction. The catalysts LaNiO<sub>3</sub> (LN) and LaNi<sub>0.5</sub>Zn<sub>0.5</sub>O<sub>3-δ</sub> (LNZn) were synthesized and characterized by XRD, H<sub>2</sub>-TPR, CH<sub>4</sub>-TPSR-MS, H<sub>2</sub>-TPHR-MS, XPS, TGA, Raman, HRTEM, and <em>quasi-in-situ</em> DRIFTS-MS, aiming to understand the role of the promoter in coke suppression. The CH<sub>4</sub>-TPSR-MS, H<sub>2</sub>-TPHR-MS, and Raman analyses revealed that the Zn-substituted catalyst exhibited higher oxygen mobility compared to the LN catalyst, attributed to the oxophilicity of Zn<sup>2+</sup>, which facilitates carbon gasification. XPS and HRTEM analyses of reduced samples confirmed the presence of metallic Zn<sup>0</sup> on the surface as Ni-Zn alloying. 30 h of TOS showed higher activity for the LN catalyst than the LNZn. However, post-reaction analysis indicated that the addition of Zn increased carbon resistance by 5 times. The formation of the Ni-Zn alloying effectively prevented the removal of Ni particles from the support and their encapsulation by carbon nanotubes. <em>Quasi-in-situ</em> DRIFTS-MS has revealed that the LNZn catalyst promotes the formation of intermediate species responsible for carbon oxidation (CH<sub>x</sub>O, HCOO<sup>⁻</sup>, and HCO<sub>3</sub><sup>⁻</sup>), clearing the anti-carbon behavior of the Zn-substituted catalyst.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120400"},"PeriodicalIF":4.7,"publicationDate":"2025-06-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144271607","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 the structure-activity relationship of Bi-doped MnO2 catalysts towards CH3OH oxidation 双掺杂MnO2催化剂对CH3OH氧化的构效关系研究
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-06-07 DOI: 10.1016/j.apcata.2025.120402
Suxin Yu, Haoyuan Gu, Qihang Wen, Yi-Fan Han, Minghui Zhu
{"title":"Elucidating the structure-activity relationship of Bi-doped MnO2 catalysts towards CH3OH oxidation","authors":"Suxin Yu,&nbsp;Haoyuan Gu,&nbsp;Qihang Wen,&nbsp;Yi-Fan Han,&nbsp;Minghui Zhu","doi":"10.1016/j.apcata.2025.120402","DOIUrl":"10.1016/j.apcata.2025.120402","url":null,"abstract":"<div><div>MnO<sub>2</sub>-based catalysts have been extensively utilized in the catalytic oxidation of volatile organic compounds due to their cost-effectiveness. In this study, a series of Bi-doped MnO<sub>2</sub> catalysts with various contents were systematically investigated to reveal the structure-activity relationship during the CH<sub>3</sub>OH oxidation reaction, which was achieved using a series of characterizations. Bi could enter the MnO<sub>2</sub> lattice and lead to the facile formation of oxygen vacancies, facilitating the generation of surface reactive oxygen species by O<sub>2</sub> dissociation. With the increase of Bi, the activity showed a volcanic trend, and the Mn<sub>7.5</sub>Bi<sub>1</sub>O<sub>x</sub> (T<sub>90</sub> = 160 °C) exhibited the lowest apparent activation energy and optimal performance. CH<sub>3</sub>OH oxidation mechanism (CH<sub>3</sub>OH → methoxy species → formate species → CO<sub>2</sub> and H<sub>2</sub>O) was revealed by <em>in situ</em> DRIFTS, and the last two oxidation processes were significantly sped up. Bi-doped MnO<sub>2</sub> exhibited high H<sub>2</sub>O tolerance due to hydroxyl-assisted CH<sub>3</sub>OH chemisorption via hydrogen bonding and hydroxyl-assisted C-H activation of methoxy species with surface reactive oxygen species. These findings are beneficial for the rational design of metal-doped catalysts with rich oxygen vacancy defects for catalytic oxidation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120402"},"PeriodicalIF":4.7,"publicationDate":"2025-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144254308","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
Electrodeposited NiMoP coating on Cu nanorods array as efficient bifunctional electrocatalysts for urea-assisted hydrogen production Cu纳米棒阵列电沉积NiMoP涂层作为高效的双功能电催化剂用于尿素辅助制氢
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-06-06 DOI: 10.1016/j.apcata.2025.120399
Mi Wang , Guangqin Chen , Yan Zhang , Jian Xiao
{"title":"Electrodeposited NiMoP coating on Cu nanorods array as efficient bifunctional electrocatalysts for urea-assisted hydrogen production","authors":"Mi Wang ,&nbsp;Guangqin Chen ,&nbsp;Yan Zhang ,&nbsp;Jian Xiao","doi":"10.1016/j.apcata.2025.120399","DOIUrl":"10.1016/j.apcata.2025.120399","url":null,"abstract":"<div><div>The development of bifunctional electrocatalyst for hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) with high catalytic activity and excellent stability can promote the application of hydrogen production by urea electrolysis. In this work, a three-dimensional composite heterogeneous electrocatalyst composed of NiMoP coating on Cu nanorods array on Cu foam (CF@Cu/NiMoP) is designed and synthesized. The CuO nanorods array constructed on Cu foam was used as the substrate for electrodeposition of NiMoP layer, while CuO substrate was reduced to Cu nanorods. The optimal deposition time was 20 min in both HER and UOR processes. Because the hierarchical nanorods array structure offers abundant active sites, accelerates electron transfer kinetics, and enables efficient multi-channel transport of electrolytes and gaseous byproducts, the optimized CF@Cu/NiMoP-20 has excellent HER and UOR performances with requiring only −94.9 mV and 1.395 V, respectively, to drive 100 mA cm<sup>−2</sup>. In addition, the overall urea-electrolysis system with CF@Cu/NiMoP-20 as bifunctional electrode provides 100 mA cm<sup>−2</sup> at a remarkably low cell voltage of 1.596 V. This energy-efficient performance can be readily powered by a commercially available mercury-free alkaline battery.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120399"},"PeriodicalIF":4.7,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144242034","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
Hierarchical MnOx loaded β zeolite as efficient catalyst for bulky aromatic hydrocarbon catalytic degradation 载MnOx分级β沸石催化降解大体积芳烃的研究
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-06-04 DOI: 10.1016/j.apcata.2025.120401
Shurui Duan , Yuan Xu , Li Xu , Si Wu , Tan Guo , Yu Wang
{"title":"Hierarchical MnOx loaded β zeolite as efficient catalyst for bulky aromatic hydrocarbon catalytic degradation","authors":"Shurui Duan ,&nbsp;Yuan Xu ,&nbsp;Li Xu ,&nbsp;Si Wu ,&nbsp;Tan Guo ,&nbsp;Yu Wang","doi":"10.1016/j.apcata.2025.120401","DOIUrl":"10.1016/j.apcata.2025.120401","url":null,"abstract":"<div><div>Conventional β zeolite exhibits limitations stemming from its constrained pore size and relatively low external surface area, impeding the efficient diffusion of bulky reactant molecules and limiting the accessibility and loading of active sites. Herein, we developed a hierarchical MnO<sub>x</sub> loaded β zeolite (MnO<sub>x</sub>/m-β) via a rational hydrothermal and subsequent redox-precipitation strategy. The hierarchical structure endows MnO<sub>x</sub>/m-β with a higher external surface area and optimized pore architecture, facilitating both the uniform dispersion of MnO<sub>x</sub> species and rapid diffusion of bulky molecules than conventional MnO<sub>x</sub>/β. Taking adsorption and catalytic oxidation of toluene, <em>o</em>-xylene, and 1,3,5-trimethylbenzene (TMB) as probe reactions, m-β exhibits significantly enhanced adsorption capacities for <em>o</em>-xylene (45.3 mg/g) and TMB (91.4 mg/g), representing 1.7 and 3.8 times increases compared to conventional β, respectively. Furthermore, MnO<sub>x</sub>/m-β achieves complete oxidation of toluene, <em>o</em>-xylene, and TMB at ca. 260 °C, 300 °C and 250 °C, respectively, significantly lower than those required for MnO<sub>x</sub>/β. This superior catalytic performance is attributed to the synergistic effects of enhanced Mn<sup>4 +</sup> -activated lattice oxygen mobility, hierarchical mass transfer channels, and abundant accessible active sites. The designed hierarchical architecture of β holds promise for the efficient removal of bulky aromatic hydrocarbon.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120401"},"PeriodicalIF":4.7,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144223318","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
Hydrogenation of 4-(2-furyl)-3-buten-2-one using Cu-double layered hydroxides modified with Zr and Ce Zr和Ce修饰cu -双层氢氧化物对4-(2-呋喃基)-3-丁烯-2-酮的加氢反应
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-06-04 DOI: 10.1016/j.apcata.2025.120394
Claudio Contreras-Díaz , Claudio Araya-Lopez , Cesar Pazo-Carballo , Marcos Flores , Vicente Diaz , Alejandro Karelovic , Ana Belén Dongil , Néstor Escalona
{"title":"Hydrogenation of 4-(2-furyl)-3-buten-2-one using Cu-double layered hydroxides modified with Zr and Ce","authors":"Claudio Contreras-Díaz ,&nbsp;Claudio Araya-Lopez ,&nbsp;Cesar Pazo-Carballo ,&nbsp;Marcos Flores ,&nbsp;Vicente Diaz ,&nbsp;Alejandro Karelovic ,&nbsp;Ana Belén Dongil ,&nbsp;Néstor Escalona","doi":"10.1016/j.apcata.2025.120394","DOIUrl":"10.1016/j.apcata.2025.120394","url":null,"abstract":"<div><div>The hydrogenation of 4-(2-furyl)-3-buten-2-one (FAc), derived from biomass through the aldol condensation of furfural and acetone, to obtain jet-fuel precursors and high-value products has been primarily performed using noble metals. In this study, the hydrogenation of FAc was studied using modified catalysts in which aluminum in CuMgAl double-layered hydroxides was partially or fully substituted with cerium (Ce) and zirconium (Zr) to induce oxygen vacancies. These vacancies were introduced to enhance catalytic performance by modifying the hydroxide structure. Characterization techniques, including N₂ adsorption–desorption, H₂-temperature-programmed reduction (TPR-H₂), N₂O-chemisorption, O₂-temperature-programmed desorption (TPD-O₂), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), were employed to characterize catalysts. The complete substitution of the Al layer with Ce or Zr significantly enhanced activity due to increased oxygen vacancy formation and improved electronic density at copper sites, resulting from variations in electronegativity. A similar product distribution at iso-conversions suggests consistent active sites across catalysts. Additionally, the Ce- and Zr-modified catalysts (CuMgCe and CuMgZr) increased selectivity toward 4-(2-furyl)-butan-2-ol, which subsequently led to the formation of 2-methyl-1,6-dioxaspiro[4,4]nonane through an intermolecular addition reaction was observed at 6 h reaction time.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120394"},"PeriodicalIF":4.7,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144291179","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
Base-free CO2 hydrogenation to methyl formate over Re/TiO2 catalysts: Effects of the crystal phase of TiO2 Re/TiO2催化剂上无碱CO2加氢制甲酸甲酯:TiO2晶相的影响
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-06-02 DOI: 10.1016/j.apcata.2025.120398
Xiyan Geng, Yali Peng, Yu Yue, Zhikun Xia, Zheng Fang, Ruiyan Sun, Kai Guo
{"title":"Base-free CO2 hydrogenation to methyl formate over Re/TiO2 catalysts: Effects of the crystal phase of TiO2","authors":"Xiyan Geng,&nbsp;Yali Peng,&nbsp;Yu Yue,&nbsp;Zhikun Xia,&nbsp;Zheng Fang,&nbsp;Ruiyan Sun,&nbsp;Kai Guo","doi":"10.1016/j.apcata.2025.120398","DOIUrl":"10.1016/j.apcata.2025.120398","url":null,"abstract":"<div><div>The crystal phase of TiO<sub>2</sub> plays a crucial role in tuning the catalytic performance of Re/TiO<sub>2</sub> catalysts for base-free CO<sub>2</sub> hydrogenation to methyl formate (MF). In this study, we investigated Re species supported on TiO<sub>2</sub> with different crystal phases (P25, rutile, and anatase) to elucidate their structure–activity relationships. Among them, P25-supported Re catalyst (denoted as Re/TiO<sub>2</sub>-P) exhibited the highest catalytic performance, achieving a turnover frequency (TOF) of 4.8 h<sup>–1</sup> at 150 °C for 2 h, along with excellent stability over five consecutive cycles. By reducing the catalyst dosage, the TOF was further increased to 10.3 h<sup>–1</sup> at 160 °C. Comprehensive characterization revealed that the superior performance of Re/TiO<sub>2</sub>-P arises from its relatively weak metal-support interaction, which facilitates the reduction of Re<sup>7+</sup> to Re<sup>4+</sup>, the key active species for H<sub>2</sub> activation. These findings highlight the crucial influence of the TiO<sub>2</sub> crystal phase on the oxidation state and catalytic behavior of Re species, offering valuable insights for designing efficient catalysts for base-free CO<sub>2</sub> hydrogenation to MF.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120398"},"PeriodicalIF":4.7,"publicationDate":"2025-06-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144223320","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
Tandem cooperative catalysis over a Zr-MOF for the synthesis of hydroxyurethanes under solvent-free conditions 无溶剂条件下Zr-MOF串联协同催化合成羟基脲
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-05-31 DOI: 10.1016/j.apcata.2025.120397
Anirban Ghosh , Sudip Bhattacharjee , Sayantan Chongdar , Tapas Sen , Soumadip Banerjee , Abhijit K. Das , Asim Bhaumik
{"title":"Tandem cooperative catalysis over a Zr-MOF for the synthesis of hydroxyurethanes under solvent-free conditions","authors":"Anirban Ghosh ,&nbsp;Sudip Bhattacharjee ,&nbsp;Sayantan Chongdar ,&nbsp;Tapas Sen ,&nbsp;Soumadip Banerjee ,&nbsp;Abhijit K. Das ,&nbsp;Asim Bhaumik","doi":"10.1016/j.apcata.2025.120397","DOIUrl":"10.1016/j.apcata.2025.120397","url":null,"abstract":"<div><div>Carbon sequestration via CO<sub>2</sub> fixation into value added chemicals is of great importance for the sustainable future of the world. Hydroxyurethane derivatives are very demanding chemical intermediate for the polymer and adhesive industries, which can be synthesized by a tandem sustainable route involving the fixing CO<sub>2</sub> on epoxides to cyclic carbonates followed by ring opening through aminolysis. In this work, we have synthesized a crystalline tritopic Zr-based metal-organic framework (MOF) having secondary building unit (SBU) as [Zr<sub>6</sub>(µ<sub>3</sub>-O)<sub>4</sub>(µ<sub>3</sub>-OH)<sub>4</sub>(OH)<sub>6</sub>(TPA-COOH)<sub>2</sub>] (TPA = triphenylamine), which we coined as Zr-TPA-MOF. This MOF was prepared through a sustainable microwave assisted synthesis route within 45 min. at 120 °C. Zr-TPA-MOF exhibited plate like morphology and possesses a good specific surface area of 312 m<sup>2</sup>g<sup>−1</sup>. Zr-TPA-MOF material displayed good reversible CO<sub>2</sub> uptakes at different temperatures (1.4 mmol at 273 K and 1.0 mmol at 298 K). We have also analyzed the thermodynamics of CO<sub>2</sub> affinity on Zr-TPA-MOF thoroughly. So, this property has been explored further, where Zr-TPA-MOF is used as a heterogeneous catalyst for the CO<sub>2</sub> fixation reaction to form hydroxyurethanes over different epoxides via tandem aminolysis. Here, we have enlightened a broader context of CO<sub>2</sub> fixation using nontoxic, cost effective Zr-MOF as a promising catalyst in isocyanate-free synthesis of hydroxyurethane derivatives.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120397"},"PeriodicalIF":4.7,"publicationDate":"2025-05-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144213322","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
Propylene oxidation to acrolein over Au@MoOx/MoO3 nanobelts driven by oxidative strong metal-support interactions 在Au@MoOx/MoO3纳米带上由氧化强金属-负载相互作用驱动的丙烯氧化成丙烯醛
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-05-31 DOI: 10.1016/j.apcata.2025.120395
Qingting Zhang , Yongbin Wu , Abouelhassan A. Gomaa , Andreas Goldbach
{"title":"Propylene oxidation to acrolein over Au@MoOx/MoO3 nanobelts driven by oxidative strong metal-support interactions","authors":"Qingting Zhang ,&nbsp;Yongbin Wu ,&nbsp;Abouelhassan A. Gomaa ,&nbsp;Andreas Goldbach","doi":"10.1016/j.apcata.2025.120395","DOIUrl":"10.1016/j.apcata.2025.120395","url":null,"abstract":"<div><div>Supported Au catalysts are widely investigated for selective oxidation processes. Here, propylene oxidation was studied over Au nanoparticles supported on MoO<sub>3</sub> nanobelts. Intriguingly, the Au particles were encapsulated by MoO<sub>x</sub> layers in oxidizing atmospheres yielding Au@MoO<sub>x</sub> aggregates which signal non-classical oxidative strong metal-support interaction (SMSI) between Au and MoO<sub>3</sub>. The core@shell particles enhanced the acrolein selectivity of MoO<sub>3</sub> from 18 % up to 81 % while its formation rate accelerated more than twentyfold to 1153 µmol g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> at 3 wt% Au loading and 350 °C. <em>In situ</em> CO DRIFTS measurements, H<sub>2</sub>-TPR and XPS analyses suggest that the Au@MoO<sub>x</sub> entities facilitate the transfer of MoO<sub>3</sub> lattice oxygen to propylene in line with the Mars-van Krevelen mechanism for acrolein formation. Apparent activation energies in the 113–163 kJ mol<sup>−1</sup> range point to re-oxidation of the ensuing oxygen-deficient MoO<sub>x</sub> moieties as rate-limiting acrolein formation step. Consequently, the oxidative SMSI strongly promotes propylene conversion to acrolein over MoO<sub>3</sub>-supported Au catalysts.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120395"},"PeriodicalIF":4.7,"publicationDate":"2025-05-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144223319","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
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信