Journal of Catalysis最新文献

筛选
英文 中文
Key role of yttrium doping on Cu/CeO2 (111) in water–gas shift reaction: Promotion of cluster dispersity 钇掺杂Cu/CeO2(111)在水气转换反应中的关键作用:促进团簇分散性
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-01 DOI: 10.1016/j.jcat.2025.116405
Yu-Xuan Zhu , Yingqi Wang , Gui-Chang Wang
{"title":"Key role of yttrium doping on Cu/CeO2 (111) in water–gas shift reaction: Promotion of cluster dispersity","authors":"Yu-Xuan Zhu ,&nbsp;Yingqi Wang ,&nbsp;Gui-Chang Wang","doi":"10.1016/j.jcat.2025.116405","DOIUrl":"10.1016/j.jcat.2025.116405","url":null,"abstract":"<div><div>Conventional theoretical models of electronic metal-support interaction (EMSI) often assume <strong><em>uniform metal dispersion</em></strong>, leading to conclusions conflicting with experimental observations. It highlights the critical need to incorporate <strong><em>metal dispersion effects</em></strong> in EMSI studies. Here, we investigate how Y<sup>3+</sup> doping regulates Cu cluster dispersion on CeO<sub>2</sub>(1 1 1) for the water–gas shift reaction (WGSR) using density functional theory (DFT), mean-field microkinetic modeling (MF-MKM), and kinetic Monte Carlo (kMC) simulations. Cohesion energy analysis reveals that on undoped ceria, bilayer clusters predominate. However, Y<sup>3+</sup> (compared to Ce<sup>4+</sup>) possesses a smaller radius and lower redox capability, which differentiates loading sites but obstructs EMSI. Excessive doping even restricts the formation of spillover oxygen (O<sub>sp</sub>), thereby favoring 3D clusters. The presence of surface spillover oxygen partially compensates for the EMSI weakening. This compensation effect causes the cohesive energy difference between bilayer and O<sub>sp</sub> planar-type clusters to become positive, resulting in the advantage of O<sub>sp</sub> planar-type clusters at lightly doping level. Kinetic simulations identify O<sub>sp</sub>-type planar copper clusters as functional active phases for undoped/lightly doped ceria, while heavily doped systems are regular planar clusters without O<sub>sp</sub>. O<sub>sp</sub>-type planar clusters exhibit extraordinary catalytic activity due to O<sub>sp</sub>-mediated adsorption and reactivity promotion, whereas bilayer clusters manifest low activity. Comprehensive analysis of cluster dispersion and structure–activity relationships discloses non-monotonic WGSR activity dependence on Y-doping: activity of sub-nanometer copper clusters peaks at low doping amount before declining at higher doping levels, aligning with experiments This work highlights the necessity of identifying both dispersion and activity of clusters for specific doping levels. These findings provide critical insights for the design of doped-supported catalysts and establish a theoretical framework for optimizing EMSI in heterogeneous catalysis.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116405"},"PeriodicalIF":6.5,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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 comprehensive theoretical study on CuOx/Cu(110) catalyzed water–gas shift reaction CuOx/Cu(110)催化水气转换反应的综合理论研究
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-01 DOI: 10.1016/j.jcat.2025.116404
Yu-Bi Huang , Yingqi Wang , Gui-Chang Wang
{"title":"A comprehensive theoretical study on CuOx/Cu(110) catalyzed water–gas shift reaction","authors":"Yu-Bi Huang ,&nbsp;Yingqi Wang ,&nbsp;Gui-Chang Wang","doi":"10.1016/j.jcat.2025.116404","DOIUrl":"10.1016/j.jcat.2025.116404","url":null,"abstract":"<div><div>In recent years, theoretical studies on Cu-based catalysts for the water–gas shift reaction (WGSR) have been conducted extensively. However, the issues concerning the oxidation state of copper atoms under reaction conditions and their roles in catalyzing WGSR remain unresolved. Surface science experiments have demonstrated that clean Cu(110) exhibits higher catalytic activity than clean Cu(111), and a previous study has theoretically indicated that the oxidation can enhance the intrinsic activity of Cu(111). Therefore, determining the surface oxides on Cu(110) and their catalytic activity is fundamental and will provide valuable insights for rational catalyst design. In this paper, ab initio atomistic thermodynamics was performed to reveal the potential phase transitions from clean Cu(110) to Cu<sub>2</sub>O (110), including added row-(4 × 1) (AR-41), added row-(2 × 1) (AR-21), as well as added strand-c(6 × 2) (AS-c62) structures. The WGSR mechanisms were systematically investigated on these distinct surfaces by density functional theory (DFT) calculations. Additionally, we identified a volcano-type relationship between the catalytic performance and the oxidation degree of Cu(110), with the mildly oxidized AR-41 structure exhibiting optimal activity, as determined by mean-field microkinetic modeling (MF-MKM) and kinetic Monte Carlo (kMC) simulations. Moreover, the degree of rate control (DRC) analysis revealed that water dissociation is no longer the rate-determining step for oxidized structures compared to clean Cu(110). Instead, the direct oxidation of CO and the production of H<sub>2</sub> may play a more critical role in CuO<sub>x</sub>/Cu(110)-catalyzed WGSR. Meanwhile, it was found that the redox and carboxyl mechanisms compete with each other. The carboxyl mechanism predominantly operates at low levels of oxidation, while the redox mechanism takes precedence at high levels of oxidation. Consequently, the appropriate oxidation state will enhance catalytic activity on Cu(110). Additionally, doping with other metal atoms was used as a strategy to improve catalyst performance, and it was found that doping with Pd or Zn may slightly promote the catalytic performance. Furthermore, a comparison between CuO<sub>x</sub>/Cu(110) and CuO<sub>x</sub>/Cu(111) was conducted, and it was found that they show different catalytic activity due to their unique interfaces of CuO<sub>x</sub> and metallic subsurface.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116404"},"PeriodicalIF":6.5,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144928589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Visible-light-driven aerobic oxidation via a dual ROS-generating manganese(II)-organic framework photocatalyst 通过双ros生成锰(II)-有机框架光催化剂的可见光驱动的好氧氧化
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-08-31 DOI: 10.1016/j.jcat.2025.116403
Hui Chen , Jiahui He , Zhen Zhou , Bin Wang , Xiong-Feng Ma , Maojun Deng , Yuanzhen Zhou , Pascal Van Der Voort
{"title":"Visible-light-driven aerobic oxidation via a dual ROS-generating manganese(II)-organic framework photocatalyst","authors":"Hui Chen ,&nbsp;Jiahui He ,&nbsp;Zhen Zhou ,&nbsp;Bin Wang ,&nbsp;Xiong-Feng Ma ,&nbsp;Maojun Deng ,&nbsp;Yuanzhen Zhou ,&nbsp;Pascal Van Der Voort","doi":"10.1016/j.jcat.2025.116403","DOIUrl":"10.1016/j.jcat.2025.116403","url":null,"abstract":"<div><div>Developing sustainable and efficient photocatalytic systems for aerobic oxidation remains a pivotal challenge in green chemistry. Herein, we report the rational design and synthesis of a novel manganese(II)-organic framework (An-MnMOF) by integrating anthracene-based photoactive ligands with Mn(II)-oxo clusters. The framework exhibits broad visible-light absorption extending up to 650 nm, efficient charge separation, and dual reactive oxygen species (ROS) generation capabilities. Structural characterization confirms a crystalline 2D lamellar architecture with hierarchical porosity, while mechanistic studies reveal a synergistic interplay between anthracene-mediated light harvesting and Mn(II)-driven redox processes. Under visible-light irradiation, An-MnMOF achieves exceptional catalytic performance in aerobic oxidation reactions, including hydroxylation of arylboronic acids (>95 % yield) and benzylic C(<em>sp</em><sup>3</sup>)-H bond activation (>85 % yield), outperforming the homogeneous Mn catalyst. The framework’s microporous channels stabilize reactive intermediates, suppressing overoxidation, while its robust chemical and thermal stability enables five consecutive recycling cycles without activity loss. This work establishes a paradigm for noble-metal-free photocatalysis by leveraging MOF-confined dual-function sites for solar-driven organic transformations, advancing sustainable synthesis methodologies.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116403"},"PeriodicalIF":6.5,"publicationDate":"2025-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924405","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Ir-catalyzed transfer hydrogenation and N-alkylation of alkynyl/alkenyl arylamines with carbonyls in water ir催化炔基/烯基芳胺与羰基在水中的转移加氢和n -烷基化反应
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-08-30 DOI: 10.1016/j.jcat.2025.116402
Jianhua Liao, Huajie Zhu, Shilin Guo, Jinhui Li, Lu Ouyang, Renshi Luo
{"title":"Ir-catalyzed transfer hydrogenation and N-alkylation of alkynyl/alkenyl arylamines with carbonyls in water","authors":"Jianhua Liao,&nbsp;Huajie Zhu,&nbsp;Shilin Guo,&nbsp;Jinhui Li,&nbsp;Lu Ouyang,&nbsp;Renshi Luo","doi":"10.1016/j.jcat.2025.116402","DOIUrl":"10.1016/j.jcat.2025.116402","url":null,"abstract":"<div><div>Herein, we advance a novel and efficient iridium-catalyzed transfer hydrogenation and <em>N</em>-alkylation of alkynyl/alkenyl arylamines with carbonyls to facilitate the streamlined synthesis of diverse amines. The reaction could be achieved direct hydrogenation and alkylation of alkynyl/alkenyl arylamines with carbonyls using H<sub>2</sub>O as reaction media and HCO<sub>2</sub>H as hydrogen donor, providing a variety of arylamine derivatives in moderate to excellent yields. Control experiments indicated the <em>N</em>-alkylation of alkynyl/alkenyl arylamines contributed to the reduction of alkynes/alkenes. The practicality of this sustainable process was evidenced by large-scale, catalyst recycling experiments and derivatization of biologically active molecules.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116402"},"PeriodicalIF":6.5,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144919085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Unraveling B, N Co-doping synergy in graphitic carbon nitride for efficient CO2 cycloaddition with styrene oxide 揭示B, N共掺杂在石墨氮化碳与苯乙烯氧化物的高效CO2环加成中的协同作用
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-08-29 DOI: 10.1016/j.jcat.2025.116399
Hafila S. Khairun , Gazala Parveen , Ripsa Rani Nayak , Jogeswar Chhatria , Sooraj Kunnikuruvan , Navneet Kumar Gupta
{"title":"Unraveling B, N Co-doping synergy in graphitic carbon nitride for efficient CO2 cycloaddition with styrene oxide","authors":"Hafila S. Khairun ,&nbsp;Gazala Parveen ,&nbsp;Ripsa Rani Nayak ,&nbsp;Jogeswar Chhatria ,&nbsp;Sooraj Kunnikuruvan ,&nbsp;Navneet Kumar Gupta","doi":"10.1016/j.jcat.2025.116399","DOIUrl":"10.1016/j.jcat.2025.116399","url":null,"abstract":"<div><div>The cycloaddition of CO<sub>2</sub> and styrene oxide to produce styrene carbonate under solvent-free conditions offers an eco-friendly, atom-efficient, and highly effective approach to CO<sub>2</sub> utilization. This study presents a highly active and selective catalytic system based on boron and nitrogen co-doped graphitic carbon nitride (BN-GCN) for the efficient production of styrene carbonate. Unlike many conventional catalysts, the BN-GCN system operates without needing solvents or metals, functioning as a metal-free heterogeneous catalyst for the cycloaddition of CO<sub>2</sub> with styrene oxide. It outperforms other heteroatom-doped graphitic carbon nitride (X-GCN) catalysts, with the enhanced activity attributed to the synergistic interaction of reactants with B and N sites. XPS analysis reveals that the N moiety and the B atom are critical active sites for cooperative catalysis. The BN-GCN catalyst achieves 75 % conversion and &gt; 90% selectivity for styrene carbonate (SC) formation under mild conditions (353 K, 2 bar CO<sub>2</sub>) within 3 h. Comprehensive material characterization, kinetic studies, and reaction data confirm that B and N co-doping facilitates the co-activation of CO<sub>2</sub> and epoxide. Based on density functional theory (DFT) calculations, and experiments, a convenient mechanism has been proposed for this unique method. The B–N bond duality in BN-GCN offers a cost-effective, sustainable, and efficient catalytic pathway for CO<sub>2</sub> utilization.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116399"},"PeriodicalIF":6.5,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144915847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Construction of visible light-driven ternary S-scheme melamine sponge MS/TpTt/ZIS heterojunction photocatalysts for enhanced photocatalytic pollutant removal and hydrogen evolution 可见光驱动三元S-scheme三聚氰胺海绵MS/TpTt/ZIS异质结光催化剂的构建
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-08-29 DOI: 10.1016/j.jcat.2025.116388
Qingmei Tang , Yuqi Wan , Yuzhuo Wan , Zhiquan Pan , Qingrong Cheng
{"title":"Construction of visible light-driven ternary S-scheme melamine sponge MS/TpTt/ZIS heterojunction photocatalysts for enhanced photocatalytic pollutant removal and hydrogen evolution","authors":"Qingmei Tang ,&nbsp;Yuqi Wan ,&nbsp;Yuzhuo Wan ,&nbsp;Zhiquan Pan ,&nbsp;Qingrong Cheng","doi":"10.1016/j.jcat.2025.116388","DOIUrl":"10.1016/j.jcat.2025.116388","url":null,"abstract":"<div><div>Charge separation critical for improving photocatalytic performance. But single semiconductor cannot realize efficient charge separation and transport. Little research has been reported on using melamine foam (MS) as a carrier. Herein, we have successfully synthesized a heterojunction MS/TpTt/ZnIn<sub>2</sub>S<sub>4</sub>-x% (MTZIS-x%) photocatalysis with MS as the carrier by solvothermal method. It was found the degradation rate of MO over MTZIS-3 % could reach almost 100 %, and the biotoxicity tests showed that degraded residual liquid of MO was almost non-biological toxicity. Moreover, the ptotocatalytic H<sub>2</sub> evolution rate of MTZIS-3 % reached to 11523.64 µmol g<sup>−1</sup>h<sup>−1</sup>, which was 7.02, 11.91 and 13.19 times than that of ZIS, MS/TpTt and COF-TpTt. And the evolution rate of photoreduction CO<sub>2</sub> to CO was 501.55 µmol g<sup>−1</sup> h<sup>−1</sup>. The excellent photocatalytic property was owing to the S-scheme band structure facilitated the separation of electron-hole efficiently and retained the highly reducing electrons. This work provided a theoretical reference for the construction of efficient new heterojunction photocatalysts using MS as a carrier.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116388"},"PeriodicalIF":6.5,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144919124","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Solventless and low-temperature ring-opening polymerization using deep eutectic solvents of ε-caprolactone and their depolymerization cycles for biodegradable polyesters ε-己内酯深共晶溶剂无溶剂低温开环聚合及其解聚循环
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-08-29 DOI: 10.1016/j.jcat.2025.116400
Puracheth Rithchumpon , Wanich Limwanich , Kraikrit Utama , Nathaporn Cheechana , Natthapol Akkravijitrkul , Padchanee Sangthong , Winita Punyodom , Puttinan Meepowpan
{"title":"Solventless and low-temperature ring-opening polymerization using deep eutectic solvents of ε-caprolactone and their depolymerization cycles for biodegradable polyesters","authors":"Puracheth Rithchumpon ,&nbsp;Wanich Limwanich ,&nbsp;Kraikrit Utama ,&nbsp;Nathaporn Cheechana ,&nbsp;Natthapol Akkravijitrkul ,&nbsp;Padchanee Sangthong ,&nbsp;Winita Punyodom ,&nbsp;Puttinan Meepowpan","doi":"10.1016/j.jcat.2025.116400","DOIUrl":"10.1016/j.jcat.2025.116400","url":null,"abstract":"<div><div>The catalytic performance of deep eutectic solvents (DESs) between choline chloride (ChCl) and organic acids was investigated for the ring-opening polymerization (ROP) of <em>ε</em>-caprolactone (CL). These organic acids act as hydrogen bond donors (HBDs), while choline chloride serves as the hydrogen bond acceptor (HBA). Among fifteen acids, (–)-camphorsulfonic acid (CSA), diphenyl phosphate (DPP), 2,5-dimethylbenzenesulfonic acid (DSA), and <em>p</em>-toluenesulfonic acid (PTSA) with ChCl at 100:1:1 M ratio could effectively poly(<em>ε</em>-caprolactone) (PCL) with the molecular weight ranging from 8,000 to 10,000 g/mol and a low dispersity (<em>Ð</em>) (1.2–1.5). The ROP kinetics was powerfully investigated differential scanning calorimetry (DSC) technique. PTSA in combination with ChCl exhibited the fastest reaction and the lowest activation energy (<em>E<sub>a</sub></em>). Additionally, the depolymerization processes of PCL back to its CL monomer was studied by thermogravimetric analysis (TGA). Notably, phosphotungstic acid (PTA) demonstrated the highest depolymerization activity achieving a 100 % yield of CL at 160 °C for 1 h under vacuum distillation.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116400"},"PeriodicalIF":6.5,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144919132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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 terphenyl phosphine TRuPhos: a novel and efficient ligand for the palladium-catalyzed arylation of hindered primary alkyl amines with mechanism clarification terphenyl phospine TRuPhos:钯催化受阻伯烷基胺芳基化的新型高效配体及其机理澄清
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-08-28 DOI: 10.1016/j.jcat.2025.116391
Lixue Zhang , Guoyu Cheng , Fabin Zhou , Xin Yang , Huicheng Cheng , Mei Yu , Dahong Jiang , Peng Zhou , He Yang , Bingxin Yuan , Wenjun Tang , Ji-cheng Shi
{"title":"The terphenyl phosphine TRuPhos: a novel and efficient ligand for the palladium-catalyzed arylation of hindered primary alkyl amines with mechanism clarification","authors":"Lixue Zhang ,&nbsp;Guoyu Cheng ,&nbsp;Fabin Zhou ,&nbsp;Xin Yang ,&nbsp;Huicheng Cheng ,&nbsp;Mei Yu ,&nbsp;Dahong Jiang ,&nbsp;Peng Zhou ,&nbsp;He Yang ,&nbsp;Bingxin Yuan ,&nbsp;Wenjun Tang ,&nbsp;Ji-cheng Shi","doi":"10.1016/j.jcat.2025.116391","DOIUrl":"10.1016/j.jcat.2025.116391","url":null,"abstract":"<div><div>Terphenyl phosphines are rising as powerful supporting ligands in the palladium-catalyzed C-N cross-coupling reactions, leading to reduced catalyst loadings and broadened substrate scope. To extend the terphenyl phosphine family, TRuPhos and TSPhos along with their 2-amino-biphenyl-ƞ<sup>2</sup>-C,N palladium precatalysts have been synthesized and characterized, including one complex by single-crystal diffraction. TRuPhos exhibits unprecedented efficiency in the palladium-catalyzed arylation of many hindered primary alkyl amines. Mechanism studies have clarified that: 1) the transmetalation <strong>path A</strong> involving amine adducts of oxidative addition product does not work by the TRuPhos-supported palladium catalyst in the arylation of hindered primary alkyl amines, but works for that in small bulk amines; 2) the <strong>path C</strong> involving the substitution of halogen atoms on oxidative addition products by <em>t</em>BuO groups seems impossible as well; 3) the reaction occurred between oxidative addition products and sodium amides forming C-N coupling products suggests that <strong>path B</strong> is a possible transmetalation pathway in Pd/TRuPhos-catalyzed arylation of hindered primary alkyl amines.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116391"},"PeriodicalIF":6.5,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144910684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Enhanced hydrogen production performance and stability simultaneously in aqueous-phase reforming of methanol over Pt/V2O3-V8C7 based on strong-weak metal support interactions 基于强-弱金属载体相互作用的Pt/V2O3-V8C7上甲醇水相重整同时增强制氢性能和稳定性
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-08-27 DOI: 10.1016/j.jcat.2025.116397
Yuhao Yang , Jie Ran , Teng Wang , Yongning Ma , Junli Zhu , Xiaolong Li , Zhuoya Zhao
{"title":"Enhanced hydrogen production performance and stability simultaneously in aqueous-phase reforming of methanol over Pt/V2O3-V8C7 based on strong-weak metal support interactions","authors":"Yuhao Yang ,&nbsp;Jie Ran ,&nbsp;Teng Wang ,&nbsp;Yongning Ma ,&nbsp;Junli Zhu ,&nbsp;Xiaolong Li ,&nbsp;Zhuoya Zhao","doi":"10.1016/j.jcat.2025.116397","DOIUrl":"10.1016/j.jcat.2025.116397","url":null,"abstract":"<div><div>Aqueous phase reforming of methanol (APRM) is an effective method for the storage and transportation of hydrogen (H<sub>2</sub>). However, this approach faces challenges due to the limited activity and stability of metal-supported catalysts. In this study, Pt/V<sub>2</sub>O<sub>3</sub>-V<sub>8</sub>C<sub>7</sub> metal-supported catalysts were prepared for APRM and the H<sub>2</sub> production of Pt/V<sub>2</sub>O<sub>3</sub>-V<sub>8</sub>C<sub>7</sub> at 200 °C was 96.52 mmol·g<sup>−1</sup>·h<sup>−1</sup>, which is 1.83 times and 1.71 times higher than the H<sub>2</sub> production performance of Pt/V<sub>2</sub>O<sub>3</sub> and Pt/V<sub>8</sub>C<sub>7</sub>, respectively. Moreover, the catalyst demonstrated remarkable stability after 10 in situ cycling tests. Structural characterization revealed that there is a strong metal-support interaction (SMSI) between Pt and V<sub>8</sub>C<sub>7</sub>, and a weak metal-support interaction (WMSI) between Pt and V<sub>2</sub>O<sub>3</sub>, which inhibits the sintering of Pt on the metal-supported catalyst. Furthermore, a straightforward experimental method has been developed that enables accurate inference of the catalytic reaction mechanism in APRM without the need for in situ material characterization. The reaction mechanism indicates that the Pt-V<sub>8</sub>C<sub>7</sub> interface serves as the active site for the methanol decomposition step, while the surface of V<sub>2</sub>O<sub>3</sub> acts as the active site for the water–gas shift reaction step. This strategy of strong–weak MSI offers a novel approach to enhancing both the stability and H<sub>2</sub> production performance in APRM.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116397"},"PeriodicalIF":6.5,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144905974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Carbazolyl-based metal organic framework for photocatalytic antibiotic degradation and H2O2 green generation assisted by silver nanoparticles 纳米银辅助下咔唑基金属有机骨架光催化抗生素降解及H2O2绿色生成
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-08-27 DOI: 10.1016/j.jcat.2025.116401
Shan Ding , Yu-Ting Hui , Qingfeng Wei , Guang-Sheng Yang , Zhe Tang , Shi-Qi Wang , Xinning Zhang , Yi-Jia Wang , Chunjie Jiang
{"title":"Carbazolyl-based metal organic framework for photocatalytic antibiotic degradation and H2O2 green generation assisted by silver nanoparticles","authors":"Shan Ding ,&nbsp;Yu-Ting Hui ,&nbsp;Qingfeng Wei ,&nbsp;Guang-Sheng Yang ,&nbsp;Zhe Tang ,&nbsp;Shi-Qi Wang ,&nbsp;Xinning Zhang ,&nbsp;Yi-Jia Wang ,&nbsp;Chunjie Jiang","doi":"10.1016/j.jcat.2025.116401","DOIUrl":"10.1016/j.jcat.2025.116401","url":null,"abstract":"<div><div>Tetracycline, a widely used antibiotic that persists in the environment, is a significant pollutant, making its efficient degradation crucial for ecosystem and human health. Meanwhile, green production of hydrogen peroxide, an important chemical raw material and green oxidant, is significant in various fields. In this study, a novel visible-light-responsive photocatalyst, the ACM-X series material, was successfully synthesized through post-synthetic modification of Cz-MOF-2, with the deposition of Ag nanoparticles on the surface significantly enhancing the photocatalytic performance, enabling efficient degradation of tetracycline (TC) and high-yield production of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) under simulated solar light irradiation. The Ag surface plasmon resonance (SPR) effect played a crucial role in improving charge separation efficiency, as confirmed by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and electrochemical measurements. The ACM-1 catalyst demonstrated exceptional photocatalytic activity, achieving over 95 % TC degradation within 60 min and a H<sub>2</sub>O<sub>2</sub> production rate of 50 μmol/h. The free radical scavenging experiments and electron paramagnetic resonance (EPR) technique confirmed that reactive oxygen species (ROS), including superoxide anion radicals (·O<sub>2</sub><sup>−</sup>), hydroxyl radicals (·OH) and singlet oxygen (<sup>1</sup>O<sub>2</sub>), were identified as key intermediates in the photocatalytic process. Density functional theory (DFT) calculations revealed that Ag modification reduced the band gap of Cz-MOF-2, enhancing light absorption and promoting electron transfer. The 2e<sup>−</sup> oxygen reduction reaction (ORR) for H<sub>2</sub>O<sub>2</sub> production was found to be spontaneous, with Ag acting as an electron and proton transfer mediator. Additionally, the degradation pathway of tetracycline (TC) was elucidated by using a mass spectrometer. The ACM − 1 catalyst exhibited excellent stability and reusability during multiple cycles of use, highlighting its potential in environmental remediation and sustainable chemical synthesis. This work provides a promising strategy for the design of advanced photocatalysts for solar energy conversion and pollutant degradation.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116401"},"PeriodicalIF":6.5,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144906336","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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