ACS Physical Chemistry Au最新文献

{"title":"","authors":"Tanja Cuk*, Jin Z. Zhang* and Gemma Solomon*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 1","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.7,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsphyschemau.4c00100","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144412126","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":"","authors":"Fábio J. Amorim,  and , Giovanni F. Caramori*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 1","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.7,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsphyschemau.4c00089","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144412122","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":"","authors":"Samuel Emilsson, Marcelo Albuquerque, Pernilla Öberg, Daniel Brandell and Mats Johansson*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 1","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.7,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsphyschemau.4c00078","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144412130","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":"","authors":"","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 1","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.7,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/pgv005i001_1891676","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144354722","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":"Understanding (La,Sr)(Co,Fe)O_3-δ Phase Instability within SOECs Using a Combined Experimental and Atomistic Modeling Approach.","authors":"Heather S Slomski, Jonas L Kaufman, Michael J Dzara, Nicholas A Strange, Cameron Priest, Jeremy L Hartvigsen, Nicholas Kane, Micah Casteel, Brandon C Wood, David S Ginley, Kyoung E Kweon, Brian P Gorman, Sarah Shulda","doi":"10.1021/acsphyschemau.4c00095","DOIUrl":"10.1021/acsphyschemau.4c00095","url":null,"abstract":"<p><p>Understanding the onset of degradation in the air electrode within solid oxide electrolysis cells (SOECs), and the subsequent impact on cell performance, is a critical step in mitigating the performance losses and stability issues of SOECs. In an effort to identify early onset degradation phenomena, SOECs were characterized as fabricated and after testing potentiostatically at 1.3 V for 1000 h at 750 °C. SOEC air electrodes composed of a 1:1 composite of La_0.6Sr_0.4Co_0.2Fe_0.8O_3-δ (6428-LSCF) and Gd_0.1Ce_0.9O_1.95 (GDC) were studied using synchrotron X-ray diffraction (XRD), scanning transmission electron microscopy coupled with energy dispersive X-ray spectroscopy (STEM-EDS), and X-ray absorption near-edge spectroscopy (XANES) to evaluate the changes in the air electrode structurally and chemically. These techniques show the migration of Sr species from the air electrode through pores in the GDC barrier layer, progressing to the electrolyte boundary, where it accumulates and reacts with (Zr_0.84Y_0.16)O_2-δ (YSZ) to form SrZrO₃. Microscopy results are paired with atomistic simulations to better understand the relationship between the thermodynamic instability of 6428-LSCF and cell fabrication/testing conditions. First-principles calculations reveal that LSCF-6428 is not stable during cell manufacturing and testing conditions, which supports the experimental identification of secondary phases in both as-fabricated and tested cells. Together, these results demonstrate that the challenging environments encountered by SOECs during cell manufacturing and operation lead to instabilities of the target 6428-LSCF anode material and underscore the need for more durable, high-performing SOEC components.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 2","pages":"207-218"},"PeriodicalIF":3.7,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11950864/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143754585","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":"Understanding (La,Sr)(Co,Fe)O3−δ Phase Instability within SOECs Using a Combined Experimental and Atomistic Modeling Approach","authors":"Heather S. Slomski,&nbsp;Jonas L. Kaufman,&nbsp;Michael J. Dzara,&nbsp;Nicholas A. Strange,&nbsp;Cameron Priest,&nbsp;Jeremy L. Hartvigsen,&nbsp;Nicholas Kane,&nbsp;Micah Casteel,&nbsp;Brandon C. Wood,&nbsp;David S. Ginley,&nbsp;Kyoung E. Kweon*,&nbsp;Brian P. Gorman* and Sarah Shulda*,&nbsp;","doi":"10.1021/acsphyschemau.4c0009510.1021/acsphyschemau.4c00095","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00095https://doi.org/10.1021/acsphyschemau.4c00095","url":null,"abstract":"<p >Understanding the onset of degradation in the air electrode within solid oxide electrolysis cells (SOECs), and the subsequent impact on cell performance, is a critical step in mitigating the performance losses and stability issues of SOECs. In an effort to identify early onset degradation phenomena, SOECs were characterized as fabricated and after testing potentiostatically at 1.3 V for 1000 h at 750 °C. SOEC air electrodes composed of a 1:1 composite of La_0.6Sr_0.4Co_0.2Fe_0.8O_3−δ (6428-LSCF) and Gd_0.1Ce_0.9O_1.95 (GDC) were studied using synchrotron X-ray diffraction (XRD), scanning transmission electron microscopy coupled with energy dispersive X-ray spectroscopy (STEM-EDS), and X-ray absorption near-edge spectroscopy (XANES) to evaluate the changes in the air electrode structurally and chemically. These techniques show the migration of Sr species from the air electrode through pores in the GDC barrier layer, progressing to the electrolyte boundary, where it accumulates and reacts with (Zr_0.84Y_0.16)O_2−δ (YSZ) to form SrZrO₃. Microscopy results are paired with atomistic simulations to better understand the relationship between the thermodynamic instability of 6428-LSCF and cell fabrication/testing conditions. First-principles calculations reveal that LSCF-6428 is not stable during cell manufacturing and testing conditions, which supports the experimental identification of secondary phases in both as-fabricated and tested cells. Together, these results demonstrate that the challenging environments encountered by SOECs during cell manufacturing and operation lead to instabilities of the target 6428-LSCF anode material and underscore the need for more durable, high-performing SOEC components.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 2","pages":"207–218 207–218"},"PeriodicalIF":3.7,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00095","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143696423","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":"Improved Skill of Rotaxanes to Recognize Cations: A Theoretical Perspective","authors":"Renato Pereira Orenha*,&nbsp;Alvaro Muñoz-Castro,&nbsp;Maurício Jeomar Piotrowski,&nbsp;Giovanni F. Caramori*,&nbsp;Renato Gonçalves Rocha and Renato Luis Tame Parreira*,&nbsp;","doi":"10.1021/acsphyschemau.4c0009010.1021/acsphyschemau.4c00090","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00090https://doi.org/10.1021/acsphyschemau.4c00090","url":null,"abstract":"<p >Cations have significant applications in fields such as medicinal inorganic chemistry and catalysis. Rotaxanes are composed of a macrocyclic structure that is mechanically interlocked with a linear molecule. These mechanically interlocked molecules (MIMs) provide a potential chemical environment that allows for the interaction with cations. In this study, the bonding situations between rotaxanes or their acyclic/cyclic molecular derivatives and: (i) transition metal (Zn²⁺ and Cd²⁺); or (ii) alkali metal (Li⁺, Na⁺, and K⁺), cations have been studied. It is notable that among the MIMs structures, the rotaxanes demonstrate enhanced interactions with cations in comparison to the cyclic and, notably, the acyclic derivative molecules. The modification of rotaxane structures through structural changes and chemical reduction represents an intriguing approach to enhance cationic recognition, which is supported by the formation of more favorable electrostatic and/or orbital interaction energies in comparison with Pauli repulsive energies. The findings of this investigation can be employed in the synthesis of compounds with enhanced cation recognition capabilities.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 2","pages":"183–194 183–194"},"PeriodicalIF":3.7,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00090","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143696465","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":"Improved Skill of Rotaxanes to Recognize Cations: A Theoretical Perspective.","authors":"Renato Pereira Orenha, Alvaro Muñoz-Castro, Maurício Jeomar Piotrowski, Giovanni F Caramori, Renato Gonçalves Rocha, Renato Luis Tame Parreira","doi":"10.1021/acsphyschemau.4c00090","DOIUrl":"10.1021/acsphyschemau.4c00090","url":null,"abstract":"<p><p>Cations have significant applications in fields such as medicinal inorganic chemistry and catalysis. Rotaxanes are composed of a macrocyclic structure that is mechanically interlocked with a linear molecule. These mechanically interlocked molecules (MIMs) provide a potential chemical environment that allows for the interaction with cations. In this study, the bonding situations between rotaxanes or their acyclic/cyclic molecular derivatives and: (i) transition metal (Zn²⁺ and Cd²⁺); or (ii) alkali metal (Li⁺, Na⁺, and K⁺), cations have been studied. It is notable that among the MIMs structures, the rotaxanes demonstrate enhanced interactions with cations in comparison to the cyclic and, notably, the acyclic derivative molecules. The modification of rotaxane structures through structural changes and chemical reduction represents an intriguing approach to enhance cationic recognition, which is supported by the formation of more favorable electrostatic and/or orbital interaction energies in comparison with Pauli repulsive energies. The findings of this investigation can be employed in the synthesis of compounds with enhanced cation recognition capabilities.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 2","pages":"183-194"},"PeriodicalIF":3.7,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11950869/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143754554","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":"Is the Future of Materials Amorphous? Challenges and Opportunities in Simulations of Amorphous Materials","authors":"Ata Madanchi,&nbsp;Emna Azek,&nbsp;Karim Zongo,&nbsp;Laurent K. Béland,&nbsp;Normand Mousseau and Lena Simine*,&nbsp;","doi":"10.1021/acsphyschemau.4c0006310.1021/acsphyschemau.4c00063","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00063https://doi.org/10.1021/acsphyschemau.4c00063","url":null,"abstract":"<p >Amorphous solids form an enormous and underutilized class of materials. In order to drive the discovery of new useful amorphous materials further we need to achieve a closer convergence between computational and experimental methods. In this review, we highlight some of the important gaps between computational simulations and experiments, discuss popular state-of-the-art computational techniques such as the Activation Relaxation Technique <i>nouveau</i> (ARTn) and Reverse Monte Carlo (RMC), and introduce more recent advances: machine learning interatomic potentials (MLIPs) and generative machine learning for simulations of amorphous matter (e.g., MAP). Examples are drawn from amorphous silicon and silica literature as well as from molecular glasses. Our outlook stresses the need for new computational methods to extend the time- and length-scales accessible through numerical simulations.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 1","pages":"3–16 3–16"},"PeriodicalIF":3.7,"publicationDate":"2024-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00063","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086803","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":"Is the Future of Materials Amorphous? Challenges and Opportunities in Simulations of Amorphous Materials.","authors":"Ata Madanchi, Emna Azek, Karim Zongo, Laurent K Béland, Normand Mousseau, Lena Simine","doi":"10.1021/acsphyschemau.4c00063","DOIUrl":"10.1021/acsphyschemau.4c00063","url":null,"abstract":"<p><p>Amorphous solids form an enormous and underutilized class of materials. In order to drive the discovery of new useful amorphous materials further we need to achieve a closer convergence between computational and experimental methods. In this review, we highlight some of the important gaps between computational simulations and experiments, discuss popular state-of-the-art computational techniques such as the Activation Relaxation Technique <i>nouveau</i> (ARTn) and Reverse Monte Carlo (RMC), and introduce more recent advances: machine learning interatomic potentials (MLIPs) and generative machine learning for simulations of amorphous matter (e.g., MAP). Examples are drawn from amorphous silicon and silica literature as well as from molecular glasses. Our outlook stresses the need for new computational methods to extend the time- and length-scales accessible through numerical simulations.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 1","pages":"3-16"},"PeriodicalIF":3.7,"publicationDate":"2024-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758375/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143047882","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}