The Journal of Physical Chemistry Letters最新文献

Reversible Hiding of Janus Structural Color Pattern Induced by ZnS Colloidal Spheres on Inverse-Opal Structure

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-22 DOI: 10.1021/acs.jpclett.5c00468

Zheng Shi, Tianyi Liu, Suli Wu

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 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

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

2D Electronic Spectroscopy Uncovers 2D Materials: Theoretical Study of Nanocavity-Integrated Monolayer Semiconductors

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

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

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

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

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

IF 6.475 2区化学

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

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

引用次数: 0

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

IF 6.475 2区化学

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

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

引用次数: 0

Polarization Switching of Photocatalytic Solar-to-Hydrogen Conversion in Two-Dimensional Single-Layer Lattices: Insights from First-Principles and Non-adiabatic Molecular Dynamics.

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-20 Epub Date: 2025-03-10 DOI: 10.1021/acs.jpclett.5c00028

Yu-Liang Liu, Yi-Dong Zhu, Run-Yang Xin, Wen-Kai Zhao, Xing-Shuai Lv, Feng Gao, Chuan-Lu Yang

{"title":"Polarization Switching of Photocatalytic Solar-to-Hydrogen Conversion in Two-Dimensional Single-Layer Lattices: Insights from First-Principles and Non-adiabatic Molecular Dynamics.","authors":"Yu-Liang Liu, Yi-Dong Zhu, Run-Yang Xin, Wen-Kai Zhao, Xing-Shuai Lv, Feng Gao, Chuan-Lu Yang","doi":"10.1021/acs.jpclett.5c00028","DOIUrl":"10.1021/acs.jpclett.5c00028","url":null,"abstract":"Two-dimensional polar materials with adjustable polarization hold significant potential to improve photocatalytic water-splitting performance. However, due to the distinct mechanism for regulating polarization and photocatalysis, achieving efficient polarization modulation for enhanced photocatalytic efficiency remains challenging. Herein, using first-principles calculations with non-adiabatic molecular dynamics simulations, we identify four single-layer materials of MoXX'N3Y (X and X' = Si and Ge; X ≠ X'; and Y = P and As), whose catalytic activity can be well-tuned by polarization switching. Adjusting electronic asymmetry contributes to effective control of electric polarization, ultimately affecting catalytic reaction paths and carrier dynamics. Consequently, P↑ MoGeSiN3Y allows spontaneous redox reactions for overall water splitting, unlike P↓ MoSiGeN3Y. Besides, the polarization switching in MoXX'N3Y monolayers enhances solar-to-hydrogen conversion efficiency and prolongs carrier lifetimes, thereby achieving a polarization-dependent photocatalytic switch. This study opens an avenue to modify the polarization and significantly improve the catalytic efficiency.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"2837-2844"},"PeriodicalIF":4.8,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143595787","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

Electrically Modulated Fluorescence in Single Rare-Earth Particles

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-20 DOI: 10.1021/acs.jpclett.5c00195

Wenjing Duan, Yibo Yang, Jianyue He, Shiyang Lyu, Yuang Chen, Wenxin Zhu, Shaokun Ling, Chen Zhang, Yan-Zhen Zheng, Jiandong Feng

{"title":"Electrically Modulated Fluorescence in Single Rare-Earth Particles","authors":"Wenjing Duan, Yibo Yang, Jianyue He, Shiyang Lyu, Yuang Chen, Wenxin Zhu, Shaokun Ling, Chen Zhang, Yan-Zhen Zheng, Jiandong Feng","doi":"10.1021/acs.jpclett.5c00195","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00195","url":null,"abstract":"Rare earth (RE)-based complexes, due to their unique electronic structures, exhibit excellent fluorescence properties with high quantum yield and a long lifetime. From an application perspective, exploring RE-based complexes in luminescent optoelectronic devices asks for effective modulation approaches that control the luminescent properties. Here we report an electrically modulated fluorescence phenomenon in an RE-based complex, namely Eu16(μ4-F)6(μ3-F)12(tBuCOO)18[N(CH2CH2O)3]4 (EuFC-16) particles, which effectively controls the optical behavior of individual particles. Frequency-dependent measurements and theoretical analysis reveal a charging mechanism on particles that rationalizes the voltage-modulated fluorescence. This charging-induced fluorescence modulation enables the localized capacitance mapping of individual RE particles at the single-pixel level. Moreover, modulation heterogeneity is observed within a single EuFC-16 particle, highlighting the importance of charge-distribution-controlled optical properties at the subparticle level. Our finding may offer a potential approach for controlling the luminescence of RE-based complexes with spatiotemporal controllability and potential scaling capability, which may enrich potential applications of RE-based electro-optical devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"26 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660891","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