Journal of Catalysis最新文献

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Consequences of altering acid strength in MFI zeolites via phosphorus modification on Friedel-Crafts acylation 磷改性对Friedel-Crafts酰化改变MFI沸石酸强度的影响
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-05 DOI: 10.1016/j.jcat.2025.116096
Ismaeel Alalq , Ana Carolina Jerdy , Huy Nguyen-Phu , Anya Zornes , Matt Wulfers , Dan Nielsen , Daniel Resasco , Jeffery L. White , Steven Crossley
{"title":"Consequences of altering acid strength in MFI zeolites via phosphorus modification on Friedel-Crafts acylation","authors":"Ismaeel Alalq ,&nbsp;Ana Carolina Jerdy ,&nbsp;Huy Nguyen-Phu ,&nbsp;Anya Zornes ,&nbsp;Matt Wulfers ,&nbsp;Dan Nielsen ,&nbsp;Daniel Resasco ,&nbsp;Jeffery L. White ,&nbsp;Steven Crossley","doi":"10.1016/j.jcat.2025.116096","DOIUrl":"10.1016/j.jcat.2025.116096","url":null,"abstract":"<div><div>Friedel-Crafts acylation is an important reaction for the formation of C<img>C bonds to produce a variety of commodity chemicals. Recent efforts have been made to reduce the environmental footprint of these reactions by utilizing renewable carboxylic acids directly (rather than halogenated species), using renewable acyl acceptors, and using zeolites as non-sacrificial catalysts. While the direct conversion of acids to valuable products is appealing, the role of acid strength and local environment on rates and stability for this reaction is unknown. Here we report the acylation of 2-methylfuran with acetic acid over phosphorus-modified MFI zeolites with various phosphorus loadings. We show that while P modification increases observed activation barriers for acylation when compared with traditional Bronsted sites, net rates of reaction can be increased. Further, selectivity is improved by reduced rates of acid self-coupling side reactions to a greater extent. Importantly, the phosphorus-modified samples also exhibit slower coke formation, and therefore deactivation, due to diminished side reactions.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116096"},"PeriodicalIF":6.5,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782770","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
Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy Ag/InOxHy中高密度受挫Lewis对促进光热催化非氧化甲烷偶联
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-05 DOI: 10.1016/j.jcat.2025.116117
Ziyuan Yan , Xiaoning Li , Xinwei Guan , Zhaoliang Wang , Jinni Shen , Tingjiang Yan , Tianyi Ma , Zizhong Zhang
{"title":"Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy","authors":"Ziyuan Yan ,&nbsp;Xiaoning Li ,&nbsp;Xinwei Guan ,&nbsp;Zhaoliang Wang ,&nbsp;Jinni Shen ,&nbsp;Tingjiang Yan ,&nbsp;Tianyi Ma ,&nbsp;Zizhong Zhang","doi":"10.1016/j.jcat.2025.116117","DOIUrl":"10.1016/j.jcat.2025.116117","url":null,"abstract":"<div><div>The photocatalytic nonoxidative coupling of methane (CH<sub>4</sub>) is crucial for sustainable energy production and chemical synthesis, however, a key challenge in advancing this process lies in the development of efficient and highly selective catalytic systems. In this study, we employ an in situ thermally induced strategy to promote the in-situ growth of oxygen vacancies (V<sub>O</sub>) for constructing a high-density In-V<sub>O</sub>-In-OH frustrated Lewis pairs (FLP) on Ag/In(OH)<sub>3</sub>-InOOH (Ag/InO<sub>x</sub>H<sub>y</sub>). Our results demonstrate that FLP can effectively polarize C–H bonds, while Ag nanoparticles serve as electron acceptors, significantly reducing the recombination of photogenerated carriers and enhancing the catalytic performance of methane coupling. Benefiting from the high density of FLP and photothermal synergistic effect, we achieve a remarkable C<sub>2</sub>H<sub>6</sub> yield of 339.2 μmol g<sub>cat</sub><sup>−1</sup>h<sup>−1</sup> over Ag/InO<sub>x</sub>H<sub>y</sub> in a flow methane atmosphere. Notably, in-situ electron<!--> <!-->paramagnetic resonance analysis not only validates this innovative strategy but also reveals a new mechanism of oxygen vacancy recycling which showcases its great potential to advance other photocatalytic processes.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116117"},"PeriodicalIF":6.5,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782771","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
Design targeted high entropy sulfides catalysts for OER by theoretical predictions 根据理论预测设计目标高熵硫化物OER催化剂
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-04 DOI: 10.1016/j.jcat.2025.116114
Mengyuan Zhang , Kongliang Luo , Peixuan Li , Hailong Li , Chuandong He , Junjun Zhang , Qiang Niu , Pengfei Zhang
{"title":"Design targeted high entropy sulfides catalysts for OER by theoretical predictions","authors":"Mengyuan Zhang ,&nbsp;Kongliang Luo ,&nbsp;Peixuan Li ,&nbsp;Hailong Li ,&nbsp;Chuandong He ,&nbsp;Junjun Zhang ,&nbsp;Qiang Niu ,&nbsp;Pengfei Zhang","doi":"10.1016/j.jcat.2025.116114","DOIUrl":"10.1016/j.jcat.2025.116114","url":null,"abstract":"<div><div>Currently, using Density Functional Theory (DFT) to drive the synthesis of targeted oxygen evolution reaction (OER) catalysts, has attracted strong attention. Herein, sulfides were selected as the models. First, the density of states (DOS), active sites and the Gibbs free energy of intermediates (ΔG) of different models were calculated respectively. DFT results indicated that d-band centers of models with sulfur vacancies, self-reconstruction, or high entropy structures possessing lower ΔG<sub>max</sub>, being closer to the Fermi level, exhibiting higher DOS at the Fermi level. To verify DFT results, thiourea was used as a precursor to prepare (CrMnCoNiMo)<sub>0.2</sub>S<sub>x</sub> for the first time. Indeed, (CrMnCoNiMo)<sub>0.2</sub>S<sub>x</sub> exhibited excellent OER activity (η<sub>100</sub> = 266 mV, Tafel slope = 57.4 mV dec<sup>−1</sup>) and strong catalytic stability. The sulfur vacancies were confirmed by EPR experiments. TEM, XPS and ICP-AES all confirmed the leaching of Cr and Mo elements after OER. XPS, TEM and In situ Raman confirmed the self-reconstruction of (CrMnCoNiMo)<sub>0.2</sub>S<sub>x</sub> during the OER. The above experimental results perfectly confirmed the initial DFT calculation.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116114"},"PeriodicalIF":6.5,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782772","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 MOF-on-MOF-derived composites with coexisting octahedrons and dodecahedrons for superior photocatalytic nitrogen fixation 八面体与十二面体共存的mof -on- mof衍生复合材料的光催化固氮性能研究
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-04 DOI: 10.1016/j.jcat.2025.116121
Runxian Hao , Zaihang Zheng , Yixin Li, Meili Zheng, Songquan Pan, Jie Hu, Hao Huang
{"title":"Construction of MOF-on-MOF-derived composites with coexisting octahedrons and dodecahedrons for superior photocatalytic nitrogen fixation","authors":"Runxian Hao ,&nbsp;Zaihang Zheng ,&nbsp;Yixin Li,&nbsp;Meili Zheng,&nbsp;Songquan Pan,&nbsp;Jie Hu,&nbsp;Hao Huang","doi":"10.1016/j.jcat.2025.116121","DOIUrl":"10.1016/j.jcat.2025.116121","url":null,"abstract":"<div><div>The photocatalytic ammonia synthesis provides a promising alternative for the sustainable production of ammonia. However, poor separation efficiency of photoinduced carriers and insufficient activation of N<sub>2</sub> remain the key obstacles to high-performance N<sub>2</sub> reduction. Herein, a MOF-on-MOF-derived material with a Z-scheme heterojunction has been reported. The Brunauer-Emmett-Teller (BET) and electrochemical impedance spectroscopy (EIS) analyses indicate that the coexistence of the two MOFs accelerates the mass transfer process at the gas-solid-liquid interface and promotes the diffusion process of nitrogen molecules to the heterogeneous interface, thereby facilitating the adsorption of N<sub>2</sub>. According to analyses of Diffuse Reflectance Spectroscopy (DRS), Mott-Schottky (M−S) and density functional theory (DFT), the MIL-101(Fe)/ZIF-67 derived material (MZ-600) complies with the charge transfer mechanism of the Z-scheme heterojunction, which realizes the effective separation of photogenerated carriers and preserves the strong redox capacity of electrons and holes. Meanwhile, it stimulates the activation of the N≡N bond and lowers the energy barrier of the rate determining step(*N<sub>2</sub>→*N<sub>2</sub>H). Therefore, the rationally designed MZ-600 heterojunction exhibits remarkable PNRR performance, with an NH<sub>3</sub> yield of 103.90 μmol·g<sup>−1</sup>·h<sup>−1</sup> and an apparent quantum yield (AQY) of 1.17 % at 465 nm. Moreover, compared to catalyst powder, the MZ-600 catalyst supported on vertical carbon paper can decrease recontamination and is convenient to be recycled.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116121"},"PeriodicalIF":6.5,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782775","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 photothermal catalytic activity of CeO2 through Co-modified for the carbonylation of amine with CO2 用共改性方法提高了CeO2的光热催化活性
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-04 DOI: 10.1016/j.jcat.2025.116122
Dalei Sun , Hongyu Li , Chen Zhou , Jinghui Cai , Zhi-Wu Liang
{"title":"Enhanced photothermal catalytic activity of CeO2 through Co-modified for the carbonylation of amine with CO2","authors":"Dalei Sun ,&nbsp;Hongyu Li ,&nbsp;Chen Zhou ,&nbsp;Jinghui Cai ,&nbsp;Zhi-Wu Liang","doi":"10.1016/j.jcat.2025.116122","DOIUrl":"10.1016/j.jcat.2025.116122","url":null,"abstract":"<div><div>The photothermal catalytic carbonylation of n-alkylamine with CO<sub>2</sub> is one of the most promising “carbon neutral” pathways due to the coupling of CO<sub>2</sub> capture and conversion. And the development of high-performance catalysts is vital to the reaction due to the inherent chemical inertness of CO<sub>2</sub>. Herein, Co-Ce composite oxides with rich oxygen vacancy (O<sub>v</sub>) were successfully synthesized via hydrothermal method and applied firstly to photothermal catalytic carbonylation of n-butyl amine with CO<sub>2</sub>. As optimizing the molar ratio of Co<sub>3</sub>O<sub>4</sub>/CeO<sub>2</sub>, Co<sub>3</sub>O<sub>4</sub>/CeO<sub>2</sub>-0.4 with up to both 95.51 % of n-butylamine conversion and 94.50 % of N,N′-dibutylurea were obtained in the presence of PEG 400 solvent using 500 W Xe lamp as the light source under 110 ℃ and 1.0 MPa for 4 h, respectively. Further characterizations such as XRD, BET, Raman, XPS, CO<sub>2</sub>/NH<sub>3</sub>-TPD, UV–Vis, PL and TPC show that both the high photocurrent density and O<sub>v</sub>-rich content on the surface of Co<sub>3</sub>O<sub>4</sub>/CeO<sub>2</sub>-0.4 enhances the adsorption-activation of CO<sub>2</sub> by facilitating the migration of d electrons from the active sites to the 2π antibonding orbitals <strong>of</strong> CO<sub>2</sub>. Finally, a Lewis acid-base interactions mechanism was also proposed in the photothermal catalytic carbonylation of amine by CO<sub>2</sub> over the Co-Ce complex oxides.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116122"},"PeriodicalIF":6.5,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782773","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
Optimizing photocatalytic degradation of dichloromethane by MOF-derived TiO2/C catalyst: Unraveling the decisive role of carbon nanolayers and reaction mechanism 优化 MOF 衍生 TiO2/C 催化剂对二氯甲烷的光催化降解:揭示碳纳米层的决定性作用和反应机理
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-04 DOI: 10.1016/j.jcat.2025.116123
Maosen Xu , Shanshan Zhao , Jinhua Feng , Yunzheng Deng , Yuemeng Ji , Yingxin Yu , Hongli Liu , Taicheng An
{"title":"Optimizing photocatalytic degradation of dichloromethane by MOF-derived TiO2/C catalyst: Unraveling the decisive role of carbon nanolayers and reaction mechanism","authors":"Maosen Xu ,&nbsp;Shanshan Zhao ,&nbsp;Jinhua Feng ,&nbsp;Yunzheng Deng ,&nbsp;Yuemeng Ji ,&nbsp;Yingxin Yu ,&nbsp;Hongli Liu ,&nbsp;Taicheng An","doi":"10.1016/j.jcat.2025.116123","DOIUrl":"10.1016/j.jcat.2025.116123","url":null,"abstract":"<div><div>In-depth dissecting the activation of C-Cl bonds and the migration transformation of dissociated chlorine species is significant to understand the mechanism underlying the formation of polychlorinated by products and chlorine poisoning deactivation of catalyst during of the photocatalytic degradation of chlorinated volatile organic compounds (CVOCs). Herein, carbon nanolayers wrapped TiO<sub>2</sub> composites (CTO), and its contrastive catalysts including defective carbon nanolayers wrapped TiO<sub>2</sub> (DCTO) and TiO<sub>2</sub> without carbon nanolayer (TO) are constructed by rational pyrolysis of titanium-based MOFs. The obtained CTO exhibits a remarkable degradation efficiency of up to 91.74 % for CH<sub>2</sub>Cl<sub>2</sub> after 3 h of UV–vis irradiation, robust stability as well as water resistance, far superior to that of DCTO and TO. Density functional theory calculations combined with <em>in-situ</em> XPS reveal that the heterogeneous interface interactions between carbon nanolayers and TiO<sub>2</sub> greatly facilitate the separation of photogenerated carriers, boosting the redox capacity of CTO. Simultaneously, the dissociated Cl species from the cleavage of the C-Cl bond can be preferentially adsorbed onto the outer carbon nanolayers, thereby inhibiting the occupation of TiO<sub>2</sub> active sites by chlorine. The preferential adsorption sites of the dissociated Cl species and optimized deep oxidation ability synergistically boost the catalytic performance and resistance of chlorine poisoning and inhibit the production of polychlorinated by-products.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116123"},"PeriodicalIF":6.5,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782974","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
Simultaneous boosting visible light-driven benzene hydroxylation reaction rate and phenol selectivity via a novel monolithic polymer photoreactive composite based on N-doped TiO2 supported CuO 基于n掺杂TiO2负载CuO的新型单片聚合物光反应复合材料同时提高可见光驱动苯羟基化反应速率和苯酚选择性
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-03 DOI: 10.1016/j.jcat.2025.116116
Antonietta Mancuso , Olga Sacco , Vincenzo Vaiano , Vincenzo Venditto
{"title":"Simultaneous boosting visible light-driven benzene hydroxylation reaction rate and phenol selectivity via a novel monolithic polymer photoreactive composite based on N-doped TiO2 supported CuO","authors":"Antonietta Mancuso ,&nbsp;Olga Sacco ,&nbsp;Vincenzo Vaiano ,&nbsp;Vincenzo Venditto","doi":"10.1016/j.jcat.2025.116116","DOIUrl":"10.1016/j.jcat.2025.116116","url":null,"abstract":"<div><div>A novel photoreactive composite consisting of CuO-loaded N-doped TiO<sub>2</sub> (CuNdT) embedded in a syndiotactic polystyrene (sPS) monolithic aerogel was developed and evaluated for the photocatalytic hydroxylation of benzene to phenol under visible light irradiation. The process was identified as biphasic, where the photoreaction occurred within the solid phase of the composite, and the surrounding liquid phase acted as a reservoir for the desired product (phenol). The composite was extensively characterized through WAXD, SEM, BET, and tomographic analyses, confirming the uniform dispersion of CuNdT particles within the porous, hydrophobic sPS matrix. Under acidic conditions (pH = 2), the composite achieved 96 % benzene conversion and &gt;99 % phenol selectivity within 180 min of irradiation, results that surpass those reported in the literature for visible-light-driven benzene hydroxylation. Kinetic modeling, based on experimentally determined partition coefficients for benzene and phenol, revealed that the composite operated entirely in a chemical regime, free from diffusional limitations. The calculated efficiency factors, all equal to 1, confirmed that the reaction was controlled solely by chemical processes occurring on the CuNdT dispersed inside the sPS matrix. The differences in kinetic constants between pH = 7 and pH = 2 highlighted the critical role of pH in driving the photocatalytic process. At pH = 2, the increased tendency of H<sub>2</sub>O<sub>2</sub> to form hydroxyl radicals enhanced the rates of benzene consumption and phenol formation. Additionally, the higher affinity of benzene for the hydrophobic sPS polymer matrix at acidic pH, as reflected by its elevated partition coefficient, further facilitated its interaction with the composite, promoting faster oxidation. In contrast, phenol displayed a lower affinity for the hydrophobic sPS matrix at pH = 2, as evidenced by its lower partition coefficient, allowing it to remain in the liquid phase, reducing over-oxidation and contributing to the higher phenol yield (96 %) observed at acidic pH. This synergistic effect between enhanced hydroxyl radical generation, increased benzene affinity and reduced phenol affinity led to a more efficient photocatalytic process under acidic conditions. These findings establish CuNdT/sPS as a highly efficient, selective, and robust photocatalytic material, combining superior performance, structural stability, and excellent reusability for multiple reaction cycles.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116116"},"PeriodicalIF":6.5,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766523","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
Linkages conversion of imine to amide promotes photocatalytic overall water splitting in Two-Dimensional covalent organic frameworks: The role of polarity effects 亚胺到酰胺的键转化促进二维共价有机框架光催化整体水分裂:极性效应的作用
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-03 DOI: 10.1016/j.jcat.2025.116118
Liqun Song , Zhonghai Lin , Zhihua Zhang , Yingcai Fan , Mingwen Zhao
{"title":"Linkages conversion of imine to amide promotes photocatalytic overall water splitting in Two-Dimensional covalent organic frameworks: The role of polarity effects","authors":"Liqun Song ,&nbsp;Zhonghai Lin ,&nbsp;Zhihua Zhang ,&nbsp;Yingcai Fan ,&nbsp;Mingwen Zhao","doi":"10.1016/j.jcat.2025.116118","DOIUrl":"10.1016/j.jcat.2025.116118","url":null,"abstract":"<div><div>Imine-based covalent organic frameworks (Im-COFs) have attracted extensive attention in photocatalytic Overall Water Splitting (OWS) due to their facile synthesis and structural stability. However, most of the Im-COFs photocatalysts face the challenge of rapid recombination of photogenerated carriers, leading to low Solar-To-Hydrogen (STH) conversion efficiency. Here, we propose that the oxidation of imine to amide linkages in two-dimensional (2D) Im-COFs would be an effective strategy to enhance the in-plane polarity and thus facilitate the separation of photogenerated carriers. Based on first principles calculations, Two amide-linked 2,4,6-triphenyl-1,3,5-triazine (TST) and Triphenylamine (TA) monolayers (Am-TST, Am-TA) were used as model to compare the photocatalytic performance with the imine-linked ones (Im-TST, Im-TA). Interestingly, both the amide-linked COFs exhibit type-II band alignments, which is absent in the imine-linked ones. Moreover, the Non-Adiabatic Molecular Dynamics (NAMD) simulations reveal the photogenerated carriers’ lifetime Am-TST monolayer (13.41 ns) is 3.45 times longer than that of Im-TST monolayer, indicating the superior ability of amide linkages in suppressing the recombination of photoexcited carriers. In addition, the Am-TST monolayer can also achieve visible-light-driven photocatalytic OWS activity, and the light absorption capability can be further improved by using the Am-TST bilayer. These findings reveal the role of imine-to-amide linkages conversion in promoting the separation of photogenerated carriers, providing a promising strategy for designing amide-based COFs photocatalysts towards OWS.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116118"},"PeriodicalIF":6.5,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766522","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
Adsorption properties of crystalline and amorphous PdIr nanoparticles. A systematic first-principles study 晶体和无定形钯金纳米粒子的吸附特性。系统的第一原理研究
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-03 DOI: 10.1016/j.jcat.2025.116102
Ilya V. Chepkasov , Viktor S. Baidyshev , Anastasiia V. Iosimovska , Ivan S. Zamulin , Alexander G. Kvashnin
{"title":"Adsorption properties of crystalline and amorphous PdIr nanoparticles. A systematic first-principles study","authors":"Ilya V. Chepkasov ,&nbsp;Viktor S. Baidyshev ,&nbsp;Anastasiia V. Iosimovska ,&nbsp;Ivan S. Zamulin ,&nbsp;Alexander G. Kvashnin","doi":"10.1016/j.jcat.2025.116102","DOIUrl":"10.1016/j.jcat.2025.116102","url":null,"abstract":"<div><div>The great interest in metal nanoparticles is due to the fact that the transition from micro to nano size leads to huge changes in the physical and chemical properties of the material. The local atomic structure and composition can significantly influence the properties of nanoparticles. First-principles calculations are used to study the influence of the structure and chemnical ordering of IrPd nanoparticles on the electronic properties, charge distribution and adsorption energy of O, H, CO, NO, OH. Three different types of PdIr bimetallic nanoparticles with different chemical ordering are considered, namely Pd-core/Ir-shell (Pd@Ir), Ir-core/Pd-shell (Ir@Pd), and bimetallic alloy (Pd-Ir) particles consisting of 79 and 321 atoms with fcc and amorphous structures. The electronic and adsorption properties of the proposed nanoparticles are extensively studied in terms of their ability to adsorb O, H, CO, NO, OH, which opens up the possibility of fine-tuning their properties by modifying the atomic structure and composition. By adjusting the core–shell ratio, the adsorption energy on the nanoparticle surface can be fine-tuned, especially in fcc nanoparticles. This results in a narrower range of adsorption energies, which cannot be achieved with bimetallic alloys. In the case of amorphous nanoparticles, the adsorption energy is highly variable because to there are many non-equivalent adsorption sites on the surface.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116102"},"PeriodicalIF":6.5,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776202","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
Synthesis, catalytic application and mechanistic studies of reusable polymer supported iron(III) complex towards efficient transfer hydrogenation of nitro compounds 可重复使用聚合物负载铁(III)配合物对硝基化合物高效转移加氢的合成、催化应用及机理研究
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-04-01 DOI: 10.1016/j.jcat.2025.116113
Priya Vimal , Babu Rajeev C.P. , Nayela Javeed , Ganga Periyasamy , Gayathri V.
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