ACS Physical Chemistry Au最新文献_第4页

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-26

Victor Somtochukwu Mbanugo, Boluwatife Stephen Ojo, Ta Chun Lin, Yue-Wern Huang, Marek Locmelis and Daoru Han*,

引用次数: 0

Choreoisosteres: Pseudoatom Variation in Macrocyclic Hinges Conserves Structure and Dynamics. Choreoisosteres：大环铰链中的假原子变异保护了结构和动力学。

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-10 eCollection Date: 2025-03-26 DOI: 10.1021/acsphyschemau.4c00103

Alexander J Menke, Joseph H Reibenspies, Casey J Patterson-Gardner, Alexander M Engstrom, R Scott Lokey, Eric E Simanek

引用次数: 0

Choreoisosteres: Pseudoatom Variation in Macrocyclic Hinges Conserves Structure and Dynamics Choreoisosteres：大环铰链中的假原子变异保护了结构和动力学

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-10 DOI: 10.1021/acsphyschemau.4c0010310.1021/acsphyschemau.4c00103

Alexander J. Menke, Joseph H. Reibenspies, Casey J. Patterson-Gardner, Alexander M. Engstrom, R. Scott Lokey and Eric E. Simanek*,

引用次数: 0

Preferred Orientation of a Physisorbed Molecular Catalyst and Implications for Selectivity. 物理吸附分子催化剂的择优取向及其选择性意义。

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-07 eCollection Date: 2025-05-28 DOI: 10.1021/acsphyschemau.5c00007

Guillaume P Laurent, Samuel L Leonard, Mita Halder, Damien B Culver, Peng Xu, Mark S Gordon, Frédéric A Perras

{"title":"Preferred Orientation of a Physisorbed Molecular Catalyst and Implications for Selectivity.","authors":"Guillaume P Laurent, Samuel L Leonard, Mita Halder, Damien B Culver, Peng Xu, Mark S Gordon, Frédéric A Perras","doi":"10.1021/acsphyschemau.5c00007","DOIUrl":"10.1021/acsphyschemau.5c00007","url":null,"abstract":"Confinement effects in stereoselective catalysis have been the topic of prolonged inquiry. Results have been largely mixed, with confinement having been reported to both enhance and degrade selectivity. Our ability to understand the surface's impact on catalytic mechanisms, and thus selectivity, has been severely hindered by the low level of details commonly seen in the structures of supported metal complexes. Recent developments in sensitivity-enhanced NMR are revealing not only the molecular structure of surface sites but also their configuration, orientation, and proximities to neighboring molecules. In studying [Rh-(cyclooctadiene)-((S)-(-)-2-aminomethyl-1-ethyl-pyrrolidine)]-CF3SO3 noncovalently immobilized to silica, an enantioselective hydrogenation catalyst, we observed a strong preference for a particular orientation of the complex relative to the support surface. We discuss how preferential adsorption may help reduce the number of competing reaction pathways and, in turn, have outsized effects on selectivity.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 3","pages":"293-301"},"PeriodicalIF":3.7,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12123549/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144200235","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

Preferred Orientation of a Physisorbed Molecular Catalyst and Implications for Selectivity 物理吸附分子催化剂的择优取向及其选择性意义

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-07 DOI: 10.1021/acsphyschemau.5c0000710.1021/acsphyschemau.5c00007

Guillaume P. Laurent, Samuel L. Leonard, Mita Halder, Damien B. Culver, Peng Xu, Mark S. Gordon and Frédéric A. Perras*,

{"title":"Preferred Orientation of a Physisorbed Molecular Catalyst and Implications for Selectivity","authors":"Guillaume P. Laurent, Samuel L. Leonard, Mita Halder, Damien B. Culver, Peng Xu, Mark S. Gordon and Frédéric A. Perras*, ","doi":"10.1021/acsphyschemau.5c0000710.1021/acsphyschemau.5c00007","DOIUrl":"https://doi.org/10.1021/acsphyschemau.5c00007https://doi.org/10.1021/acsphyschemau.5c00007","url":null,"abstract":"Confinement effects in stereoselective catalysis have been the topic of prolonged inquiry. Results have been largely mixed, with confinement having been reported to both enhance and degrade selectivity. Our ability to understand the surface’s impact on catalytic mechanisms, and thus selectivity, has been severely hindered by the low level of details commonly seen in the structures of supported metal complexes. Recent developments in sensitivity-enhanced NMR are revealing not only the molecular structure of surface sites but also their configuration, orientation, and proximities to neighboring molecules. In studying [Rh(cyclooctadiene)((S)-(−)-2-aminomethyl-1-ethyl-pyrrolidine)]CF3SO3 noncovalently immobilized to silica, an enantioselective hydrogenation catalyst, we observed a strong preference for a particular orientation of the complex relative to the support surface. We discuss how preferential adsorption may help reduce the number of competing reaction pathways and, in turn, have outsized effects on selectivity.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 3","pages":"293–301 293–301"},"PeriodicalIF":3.7,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.5c00007","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144146487","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

Elastic Electron Collisions with Cyanoacetylene 与氰乙炔的弹性电子碰撞

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-05 DOI: 10.1021/acsphyschemau.5c0000610.1021/acsphyschemau.5c00006

Victor A. S. daMata*, Giseli M. Moreira, Adevânia J. da Silva, Romarly F. da Costa, Luiz A. V. Mendes and Manoel G. P. Homem,

{"title":"Elastic Electron Collisions with Cyanoacetylene","authors":"Victor A. S. daMata*, Giseli M. Moreira, Adevânia J. da Silva, Romarly F. da Costa, Luiz A. V. Mendes and Manoel G. P. Homem, ","doi":"10.1021/acsphyschemau.5c0000610.1021/acsphyschemau.5c00006","DOIUrl":"https://doi.org/10.1021/acsphyschemau.5c00006https://doi.org/10.1021/acsphyschemau.5c00006","url":null,"abstract":"A comprehensive theoretical investigation involving electron collisions with cyanoacetylene is reported. Differential cross sections (DCSs), integral cross sections (ICSs), and momentum-transfer cross sections (MTCSs) for the elastic electron scattering were calculated using the Schwinger multichannel (SMC) method at the static-exchange plus polarization (SEP) level of approximation for energies ranging from 0.5 to 30 eV. The Schwinger variational method combined with Padé’s approximants (SVPA), considering static-exchange-polarization plus absorption (SEPA), was also applied for impact energies from 0.1 to 1000 eV. These results were complemented by calculations performed according to the screen-corrected independent atom model (SCIAM). Furthermore, original measurements of absolute elastic (DCSs) at 20 eV were conducted in a crossed-beam apparatus. The theoretical results display an outstanding agreement with each other and an overall agreement with the calculated cross sections available in the literature. The agreement between the calculated and measured results is quite encouraging, further validating the thoroughness of the current research.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 3","pages":"283–292 283–292"},"PeriodicalIF":3.7,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.5c00006","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144146486","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

Elastic Electron Collisions with Cyanoacetylene. 与氰乙炔的弹性电子碰撞。

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-05 eCollection Date: 2025-05-28 DOI: 10.1021/acsphyschemau.5c00006

Victor A S da Mata, Giseli M Moreira, Adevânia J da Silva, Romarly F da Costa, Luiz A V Mendes, Manoel G P Homem

{"title":"Elastic Electron Collisions with Cyanoacetylene.","authors":"Victor A S da Mata, Giseli M Moreira, Adevânia J da Silva, Romarly F da Costa, Luiz A V Mendes, Manoel G P Homem","doi":"10.1021/acsphyschemau.5c00006","DOIUrl":"10.1021/acsphyschemau.5c00006","url":null,"abstract":"A comprehensive theoretical investigation involving electron collisions with cyanoacetylene is reported. Differential cross sections (DCSs), integral cross sections (ICSs), and momentum-transfer cross sections (MTCSs) for the elastic electron scattering were calculated using the Schwinger multichannel (SMC) method at the static-exchange plus polarization (SEP) level of approximation for energies ranging from 0.5 to 30 eV. The Schwinger variational method combined with Padé's approximants (SVPA), considering static-exchange-polarization plus absorption (SEPA), was also applied for impact energies from 0.1 to 1000 eV. These results were complemented by calculations performed according to the screen-corrected independent atom model (SCIAM). Furthermore, original measurements of absolute elastic (DCSs) at 20 eV were conducted in a crossed-beam apparatus. The theoretical results display an outstanding agreement with each other and an overall agreement with the calculated cross sections available in the literature. The agreement between the calculated and measured results is quite encouraging, further validating the thoroughness of the current research.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 3","pages":"283-292"},"PeriodicalIF":3.7,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12123550/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144200231","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

Impact of the Channel Length in Nanoporous Electric Double-Layer Capacitors on the Charge Transport Explored by Metal–Organic Framework Films 纳米多孔双电层电容器通道长度对金属-有机骨架膜探索的电荷输运的影响

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-04 DOI: 10.1021/acsphyschemau.4c0010410.1021/acsphyschemau.4c00104

Yidong Liu, Abhinav Chandresh and Lars Heinke*,

{"title":"Impact of the Channel Length in Nanoporous Electric Double-Layer Capacitors on the Charge Transport Explored by Metal–Organic Framework Films","authors":"Yidong Liu, Abhinav Chandresh and Lars Heinke*, ","doi":"10.1021/acsphyschemau.4c0010410.1021/acsphyschemau.4c00104","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00104https://doi.org/10.1021/acsphyschemau.4c00104","url":null,"abstract":"For enhancing the performance of electric double-layer capacitors, the porous electrodes must be further optimized. While many studies on electrolyte and electrode structures enable detailed insights, the length of the pore channels of the electrode has been overlooked. Here, we use films of two-dimensional conductive metal–organic frameworks, where the film thickness (and thus the pore channel length) is rationally tuned over a wide range. Cyclic voltammetry experiments with two different electrolytes were conducted, revealing the charge transport kinetics in the porous electrodes. For the highly mobile electrolyte, the kinetics is not limited by ion transport (i.e., diffusion) even for thick films, exhibiting mainly surface-controlled kinetic behavior. In contrast, for the less mobile electrolyte, the kinetics is primarily limited by ion diffusion, and the pore channel length has a severe impact, where long channels result in strongly decreased capacitances, highlighting the importance of adjusting the channel length.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 3","pages":"266–273 266–273"},"PeriodicalIF":3.7,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00104","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144146485","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

Impact of the Channel Length in Nanoporous Electric Double-Layer Capacitors on the Charge Transport Explored by Metal-Organic Framework Films. 纳米多孔双电层电容器通道长度对金属-有机骨架膜探索的电荷输运的影响。

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-03-04 eCollection Date: 2025-05-28 DOI: 10.1021/acsphyschemau.4c00104

Yidong Liu, Abhinav Chandresh, Lars Heinke

{"title":"Impact of the Channel Length in Nanoporous Electric Double-Layer Capacitors on the Charge Transport Explored by Metal-Organic Framework Films.","authors":"Yidong Liu, Abhinav Chandresh, Lars Heinke","doi":"10.1021/acsphyschemau.4c00104","DOIUrl":"10.1021/acsphyschemau.4c00104","url":null,"abstract":"For enhancing the performance of electric double-layer capacitors, the porous electrodes must be further optimized. While many studies on electrolyte and electrode structures enable detailed insights, the length of the pore channels of the electrode has been overlooked. Here, we use films of two-dimensional conductive metal-organic frameworks, where the film thickness (and thus the pore channel length) is rationally tuned over a wide range. Cyclic voltammetry experiments with two different electrolytes were conducted, revealing the charge transport kinetics in the porous electrodes. For the highly mobile electrolyte, the kinetics is not limited by ion transport (i.e., diffusion) even for thick films, exhibiting mainly surface-controlled kinetic behavior. In contrast, for the less mobile electrolyte, the kinetics is primarily limited by ion diffusion, and the pore channel length has a severe impact, where long channels result in strongly decreased capacitances, highlighting the importance of adjusting the channel length.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 3","pages":"266-273"},"PeriodicalIF":3.7,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12123543/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144200232","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

"Button-on-a-String" Mechanism in Water, the Ultrafast UV-to-Heat Conversion by Mycosporine-like Amino Acid Porphyra-334 of Natural Sunscreen Compound. 天然防晒化合物类真菌菌素类氨基酸卟啉-334在水中的超快uv -热转化机理

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-02-26 eCollection Date: 2025-05-28 DOI: 10.1021/acsphyschemau.4c00107

Makoto Hatakeyama, Shinichiro Nakamura

{"title":"\"Button-on-a-String\" Mechanism in Water, the Ultrafast UV-to-Heat Conversion by Mycosporine-like Amino Acid Porphyra-334 of Natural Sunscreen Compound.","authors":"Makoto Hatakeyama, Shinichiro Nakamura","doi":"10.1021/acsphyschemau.4c00107","DOIUrl":"10.1021/acsphyschemau.4c00107","url":null,"abstract":"Mycosporine-like amino acids (MAAs) are a family of hydrophilic sunscreen compounds synthesized by aquatic organisms, such as algae and cyanobacteria. In this study, we demonstrate that porphyra-334, which is a common MAA, decays nonradiatively within several hundred femtoseconds after ultraviolet (UV) light absorption in water by rotating the intramolecular cyclohexenimine ring. The ring rotation resulted from the UV excitation of the intramolecular π-conjugation, and the ring rotation proceeded while preserving the hydrogen bonds with the surrounding water molecules. The hydrogen bonds were preserved due to the structural flexibility of the ring-attached amino acids of porphyra-334. The amino acids maintained their center of mass positions during the ring-rotating nonradiative decay. The amino acids and cyclohexenimine ring are analogous to the string and button of a button-on-a-string spinner, otherwise known as button whirligigs. Thus, we refer to the ring-rotating nonradiative decay of porphyra-334 as a button-on-a-string mechanism. We also show that this mechanism results from porphyra-334 itself rather than from the surrounding water molecules. The present results indicate that the molecular \"spinner\" exists in aquatic organisms and protects them from UV with the aid of water.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 3","pages":"274-282"},"PeriodicalIF":3.7,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12123545/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144200229","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