{"title":"Enhancing Optical and Electrical Performances via Nanocrystalline Si-Based Thin Films for Si Heterojunction Solar Cells","authors":"Bingquan Liang, Xinliang Chen*, Heze Yuan, Xuejiao Wang, Guofu Hou, Ying Zhao and Xiaodan Zhang, ","doi":"10.1021/acsomega.4c0908010.1021/acsomega.4c09080","DOIUrl":"https://doi.org/10.1021/acsomega.4c09080https://doi.org/10.1021/acsomega.4c09080","url":null,"abstract":"<p >Silicon heterojunction (SHJ) solar cells, as one of the most promising passivated contact solar cell technologies of the next generation, have the advantages of high conversion efficiency, high open-circuit voltage, low-temperature coefficient, and no potential-induced degradation. For the single-side rear-emitter SHJ solar cells, the n-type carrier selective layer, which serves as the light-incident side, plays a pivotal role in determining the performance of heterojunction devices. Consequently, a superior n-doped layer should exhibit high optical transmittance and minimal optical absorption, along with a substantial effective doping level to guarantee the formation of dark conductivity (σ<sub>d</sub>) and electron-transport capacity. In this work, we investigated the optical and electrical properties of different n-type monolayers and stacked gradient multilayers, including monolayer, bilayer, and trilayer Si-based thin films, acting as electron-transport layers (ETL) prepared by plasma-enhanced chemical vapor deposition, and studied the influences of these above layers on the performance of SHJ solar cells. The experimental results demonstrate that the ETL with an n-nc-Si:H/n-nc-SiOx:H/n<sup>+</sup>-nc-Si:H trilayer structure exhibits the potential to boost highly efficient solar cells. The bottom highly crystallized, lightly phosphorus-doped n-nc-Si:H film promotes rapid nucleation of the intermediate n-nc-SiOx:H film and thus reduces the thickness of the incubation layer, as well as improves the passivation contact. The n-nc-SiOx:H film in the middle layer provides excellent optical properties and reduces parasitic absorption, thereby increasing the short-circuit current density. Furthermore, the highly doped n<sup>+</sup>-nc-Si:H at the top offers an optimal ohmic contact with the reactive plasma deposition-grown TCO layer, which ultimately enhances the fill factor. Ultimately, a conversion efficiency of 20.41%, with an open-circuit voltage of 720 mV, a short-circuit current density of 39.34 mA/cm<sup>2</sup>, and a filling factor of 72.05%, was achieved in the SHJ solar cell using a typical trilayer structure. This kind of trilayer structure has a particular significance for potential industrialized applications as it allows for efficient utilization of solar energy.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49935–49944 49935–49944"},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c09080","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842507","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}
ACS OmegaPub Date : 2024-12-06eCollection Date: 2024-12-17DOI: 10.1021/acsomega.4c06566
Jakub S Cyniak, Artur Kasprzak
{"title":"Mechanochemical Synthesis of Molecular Chemoreceptors.","authors":"Jakub S Cyniak, Artur Kasprzak","doi":"10.1021/acsomega.4c06566","DOIUrl":"10.1021/acsomega.4c06566","url":null,"abstract":"<p><p>The design of environmentally friendly methods for synthesizing molecular receptors is an expanding area within applied organic chemistry. This work systematically summarizes advances in the mechanochemical synthesis of molecular chemoreceptors. It discusses key achievements related to the synthesis of chemoreceptors containing azine, Schiff base, thiosemicarbazone, hydrazone, rhodamine 6G, imide, or amide moieties. Additionally, it highlights the application potential of mechanochemically synthesized molecular chemoreceptors in the recognition of ions and small molecules, along with a discussion of the mechanisms of detection processes.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"48870-48883"},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11656220/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142875356","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}
{"title":"Enhancing Optical and Electrical Performances via Nanocrystalline Si-Based Thin Films for Si Heterojunction Solar Cells.","authors":"Bingquan Liang, Xinliang Chen, Heze Yuan, Xuejiao Wang, Guofu Hou, Ying Zhao, Xiaodan Zhang","doi":"10.1021/acsomega.4c09080","DOIUrl":"10.1021/acsomega.4c09080","url":null,"abstract":"<p><p>Silicon heterojunction (SHJ) solar cells, as one of the most promising passivated contact solar cell technologies of the next generation, have the advantages of high conversion efficiency, high open-circuit voltage, low-temperature coefficient, and no potential-induced degradation. For the single-side rear-emitter SHJ solar cells, the n-type carrier selective layer, which serves as the light-incident side, plays a pivotal role in determining the performance of heterojunction devices. Consequently, a superior n-doped layer should exhibit high optical transmittance and minimal optical absorption, along with a substantial effective doping level to guarantee the formation of dark conductivity (σ<sub>d</sub>) and electron-transport capacity. In this work, we investigated the optical and electrical properties of different n-type monolayers and stacked gradient multilayers, including monolayer, bilayer, and trilayer Si-based thin films, acting as electron-transport layers (ETL) prepared by plasma-enhanced chemical vapor deposition, and studied the influences of these above layers on the performance of SHJ solar cells. The experimental results demonstrate that the ETL with an n-nc-Si:H/n-nc-SiOx:H/n<sup>+</sup>-nc-Si:H trilayer structure exhibits the potential to boost highly efficient solar cells. The bottom highly crystallized, lightly phosphorus-doped n-nc-Si:H film promotes rapid nucleation of the intermediate n-nc-SiOx:H film and thus reduces the thickness of the incubation layer, as well as improves the passivation contact. The n-nc-SiOx:H film in the middle layer provides excellent optical properties and reduces parasitic absorption, thereby increasing the short-circuit current density. Furthermore, the highly doped n<sup>+</sup>-nc-Si:H at the top offers an optimal ohmic contact with the reactive plasma deposition-grown TCO layer, which ultimately enhances the fill factor. Ultimately, a conversion efficiency of 20.41%, with an open-circuit voltage of 720 mV, a short-circuit current density of 39.34 mA/cm<sup>2</sup>, and a filling factor of 72.05%, was achieved in the SHJ solar cell using a typical trilayer structure. This kind of trilayer structure has a particular significance for potential industrialized applications as it allows for efficient utilization of solar energy.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49935-49944"},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11656382/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142875369","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}
{"title":"Sensing the Future-Frontiers in Biosensors: Exploring Classifications, Principles, and Recent Advances.","authors":"Sumitha Manoharan Nair Sudha Kumari, Xavier Thankappan Suryabai","doi":"10.1021/acsomega.4c07991","DOIUrl":"10.1021/acsomega.4c07991","url":null,"abstract":"<p><p>Biosensors are transforming healthcare by delivering swift, precise, and economical diagnostic solutions. These analytical instruments combine biological indicators with physical transducers to identify and quantify biomarkers, thereby improving illness detection, management, and patient surveillance. Biosensors are widely utilized in healthcare for the diagnosis of chronic and infectious diseases, tailored treatment, and real-time health monitoring. This thorough overview examines several categories of biosensors and their uses in the detection of numerous biomarkers, including glucose, proteins, nucleic acids, and infections. Biosensors are commonly classified based on the type of transducer employed or the specific biorecognition element utilized. This review introduces a novel classification based on substrate morphology, offering a comprehensive perspective on biosensor categorization. Considerable emphasis is placed on the advancement of point-of-care biosensors, facilitating decentralized diagnostics and alleviating the strain on centralized healthcare systems. Recent advancements in nanotechnology have significantly improved the sensitivity, selectivity, and downsizing of biosensors, rendering them more efficient and accessible. The study examines problems such as stability, reproducibility, and regulatory approval that must be addressed to enable the widespread implementation of biosensors in clinical environments. The study examines the amalgamation of biosensors with wearable devices and smartphones, emphasizing the prospects for ongoing health surveillance and individualized medical care. This viewpoint clarifies the distinct types of biosensors and their particular roles, together with recent developments in the \"smart biosensor\" sector, facilitated by artificial intelligence and the Internet of Medical Things (IoMT). This novel approach seeks to deliver a comprehensive evaluation of the present condition of biosensor technology in healthcare, recent developments, and prospective paths, emphasizing their significance in influencing the future of medical diagnostics and patient care.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"48918-48987"},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11656264/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142875394","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}
ACS OmegaPub Date : 2024-12-06eCollection Date: 2024-12-17DOI: 10.1021/acsomega.4c07419
Beata Salamon-Baran, Jan Kapała, Leszek Rycerz, Irena Szczygieł
{"title":"Thermodynamics of Tl<sub>2</sub>PrBr<sub>5</sub> Compound and Re-examination of Phase Equilibria in the PrBr<sub>3</sub>-TlBr System.","authors":"Beata Salamon-Baran, Jan Kapała, Leszek Rycerz, Irena Szczygieł","doi":"10.1021/acsomega.4c07419","DOIUrl":"10.1021/acsomega.4c07419","url":null,"abstract":"<p><p>The PrBr<sub>3</sub>-TlBr phase diagram was first established in the 1970s. Due to some inaccuracies, it was redetermined using differential scanning calorimetry. The results obtained differ significantly from those in the literature, which has been discussed in this paper. Only one congruently melting Tl<sub>2</sub>PrBr<sub>5</sub> was confirmed, and the thermodynamic characterization of molar heat capacity temperature dependence was carried out for this compound. The compatibility of the obtained data was examined by using the CALPHAD method. The dependences of mixing enthalpy and mixing entropy of the liquid phase on the mole fraction were estimated.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49539-49544"},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11656224/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142875465","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}
ACS OmegaPub Date : 2024-12-06DOI: 10.1021/acsomega.4c0799110.1021/acsomega.4c07991
Sumitha ManoharanNair Sudha Kumari*, and , Xavier Thankappan Suryabai*,
{"title":"Sensing the Future─Frontiers in Biosensors: Exploring Classifications, Principles, and Recent Advances","authors":"Sumitha ManoharanNair Sudha Kumari*, and , Xavier Thankappan Suryabai*, ","doi":"10.1021/acsomega.4c0799110.1021/acsomega.4c07991","DOIUrl":"https://doi.org/10.1021/acsomega.4c07991https://doi.org/10.1021/acsomega.4c07991","url":null,"abstract":"<p >Biosensors are transforming healthcare by delivering swift, precise, and economical diagnostic solutions. These analytical instruments combine biological indicators with physical transducers to identify and quantify biomarkers, thereby improving illness detection, management, and patient surveillance. Biosensors are widely utilized in healthcare for the diagnosis of chronic and infectious diseases, tailored treatment, and real-time health monitoring. This thorough overview examines several categories of biosensors and their uses in the detection of numerous biomarkers, including glucose, proteins, nucleic acids, and infections. Biosensors are commonly classified based on the type of transducer employed or the specific biorecognition element utilized. This review introduces a novel classification based on substrate morphology, offering a comprehensive perspective on biosensor categorization. Considerable emphasis is placed on the advancement of point-of-care biosensors, facilitating decentralized diagnostics and alleviating the strain on centralized healthcare systems. Recent advancements in nanotechnology have significantly improved the sensitivity, selectivity, and downsizing of biosensors, rendering them more efficient and accessible. The study examines problems such as stability, reproducibility, and regulatory approval that must be addressed to enable the widespread implementation of biosensors in clinical environments. The study examines the amalgamation of biosensors with wearable devices and smartphones, emphasizing the prospects for ongoing health surveillance and individualized medical care. This viewpoint clarifies the distinct types of biosensors and their particular roles, together with recent developments in the “smart biosensor” sector, facilitated by artificial intelligence and the Internet of Medical Things (IoMT). This novel approach seeks to deliver a comprehensive evaluation of the present condition of biosensor technology in healthcare, recent developments, and prospective paths, emphasizing their significance in influencing the future of medical diagnostics and patient care.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"48918–48987 48918–48987"},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c07991","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850096","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}
ACS OmegaPub Date : 2024-12-06DOI: 10.1021/acsomega.4c0683010.1021/acsomega.4c06830
Kyunghoon Han*, Ariadni Boziki, Alexandre Tkatchenko and Joshua T. Berryman,
{"title":"TIHI Toolkit: A Peak Finder and Analyzer for Spectroscopic Data","authors":"Kyunghoon Han*, Ariadni Boziki, Alexandre Tkatchenko and Joshua T. Berryman, ","doi":"10.1021/acsomega.4c0683010.1021/acsomega.4c06830","DOIUrl":"https://doi.org/10.1021/acsomega.4c06830https://doi.org/10.1021/acsomega.4c06830","url":null,"abstract":"<p >Complex signal vectors, particularly spectra, are integral to many scientific domains. Interpreting these signals often involves decomposing them into contributions from independent components and subtraction or deconvolution of the channel and instrument noise. Despite the fundamental nature of this task, researchers frequently rely on costly commercial tools. To make such tools accessible to all, we present <i>Tihi</i>, interactive, open-source multiplatform software for interpolation, denoising, baseline correction, peak detection, and signal decomposition. <i>Tihi</i> provides a user-friendly graphical interface (GUI) that facilitates the analysis of spectroscopic data and more. It allows researchers to contribute to and freely distribute these tools, ensuring broad accessibility and fostering collaborative improvements. We present examples demonstrating the efficiency of the program using the spectra of different systems acquired by different spectroscopic techniques, including Raman (aspirin), IR (solid ammonia), XRD (anatase), and UV–vis (petal tip from the <i>Puya alpestris</i> flower). These examples showcase a variety of spectra that differ significantly, from signals with narrow profiles to signals with very broad profiles. This demonstrates the versatility of <i>Tihi</i> for peak identification in a wide range of spectroscopic techniques.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49397–49410 49397–49410"},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c06830","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850098","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}
ACS OmegaPub Date : 2024-12-06eCollection Date: 2024-12-17DOI: 10.1021/acsomega.4c06171
Melika Eshaghi Kenari, Sayan Maiti, Jianheng Ling, Xena El-Shamy, Hiren Bagga, Matthew A Addicoat, Phillip J Milner, Anindita Das
{"title":"Toward Pore Size-Selective Photoredox Catalysis Using Bifunctional Microporous 2D Triazine-Based Covalent Organic Frameworks.","authors":"Melika Eshaghi Kenari, Sayan Maiti, Jianheng Ling, Xena El-Shamy, Hiren Bagga, Matthew A Addicoat, Phillip J Milner, Anindita Das","doi":"10.1021/acsomega.4c06171","DOIUrl":"https://doi.org/10.1021/acsomega.4c06171","url":null,"abstract":"<p><p>The design and synthesis of photoactive metal-free 2D materials for selective heterogeneous photoredox catalysis continue to be challenging due to issues related to nonrecyclability, and limited photo- and chemical stability. Herein, we report the photocatalytic properties of a triazine-based porous COF, <b>TRIPTA</b>, which is found to be capable of facilitating both SET (single electron transfer) for photocatalytic reductive debromination of phenacyl bromide in absence of oxygen and generation of reactive oxygen species (ROS) for benzylamine photo-oxidation in the presence of oxygen, respectively, under visible light irradiation. Inspired by the latter results, we further systematically investigated different-sized benzylamine substrates in this single-component reaction and compared the results with an analogous COF (<b>Micro-COF-2</b>) exhibiting a larger pore size. We observed a marked improvement in the conversion of larger-sized substrates with the latter COF, thereby demonstrating angstrom-level pore size-selective photocatalytic activity of COFs.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49249-49258"},"PeriodicalIF":3.7,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11656359/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142875469","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}
ACS OmegaPub Date : 2024-12-05DOI: 10.1021/acsomega.4c0617110.1021/acsomega.4c06171
Melika Eshaghi Kenari, Sayan Maiti, Jianheng Ling, Xena El-Shamy, Hiren Bagga, Matthew A. Addicoat, Phillip J. Milner and Anindita Das*,
{"title":"Toward Pore Size-Selective Photoredox Catalysis Using Bifunctional Microporous 2D Triazine-Based Covalent Organic Frameworks","authors":"Melika Eshaghi Kenari, Sayan Maiti, Jianheng Ling, Xena El-Shamy, Hiren Bagga, Matthew A. Addicoat, Phillip J. Milner and Anindita Das*, ","doi":"10.1021/acsomega.4c0617110.1021/acsomega.4c06171","DOIUrl":"https://doi.org/10.1021/acsomega.4c06171https://doi.org/10.1021/acsomega.4c06171","url":null,"abstract":"<p >The design and synthesis of photoactive metal-free 2D materials for selective heterogeneous photoredox catalysis continue to be challenging due to issues related to nonrecyclability, and limited photo- and chemical stability. Herein, we report the photocatalytic properties of a triazine-based porous COF, <b>TRIPTA</b>, which is found to be capable of facilitating both SET (single electron transfer) for photocatalytic reductive debromination of phenacyl bromide in absence of oxygen and generation of reactive oxygen species (ROS) for benzylamine photo-oxidation in the presence of oxygen, respectively, under visible light irradiation. Inspired by the latter results, we further systematically investigated different-sized benzylamine substrates in this single-component reaction and compared the results with an analogous COF (<b>Micro-COF-2</b>) exhibiting a larger pore size. We observed a marked improvement in the conversion of larger-sized substrates with the latter COF, thereby demonstrating angstrom-level pore size-selective photocatalytic activity of COFs.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49249–49258 49249–49258"},"PeriodicalIF":3.7,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c06171","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842436","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}
ACS OmegaPub Date : 2024-12-05DOI: 10.1021/acsomega.4c0925410.1021/acsomega.4c09254
Narayan Ch. Jana, Zvonko Jagličić, Paula Brandão and Anangamohan Panja*,
{"title":"Supramolecular Dimeric MnIII Complexes: Synthesis, Structure, Magnetic Properties, and Catalytic Oxidation Studies","authors":"Narayan Ch. Jana, Zvonko Jagličić, Paula Brandão and Anangamohan Panja*, ","doi":"10.1021/acsomega.4c0925410.1021/acsomega.4c09254","DOIUrl":"https://doi.org/10.1021/acsomega.4c09254https://doi.org/10.1021/acsomega.4c09254","url":null,"abstract":"<p >In this study, a tetradentate Schiff-base ligand (H<sub>2</sub>L), synthesized by the condensation of ethylenediamine with 2-hydroxy-3-methoxy-5-methylbenzaldehyde, was reacted with either manganese salts or manganese salts in the presence of various pseudohalides in methanol. This reaction resulted in the formation of five mononuclear Mn<sup>III</sup> complexes: [Mn(L)(H<sub>2</sub>O)<sub>2</sub>](NO<sub>3</sub>)·1/2H<sub>2</sub>O·1/2CH<sub>3</sub>OH (<b>1</b>), [Mn(L)(H<sub>2</sub>O)<sub>2</sub>](ClO<sub>4</sub>)·H<sub>2</sub>O (<b>2</b>), [Mn(L)(N<sub>3</sub>)(H<sub>2</sub>O)]·1/3H<sub>2</sub>O (<b>3</b>), [Mn(L)(NCS)(H<sub>2</sub>O)] (<b>4</b>), and [Mn(L)(H<sub>2</sub>O)<sub>2</sub>](dca) (<b>5</b>) (where dca is dicyanamide ion). X-ray crystallography revealed that the Mn<sup>III</sup> centers adopt a hexa-coordinate pseudo-octahedral geometry, where the equatorial plane is constructed with phenoxo oxygen and imine nitrogen atoms from the Schiff base ligand, while the axial positions are occupied by water molecules or a combination of water and pseudohalides. Supramolecular interactions, primarily π–π stacking and hydrogen bonding, contribute to the formation of pseudodimeric structures in the solid state. Magnetic susceptibility measurements indicated antiferromagnetic coupling within quasi-dimers, primarily through hydrogen bonds. Catalytic studies showed that the complexes effectively catalyze the aerobic oxidation of substrates such as 2-aminophenol and 3,5-di-<i>tert</i>-butylcatechol to yield 2-aminophenoxazin-3-one and 3,5-di-<i>tert</i>-butylquinone, respectively. They also catalyze the oxidation of styrene to its corresponding oxirane, demonstrating their versatile catalytic proficiency. Mechanistic insights, supported by ESI mass spectrometry and EPR studies, suggest that catalysis involves the formation of a complex–substrate aggregate, followed by an intramolecular electron transfer.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49953–49965 49953–49965"},"PeriodicalIF":3.7,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c09254","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850049","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}