Journal of Catalysis最新文献_第5页

Reusable metal-free mesoporous carbon-catalyzed reductive N-formylation of nitroarenes and quinolines 可重复使用的无金属介孔碳催化硝基烯烃和喹啉的还原 N-甲酰化反应

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.jcat.2024.115826

Xiangzhu Yu, Meng Miao, Shuxiao Huo, Shaowei Liu, Hao Dong, Lianyue Wang

{"title":"Reusable metal-free mesoporous carbon-catalyzed reductive N-formylation of nitroarenes and quinolines","authors":"Xiangzhu Yu, Meng Miao, Shuxiao Huo, Shaowei Liu, Hao Dong, Lianyue Wang","doi":"10.1016/j.jcat.2024.115826","DOIUrl":"10.1016/j.jcat.2024.115826","url":null,"abstract":"<div><div>The high-value transformation of nitrogen-containing compounds through a facile, cost-effective, and eco-friendly one-pot strategy holds significant importance. However, this process typically involves the use of metal catalysts and is limited by low activity as well as the requirement of high temperature and pressure. Herein, we describe a general and efficient metal-free N-doped mesoporous carbon material using well-defined ligand 1,10-phenanthroline as the precursor and silica colloid as the hard template. Formic acid is both a reducing agent and a formylation reagent, and structurally distinct mono- or multi-substituted nitroarenes and quinolines can be selectively <em>N</em>-formylation in a one-pot method. The catalyst can be easily recovered without observable loss of efficiency for ten consecutive uses. The control experiments and density functional theory (DFT) calculations indicate that formic acid mainly obtains active hydrogen in the form of O–H bond cleavage, which benefits from the strong adsorption and enhanced activity generated by the interaction between graphitic nitrogen species in the catalyst and formic acid. The excellent catalytic performance of the <em>meso</em>-phen-X catalyst is attributed to the synergistic effect of graphitic N and large specific surface area, providing a promising method for the development of non-metallic catalyst-modified carbon materials.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115826"},"PeriodicalIF":6.5,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519383","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}

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Highly efficient selective hydrogenation of furfural to tetrahydrofurfuryl alcohol over MOF-derived Co-Ni bimetallic catalysts: The effects of Co-Ni alloy and adsorption configuration 在 MOF 衍生 Co-Ni 双金属催化剂上高效选择性加氢将糠醛转化为四氢糠醇：Co-Ni 合金和吸附构型的影响

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.jcat.2024.115824

Zonghao Zhang , Ruizhuo Liu , Lei Huang , Pingle Liu

{"title":"Highly efficient selective hydrogenation of furfural to tetrahydrofurfuryl alcohol over MOF-derived Co-Ni bimetallic catalysts: The effects of Co-Ni alloy and adsorption configuration","authors":"Zonghao Zhang , Ruizhuo Liu , Lei Huang , Pingle Liu","doi":"10.1016/j.jcat.2024.115824","DOIUrl":"10.1016/j.jcat.2024.115824","url":null,"abstract":"<div><div>The targeted conversion of furfural (FA) over inexpensive catalyst is a critical and challenging project. Herein, CoNi alloy catalysts (xCoyNi/C) were prepared through one-step pyrolysis of metal–organic frameworks and used in furfural (FA) hydrogenation to tetrahydrofurfuryl alcohol (TFOL). The formation of CoNi alloy leads to a reconfiguration of the electronic structure on the metal surface, which affects the adsorption of functional groups on FA and furfuryl alcohol (FOL). <em>In situ</em> FT-IR analysis and DFT calculations verify that bimetallic CoNi alloy catalyst exhibits more suitable reactants adsorption and hydrogenation rate in comparison with the monometallic Co and monometallic Ni catalysts. Meanwhile, CoNi alloy significantly reduces the activation barrier from FOL to TFOL. Hence, the 1Co1Ni/C catalyst gives the highest TFOL yield of > 99 %. This study provides a simple strategy for the preparation of alloy catalysts for tuning product selectivity and presents practical potential for upgrading biomass-derived platform molecules.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115824"},"PeriodicalIF":6.5,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519389","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}

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Catalytic and electrochemical evaluation of the role of metal oxides on Pd nano-catalysts for complete methane oxidation 钯纳米催化剂上的金属氧化物对甲烷完全氧化作用的催化和电化学评估

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.jcat.2024.115827

Najmeh Ahledel , Komalpreet Kaur Saini , Martin Couillard , Elena A. Baranova

{"title":"Catalytic and electrochemical evaluation of the role of metal oxides on Pd nano-catalysts for complete methane oxidation","authors":"Najmeh Ahledel , Komalpreet Kaur Saini , Martin Couillard , Elena A. Baranova","doi":"10.1016/j.jcat.2024.115827","DOIUrl":"10.1016/j.jcat.2024.115827","url":null,"abstract":"<div><div>Catalytic complete methane oxidation over Pd-MOx (MO<sub>x</sub> = SnO<sub>2</sub>, FeO<sub>x</sub>, and ZnO) nanoparticles deposited on YSZ solid electrolyte was evaluated for and compared to a monometallic Pd catalyst. To this end, the nanoparticles were synthesized via the polyol method and tested for methane oxidation in a temperature range from 200 to 475 °C under reducing, stoichiometric, and oxidizing reaction conditions in open-circuit conditions. The light-off experiments revealed that the presence of a second phase in the form of metal oxide (SnO<sub>2</sub> and ZnO) increased the catalytic rate of the reaction compared to monometallic palladium in all gas compositions. However, the addition of iron oxide to Pd showed a different behaviour, i.e., a strong inhibition of the reaction rate in the oxidizing and stoichiometric conditions and significant promotion in the reducing conditions. To gain an insight into the role of MO<sub>x</sub> in various conditions, the detailed electrochemical measurements were carried out at selected temperatures. The exchange current density (<em>i</em><sub>o</sub>) of the electrochemical process at the three phase bpoundary was found to depend on the oxidation state of the catalyst, which in turn influences the catalytic rate of Pd-MO<sub>x</sub>. Overall, the addition of the cheaper oxide to Pd significantly promotes the catalytic reaction, and the inverse relation between the catalytic rate and <em>i</em><sub>o</sub> was found in agreement with the electrochemical promotion of catalysis (EPOC) mechanism, where the lower exchange current density values correspond to the higher catalytic reaction rate of complete methane oxidaiton.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115827"},"PeriodicalIF":6.5,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142536421","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Detailed mechanistic studies on PNN-palladium pincer complex catalyzed Suzuki-Miyaura cross-coupling reaction proceeding through a PdII/PdIII/PdIV catalytic cycle 通过 PdII/PdIII/PdIV 催化循环进行的 PNN-钯钳形复合物催化铃木-宫浦拉交叉偶联反应的详细机理研究

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.jcat.2024.115825

Gazal Sabharwal , Khilesh C. Dwivedi , Chandan Das , Thakur Rochak Kumar Rana , Arnab Dutta , Gopalan Rajaraman , Maravanji S. Balakrishna

{"title":"Detailed mechanistic studies on PNN-palladium pincer complex catalyzed Suzuki-Miyaura cross-coupling reaction proceeding through a PdII/PdIII/PdIV catalytic cycle","authors":"Gazal Sabharwal , Khilesh C. Dwivedi , Chandan Das , Thakur Rochak Kumar Rana , Arnab Dutta , Gopalan Rajaraman , Maravanji S. Balakrishna","doi":"10.1016/j.jcat.2024.115825","DOIUrl":"10.1016/j.jcat.2024.115825","url":null,"abstract":"<div><div>In this paper, synthesis, Pd and Pt complexes and catalytic investigations of a tridentate pincer ligand 2-(diphenylphosphaneyl)-N-(pyridine-2-ylmethyl)benzamide, {(<em>o</em>-PPh<sub>2</sub>)C<sub>6</sub>H<sub>4</sub>C(O)N(H)CH<sub>2</sub>(C<sub>6</sub>H<sub>5</sub>N)} (<strong>1</strong>), (hereafter referred to as “PN(H)N” and its anionic form as “PNN”) is described. Reaction of <strong>1</strong> with MCl<sub>2</sub>(COD) resulted in pincer complexes [MCl(PNN-κ<sup>3</sup>-P,N,N)] (Pd <strong>2</strong>, Pt <strong>3</strong>), whereas the same reaction with Pd(OAc)<sub>2</sub> afforded [CH<sub>3</sub>C(O)OPd(PNN-κ<sup>3</sup>-P,N,N)] (<strong>4</strong>). The structures of all of the compounds are confirmed by single-crystal X-ray analysis. The palladium complex <strong>4</strong> promoted the Suzuki-Miyaura cross-coupling reaction between aryl halides and boronic acids to form the corresponding biphenyls in excellent yields. The catalytic investigation supported by spectroscopic studies and DFT calculations suggested the involvement of Pd<sup>II</sup>/Pd<sup>IV</sup> catalytic cycle <em>via</em> a short lived Pd<sup>III</sup> intermediate, which transforms into Pd<sup>IV</sup> species rapidly. The catalytic process proceeded with a very low catalyst loading under relatively mild reaction conditions.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115825"},"PeriodicalIF":6.5,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519969","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

Enumeration of surface site nuclearity and shape in a database of intermetallic low-index surface facets 金属间低指数表面面数据库中表面位点核性和形状的列举

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.jcat.2024.115795

Unnatti Sharma , Angela Nguyen , John R. Kitchin , Zachary W. Ulissi , Michael J. Janik

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Highly para-selective alkylation of toluene by methyl mercaptan over silylated ZSM-5 zeolite 硅烷化 ZSM-5 沸石上甲基硫醇对甲苯的高副选择性烷基化反应

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.jcat.2024.115828

Abdelilah Bayout , Claudia Cammarano , Izabel Medeiros Costa , Gleb Veryasov , Alexander Sachse , Vasile Hulea

{"title":"Highly para-selective alkylation of toluene by methyl mercaptan over silylated ZSM-5 zeolite","authors":"Abdelilah Bayout , Claudia Cammarano , Izabel Medeiros Costa , Gleb Veryasov , Alexander Sachse , Vasile Hulea","doi":"10.1016/j.jcat.2024.115828","DOIUrl":"10.1016/j.jcat.2024.115828","url":null,"abstract":"<div><div>Friedel-Crafts alkylation of toluene with methyl mercaptan has been investigated in the presence of H-ZSM-5 and SiO<sub>2</sub>/H-ZSM-5 catalysts. The silica layers have been built on H-ZSM-5 zeolite by chemical liquid deposition of tetraethyl orthosilicate. The passivation with silica of the external surface of H-ZSM-5 zeolite has been confirmed by FT-IR spectroscopy and mesitylene isomerization, used as a model reaction. All catalysts exhibited notable behavior in the alkylation of toluene to xylenes. Efficiencies higher than 98 % in alkylation for both toluene and methyl mercaptan were obtained at 375 °C. In terms of <em>para</em>-selectivity, outstanding performance was revealed by the silylated zeolites. Thus, over 12 % SiO<sub>2</sub>/H-ZSM-5, at 375 °C and WHSV = 9.4 g<sub>toluene+CH3SH</sub> g<sub>cat</sub><sup>-1</sup>h<sup>−1</sup>, the <em>para</em>-xylene selectivity was close to 100 %. The experimental apparent activation energy for the toluene alkylation with methyl mercaptan catalyzed by H-ZSM-5 was 80 kJ/mol.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115828"},"PeriodicalIF":6.5,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519375","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Deactivation of Cu/ZnO/Al2O3 catalysts by sintering in liquid phase assisted methanol synthesis from CO2/H2 and a way to counteract it Cu/ZnO/Al2O3 催化剂在液相辅助 CO2/H2 合成甲醇过程中的烧结失活问题及解决方法

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.jcat.2024.115829

Dominic Walter , Jonathan Hackebeil , Conrad Hübler , Erik Schumann , Andreas Lißner , Bianca Störr , Mykhaylo Motylenko , David Rafaja , Florian Mertens

引用次数: 0

Kinetic analysis of the self-discharge of the NiOOH OER active phase in KOH electrolyte: insights from in-situ Raman and UV–Vis reflectance spectroscopies KOH 电解液中 NiOOH OER 活性相的自放电动力学分析：原位拉曼光谱和紫外可见反射光谱的启示

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-26 DOI: 10.1016/j.jcat.2024.115823

Harol Moreno Fernández , Achim Alkemper , Kai Wang , Crizaldo Jr. Mempin , Julia Gallenbeger , Jan P. Hofmann

{"title":"Kinetic analysis of the self-discharge of the NiOOH OER active phase in KOH electrolyte: insights from in-situ Raman and UV–Vis reflectance spectroscopies","authors":"Harol Moreno Fernández , Achim Alkemper , Kai Wang , Crizaldo Jr. Mempin , Julia Gallenbeger , Jan P. Hofmann","doi":"10.1016/j.jcat.2024.115823","DOIUrl":"10.1016/j.jcat.2024.115823","url":null,"abstract":"<div><div>NiOOH has been established as the active phase of NiO-based electrocatalysts in the alkaline Oxygen Evolution Reaction (OER). Here, we investigate the self-discharge behavior of NiOOH electrodes under open circuit potential (OCP) conditions in 1 M KOH electrolyte by monitoring phase changes via in-situ Raman and UV–Vis reflectance spectroscopies and performing kinetic analyses on the OCP and spectroscopic data. Our findings reveal a linear phase change from NiOOH to Ni(OH)<sub>2</sub> over time, indicative of a 0<sup>th</sup>-order reduction reaction. Contrarily, the OCP evolution associated with this phase reduction displayed a combination of linear and exponential decay patterns as a result of various kinetics, including Faradaic processes and diffusion-controlled mechanisms, influencing the self-discharge potential over 1.25 V (vs RHE). An additional linear region at lower potentials (<1.25 V (vs RHE)) suggests that charge redistribution due to the phase change from α-Ni(OH)<sub>2</sub> to β-Ni(OH)<sub>2</sub> dominates the self-discharge, a behavior confirmed by in-situ UV–Vis reflectance spectroscopy. These findings highlight the effectiveness of combining in-situ Raman and UV–Vis spectroscopy with electrochemical data for real-time monitoring of electrochemical processes, here potential-dependent electrocatalyst phase changes, leading to a more detailed and accurate understanding of the dynamic behavior, phase change kinetics, and self-discharge behaviors of solid electrocatalysts that can guide the design of more efficient and durable energy storage and conversion materials.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115823"},"PeriodicalIF":6.5,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Efficient photoreforming of plastic waste using a high-entropy oxide catalyst 使用高熵氧化物催化剂对塑料废弃物进行高效光转化

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-24 DOI: 10.1016/j.jcat.2024.115808

Thanh Tam Nguyen , Kaveh Edalati

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Enhancing coke resistance of Ni-based spinel-type oxides by tuning the configurational entropy 通过调整构型熵增强镍基尖晶石型氧化物的抗焦性

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-10-24 DOI: 10.1016/j.jcat.2024.115819

Shuangshuang Zhang , Ying Gao , Qiang Niu , Pengfei Zhang

{"title":"Enhancing coke resistance of Ni-based spinel-type oxides by tuning the configurational entropy","authors":"Shuangshuang Zhang , Ying Gao , Qiang Niu , Pengfei Zhang","doi":"10.1016/j.jcat.2024.115819","DOIUrl":"10.1016/j.jcat.2024.115819","url":null,"abstract":"<div><div>The reforming of CH<sub>4</sub> and CO<sub>2</sub> into syngas is a highly relevant technology for energy conservation and reducing greenhouse gas emissions, attracting widespread attention in the industry. Inspired by this, this work proposes a general criterion for coke-resistant nickel-based catalysts. By leveraging the high-entropy effect and the lattice distortion of the structure, a high-entropy (NiCaMgZnCo)Al<sub>10</sub>O<sub>x</sub> catalyst was synthesized. The high-entropy oxide exhibited good activity and stability during the DRM reaction over 100 h at 800°C and 650°C, producing only a minimal amount of easily removable carbon deposition. O<sub>2</sub>-TPO, CO<sub>2</sub>-TPD, CH<sub>4</sub>-TPSR, CO<sub>2</sub>-TPSR, DFT and in situ DRIFT were employed to investigate the mechanism of carbon deposition elimination on the surface of the high-entropy catalyst. Then, a high-entropy strategy for designing coke-resistant catalysts was proposed. This strategy may soon inspire the development of catalysts with enhanced stability and anti-coke deposition properties for various catalytic applications.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115819"},"PeriodicalIF":6.5,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142488179","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