ACS Physical Chemistry Au最新文献_第3页

Improved Skill of Rotaxanes to Recognize Cations: A Theoretical Perspective

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-01-06 DOI: 10.1021/acsphyschemau.4c0009010.1021/acsphyschemau.4c00090

Renato Pereira Orenha*, Alvaro Muñoz-Castro, Maurício Jeomar Piotrowski, Giovanni F. Caramori*, Renato Gonçalves Rocha and Renato Luis Tame Parreira*,

{"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 and Renato Luis Tame Parreira*, ","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":"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.","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}

引用次数: 0

Improved Skill of Rotaxanes to Recognize Cations: A Theoretical Perspective.

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-01-06 eCollection Date: 2025-03-26 DOI: 10.1021/acsphyschemau.4c00090

Renato Pereira Orenha, Alvaro Muñoz-Castro, Maurício Jeomar Piotrowski, Giovanni F Caramori, Renato Gonçalves Rocha, Renato Luis Tame Parreira

{"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":"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.","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}

引用次数: 0

Is the Future of Materials Amorphous? Challenges and Opportunities in Simulations of Amorphous Materials

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-12-31 DOI: 10.1021/acsphyschemau.4c0006310.1021/acsphyschemau.4c00063

Ata Madanchi, Emna Azek, Karim Zongo, Laurent K. Béland, Normand Mousseau and Lena Simine*,

{"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 and Lena Simine*, ","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":"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 nouveau (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.","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}

引用次数: 0

Is the Future of Materials Amorphous? Challenges and Opportunities in Simulations of Amorphous Materials.

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-12-31 eCollection Date: 2025-01-22 DOI: 10.1021/acsphyschemau.4c00063

Ata Madanchi, Emna Azek, Karim Zongo, Laurent K Béland, Normand Mousseau, Lena Simine

引用次数: 0

Design Criteria for Active and Selective Catalysts in the Nitrogen Oxidation Reaction

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-12-24 DOI: 10.1021/acsphyschemau.4c0005810.1021/acsphyschemau.4c00058

Muhammad Usama, Samad Razzaq and Kai S. Exner*,

{"title":"Design Criteria for Active and Selective Catalysts in the Nitrogen Oxidation Reaction","authors":"Muhammad Usama, Samad Razzaq and Kai S. Exner*, ","doi":"10.1021/acsphyschemau.4c0005810.1021/acsphyschemau.4c00058","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00058https://doi.org/10.1021/acsphyschemau.4c00058","url":null,"abstract":"The direct conversion of dinitrogen to nitrate is a dream reaction to combine the Haber–Bosch and Ostwald processes as well as steam reforming using electrochemistry in a single process. Regrettably, the corresponding nitrogen oxidation (NOR) reaction is hampered by a selectivity problem, since the oxygen evolution reaction (OER) is both thermodynamically and kinetically favored in the same potential range. This opens the search for the identification of active and selective NOR catalysts to enable nitrate production under anodic reaction conditions. While theoretical considerations using the computational hydrogen electrode approach have helped in identifying potential material motifs for electrocatalytic reactions over the last decades, the inherent complexity of the NOR, which consists of ten proton-coupled electron transfer steps and thus at least nine intermediate states, poses a challenge for electronic structure theory calculations in the realm of materials screening. To this end, we present a different strategy to capture the competing NOR and OER at the atomic scale. Using a data-driven method, we provide a framework to derive generalized design criteria for materials with selectivity toward NOR. This leads to a significant reduction of the computational costs, since only two free-energy changes need to be evaluated to draw a first conclusion on NOR selectivity.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 1","pages":"38–46 38–46"},"PeriodicalIF":3.7,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00058","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086486","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}

引用次数: 0

Design Criteria for Active and Selective Catalysts in the Nitrogen Oxidation Reaction.

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-12-24 eCollection Date: 2025-01-22 DOI: 10.1021/acsphyschemau.4c00058

Muhammad Usama, Samad Razzaq, Kai S Exner

{"title":"Design Criteria for Active and Selective Catalysts in the Nitrogen Oxidation Reaction.","authors":"Muhammad Usama, Samad Razzaq, Kai S Exner","doi":"10.1021/acsphyschemau.4c00058","DOIUrl":"10.1021/acsphyschemau.4c00058","url":null,"abstract":"The direct conversion of dinitrogen to nitrate is a dream reaction to combine the Haber-Bosch and Ostwald processes as well as steam reforming using electrochemistry in a single process. Regrettably, the corresponding nitrogen oxidation (NOR) reaction is hampered by a selectivity problem, since the oxygen evolution reaction (OER) is both thermodynamically and kinetically favored in the same potential range. This opens the search for the identification of active and selective NOR catalysts to enable nitrate production under anodic reaction conditions. While theoretical considerations using the computational hydrogen electrode approach have helped in identifying potential material motifs for electrocatalytic reactions over the last decades, the inherent complexity of the NOR, which consists of ten proton-coupled electron transfer steps and thus at least nine intermediate states, poses a challenge for electronic structure theory calculations in the realm of materials screening. To this end, we present a different strategy to capture the competing NOR and OER at the atomic scale. Using a data-driven method, we provide a framework to derive generalized design criteria for materials with selectivity toward NOR. This leads to a significant reduction of the computational costs, since only two free-energy changes need to be evaluated to draw a first conclusion on NOR selectivity.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 1","pages":"38-46"},"PeriodicalIF":3.7,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11758373/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143047861","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}

引用次数: 0

Unveiling the Impact of Spin and Cation Dynamics on Raman Spectroscopy in Co-Ferrite.

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-12-20 eCollection Date: 2025-03-26 DOI: 10.1021/acsphyschemau.4c00088

Tahani Saad Almutairi

{"title":"Unveiling the Impact of Spin and Cation Dynamics on Raman Spectroscopy in Co-Ferrite.","authors":"Tahani Saad Almutairi","doi":"10.1021/acsphyschemau.4c00088","DOIUrl":"10.1021/acsphyschemau.4c00088","url":null,"abstract":"Raman spectroscopy offers profound insights into the vibrational dynamics of spinel ferrites, yet the precise assignment of these modes presents a notable challenge. This difficulty stems from the complex structure of spinel ferrites, where metal cations of varying spins populate distinct lattice sites, complicating the spectroscopic characterization. Specifically, cobalt ferrite is extensively utilized in electronic applications due to its superior magnetic properties, influenced significantly by the degree of inversion, denoted as (x), and the spin configurations within the crystal. While the magnetic influences of (x) are well-documented, its impact on other material properties has not been thoroughly investigated through first-principles calculations. This study delves into how varying degrees of inversion from (x = 0) to (x = 1) and different magnetic interactions-ferromagnetism, ferrimagnetism, and antiferromagnetism-affect the Raman vibrational modes of cobalt ferrite. We introduce a new perspective on the mode assignments by comparing our findings with existing experimental data. These insights could significantly refine experimental synthesis protocols, ensuring the production of materials optimized for specific applications. The interplay between inversion and spin configurations not only elucidates the vibrational properties but also enhances our understanding of the fundamental physics governing these versatile materials.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 2","pages":"171-182"},"PeriodicalIF":3.7,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11950867/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143754588","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}

引用次数: 0

Unveiling the Impact of Spin and Cation Dynamics on Raman Spectroscopy in Co-Ferrite

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-12-20 DOI: 10.1021/acsphyschemau.4c0008810.1021/acsphyschemau.4c00088

Tahani Saad Almutairi*,

{"title":"Unveiling the Impact of Spin and Cation Dynamics on Raman Spectroscopy in Co-Ferrite","authors":"Tahani Saad Almutairi*, ","doi":"10.1021/acsphyschemau.4c0008810.1021/acsphyschemau.4c00088","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00088https://doi.org/10.1021/acsphyschemau.4c00088","url":null,"abstract":"Raman spectroscopy offers profound insights into the vibrational dynamics of spinel ferrites, yet the precise assignment of these modes presents a notable challenge. This difficulty stems from the complex structure of spinel ferrites, where metal cations of varying spins populate distinct lattice sites, complicating the spectroscopic characterization. Specifically, cobalt ferrite is extensively utilized in electronic applications due to its superior magnetic properties, influenced significantly by the degree of inversion, denoted as (x), and the spin configurations within the crystal. While the magnetic influences of (x) are well-documented, its impact on other material properties has not been thoroughly investigated through first-principles calculations. This study delves into how varying degrees of inversion from (x = 0) to (x = 1) and different magnetic interactions─ferromagnetism, ferrimagnetism, and antiferromagnetism─affect the Raman vibrational modes of cobalt ferrite. We introduce a new perspective on the mode assignments by comparing our findings with existing experimental data. These insights could significantly refine experimental synthesis protocols, ensuring the production of materials optimized for specific applications. The interplay between inversion and spin configurations not only elucidates the vibrational properties but also enhances our understanding of the fundamental physics governing these versatile materials.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 2","pages":"171–182 171–182"},"PeriodicalIF":3.7,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00088","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143696323","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}

引用次数: 0

Ultrafast Spectroscopy of Chemical Transformations

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-12-17 DOI: 10.1021/acsphyschemau.4c0010010.1021/acsphyschemau.4c00100

Tanja Cuk*, Jin Z. Zhang* and Gemma Solomon*,

引用次数: 0

Ultrafast Spectroscopy of Chemical Transformations.

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-12-17 eCollection Date: 2025-01-22 DOI: 10.1021/acsphyschemau.4c00100

Tanja Cuk, Jin Z Zhang, Gemma Solomon

引用次数: 0