The Journal of Physical Chemistry Letters最新文献_第7页

Manipulating the Interface Relay Jumps of OH–ad Species to Accelerate the Anode Reaction Kinetics in Direct Ammonia Fuel Cells

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c00384

Xiaohui Xu, Yu Cheng, Xinnan Xu, Weidong Tang, SiSi Liu, Chunlin Mu, Yinshi Huang, Baocong Guo, Chenglin Yan, Tao Qian

{"title":"Manipulating the Interface Relay Jumps of OH–ad Species to Accelerate the Anode Reaction Kinetics in Direct Ammonia Fuel Cells","authors":"Xiaohui Xu, Yu Cheng, Xinnan Xu, Weidong Tang, SiSi Liu, Chunlin Mu, Yinshi Huang, Baocong Guo, Chenglin Yan, Tao Qian","doi":"10.1021/acs.jpclett.5c00384","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00384","url":null,"abstract":"Ammonia is a hydrogen-dense, carbon-neutral energy carrier, but sluggish oxidation kinetics and catalyst toxicity limit its large-scale use in low-temperature alkaline direct ammonia fuel cells (DAFCs). Inspired by the “Grotthuss hopping” theory, we designed a hydroxyl group-modified membrane electrode catalyst system through the modification of interface key groups. This system can interact with adsorbed OH– (hereafter, OH–ad), thus being similar to a “relay” that allows OH–ad to jump from one active site to another and then react with ammonia intermediates, injecting more impetus into the kinetic process of the orderly release of OH–ad. The results of molecular dynamics (MD) simulations and operando Fourier transform infrared spectroscopy (operando-FTIR) further demonstrated and confirmed that this process follows the Gerischer–Mauerer (G–M) mechanism. Consequently, the mass activity of the best membrane electrode catalyst in this series, PtNiNC@OH0.05 (373 A g–1Pt), has been significantly enhanced in alkaline media, which is 3.2 times higher than that of the commercial 20% Pt/C (116 A g–1Pt) catalyst. Even more surprisingly, the DAFC of the membrane electrode catalyst as an anode achieves a peak power density of 17.4 mW cm–2 at 60 °C, which is 9.89-fold higher than that of 20% Pt/C (1.76 mW cm–2). The interface modification method based on the “relay” jumps proposed by us provides a way to fabricate DAFC membrane electrode catalysts.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"1 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Circularly Polarized Light-Induced Microwave Conductivity Measurement: Rapid Screening Technique of Electronic Conductivity in Chiral Molecular Materials 圆偏振光诱导微波电导率测量：手性分子材料电子电导率的快速筛选技术

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c00370

Yun Hee Koo, Yusuke Tsutsui, Mikito Omoto, Yohei Yomogida, Kazuhiro Yanagi, Yuichiro K. Kato, M. Alejandra Hermosilla-Palacios, Jeffrey L. Blackburn, Shu Seki

{"title":"Circularly Polarized Light-Induced Microwave Conductivity Measurement: Rapid Screening Technique of Electronic Conductivity in Chiral Molecular Materials","authors":"Yun Hee Koo, Yusuke Tsutsui, Mikito Omoto, Yohei Yomogida, Kazuhiro Yanagi, Yuichiro K. Kato, M. Alejandra Hermosilla-Palacios, Jeffrey L. Blackburn, Shu Seki","doi":"10.1021/acs.jpclett.5c00370","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00370","url":null,"abstract":"We developed circularly polarized light–time-resolved microwave conductivity (CPL–TRMC) for investigation of the CPL-dependent photoinduced charge carrier dynamics in chiral materials with chiroptical properties. Chiral R- or S-perylenediimide (PDI) molecular thin films were paired with handedness-sorted (6,5) and (11,–5) single-walled carbon nanotube (SWCNT) films to compose a donor (D)–acceptor (A) system for the spin-dependent charge separation process, and the D–A system was examined through linear and circular polarization-dependent steady-state and time-resolved measurements. The R-PDI-(6,5) film exhibited strong enhancement in circular dichroism (CD) and revealed a reversed transient conductivity signal, relative to the polarity of CD in CPL–TRMC measurement upon excitation of the E11 state, which is interpreted as arising from a spin-dependent initial charge separation process. Through linear polarization-dependent flash photolysis TRMC and circular polarization-resolved femtosecond transient absorption, we could deduce that sub-picosecond intertubular charge separation upon E11 excitation in SWCNT was responsible for the spin-dependent photoconductivity transients observed in CPL–TRMC measurements.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"46 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672593","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Reflection on the Use of Molecular Simulation to Respond to SARS-CoV-2 Pandemic Threats

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.4c0365410.1021/acs.jpclett.4c03654

Lorenzo Casalino, Carlos A. Ramos-Guzmán, Rommie E. Amaro*, Carlos Simmerling*, Alessio Lodola*, Adrian J. Mulholland*, Katarzyna Świderek* and Vicent Moliner*,

引用次数: 0

Manipulating the Interface Relay Jumps of OH–ad Species to Accelerate the Anode Reaction Kinetics in Direct Ammonia Fuel Cells

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c0038410.1021/acs.jpclett.5c00384

Xiaohui Xu, Yu Cheng*, Xinnan Xu, Weidong Tang, SiSi Liu, Chunlin Mu, Yinshi Huang, Baocong Guo, Chenglin Yan and Tao Qian*,

{"title":"Manipulating the Interface Relay Jumps of OH–ad Species to Accelerate the Anode Reaction Kinetics in Direct Ammonia Fuel Cells","authors":"Xiaohui Xu, Yu Cheng*, Xinnan Xu, Weidong Tang, SiSi Liu, Chunlin Mu, Yinshi Huang, Baocong Guo, Chenglin Yan and Tao Qian*, ","doi":"10.1021/acs.jpclett.5c0038410.1021/acs.jpclett.5c00384","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00384https://doi.org/10.1021/acs.jpclett.5c00384","url":null,"abstract":"Ammonia is a hydrogen-dense, carbon-neutral energy carrier, but sluggish oxidation kinetics and catalyst toxicity limit its large-scale use in low-temperature alkaline direct ammonia fuel cells (DAFCs). Inspired by the “Grotthuss hopping” theory, we designed a hydroxyl group-modified membrane electrode catalyst system through the modification of interface key groups. This system can interact with adsorbed OH– (hereafter, OH–ad), thus being similar to a “relay” that allows OH–ad to jump from one active site to another and then react with ammonia intermediates, injecting more impetus into the kinetic process of the orderly release of OH–ad. The results of molecular dynamics (MD) simulations and operando Fourier transform infrared spectroscopy (operando-FTIR) further demonstrated and confirmed that this process follows the Gerischer–Mauerer (G–M) mechanism. Consequently, the mass activity of the best membrane electrode catalyst in this series, PtNiNC@OH0.05 (373 A g–1Pt), has been significantly enhanced in alkaline media, which is 3.2 times higher than that of the commercial 20% Pt/C (116 A g–1Pt) catalyst. Even more surprisingly, the DAFC of the membrane electrode catalyst as an anode achieves a peak power density of 17.4 mW cm–2 at 60 °C, which is 9.89-fold higher than that of 20% Pt/C (1.76 mW cm–2). The interface modification method based on the “relay” jumps proposed by us provides a way to fabricate DAFC membrane electrode catalysts.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3212–3224 3212–3224"},"PeriodicalIF":4.8,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

2D Electronic Spectroscopy Uncovers 2D Materials: Theoretical Study of Nanocavity-Integrated Monolayer Semiconductors 二维电子能谱揭示二维材料：纳米空腔集成单层半导体的理论研究

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c00280

Kaijun Shen, Kewei Sun, Maxim F. Gelin, Yang Zhao

引用次数: 0

Enhancement of Dendrite-Free Lithium Metal Anode Performance through LiF-Rich Protective Layer for Lithium Metal Batteries

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c0045910.1021/acs.jpclett.5c00459

Changlian Wang, Kun Zhang, Yuning Cui, Qingtian Li, Tengwei Ma, Fangyuan Li, Hailong Qiu* and Di Jin*,

{"title":"Enhancement of Dendrite-Free Lithium Metal Anode Performance through LiF-Rich Protective Layer for Lithium Metal Batteries","authors":"Changlian Wang, Kun Zhang, Yuning Cui, Qingtian Li, Tengwei Ma, Fangyuan Li, Hailong Qiu* and Di Jin*, ","doi":"10.1021/acs.jpclett.5c0045910.1021/acs.jpclett.5c00459","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00459https://doi.org/10.1021/acs.jpclett.5c00459","url":null,"abstract":"Lithium metal batteries represent a cutting-edge class of energy storage devices, yet the high surface diffusion energy barrier of lithium metal prompts preferential Li+ accumulation and deposition, fostering the growth of lithium dendrites. To address this challenge, a straightforward solvent-based approach is employed to create a LiF-rich protective layer on the lithium anode. The uniform LiF interface facilitates the transport of Li+ and effectively induces the uniform plating and stripping of lithium while inhibiting the formation of dendrites. Notably, the symmetric battery incorporating a lithium anode modified with appropriate LiF demonstrates substantially enhanced cycling performance. Importantly, the full cell matched with LiFePO4 displays an initial capacity of 146.3 mAh g–1 and a capacity retention rate of 92.7% after 300 cycles. Its practical application has also been verified in symmetric batteries and full batteries for PEO solid-state batteries. This work underscores the potential of the LiF protective layer to boost the dendrite-free lithium metal anode.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3240–3248 3240–3248"},"PeriodicalIF":4.8,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758907","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Predicting Thermodynamic Stability at Protein G Sites with Deleterious Mutations Using λ-Dynamics with Competitive Screening

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c00260

Christopher Yeh, Ryan L. Hayes

{"title":"Predicting Thermodynamic Stability at Protein G Sites with Deleterious Mutations Using λ-Dynamics with Competitive Screening","authors":"Christopher Yeh, Ryan L. Hayes","doi":"10.1021/acs.jpclett.5c00260","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00260","url":null,"abstract":"Free energy predictions are useful in protein design and computer-aided drug design. Alchemical free energy methods are highly accurate, and the alchemical method λ-dynamics significantly improves computational cost. Recent progress made simulations of dozens of perturbations at a single site possible, enabling in silico site-saturation mutagenesis with λ-dynamics. Site-saturation mutagenesis may require increased sampling to characterize many mutations and to accommodate structural disruptions around deleterious mutations. We reintroduce the neglected idea of competitive screening with λ-dynamics to address both issues. Traditional landscape flattening tunes two distinct biases to sample all mutations equally in the folded and unfolded states. Competitive screening transfers the unfolded bias to the folded state so that only reasonable mutations are sampled. Competitive screening is demonstrated on four surface sites and four buried sites in protein G and provides improvements for buried sites. Consequently, competitive screening provides new opportunities for molecular design within larger chemical spaces.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"34 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Circularly Polarized Light-Induced Microwave Conductivity Measurement: Rapid Screening Technique of Electronic Conductivity in Chiral Molecular Materials

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c0037010.1021/acs.jpclett.5c00370

Yun Hee Koo, Yusuke Tsutsui*, Mikito Omoto, Yohei Yomogida, Kazuhiro Yanagi*, Yuichiro K. Kato, M. Alejandra Hermosilla-Palacios, Jeffrey L. Blackburn* and Shu Seki*,

{"title":"Circularly Polarized Light-Induced Microwave Conductivity Measurement: Rapid Screening Technique of Electronic Conductivity in Chiral Molecular Materials","authors":"Yun Hee Koo, Yusuke Tsutsui*, Mikito Omoto, Yohei Yomogida, Kazuhiro Yanagi*, Yuichiro K. Kato, M. Alejandra Hermosilla-Palacios, Jeffrey L. Blackburn* and Shu Seki*, ","doi":"10.1021/acs.jpclett.5c0037010.1021/acs.jpclett.5c00370","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00370https://doi.org/10.1021/acs.jpclett.5c00370","url":null,"abstract":"We developed circularly polarized light–time-resolved microwave conductivity (CPL–TRMC) for investigation of the CPL-dependent photoinduced charge carrier dynamics in chiral materials with chiroptical properties. Chiral R- or S-perylenediimide (PDI) molecular thin films were paired with handedness-sorted (6,5) and (11,–5) single-walled carbon nanotube (SWCNT) films to compose a donor (D)–acceptor (A) system for the spin-dependent charge separation process, and the D–A system was examined through linear and circular polarization-dependent steady-state and time-resolved measurements. The R-PDI-(6,5) film exhibited strong enhancement in circular dichroism (CD) and revealed a reversed transient conductivity signal, relative to the polarity of CD in CPL–TRMC measurement upon excitation of the E11 state, which is interpreted as arising from a spin-dependent initial charge separation process. Through linear polarization-dependent flash photolysis TRMC and circular polarization-resolved femtosecond transient absorption, we could deduce that sub-picosecond intertubular charge separation upon E11 excitation in SWCNT was responsible for the spin-dependent photoconductivity transients observed in CPL–TRMC measurements.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3232–3239 3232–3239"},"PeriodicalIF":4.8,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758901","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Imaging the Rovibrational Ground State of the Helium–Neon Dimers 4He20Ne and 4He22Ne

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c0037710.1021/acs.jpclett.5c00377

J. Kruse, J. Schröder, D. Blume, R. Dörner* and M. Kunitski*,

{"title":"Imaging the Rovibrational Ground State of the Helium–Neon Dimers 4He20Ne and 4He22Ne","authors":"J. Kruse, J. Schröder, D. Blume, R. Dörner* and M. Kunitski*, ","doi":"10.1021/acs.jpclett.5c0037710.1021/acs.jpclett.5c00377","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00377https://doi.org/10.1021/acs.jpclett.5c00377","url":null,"abstract":"The helium–neon dimer has been subject to many theoretical studies, in which the interaction potential of the helium–neon system has been calculated with ever increasing accuracy. Calculations predict that the helium–neon system supports only a few bound states, which makes the system inaccessible to standard spectroscopic techniques. Previous experiments have probed the helium–neon potential by comparing measured and predicted scattering cross sections. However, the spatial structure and energetics of the bound states of the helium–neon system have not been studied experimentally in great detail. We employ Coulomb explosion imaging (CEI) to measure the pair distance distributions of the helium–neon dimers 4He20Ne and 4He22Ne in their rovibrational ground state. For each dimer, the binding energy is extracted from the measured pair distance distribution. Additionally, the pair distance distribution provides access to the helium–neon potential.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3225–3231 3225–3231"},"PeriodicalIF":4.8,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.5c00377","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758904","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhancement of Dendrite-Free Lithium Metal Anode Performance through LiF-Rich Protective Layer for Lithium Metal Batteries 通过富含 LiF 的保护层提高金属锂锂电池的无枝晶型金属锂负极性能

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-21 DOI: 10.1021/acs.jpclett.5c00459

Changlian Wang, Kun Zhang, Yuning Cui, Qingtian Li, Tengwei Ma, Fangyuan Li, Hailong Qiu, Di Jin

{"title":"Enhancement of Dendrite-Free Lithium Metal Anode Performance through LiF-Rich Protective Layer for Lithium Metal Batteries","authors":"Changlian Wang, Kun Zhang, Yuning Cui, Qingtian Li, Tengwei Ma, Fangyuan Li, Hailong Qiu, Di Jin","doi":"10.1021/acs.jpclett.5c00459","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00459","url":null,"abstract":"Lithium metal batteries represent a cutting-edge class of energy storage devices, yet the high surface diffusion energy barrier of lithium metal prompts preferential Li+ accumulation and deposition, fostering the growth of lithium dendrites. To address this challenge, a straightforward solvent-based approach is employed to create a LiF-rich protective layer on the lithium anode. The uniform LiF interface facilitates the transport of Li+ and effectively induces the uniform plating and stripping of lithium while inhibiting the formation of dendrites. Notably, the symmetric battery incorporating a lithium anode modified with appropriate LiF demonstrates substantially enhanced cycling performance. Importantly, the full cell matched with LiFePO4 displays an initial capacity of 146.3 mAh g–1 and a capacity retention rate of 92.7% after 300 cycles. Its practical application has also been verified in symmetric batteries and full batteries for PEO solid-state batteries. This work underscores the potential of the LiF protective layer to boost the dendrite-free lithium metal anode.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"10 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672596","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0