Precision Chemistry最新文献

{"title":"Controlled Synthesis and Phase Transition Mechanisms of Palladium Selenide: A First-Principles Study","authors":"Mingxiang Zhang,&nbsp;Aixinye Zhang,&nbsp;Hao Ren,&nbsp;Wenyue Guo,&nbsp;Feng Ding and Wen Zhao*,&nbsp;","doi":"10.1021/prechem.4c0004910.1021/prechem.4c00049","DOIUrl":"https://doi.org/10.1021/prechem.4c00049https://doi.org/10.1021/prechem.4c00049","url":null,"abstract":"<p >Using density functional theory, we carefully calculated the relative stability of monolayer, few-layer, and cluster structures with Penta PdSe₂, T-phase PdSe₂, and Pd₂Se₃-phase. We found that the stability of Penta PdSe₂ increases with the number of layers. The Penta PdSe₂, T-phase PdSe₂, and Pd₂Se₃ monolayers are all semiconducting, with band gaps of 1.77, 0.81, and 0.65 eV, respectively. The formation energy of palladium selenide clusters with different phase structures is calculated, considering the cluster size, stoichiometry, and chemical environment. Under typical experimental conditions, Pd₂Se₃ phase clusters are found to be dominant, having the lowest formation energy among all of the phases considered, with this dominance increasing as cluster size grows. Adjusting the Pd–Se ratio in the environment allows for controlled synthesis of specific palladium selenide phases, providing theoretical insights into the nucleation mechanisms of PdSe₂ and other transition metal chalcogenides.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 10","pages":"545–552 545–552"},"PeriodicalIF":0.0,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00049","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Achieving Linear α-Macro-olefins in Ethylene Polymerization through Precisely Tuned Bis(imino)pyridylcobalt Precatalysts with Steric and Electronic Parameters","authors":"Kainat Fatima Tahir,&nbsp;Yanping Ma*,&nbsp;Qaiser Mahmood*,&nbsp;Geng Ren,&nbsp;Areej Khalid,&nbsp;Yizhou Wang,&nbsp;Song Zou,&nbsp;Tongling Liang and Wen-Hua Sun*,&nbsp;","doi":"10.1021/prechem.4c0006710.1021/prechem.4c00067","DOIUrl":"https://doi.org/10.1021/prechem.4c00067https://doi.org/10.1021/prechem.4c00067","url":null,"abstract":"<p >Synthesis of functional polyethylene from ethylene alone is tricky and heavily dependent on both the type and structure of the precatalyst and the choice of cocatalyst used in the polymerization. In the present study, a series of cobalt precatalysts was prepared and investigated for ethylene polymerization under various conditions. By incorporation of strong electron-withdrawing groups (F and NO₂) and a steric component (benzhydryl) into the parent bis(imino)pyridine ligand, the catalytic performance of these precatalysts was optimized. On activation with MAO or MMAO, these precatalysts with relatively open structure achieved unprecedented ethylene polymerization rates at 60 °C (up to 27.6 × 10⁶ g mol^–1 h^–1) and remained effective at temperatures up to 100 °C. Chain growth reactions were moderate, resulting in polyethylene with molecular weights up to 61.0 kg/mol and broad bimodal dispersity index. High crystallinity and melt temperature indicated a strictly linear microstructure, as further confirmed by high-temperature ¹H/¹³C NMR measurements. Of significant note that chain termination predominantly occurred through β-elimination (up to 84.5%), yielding vinyl-terminated long-chain olefins. These functional α-macro-olefins are valuable as precursors for postfunctionalization, expanding the potential applications of polyethylene across various sectors.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 12","pages":"655–668 655–668"},"PeriodicalIF":0.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00067","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874977","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Achieving Linear α-Macro-olefins in Ethylene Polymerization through Precisely Tuned Bis(imino)pyridylcobalt Precatalysts with Steric and Electronic Parameters.","authors":"Kainat Fatima Tahir, Yanping Ma, Qaiser Mahmood, Geng Ren, Areej Khalid, Yizhou Wang, Song Zou, Tongling Liang, Wen-Hua Sun","doi":"10.1021/prechem.4c00067","DOIUrl":"10.1021/prechem.4c00067","url":null,"abstract":"<p><p>Synthesis of functional polyethylene from ethylene alone is tricky and heavily dependent on both the type and structure of the precatalyst and the choice of cocatalyst used in the polymerization. In the present study, a series of cobalt precatalysts was prepared and investigated for ethylene polymerization under various conditions. By incorporation of strong electron-withdrawing groups (F and NO₂) and a steric component (benzhydryl) into the parent bis(imino)pyridine ligand, the catalytic performance of these precatalysts was optimized. On activation with MAO or MMAO, these precatalysts with relatively open structure achieved unprecedented ethylene polymerization rates at 60 °C (up to 27.6 × 10⁶ g mol^-1 h^-1) and remained effective at temperatures up to 100 °C. Chain growth reactions were moderate, resulting in polyethylene with molecular weights up to 61.0 kg/mol and broad bimodal dispersity index. High crystallinity and melt temperature indicated a strictly linear microstructure, as further confirmed by high-temperature ¹H/¹³C NMR measurements. Of significant note that chain termination predominantly occurred through β-elimination (up to 84.5%), yielding vinyl-terminated long-chain olefins. These functional α-macro-olefins are valuable as precursors for postfunctionalization, expanding the potential applications of polyethylene across various sectors.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 12","pages":"655-668"},"PeriodicalIF":0.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11672542/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142903803","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Triplet-Triplet Annihilation-Based Photon Upconversion with a Macrocyclic Parallel Dimer.","authors":"Catherine H Mulyadi, Masanori Uji, Bhavesh Parmar, Kana Orihashi, Nobuhiro Yanai","doi":"10.1021/prechem.4c00050","DOIUrl":"10.1021/prechem.4c00050","url":null,"abstract":"<p><p>The integration of multiple chromophore units into a single molecule is expected to improve the performance of photon upconversion based on triplet-triplet annihilation (TTA-UC) that can convert low energy photons to higher energy photons at low excitation intensity. In this study, a macrocyclic parallel dimer of 9,10-diphenylanthracene (DPA) with a precisely parallel orientation, named MPD-2, is synthesized, and its TTA-UC properties are investigated. MPD-2 shows a green-to-blue TTA-UC emission in the presence of a triplet sensitizer, platinum octaethylporphyrin (PtOEP). Compared to monomeric DPA, MPD-2 results in an enhancement of the spin statistical factor of TTA and a decrease in the excitation light intensity due to the intramolecular TTA process. The obtained structure-property relationship provides important information for the further improvement of TTA-UC properties.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 10","pages":"539-544"},"PeriodicalIF":0.0,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11522992/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142558988","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Triplet–Triplet Annihilation-Based Photon Upconversion with a Macrocyclic Parallel Dimer","authors":"Catherine H. Mulyadi,&nbsp;Masanori Uji,&nbsp;Bhavesh Parmar,&nbsp;Kana Orihashi and Nobuhiro Yanai*,&nbsp;","doi":"10.1021/prechem.4c0005010.1021/prechem.4c00050","DOIUrl":"https://doi.org/10.1021/prechem.4c00050https://doi.org/10.1021/prechem.4c00050","url":null,"abstract":"<p >The integration of multiple chromophore units into a single molecule is expected to improve the performance of photon upconversion based on triplet–triplet annihilation (TTA-UC) that can convert low energy photons to higher energy photons at low excitation intensity. In this study, a macrocyclic parallel dimer of 9,10-diphenylanthracene (DPA) with a precisely parallel orientation, named MPD-2, is synthesized, and its TTA-UC properties are investigated. MPD-2 shows a green-to-blue TTA-UC emission in the presence of a triplet sensitizer, platinum octaethylporphyrin (PtOEP). Compared to monomeric DPA, MPD-2 results in an enhancement of the spin statistical factor of TTA and a decrease in the excitation light intensity due to the intramolecular TTA process. The obtained structure–property relationship provides important information for the further improvement of TTA-UC properties.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 10","pages":"539–544 539–544"},"PeriodicalIF":0.0,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00050","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551716","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Water-Mediated Proton Hopping Mechanisms at the SnO₂(110)/H₂O Interface from Ab Initio Deep Potential Molecular Dynamics.","authors":"Mei Jia, Yong-Bin Zhuang, Feng Wang, Chao Zhang, Jun Cheng","doi":"10.1021/prechem.4c00056","DOIUrl":"10.1021/prechem.4c00056","url":null,"abstract":"<p><p>The interfacial proton transfer (PT) reaction on the metal oxide surface is an important step in many chemical processes including photoelectrocatalytic water splitting, dehydrogenation, and hydrogen storage. The investigation of the PT process, in terms of thermodynamics and kinetics, has received considerable attention, but the individual free energy barriers and solvent effects for different PT pathways on rutile oxide are still lacking. Here, by applying a combination of ab initio and deep potential molecular dynamics methods, we have studied interfacial PT mechanisms by selecting the rutile SnO₂(110)/H₂O interface as an example of an oxide with the characteristic of frequently interfacial PT processes. Three types of PT pathways among the interfacial groups are found, i.e., proton transfer from terminal adsorbed water to bridge oxygen directly (surface-PT) or via a solvent water (mediated-PT), and proton hopping between two terminal groups (adlayer PT). Our simulations reveal that the terminal water in mediated-PT prefers to point toward the solution and forms a shorter H-bond with the assisted solvent water, leading to the lowest energy barrier and the fastest relative PT rate. In particular, it is found that the full solvation environment plays a crucial role in water-mediated proton conduction, while having little effect on direct PT reactions. The PT mechanisms on aqueous rutile oxide interfaces are also discussed by comparing an oxide series composed of SnO₂, TiO₂, and IrO₂. Consequently, this work provides valuable insights into the ability of a deep neural network to reproduce the ab initio potential energy surface, as well as the PT mechanisms at such oxide/liquid interfaces, which can help understand the important chemical processes in electrochemistry, photoelectrocatalysis, colloid science, and geochemistry.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 12","pages":"644-654"},"PeriodicalIF":0.0,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11672534/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142903487","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Water-Mediated Proton Hopping Mechanisms at the SnO2(110)/H2O Interface from Ab Initio Deep Potential Molecular Dynamics","authors":"Mei Jia,&nbsp;Yong-Bin Zhuang,&nbsp;Feng Wang,&nbsp;Chao Zhang and Jun Cheng*,&nbsp;","doi":"10.1021/prechem.4c0005610.1021/prechem.4c00056","DOIUrl":"https://doi.org/10.1021/prechem.4c00056https://doi.org/10.1021/prechem.4c00056","url":null,"abstract":"<p >The interfacial proton transfer (PT) reaction on the metal oxide surface is an important step in many chemical processes including photoelectrocatalytic water splitting, dehydrogenation, and hydrogen storage. The investigation of the PT process, in terms of thermodynamics and kinetics, has received considerable attention, but the individual free energy barriers and solvent effects for different PT pathways on rutile oxide are still lacking. Here, by applying a combination of ab initio and deep potential molecular dynamics methods, we have studied interfacial PT mechanisms by selecting the rutile SnO₂(110)/H₂O interface as an example of an oxide with the characteristic of frequently interfacial PT processes. Three types of PT pathways among the interfacial groups are found, i.e., proton transfer from terminal adsorbed water to bridge oxygen directly (surface-PT) or via a solvent water (mediated-PT), and proton hopping between two terminal groups (adlayer PT). Our simulations reveal that the terminal water in mediated-PT prefers to point toward the solution and forms a shorter H-bond with the assisted solvent water, leading to the lowest energy barrier and the fastest relative PT rate. In particular, it is found that the full solvation environment plays a crucial role in water-mediated proton conduction, while having little effect on direct PT reactions. The PT mechanisms on aqueous rutile oxide interfaces are also discussed by comparing an oxide series composed of SnO₂, TiO₂, and IrO₂. Consequently, this work provides valuable insights into the ability of a deep neural network to reproduce the ab initio potential energy surface, as well as the PT mechanisms at such oxide/liquid interfaces, which can help understand the important chemical processes in electrochemistry, photoelectrocatalysis, colloid science, and geochemistry.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 12","pages":"644–654 644–654"},"PeriodicalIF":0.0,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00056","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874924","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Single-Molecule Bioelectronic Sensors with AI-Aided Data Analysis: Convergence and Challenges.","authors":"Yuxin Yang, Yueqi Li, Longhua Tang, Jinghong Li","doi":"10.1021/prechem.4c00048","DOIUrl":"10.1021/prechem.4c00048","url":null,"abstract":"<p><p>Single-molecule bioelectronic sensing, a groundbreaking domain in biological research, has revolutionized our understanding of molecules by revealing deep insights into fundamental biological processes. The advent of emergent technologies, such as nanogapped electrodes and nanopores, has greatly enhanced this field, providing exceptional sensitivity, resolution, and integration capabilities. However, challenges persist, such as complex data sets with high noise levels and stochastic molecular dynamics. Artificial intelligence (AI) has stepped in to address these issues with its powerful data processing capabilities. AI algorithms effectively extract meaningful features, detect subtle changes, improve signal-to-noise ratios, and uncover hidden patterns in massive data. This review explores the synergy between AI and single-molecule bioelectronic sensing, focusing on how AI enhances signal processing and data analysis to boost accuracy and reliability. We also discuss current limitations and future directions for integrating AI, highlighting its potential to advance biological research and technological innovation.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 10","pages":"518-538"},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11523000/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142558986","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthesis of Ultralow-Density Polyethylene Elastomers Using Triarylnaphthyl Iminopyridyl Ni(II) Catalysts.","authors":"Wenbin Yuan, Shengyu Dai","doi":"10.1021/prechem.4c00057","DOIUrl":"10.1021/prechem.4c00057","url":null,"abstract":"<p><p>Recently, the chain-walking ethylene polymerization strategy has garnered widespread attention as an efficient and straightforward method for preparing polyolefin elastomers. In this study, a series of 2,4,8-triarylnaphthyl iminopyridyl nickel catalysts were synthesized and used in ethylene polymerization. These catalysts demonstrated moderate catalytic activity (10⁵ g mol^-1 h^-1), producing high-molecular-weight (up to 145.5 kg/mol) polyethylene materials with high branching degrees (75-95/1000C) and correspondingly low melting points. Detailed analysis using ¹³C NMR spectroscopy revealed that the polyethylenes primarily featured methyl and long-chain branches. Mechanical testing of the polyethylene samples obtained from catalysts <b>Ni1</b>-<b>Ni3</b> exhibited moderate stress at break (4.64-6.97 MPa) coupled with a very high strain at break (1650-3752%), indicating their very good ductility. Furthermore, these polyethylenes showcased great elastic recovery abilities, with strain recovery values ranging from 72% to 85%. In contrast, the polyethylene produced by <b>Ni4</b> displayed notably inferior tensile strength (0.16 MPa) and tensile recovery (43%). To the best of our knowledge, this study represents the inaugural utilization of a nickel iminopyridyl catalyst in the preparation of a polyethylene thermoplastic elastomer.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 10","pages":"553-558"},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11522993/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142558987","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthesis of Ultralow-Density Polyethylene Elastomers Using Triarylnaphthyl Iminopyridyl Ni(II) Catalysts","authors":"Wenbin Yuan,&nbsp; and ,&nbsp;Shengyu Dai*,&nbsp;","doi":"10.1021/prechem.4c0005710.1021/prechem.4c00057","DOIUrl":"https://doi.org/10.1021/prechem.4c00057https://doi.org/10.1021/prechem.4c00057","url":null,"abstract":"<p >Recently, the chain-walking ethylene polymerization strategy has garnered widespread attention as an efficient and straightforward method for preparing polyolefin elastomers. In this study, a series of 2,4,8-triarylnaphthyl iminopyridyl nickel catalysts were synthesized and used in ethylene polymerization. These catalysts demonstrated moderate catalytic activity (10⁵ g mol^–1 h^–1), producing high-molecular-weight (up to 145.5 kg/mol) polyethylene materials with high branching degrees (75–95/1000C) and correspondingly low melting points. Detailed analysis using ¹³C NMR spectroscopy revealed that the polyethylenes primarily featured methyl and long-chain branches. Mechanical testing of the polyethylene samples obtained from catalysts <b>Ni1</b>–<b>Ni3</b> exhibited moderate stress at break (4.64–6.97 MPa) coupled with a very high strain at break (1650–3752%), indicating their very good ductility. Furthermore, these polyethylenes showcased great elastic recovery abilities, with strain recovery values ranging from 72% to 85%. In contrast, the polyethylene produced by <b>Ni4</b> displayed notably inferior tensile strength (0.16 MPa) and tensile recovery (43%). To the best of our knowledge, this study represents the inaugural utilization of a nickel iminopyridyl catalyst in the preparation of a polyethylene thermoplastic elastomer.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 10","pages":"553–558 553–558"},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00057","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551790","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}