ChemCatChem最新文献_第9页

Organo-Soluble MoS₂ Quantum Dots Mediated Photocatalytic Generation of Imminium Intermediate for Effective Synthesis of Bis(indolyl)Methanes Derivatives 有机可溶性MoS 2量子点介导光催化合成双（吲哚基）甲烷衍生物的最小中间体

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-20 DOI: 10.1002/cctc.202500977

Abir Kayal, Mrinmoy De

{"title":"Organo-Soluble MoS₂ Quantum Dots Mediated Photocatalytic Generation of Imminium Intermediate for Effective Synthesis of Bis(indolyl)Methanes Derivatives","authors":"Abir Kayal, Mrinmoy De","doi":"10.1002/cctc.202500977","DOIUrl":"10.1002/cctc.202500977","url":null,"abstract":"Iminium intermediates play a pivotal role in the synthesis of diverse organic molecules due to their exceptional reactivity and capacity to participate in a wide range of transformative reactions. However, their inherent instability in aqueous media, commonly employed in nanomaterial-based catalysis presents a significant challenge. Even though there are few reports of organo-soluble nanophotocatalysis, it has never been explored for iminium ion-mediated pharmaceutically important bis(indolyl)methanes (BIMs) synthesis. In this study, we report the use of organo-soluble MoS₂ quantum dots (QDs) as photocatalysts for the in situ generation of stable iminium ions, which serve as key intermediates in the synthesis of bis(indolyl)methanes (BIMs). Leveraging the unique electronic properties and high surface area of MoS₂ QDs, we achieve efficient substrate activation under mild, environmentally benign conditions, eliminating the need for harsh reagents or elevated temperatures. The in situ generated iminium ions undergo nucleophilic attack by indoles, affording bisindoline derivatives, structural motifs commonly found in biologically active natural products and pharmaceutical agents. Our findings highlight the potential of MoS₂ QDs as sustainable and versatile photocatalysts in organic synthesis, offering a novel and efficient strategy for constructing bisindoline frameworks. This approach not only advances synthetic methodologies but also opens new avenues for the design of catalytic systems aimed at accelerating the discovery of therapeutic agents and bioactive molecules.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145102061","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

Mechanical Understanding of the Roles of Crystal Facets and the Aqueous Solution for the Hydrogenation of LGO to Cyrene with the Pd/Pt Catalysts Pd/Pt催化剂催化LGO加氢制昔烯过程中晶面和水溶液作用的力学理解

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-20 DOI: 10.1002/cctc.202500889

Han-xian Meng, Hao-ze Chen, Bin Hu, Ji Liu, Yang-wen Wu, Kai Li, Yao-bing Huang, Qiang Lu

{"title":"Mechanical Understanding of the Roles of Crystal Facets and the Aqueous Solution for the Hydrogenation of LGO to Cyrene with the Pd/Pt Catalysts","authors":"Han-xian Meng, Hao-ze Chen, Bin Hu, Ji Liu, Yang-wen Wu, Kai Li, Yao-bing Huang, Qiang Lu","doi":"10.1002/cctc.202500889","DOIUrl":"10.1002/cctc.202500889","url":null,"abstract":"Hydrogenation of biomass-derived levoglucosenone (LGO) into versatile dihydroleveglucosenone (Cyrene) is one of the most attractive biomass transformations due to its widespread application in chemical synthesis. LGO hydrogenation is commonly catalyzed by Pd/Pt catalysts, with the reaction being influenced by their crystal facets and reaction environment. Regrettably, the current understanding of the hydrogenation mechanism of LGO to Cyrene over these catalysts is limited. Herein, the catalytic hydrogenation mechanism of LGO to Cyrene on Pd/Pt catalysts was systematically studied based on the first principle calculations. Particularly, the roles of exposed crystal facets and the aqueous solution have been discussed. The hydrogenation of LGO begins with the absorption of its C═C bond, and the optimal pathways over Pd/Pt catalysts vary depending on different crystal facets. In addition, Pd(101) exhibits superior catalytic activity for LGO hydrogenation than that of Pt(111) when comparing the optimal facets of Pb and Pt catalysts (19.50 versus 185.05 kJ mol⁻¹). H2O chiefly affects the hydrogenation reactions by forming a hydrated derivative with LGO, altering the hydrogenation pathway for Cyrene production. This work can provide a theoretical basis for developing high-performance catalysts and exploring new ways to realize the efficient hydrogenation of LGO to Cyrene.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145102060","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

Metallogels as Functional Catalysts: Bridging Soft Materials with Sustainable Transformations 金属凝胶作为功能催化剂：桥接软材料与可持续转变

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-20 DOI: 10.1002/cctc.202500640

Sumit Mondal, Joydeep Ray, Debajit Sarma

引用次数: 0

Sulfonic Acid-Functionalized KIT-6 Solid Acid Catalysts for Glycerol Acetylation 磺酸功能化KIT-6固体酸催化剂的甘油乙酰化研究

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-20 DOI: 10.1002/cctc.202500808

Nattha Baingam, Li-Yu Wang, Dr. Shih-Yuan Chen, Fitrah Hardhana, Dr. Chung-Kai Chang, Dr. Hiroyuki Tateno, Dr. Takehisa Mochizuki, Prof. Chia-Min Yang, Prof. Apanee Luengnaruemitchai

{"title":"Sulfonic Acid-Functionalized KIT-6 Solid Acid Catalysts for Glycerol Acetylation","authors":"Nattha Baingam, Li-Yu Wang, Dr. Shih-Yuan Chen, Fitrah Hardhana, Dr. Chung-Kai Chang, Dr. Hiroyuki Tateno, Dr. Takehisa Mochizuki, Prof. Chia-Min Yang, Prof. Apanee Luengnaruemitchai","doi":"10.1002/cctc.202500808","DOIUrl":"10.1002/cctc.202500808","url":null,"abstract":"Blending biodiesel fuel (BDF) with petrodiesel effectively reduces CO₂ emissions in the transportation sector. The carbon footprint can be further minimized by converting crude glycerol, a byproduct of the BDF industry, into high-value products like triacetin, which can serve as a biofuel additive. This study demonstrated the acetylation of glycerol with acetic acid using propylsulfonic acid-functionalized KIT-6 mesoporous silica (PA-KIT-6) as a solid catalyst to produce triacetin. A series of PA-KIT-6 catalysts was synthesized by post-synthesis (grafting) and direct-synthesis (co-condensation) methods with varying sulfonic acid loading, using 3-mercaptopropyltrimethoxysilane (MPTMS) and hydrogen peroxide as precursor and oxidant. In-situ diffuse reflectance infrared Fourier transform spectroscopy and X-ray photoelectron spectra confirm that all catalysts contained Brønsted acid sites, which increased with sulfonic acid loading. The P-20PA-KIT-6 catalyst, with 0.25 mmol g⁻¹ sulfonic acid loading, exhibited the best performance. Glycerol was rapidly consumed, and 52% selectivity for triacetin was achieved using a 1:9 glycerol-to-acetic acid molar ratio and 2.83 wt.% catalyst at 115 °C for 8 h. This catalyst was reusable, maintaining its activity and selectivity over four cycles. This study highlights the intrinsic activity of sulfonic acid-based solid acids with Brønsted acidity in glycerol acetylation, effectively producing triacetin.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202500808","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145102059","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

Front Cover: Engineering Substrate Acceptance of Resveratrol O-Methyltransferase from Vitis vinifera for the Selective Synthesis of O-Methyl Protected Biobased Hydroxystyrenes (ChemCatChem 14/2025) 封面：葡萄白藜芦醇o -甲基转移酶用于选择性合成o -甲基保护的生物基羟基苯乙烯的工程底物验收（ChemCatChem 14/2025）

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-19 DOI: 10.1002/cctc.70194

Kamela Myrtollari, Andrea M. Chánique, Daniel Kracher, Daniela P. Herrera, Joaquin Gutierrez-Benavente, Andreas Schüller, Robert Kourist

引用次数: 0

Graph-Based High-Throughput Framework for Screening Selective Propane Dehydrogenation Catalysts 基于图的筛选选择性丙烷脱氢催化剂的高通量框架

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-19 DOI: 10.1002/cctc.202500803

Ranga Rohit Seemakurthi, Siddharth Deshpande, David P. Dean, Jessica A. Muhlenkamp, Ryan N. Alcala, Aubrey L. Jeffries, Russell J. Clarke, Isha S. Chavan, Justin Senyk, Yinan Xu, Anne Serban, Casey P. O Brien, Abhaya K. Datye, Jason C. Hicks, Jeffrey T. Miller, Jeffrey Greeley

{"title":"Graph-Based High-Throughput Framework for Screening Selective Propane Dehydrogenation Catalysts","authors":"Ranga Rohit Seemakurthi, Siddharth Deshpande, David P. Dean, Jessica A. Muhlenkamp, Ryan N. Alcala, Aubrey L. Jeffries, Russell J. Clarke, Isha S. Chavan, Justin Senyk, Yinan Xu, Anne Serban, Casey P. O Brien, Abhaya K. Datye, Jason C. Hicks, Jeffrey T. Miller, Jeffrey Greeley","doi":"10.1002/cctc.202500803","DOIUrl":"10.1002/cctc.202500803","url":null,"abstract":"High-throughput computational screening is a powerful approach in accelerating the identification of highly selective and stable catalysts. However, it is often hindered by lack of generalized descriptors and the complexity of handling numerous multidentate adsorption configurations. In this study, we propose a computational framework integrating graph theory and python-based databasing tools with robust catalytic descriptors to enable high-throughput screening of alloys for nonoxidative propane dehydrogenation. We derive mechanistic Brønsted–Evans-Polanyi (BEP) correlations for C─H and C─C bond breaking, highlighting the role of metastable binding configurations in transition states involving more than three surface atoms. Although activity and stability descriptors exhibit strong scaling, these descriptors are uncorrelated, enabling construction of a pareto-optimal line identifying alloys with the best balance between activity and selectivity. Known optimal catalysts, including PtZn, PdZn, PtSn, and PdIn, lie on this pareto-optimal line validating the framework. Furthermore, Ir and Rh, typically known for hydrogenolysis, can be engineered for high selectivity by site-isolating active ensembles with high promoter compositions. Experimental validation confirms that Ir1Sn1 remains highly stable and selective over 15 h. Overall, our approach highlights the power of generalized descriptors combined with high-throughput screening and experimental benchmarking to extract key mechanistic insights and computationally design novel catalysts.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202500803","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145102092","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

Cover Feature: Manganese-Triazolylidene Catalysis for The Synthesis of 1,2,3,4-Tetrahydroquinoxalines and Selective Alkylation of Diamines and Anilines with Alcohols and Diols (ChemCatChem 14/2025) 封面专题：锰-三氮吡啶催化1,2,3,4-四氢喹啉的合成及二胺和苯胺与醇和二醇的选择性烷基化（ChemCatChem 14/2025）

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-19 DOI: 10.1002/cctc.70193

Beatriz Garcia, Sofia Friães, Daniel Raydan, M. Manuel B. Marques, Beatriz Royo

引用次数: 0

Role of Gas Dropouts in CO₂ Methanation over MOF-Derived Ni₃Fe@C Catalysts: An In Situ XAS and PDF Study mof衍生Ni₃Fe@C催化剂上气体脱出在CO₂甲烷化中的作用：原位XAS和PDF研究

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-17 DOI: 10.1002/cctc.202500859

Fabio Manzoni, Sven Strübbe, Leif Rohrbach, Maxime Boniface, Thomas Lunkenbein, Roland Schoch, Wolfgang Kleist, Matthias Bauer, Mirijam Zobel

{"title":"Role of Gas Dropouts in CO₂ Methanation over MOF-Derived Ni₃Fe@C Catalysts: An In Situ XAS and PDF Study","authors":"Fabio Manzoni, Sven Strübbe, Leif Rohrbach, Maxime Boniface, Thomas Lunkenbein, Roland Schoch, Wolfgang Kleist, Matthias Bauer, Mirijam Zobel","doi":"10.1002/cctc.202500859","DOIUrl":"10.1002/cctc.202500859","url":null,"abstract":"With industrial chemical processes facing the challenges of renewable energy supply, catalysts are needed that withstand fluctuations of operating conditions. For methanation reactions using hydrogen from electrocatalytic water splitting, dropouts of hydrogen are amongst the realistic scenarios. While Ni-based catalysts are the most widely used, bimetallic Ni/Fe-based catalysts recently emerged as superior. A new method of preparing highly active metallic catalysts is the decomposition of metal-organic frameworks. Even though it is difficult to control the particle size distribution and the homogeneity of the formed nanoparticles with this method, the carbonaceous features present between the nanoparticles permit avoiding the use of support, leading to a high-loading catalyst with superior stability. Here, we investigate with in situ X-ray absorption spectroscopy and pair distribution function analysis the structural details of a Ni3Fe@C methanation catalyst derived from a metal-organic framework during its activation and catalysis under H2-dropout conditions. Despite the similarity of these phases, it was possible to identify two fcc phases of Ni3Fe and Ni coexisting during catalytic cycling, with a Fe2NiO4 spinel phase appearing during dropouts. This indicates oxidation of the particle surface in the absence of hydrogen, which can be fully recovered by reactivation in pure hydrogen atmosphere, providing high stability of the catalyst during an industrially relevant dropout scenario.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202500859","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145101661","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

Pd/Pt-PW Keggin Systems for H2 Generation: A DFT Study Pd/Pt-PW Keggin制氢系统的DFT研究

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-17 DOI: 10.1002/cctc.202500745

Renata Tokarz-Sobieraj, Dorota Rutkowska-Zbik

引用次数: 0

Sonochemical Exfoliation of AlB2 into Few-Layer-Thick Chemically Functionalized Borophene with Inherent Reducing Capability 声化学剥离AlB2成具有固有还原能力的薄层化学功能化硼罗芬

IF 3.9 3区化学

ChemCatChem Pub Date : 2025-07-17 DOI: 10.1002/cctc.202500661

Parth Shah, Kabeer Jasuja

{"title":"Sonochemical Exfoliation of AlB2 into Few-Layer-Thick Chemically Functionalized Borophene with Inherent Reducing Capability","authors":"Parth Shah, Kabeer Jasuja","doi":"10.1002/cctc.202500661","DOIUrl":"10.1002/cctc.202500661","url":null,"abstract":"Ultrasonication-assisted liquid-phase exfoliation of layered metal diborides has emerged as a promising path for obtaining metal-deficient quasi-2D nanostructures. In this study, we show that ultrasonication can be combined with chelation to achieve exfoliation of AlB2 in high yields. We show that ultrasonicating AlB2 crystals in a solution containing ethylenediaminetetraacetate results in nearly metal-free, few-layer-thick nanosheets rich in boron. These nanosheets exhibit crumpled morphology with several instances of crystalline regions. AFM indicates thickness values between 1 and 6 nm with lateral dimensions extending up to a few microns. Chemical analyses show ultra-low aluminum content (Al:B molar ratio as low as 0.04:2) and presence of oxy, hydroxy, and hydride functional groups, rendering these as chemically functionalized borophene (CFB) nanosheets. We found that the yield of nanosheets can be increased up to 30% by choosing an appropriate pH. We further show that these nanosheets exhibit an inherent reducing capability and can catalyze the reduction of gold salt into gold nanoparticles while simultaneously serving as templates to stabilize them, with the growth of nanoparticles up to 10 nm. This study lays the ground for top-down approaches to synthesize chemically functionalized borophene in high yield and presents its potential as an active reducing agent.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145101660","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