ChemCatChem最新文献_第5页

Effect of Alkali Metals on CoMo2C/Al2O3 Catalysts for Syngas to Higher Alcohols 碱金属对用于合成气制取高级醇的 CoMo2C/Al2O3 催化剂的影响

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-24 DOI: 10.1002/cctc.202402143

Zhi Yang, Mingsheng Luo, Qinglong Liu, Roshni Rahman

{"title":"Effect of Alkali Metals on CoMo2C/Al2O3 Catalysts for Syngas to Higher Alcohols","authors":"Zhi Yang, Mingsheng Luo, Qinglong Liu, Roshni Rahman","doi":"10.1002/cctc.202402143","DOIUrl":"https://doi.org/10.1002/cctc.202402143","url":null,"abstract":"The development of catalysts for the direct one-step conversion of syngas to higher alcohols is still a challenge. In this study, different alkali metal-modified MCoMo/Al2O3 (M = Li, Na, K, and Cs) catalysts were prepared by impregnation and temperature-programmed carbonization process. Characterization by XRD, H2-TPR, and XPS revealed that the introduction of alkali metals increases the crystallinity of Mo2C, decreases the reducibility of the catalyst, as well as increases the surface high-valent Mo content. The catalysts were evaluated for activity at 300 °C, 3.0 MPa, 18,000 mL·gMo−1·h−1, H2/CO = 2. The evaluation results found that with the increase in the electron-giving capacity of alkali metals, the CO conversion rate gradually decreased from 98.8% to 46.3%. While the alcohol selectivity showed the opposite trend, increasing from 14.4% to 54.9%. Notably, the addition of K and Cs significantly increased the alcohol selectivity in the catalyst product, from 8.3% to 50.5% and 54.9%, respectively. Moreover, the ratio of higher alcohols in the alcohol product increased significantly from 10.5% to nearly 80%. Finally, in situ DRIFT characterization of the catalysts with different alkali metal modifications was carried out to investigate the changes in the reaction process intermediates and to summarize the possible reaction routes.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836372","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Defective Titania Photocatalyst Modified with Iron Oxides for Oxidative Decomposition of Organic Compounds

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-24 DOI: 10.1002/cctc.202500053

Zhishun Wei, Junhao Qin, Yuanyuan Ji, Zuzanna Bielan, Limeng Wu, Xin Yue, Sha Chen, Guoqiang Yi, Ying Chang, Ewa Kowalska

{"title":"Defective Titania Photocatalyst Modified with Iron Oxides for Oxidative Decomposition of Organic Compounds","authors":"Zhishun Wei, Junhao Qin, Yuanyuan Ji, Zuzanna Bielan, Limeng Wu, Xin Yue, Sha Chen, Guoqiang Yi, Ying Chang, Ewa Kowalska","doi":"10.1002/cctc.202500053","DOIUrl":"https://doi.org/10.1002/cctc.202500053","url":null,"abstract":"Ultrafine anatase titania of high crystallinity, composed of ≈10-nm uniform particles, was prepared by a simple solvothermal method, without any additional heat treatment. Subsequently, the photodeposition method was chosen for the surface titania modification with different contents of iron. The properties of obtained samples were estimated by various methods, including, X-ray diffraction, diffuse reflection spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, energy dispersive X-ray spectroscopy, and transmission electron microscopy. Moreover, photoelectrochemical properties were investigated via measurements of photocurrent, electrochemical impedance and cyclic voltammetry. The photocatalytic activity was tested towards oxidative decomposition of acetic acid and different antibiotics from tetracycline (TC) group under UV and/or vis irradiation, including also scavengers’ tests. It was found that optimized conditions of solvothermal reaction allowed an easy control of samples’ properties. Interestingly, the bare titania sample exhibit vis activity (even at 550 nm) due to its defective structure, probably resulting from carbon species (dopants). The modification of titania with deposits of mixed iron oxides results in preparation of highly active samples at broad irradiation ranges, with a real possibility to replace noble metals as titania modifiers. It was also found that superoxide radicals were the main oxidative species under vis irradiation, suggesting the Z-scheme mechanism.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836371","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Efficient Brønsted Acid Sites Accessibility of ZSM-5 Nanosheets Promoting One-Step Lactide Synthesis

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-24 DOI: 10.1002/cctc.202402094

Long Zhang, Linjie Guan, Jiashu Liu, Prof. Song Song, Prof. Ye Tian, Prof. Xingang Li

{"title":"Efficient Brønsted Acid Sites Accessibility of ZSM-5 Nanosheets Promoting One-Step Lactide Synthesis","authors":"Long Zhang, Linjie Guan, Jiashu Liu, Prof. Song Song, Prof. Ye Tian, Prof. Xingang Li","doi":"10.1002/cctc.202402094","DOIUrl":"https://doi.org/10.1002/cctc.202402094","url":null,"abstract":"Lactide (LD) is the key building block of high-quality polylactic acid (PLA), a biodegradable polymer with broad industrial applications. Developing an efficient catalyst for one-step conversion of lactic acid to LD is critical for the PLA industry. Herein, N-ZSM-5–40 nanosheets with a thickness of about 20 nm were successfully synthesized and first applied to this esterification reaction. The yield of LD over N-ZSM-5–40 reaches 60.5% after reaction at an oil bath temperature of 140 °C for 5 h. Systematic characterization revealed that reducing the b-axis thickness of MFI-type nanosheet zeolites improves Brønsted acid sites (BASs) accessibility, which was identified as a critical factor governing the yield of LD. Time-dependent product distribution experiments demonstrate that the nanosheet structure of N-ZSM-5–40 facilitates faster cyclization of L2A to LD, compared to commercial C-ZSM-5–40. In-situ FTIR results reveal that N-ZSM-5–40 nanosheets have a strong ability to adsorb and activate carbonyl groups, which promotes the rapid conversion of lactic acid to LD. Given the aforementioned advantages, ZSM-5 nanosheets hold great potential for guiding the development of industrial catalysts for sustainable LD synthesis.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Copper-Based Nitrides Outperform Phosphides in Nitrate Electroreduction to Ammonia: The Cooperative Role of the Cu3N/CuO Interface

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-23 DOI: 10.1002/cctc.202500156

Paz Stein, Henry Hall, Ran Shimoni, Noam E. Amitay, Dyuti Bandyopadhyay, Alevtina Neyman, Ronen Bar-Ziv, Maya Bar Sadan

{"title":"Copper-Based Nitrides Outperform Phosphides in Nitrate Electroreduction to Ammonia: The Cooperative Role of the Cu3N/CuO Interface","authors":"Paz Stein, Henry Hall, Ran Shimoni, Noam E. Amitay, Dyuti Bandyopadhyay, Alevtina Neyman, Ronen Bar-Ziv, Maya Bar Sadan","doi":"10.1002/cctc.202500156","DOIUrl":"https://doi.org/10.1002/cctc.202500156","url":null,"abstract":"Binary compounds consisting of Cu(I) and moderately electronegative elements (N, P) are attractive semiconductors for optoelectronic and electrocatalytic applications. This study investigates the electrochemical reduction of nitrate to ammonia (NO3RR) using copper-based catalysts, specifically Cu3N and Cu3P. Inhibiting the competitive hydrogen evolution reaction and ensuring active hydrogen (H*) for NH3 production during NO3RR pose significant challenges. Our research demonstrates that while Cu₃P is effective in the initial reduction of nitrate to nitrite, it fails to produce NH₃ at more negative potentials due to competition with the hydrogen evolution reaction (HER). In contrast, Cu₃N exhibits remarkable performance, achieving an ammonia yield rate of 48.8 mmol h−1 mmol−1cat at −0.9 VRHE, accompanied by considerable Faradaic efficiency and durability. The formation of a Cu3N/CuO interface during the catalysis is crucial for its activity, facilitating efficient NO3RR through a stepwise reduction mechanism. The study provides insights into the surface modifications and mechanistic aspects of these catalysts during NO3RR, offering guidance for strategically developing more efficient catalysts for nitrate reduction to ammonia.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202500156","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836450","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Construction of In-Plane ZnIn2S4/In(OH)3 Heterojunction with Boosted CO2 Photoreduction Performance by a Three-Phase Etching-Hydrolysis Strategy

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-23 DOI: 10.1002/cctc.202402051

Jun Du, Jiaming Wu, Keyan Li, Siyang Yan, Jiaxu Liu, Ziwei Liu, Chunshan Song, Xinwen Guo

{"title":"Construction of In-Plane ZnIn2S4/In(OH)3 Heterojunction with Boosted CO2 Photoreduction Performance by a Three-Phase Etching-Hydrolysis Strategy","authors":"Jun Du, Jiaming Wu, Keyan Li, Siyang Yan, Jiaxu Liu, Ziwei Liu, Chunshan Song, Xinwen Guo","doi":"10.1002/cctc.202402051","DOIUrl":"https://doi.org/10.1002/cctc.202402051","url":null,"abstract":"In this work, an in-plane ZnIn2S4/In(OH)3 (ZIS/IOH) heterojunction was fabricated with a gas–solid–liquid three-phase etching-hydrolysis strategy utilizing single-unit-cell ZnIn2S4 nanosheets as the precursor. A portion of ZnIn2S4, which was dispersed in water, was in situ converted to crystalline and amorphous In(OH)3 under hydrothermal condition, while the sulfur escaped in the gas phase was captured by Cu foam placed on a free-standing porous rack above water. This unique approach enabled all In elements to retain in the lattice and prevented the incorporation of Cu impurity into the heterojunction. ZIS/IOH heterojunction exhibited remarkably boosted photocatalytic CO2 reduction performance. The CO generation rate and selectivity reached 1807 µmol g−1 h−1 and 82%, respectively, significantly surpassing those of pure ZnIn2S4 (842 µmol g−1 h−1 and 65%). The resulting heterojunction inherited ultrathin nanosheet morphology coupled with a chemically bonded interface. Moreover, In(OH)3 functions as both electron-accepting platform and reactant adsorption sites, greatly enhancing charge separation efficiency as well as the reaction between CO2 and H2O. The synergy of improved charge separation and increased active sites lead to the remarkably boosted photocatalytic CO2 reduction performance. This work provides a new strategy for the fabrication of 2D in-plane heterojunctions for photocatalytic applications.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836447","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Enantioselective Preparation of Chiral Succinimide Derivatives by Mechanochemical Catalytic Michael Addition

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-23 DOI: 10.1002/cctc.202402021

Dr. György Szőllősi, Kristóf András Kőszegi, Dr. Ákos Kukovecz, Dr. Márton Szabados

{"title":"Enantioselective Preparation of Chiral Succinimide Derivatives by Mechanochemical Catalytic Michael Addition","authors":"Dr. György Szőllősi, Kristóf András Kőszegi, Dr. Ákos Kukovecz, Dr. Márton Szabados","doi":"10.1002/cctc.202402021","DOIUrl":"https://doi.org/10.1002/cctc.202402021","url":null,"abstract":"Mechanochemical activation of organic reactions is a simple and efficient way of preparing complex molecules by an environmentally benign method. Although, various asymmetric catalytic reactions were found to proceed smoothly by milling, enantioselective Michael additions of nucleophiles to maleimide derivatives, providing valuable chiral succinimides, have not yet been attempted. Here we report the mechanochemical addition of isobutyraldehyde to various N-substituted maleimides using a recently developed recyclable heterogeneous chiral hybrid catalyst prepared by adsorption of l-phenylalanine on the surface of layered cation-exchanger inorganic oxides, such as laponite or bentonite. Good conversions and isolated yields were achieved after short millings under solvent free conditions accompanied by high enantioselectivities. The mechanochemical activation was also extended to the asymmetric addition of aldehydes to nitrostyrene catalyzed by l-proline adsorbed on laponite. The chiral catalyst was easily recovered and could be efficiently recycled, as long as small amount of amino acid is supplied upon reuse, which could complement the chirality source leached from the surface, as shown by characterization of the solids using thermal analysis, infrared spectroscopy, X-ray diffractometry, and scanning electron microscopy.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202402021","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Perspectives and Emerging Trends in Plasma Catalysis: Facing the Challenge of Chemical Production Electrification

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-23 DOI: 10.1002/cctc.202401938

Annemie Bogaerts, Gabriele Centi, Volker Hessel, Evgeny Rebrov

引用次数: 0

Bio-Inspired In Situ Tuning of the Hydrophobic Environment Around Catalytically Active Organic Ligand-Stabilized Ruthenium Nanoparticles

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-22 DOI: 10.1002/cctc.202500275

Sayed Abu Sufyan, Paul F. Oblad, Brian van Devener, Jesus Paulo L. Perez, Ahmad Dousti, Samira Shiri, Michael M. Nigra

{"title":"Bio-Inspired In Situ Tuning of the Hydrophobic Environment Around Catalytically Active Organic Ligand-Stabilized Ruthenium Nanoparticles","authors":"Sayed Abu Sufyan, Paul F. Oblad, Brian van Devener, Jesus Paulo L. Perez, Ahmad Dousti, Samira Shiri, Michael M. Nigra","doi":"10.1002/cctc.202500275","DOIUrl":"https://doi.org/10.1002/cctc.202500275","url":null,"abstract":"The organic ligand environment surrounding enzymatic and homogeneous catalytic active sites often determines catalytic activity. Ruthenium nanoparticles, ≤1 nm in diameter, are synthesized using monodentate thiol, monodentate phosphine, and bidentate bisphosphine ligands. Even though some of the ruthenium surface is blocked by the ligands, catalytic activity is still observed for CO oxidation and H2O2 decomposition. All three ligand-stabilized ruthenium nanoparticles have similar CO oxidation rates; however, the bisphosphine-stabilized Ru nanoparticles are approximately 2.5 times less active than the monothiol-stabilized and monophosphine-stabilized ruthenium nanoparticles for H2O2 decomposition. It is observed that the organic ligand environment is modulated in situ during nanoparticle synthesis via partial oxidation of the bisphosphine as confirmed by 31P NMR measurements. We hypothesize that bisphosphine-bound Ru nanoparticles consist of a Ru core with some of the ligands bound in a monodentate manner where the other P atom is oxidized and not bound to the Ru surface leading to a thicker hydrophobic layer around the Ru nanoparticles. The increase in hydrophobicity is confirmed via contact angle and zeta potential measurements. H2O2 decomposition rates are known to decrease with increasing hydrophobicity, and this work illustrates a pathway for increasing hydrophobicity in situ using ligand-bound metallic nanoparticles.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 8","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202500275","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836290","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ru(II)-Catalyzed Aldehyde-Directed Cascade Annulation of Aromatic Aldehydes With Acrylates to Access Indenes

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-20 DOI: 10.1002/cctc.202402109

Hong-Yu Ma, Juan Fan, Wen-Ting Wei, Jia-Xin Chang, Yi-Hao Wang, Prof. Dr. Xian-Ying Shi

引用次数: 0

In-situ Chemical Bonded Tubular Titanium Dioxide With Covalent Organic Frameworks Promoted Photocatalytic Activity 具有共价有机框架的原位化学键合管状二氧化钛促进了光催化活性

IF 3.8 3区化学

ChemCatChem Pub Date : 2025-02-20 DOI: 10.1002/cctc.202401977

Yuqing Gao, Yu Liu, Xiaojie Cao, Prof. Liping Guo, Prof. Lijun Liao, Prof. Zhenzi Li, Prof. Wei Zhou, Prof. Mingxia Li, Prof. Xuepeng Wang

引用次数: 0