{"title":"Cover Feature: Bifunctional Strontium Cobalt Molybdenum Oxide (Sr2CoMoO6) Perovskite as an Efficient Catalyst for Electrochemical Water Splitting Reactions in Alkaline Media (ChemCatChem 17/2024)","authors":"Shahan Atif, Abhisek Padhy, Pawan Kumar Jha, Dorothy Sachdeva, Dr. Prabeer Barpanda","doi":"10.1002/cctc.202481702","DOIUrl":"https://doi.org/10.1002/cctc.202481702","url":null,"abstract":"<p><b>The Cover Feature</b> highlights the concept that, for water-splitting reaction and related clean energy technology, it is imperative to design earth-abundant low-cost electrocatalysts. In this spirit, the work by Abhisek Padhy, Prabeer Barpanda, and co-workers introduces double perovskite-based strontium cobalt molybdenum oxide (SCMO) as an efficient bifunctional electrocatalyst showing both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Prepared by scalable autocombustion synthesis, the bulk SCMO perovskite exhibits stable electrocatalytic performance attributed to its substantial electrochemical active surface area. Double perovskite electrocatalysts can be harnessed for sustainable energy technologies. More information can be found in the Research Article by Shahan Atif et al. (DOI: 10.1002/cctc.202400217).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 17","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202481702","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142165619","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}
ChemCatChemPub Date : 2024-09-09DOI: 10.1002/cctc.202401385
Bohai Gao, Weijie Li, Yuchao Chai, Guangjun Wu, Landong Li
{"title":"Heteroatom‐Containing Zeolites as Solid Lewis Acid Catalysts for the Cycloaddition of CO2 to Epoxides","authors":"Bohai Gao, Weijie Li, Yuchao Chai, Guangjun Wu, Landong Li","doi":"10.1002/cctc.202401385","DOIUrl":"https://doi.org/10.1002/cctc.202401385","url":null,"abstract":"The catalytic cycloaddition of CO2 to epoxides to produce valuable cyclic carbonates represents a simple and promising strategy for CO2 utilization, circumventing the ineffective CO2 reduction process. Despite current progresses, there remains an impending demand for highly‐active, cost‐effective and stable catalysts especially the ideal heterogeneous catalytic systems. Herein, we report the preparation of heteroatom‐containing zeolites through a two‐step process comprising of framework dealumination and subsequent heteroatom incorporation, and their catalytic applications in CO2 cycloaddition to epoxides. Characterization results reveal the successful incorporation of heteroatoms into framework to derive Lewis acidic M‐Beta zeolites (M=Ti, Zr or Hf). The as‐prepared M‐Beta Lewis acids show remarkable performance in the model reaction of CO2 cycloaddition to propylene oxide with the assistance of potassium iodide under solvent‐free conditions. The reaction parameters have been optimized employing Ti‐Beta catalyst and the substrate scope has been investigated. Finally, the impact of Lewis acidity on the cycloaddition reaction is discussed and the actual bifunctional Ti‐Beta/KI catalyst system is proposed, which is of important significance for the understanding of CO2 catalytic cycloaddition to epoxides.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"47 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208896","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}
ChemCatChemPub Date : 2024-09-09DOI: 10.1002/cctc.202401337
Michael A Unkrig-Bau, Sara L Leijendekker, Jan Streuff
{"title":"Exploring Dinuclear Titanium Complexes in Titanium(III) Catalysis","authors":"Michael A Unkrig-Bau, Sara L Leijendekker, Jan Streuff","doi":"10.1002/cctc.202401337","DOIUrl":"https://doi.org/10.1002/cctc.202401337","url":null,"abstract":"The synthesis of one achiral and two chiral propylene‐bridged dititanocenes and their evaluation as catalysts in titanium(III) catalyzed ketone‐nitrile coupling reactions is reported. A reaction progress kinetics analysis of the cross‐coupling between acetophenone and benzyl cyanide reveals that, using a dinuclear titanocene catalyst, the order in catalyst is reduced from two to one in comparison to a mononuclear catalyst. Although the obtained coupling yields and enantioselectivities did not reach the results obtained with the latter, these examples constitute a proof‐of‐concept for the templated C‐C coupling through coordination of ketone and nitrile to the two tethered titanium centers of a dinuclear catalyst.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"262 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208899","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}
ChemCatChemPub Date : 2024-09-09DOI: 10.1002/cctc.202401302
Jinju Hong, Jonghyun Jeon, Hee Hwan Kim, Kyung Soo Shin, Sung June Cho, Kyoung-Su Ha
{"title":"Effects of Acid Sites on Thin MCM‐22 Zeolite Catalysts and Their Catalytic Applications for Acetylene Aromatization","authors":"Jinju Hong, Jonghyun Jeon, Hee Hwan Kim, Kyung Soo Shin, Sung June Cho, Kyoung-Su Ha","doi":"10.1002/cctc.202401302","DOIUrl":"https://doi.org/10.1002/cctc.202401302","url":null,"abstract":"Two types of thin zeolite MCM‐22 catalysts were prepared by using a carbon sphere template. By different calcination methods, a hollow sphere‐type MCM‐22 (HS‐MCM‐22) and a nanosheet‐type MCM‐22 (NS‐MCM‐22) were synthesized. Those catalysts were tested and evaluated for acetylene aromatization to see the effects of thin structures. The two types of thin catalysts were found to have higher amount of acid sites than that of the conventional MCM‐22 catalyst. It was found that the extremely short diffusion length not only enhanced the aromatic yield, but also suppressed the formation of graphitic coke. Notably, the diffusion length of NS‐MCM‐22 was found to be at least 15 times shorter than that of conventional MCM‐22, leading to an 11 % and 18 % increase in benzene yield, respectively. The thin structure seemed to help the produced aromatics efficiently desorb before they further converted into carbon precursors and coke. The carbon species in the spent thin catalysts were found less graphitic than that of the conventional MCM‐22 catalyst. Because of this, the thin MCM‐22 catalysts were believed to show higher coke removal capability. Especially, the coke removal rate of NS‐MCM‐22 was estimated over 90% despite the severe carbon deposition during reaction.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"55 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208897","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}
ChemCatChemPub Date : 2024-09-06DOI: 10.1002/cctc.202400874
Agnès Labande, Illia Ruzhylo, Anna Vorozhbian, Sandrine Vincendeau, Tanguy Saget, Sonia Mallet-Ladeira, Philippe Dauban, Eric Manoury
{"title":"[Rh2(phesp)2]: a Bulkier [Rh2(esp)2] Analog to Tune the Site‐Selectivity in Carbene C–H Insertion Reactions","authors":"Agnès Labande, Illia Ruzhylo, Anna Vorozhbian, Sandrine Vincendeau, Tanguy Saget, Sonia Mallet-Ladeira, Philippe Dauban, Eric Manoury","doi":"10.1002/cctc.202400874","DOIUrl":"https://doi.org/10.1002/cctc.202400874","url":null,"abstract":"[Rh2(phesp)2], a new dirhodium(II) complex bearing a bulky bidentate bis‐carboxylate ligand, has been prepared in two steps from commercially available compounds. Its X‐ray structure revealed distinctive features with a strong distortion around the dirhodium(II) core, illustrated by important torsion angles of up to 9.0°. It has been evaluated as catalyst as a bulky version of the prominent [Rh2(esp)2] complex in carbene C–H insertion reactions. [Rh2(phesp)2] proved as active as [Rh2(esp)2], and showed an intermediate selectivity between [Rh2(esp)2] and bulky [Rh2(tpa)4] in both intra‐ and intermolecular reactions with donor‐acceptor and acceptor‐acceptor diazo compounds, comprising challenging C(sp3)–H insertion into pentane.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"25 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208900","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}
{"title":"Oxidase‐like nanozyme activity of ultrathin copper metal‐organic framework nanosheets with high specificity for catechol oxidation","authors":"Ajit Kumar Singh, Deepika Sharma, Devesh Kumar Singh, Sonu Sarraf, Aviru Kumar Basu, Vellaichamy Ganesan, Avishek Saha, Arindam Indra","doi":"10.1002/cctc.202401029","DOIUrl":"https://doi.org/10.1002/cctc.202401029","url":null,"abstract":"In nature, catechol oxidase catalyzes the oxidation of o‐diphenol to o‐quinone to produce a series of highly important polyphenolic natural products. Although mimicking the functionality of natural enzyme using a nanozyme was found to be beneficial, attaining a high specificity is challenging. Herein, we have explored the thickness‐dependent oxidase activity and specificity of Cu‐metal‐organic framework (MOF) nanosheets. The unique synthetic method offers control over the thickness of the Cu‐MOF nanosheets. The ultrathin (4 nm) Cu‐MOF (Cu‐UMOF) nanosheets as an oxidase nanozyme exhibit high specificity for catechol oxidation without having any peroxidase activity. Interestingly, the specificity is lost for the thicker (20‐30 nm) Cu‐MOF nanosheets. The binuclear Cu‐center, coordinative and electronic unsaturation tuned electronic structure in Cu‐UMOF, resulting in higher specificity for catechol oxidation than thicker Cu‐MOF.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"73 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208737","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}
{"title":"Synthesis of Coke‐Resistant Catalyst Using NiAl2O4 Support for Hydrogen Production via Autothermal Dry Reforming of Methane","authors":"Yasin Khani, Sumin Pyo, Farzad Bahadoran, Kanghee Cho, Kwang-Eun Jeong, Young-Kwon Park","doi":"10.1002/cctc.202401015","DOIUrl":"https://doi.org/10.1002/cctc.202401015","url":null,"abstract":"A highly porous NiAl2O4 spinel structure was synthesized and employed as a support for catalysts in the autothermal dry reforming of methane (ATDRM) in a monolithic‐type reactor. A series of catalyst with various metal species, X/NiAl2O4@monolith (X: Ni, Co, Pt, Rh, and Ru), was prepared. NiAl2O4 support provides a high dispersion of active metal species with a uniform size distribution, due to its high surface area, and large pore volume. These features enable catalysts to maximize catalytic performance by improving the adsorption and reaction rates of reactants. More notably, the use of NiAl2O4 support enhanced catalyst longevity by retarding coke formation during the ATDRM, due to its improved catalyst acidity compared to conventional alumina support. The conversion of feeed, CH4 and CO2 on X/NiAl2O4 catalysts increases in the order of Rh > Ni > Ru > Co > Pt. Notably, the inexpensive Ni catalyst exhibits slightly lower but comparable CH4 conversion to the expensive noble metal Rh when using NiAl2O4 as a supporting material: 93.7% for Ni vs. 95.2% for Rh. Moreover, applying monolithic reactors considerably increased methane conversion compared with fixed bed reactors due to the better distribution of active metal, increased activity per unit volume, high mass/heat transfer.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"9 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208740","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}
ChemCatChemPub Date : 2024-09-05DOI: 10.1002/cctc.202401358
Jie Zhou, Yuanyuan Wu, Yonghong Liu, Na Li, Zhen Yang, Jiadi Ying, Xiaorong Ren, Tao Zhang, Wei Xu, Jinyang Chen, Xingzhong Cao, Runsheng Yu, Minfeng Zeng
{"title":"Pd nanoparticle supported on N‐doped carbon derived from sodium alginate/melamine blends as efficient heterogeneous catalyst for Heck reactions","authors":"Jie Zhou, Yuanyuan Wu, Yonghong Liu, Na Li, Zhen Yang, Jiadi Ying, Xiaorong Ren, Tao Zhang, Wei Xu, Jinyang Chen, Xingzhong Cao, Runsheng Yu, Minfeng Zeng","doi":"10.1002/cctc.202401358","DOIUrl":"https://doi.org/10.1002/cctc.202401358","url":null,"abstract":"N‐doped porous carbon shows great potential in the field of heterogenous supports due to its high porosity, large surface area, rich active sites, and strong chelation with catalytic active metals species. Here, we successfully fabricated novel N‐doped porous carbon derived from alginate/melamine blends with different mass ratio by simple carbonization and activation process. Hierarchical porous structure of the derived N‐doped carbon has been confirmed with the SEM, TEM and N2 adsorption characterization. After Na2PdCl4 solution impregnation and further reduction process, Pd0 nanoparticles have been uniformly immobilized on the SMCNC support to produce novel Pd@SAMNC catalyst. The optimated Pd@SAMNC‐0.6 possesses a high N content (5.13%), Pd content (5.90%), large BET specific surface area of 1884.5 m2/g. Positron annihilation lifetime spectroscopy (PALS) investigation of the porous carbon materials provided the sub‐nano level microporous information proofs of Pd@SAMNC‐0.6 had the capability to provide more active sites for reactions than commercial Pd@AC. Pd@SAMNC‐0.6 catalyst showed superior catalytic efficiency in Heck coupling reaction between aromatic halides and alkenes and can be recycled for 17 runs without significant decrease in catalytic efficiency.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"7 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208901","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}
ChemCatChemPub Date : 2024-09-05DOI: 10.1002/cctc.202400765
Paula Vidal, Ana Robles-Martín, Laura Fernandez-Lopez, Jose L. Gonzalez-Alfonso, David Almendral, Ruben Muñoz-Tafalla, Francisco J. Plou, Víctor Guallar, Manuel Ferrer
{"title":"Unlocking a Key Residue in a Lipase for Efficient Polyethylene Terephthalate (PET) Hydrolysis and Influencing Depolymerization Product Profiles","authors":"Paula Vidal, Ana Robles-Martín, Laura Fernandez-Lopez, Jose L. Gonzalez-Alfonso, David Almendral, Ruben Muñoz-Tafalla, Francisco J. Plou, Víctor Guallar, Manuel Ferrer","doi":"10.1002/cctc.202400765","DOIUrl":"https://doi.org/10.1002/cctc.202400765","url":null,"abstract":"Polyethylene terephthalate (PET) pollution is a global challenge. Advancing the bioprospecting of PET‐degrading enzymes through metagenomics and using computational and functional methods to identify key positions influencing the catalytic rate and selectivity are part of the solution. Here, we report PETase activity in the metagenomic lipase LipMRD9, which exhibits peak activity at 30 °C and pH 9.0 and has a denaturation temperature of 42 °C. In addition to acting on long‐chain triglycerides (up to 13 units (U)/mg, pH 8.0, 30 °C) and a wide range of 34 other esters (up to 228 U/g), LipMRD9 hydrolyses mono(2‐hydroxyethyl) terephthalate (57 U/g) and bis(2‐hydroxyethyl) terephthalate (131 U/g). It also efficiently deconstructs GoodFellow amorphous submicro‐ and nanosized PET particles (984/2238 µM degradation products at 30/40 °C, pH 7.0, 21.5 h) and films (112/198 µM degradation products at 30/40 °C, pH 7.0, 7 days). Through molecular modelling and experimental analysis, the active site of LipMRD9 was revealed, identifying a key residue contributing to its PETase activity compared with those of its closest homologues. This residue plays a crucial role in determining the distinct profiles of degradation products from PET hydrolysis and should be studied in other PETases for its influence on the catalytic process.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"21 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208902","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}
{"title":"Ce‐Pr co‐doped Co3O4 with enriched oxygen vacancies for the efficient decomposition of N2O","authors":"Haiqiang Wang, Yuxin Sun, Yunshuo Wu, Zhuoyi Zhang, Xuanhao Wu, Zhongbiao Wu","doi":"10.1002/cctc.202401060","DOIUrl":"https://doi.org/10.1002/cctc.202401060","url":null,"abstract":"Nitrous oxide (N2O) has gained increasing attention as a non‐carbon dioxide greenhouse gas, and catalytic decomposition is an effective method for mitigating its emissions. In this study, Ce‐Pr co‐doped Co3O4 was synthesised via a coprecipitation method and used for the catalytic decomposition of N2O. The experimental results revealed that the N2O decomposition achieved 100% conversion at 400 °C on the catalyst with a Pr/Ce/Co molar ratio of 0.02:0.2:1, exhibiting an 80 °C decrease of T100 compared with that of Co3O4. The introduction of Ce reduced the size and crystallisation of Co3O4 particles, increased the activity of the lattice oxygen of Co3O4, and facilitated the formation of oxygen vacancies, thereby enhancing the activation of N2O. However, the introduction of Ce inhibited the crystallisation of Co3O4 and the surface coverage of CeO2 decreased the exposure degree of N2O molecules to the Co3O4 surface. Co‐doping strategy of Ce‐Pr was performed to alleviate the negative effects of ceria. Consequently, the incorporation of Ce and Pr species enhanced the redox properties of Co3O4, leading to remarkable catalytic performance of N2O decomposition. This study elucidated the interaction between Ce and Pr dopants and Co3O4, and encouraged more attention on designing novel catalysts for N2O mitigation.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"11 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208742","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}