The Journal of Physical Chemistry Letters最新文献_第9页

Interpretable Multimodal Deep Ensemble Framework Dissecting Bloodbrain Barrier Permeability with Molecular Features. 可解释的多模态深系综框架与分子特征解剖血脑屏障通透性。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 Epub Date: 2025-06-03 DOI: 10.1021/acs.jpclett.5c01077

Dushuo Feng, Lulu Guan, Yunxiang Sun, Bote Qi, Yu Zou

{"title":"Interpretable Multimodal Deep Ensemble Framework Dissecting Bloodbrain Barrier Permeability with Molecular Features.","authors":"Dushuo Feng, Lulu Guan, Yunxiang Sun, Bote Qi, Yu Zou","doi":"10.1021/acs.jpclett.5c01077","DOIUrl":"10.1021/acs.jpclett.5c01077","url":null,"abstract":"Blood-brain barrier permeability (BBBP) prediction plays a critical role in the drug discovery process, particularly for compounds targeting the central nervous system. While machine learning (ML) has significantly advanced the prediction of BBBP, there remains an urgent need for interpretable ML models that can reveal the physicochemical principles governing BBB permeability. In this study, we propose a multimodal ML framework that integrates molecular fingerprints (Morgan, MACCS, RDK) and image features to improve BBBP prediction. The classification task (BBB-permeable vs nonpermeable) is addressed with a stacking ensemble model combining multiple base classifiers. The proposed framework demonstrates competitive predictive stability, generalization ability, and feature interpretability compared with recent approaches, under comparable evaluation settings. Beyond predictive performance, our framework incorporates Principal Component Analysis (PCA) and Shapley Additive Explanations (SHAP) analysis to highlight key fingerprint features contributing to predictions. The regression task (logBB value prediction) is tackled by a multi-input deep learning framework, incorporating a Transformer encoder for fingerprint processing, a convolutional neural network (CNN) for image feature extraction, and a Multi-Head Attention fusion mechanism to enhance feature interactions. Attention maps derived from the multimodal features reveal token-level relationships within molecular representations. This work provides an interpretable framework for modeling BBBP with enhanced transparency and mechanistic insight and lays the foundation for future studies incorporating transparent descriptors and physics-informed features.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"5806-5819"},"PeriodicalIF":4.8,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144214384","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

Warp-Driven Dual-Side Adsorption for Superior Surface-Enhanced Raman Scattering Performance of Transition Metal Dichalcogenides Nanosheets 翘曲驱动的双面吸附对过渡金属二硫族化合物纳米片表面增强拉曼散射性能的影响

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 DOI: 10.1021/acs.jpclett.5c0119710.1021/acs.jpclett.5c01197

Tong Xiang, Qiao Wang, Biwen He, Jibo Zhang, Xixi Huang, Wei Chen, Siwei Luo* and Xiang Qi,

{"title":"Warp-Driven Dual-Side Adsorption for Superior Surface-Enhanced Raman Scattering Performance of Transition Metal Dichalcogenides Nanosheets","authors":"Tong Xiang, Qiao Wang, Biwen He, Jibo Zhang, Xixi Huang, Wei Chen, Siwei Luo* and Xiang Qi, ","doi":"10.1021/acs.jpclett.5c0119710.1021/acs.jpclett.5c01197","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01197https://doi.org/10.1021/acs.jpclett.5c01197","url":null,"abstract":"Surface-enhanced Raman scattering (SERS) technology is highly sensitive but limited by the high cost of noble-metal substrates and the low enhancement of two-dimensional (2D) materials. This work proposes a dual-sided adsorption strategy utilizing warped structures at the cracks and edges of WSe2 and MoSe2 nanosheets grown by Chemical Vapor Deposition (CVD). Driven by capillary forces, probe molecules infiltrate the nanosheet–substrate interface, enabling dual-sided adsorption on both the upper and lower surfaces. This approach enhances SERS signals by up to 20-fold, with a detection limit of 10–10 M, surpassing most reported traditional single-sided adsorption modes. Additionally, it improves stability by isolating the probe molecules from oxygen. This study further enhanced the formation efficiency and coverage area of the dual-sided adsorption mode by leveraging wide warped structures. It offers new perspectives on the application of crack defects and the potential for the development of high-performance and highly stable SERS substrates.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"6212–6218 6212–6218"},"PeriodicalIF":4.8,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312375","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

In Silico Design of Methyl-Driven Overhauser Dynamic Nuclear Polarization Agents 甲基驱动高压动态核极化剂的计算机设计

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 DOI: 10.1021/acs.jpclett.5c0137510.1021/acs.jpclett.5c01375

Scott A. Southern, Georgia A. Zissimou, Dragos F. Flesariu, Fadwat Bazzi, Constantinos Nicolaides, Theodossis Trypiniotis, Christos P. Constantinides*, Panayiotis A. Koutentis* and Frédéric A. Perras*,

引用次数: 0

Investigation of Methionine Metabolism in Coccolithophore by In Situ Light-Coupled Nuclear Magnetic Resonance Spectroscopy. 用原位光耦合核磁共振光谱法研究球石藻中蛋氨酸代谢。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 Epub Date: 2025-06-03 DOI: 10.1021/acs.jpclett.5c01316

Yi-Shan Wu, Li-Kang Chu, Tsyr-Yan Yu

{"title":"Investigation of Methionine Metabolism in Coccolithophore by In Situ Light-Coupled Nuclear Magnetic Resonance Spectroscopy.","authors":"Yi-Shan Wu, Li-Kang Chu, Tsyr-Yan Yu","doi":"10.1021/acs.jpclett.5c01316","DOIUrl":"10.1021/acs.jpclett.5c01316","url":null,"abstract":"Coccolithophores play critical roles in global carbon and sulfur cycles. They contribute to the carbon cycle through photosynthesis and calcification and the sulfur cycle by producing dimethylsulfoniopropionate (DMSP). Despite their ecological importance, the details and dynamics of methionine metabolism in coccolithophores are poorly understood. Here, we introduce an in situ light-coupled nuclear magnetic resonance (NMR) spectroscopy setup to monitor methionine metabolism directly in coccolithophore cultures under varying environmental conditions. Combining in situ light-coupled NMR spectroscopy and 13C magic angle spinning (MAS) spectroscopy, we observed that coccolithophores can take up methionine and convert it into 4-methylthio-2-oxobutyrate (MTOB), which is subsequently secreted into the culture medium, while DMSP was detected only intracellularly. Furthermore, environmental factors, such as elevated temperatures at 24.8 °C, which is 6.8 °C higher than the typical growth temperature for coccolithophores, and darkness, accelerated methionine consumption but reduced its incorporation into proteins and its conversion into MTOB, suggesting a shift toward alternative metabolic pathways under stress. In contrast, seawater acidification had minimal effects on the methionine metabolism. These findings provide new insights into how environmental conditions influence sulfur metabolism in coccolithophores, with potential consequences for their ecological functioning under future climate scenarios.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"5800-5805"},"PeriodicalIF":4.8,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12169660/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144214385","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

Self-Catalyzed Carbon Nanotubes with Dual-Active-Site Co/CoN4 Motifs for High-Efficiency Bifunctional Oxygen Electrocatalysis 具有双活性位点Co/CoN4基序的自催化碳纳米管用于高效双功能氧电催化

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 DOI: 10.1021/acs.jpclett.5c0110510.1021/acs.jpclett.5c01105

Wenhui Deng, Yuhao Luo, Kewei Wu, Yanqiu Wang, Hongtao Liu, Xiaoqing Qiu, Kang Liu, Junwei Fu, Wenzhang Li* and Min Liu*,

{"title":"Self-Catalyzed Carbon Nanotubes with Dual-Active-Site Co/CoN4 Motifs for High-Efficiency Bifunctional Oxygen Electrocatalysis","authors":"Wenhui Deng, Yuhao Luo, Kewei Wu, Yanqiu Wang, Hongtao Liu, Xiaoqing Qiu, Kang Liu, Junwei Fu, Wenzhang Li* and Min Liu*, ","doi":"10.1021/acs.jpclett.5c0110510.1021/acs.jpclett.5c01105","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01105https://doi.org/10.1021/acs.jpclett.5c01105","url":null,"abstract":"Carbon nanotubes (CNTs) have garnered significant attention due to their large specific surface area and efficient mass transfer properties. However, the construction of well-ordered CNT catalysts with high-efficiency bifunctional oxygen electrocatalytic activity remains a significant challenge. Herein, the uniform size of CNTs with high-density dual-active-site Co/CoN4 motifs (A-Co/Co-NC) is rationally designed and fabricated through an in situ metal–ligand anchoring method (N → Co2+) followed by a pyrolysis process. The selected 2,6-diaminopurine (DAP) can anchor and disperse Co ions in N sites, which will form uniform CNTs with Co NPs and CoN4 active sites during the pyrolysis process. Theoretical calculation and in situ characteristics clearly proved that Co NP works as an OER active unit and that CoN4 acts as an ORR active site. Benefiting from the high-density dual-active-site Co/CoN4 motifs, the A-Co/Co-NC catalyst displays superior bifunctional performance (ΔE = 0.76 V). Therefore, the A-Co/Co-NC-based zinc–air battery (ZAB) exhibits distinguished reversibility. Remarkably, the A-Co/Co-NC-based Al–air battery (AAB) has a high power density (129.12 mW cm–2). This work provides a feasible design concept to obtain well-organized CNTs with highly dispersed active sites.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"6202–6211 6202–6211"},"PeriodicalIF":4.8,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312377","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

Reaction Kinetics with Multiorder Cavity Modes under Vibrational Strong Coupling. 振动强耦合下多级腔模式反应动力学。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 Epub Date: 2025-06-03 DOI: 10.1021/acs.jpclett.5c00264

Tomohiro Fukushima, Masaki Itatani, Kei Murakoshi

引用次数: 0

Anomalous versus Fickian-but-Not-Gaussian Diffusion in Heterogeneous Systems Depends on the Time Scale of Observation 异质系统中的反常扩散与菲克但非高斯扩散取决于观测的时间尺度

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 DOI: 10.1021/acs.jpclett.5c00780

Hongbo Chen, Jingrui Shi, Ming Hu, Anni Shi, Daniel K. Schwartz, Dapeng Wang

{"title":"Anomalous versus Fickian-but-Not-Gaussian Diffusion in Heterogeneous Systems Depends on the Time Scale of Observation","authors":"Hongbo Chen, Jingrui Shi, Ming Hu, Anni Shi, Daniel K. Schwartz, Dapeng Wang","doi":"10.1021/acs.jpclett.5c00780","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00780","url":null,"abstract":"Both Fickian-but-not-Gaussian diffusion (FnGD) and anomalous diffusion have been observed in various heterogeneous systems. It remains unclear whether FnGD is an independent diffusion process and what factors determine whether anomalous diffusion or FnGD will be observed. Here, we studied two well-defined heterogeneous systems. The first system involves the simulation of polymer diffusion within polymer–nanoparticle mixtures (exhibiting temporal and population heterogeneity), and the second system involves single-molecule fluorescence tracking experiments of nanoparticle diffusion in inverse opals (exhibiting spatial heterogeneity). Despite the qualitative physical differences between these two systems, different types of diffusion, including anomalous diffusion, FnGD, and Brownian diffusion can emerge at varying time scales provided the system is ergodic. The observed phenomena are contingent upon the specific observation time window. Within the same system, diffusion that emerged at different time scales can be interpreted through different diffusion models. These observations suggest that future research should consider characterization across multiple time scales to fully elucidate the underlying mechanisms of heterogeneous systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"6 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144269438","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

Structural Fluctuations at Nanoscale and Cooperative Molecular Dynamics in Bulk Water. 纳米尺度结构波动与散装水中协同分子动力学。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 Epub Date: 2025-06-04 DOI: 10.1021/acs.jpclett.5c00735

Margarita Russina, Gerrit Günther, Bela Farago, Earl Babcock, Zahir Salhi, Alexander Ioffe, Ferenc Mezei

引用次数: 0

Structural Changes in the Retinal Chromophore and Ion-Conducting Pathway of an Anion Channelrhodopsin GtACR1 视网膜发色团的结构变化和阴离子通道视紫质GtACR1的离子传导途径

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 DOI: 10.1021/acs.jpclett.5c0100810.1021/acs.jpclett.5c01008

Keisei Shibata*, Yuma Kawasaki, Shunki Takaramoto, Masaya Watanabe, Masahiro Fukuda, Ryohei Ono, Hideaki E. Kato, Hidefumi Akiyama and Keiichi Inoue*,

{"title":"Structural Changes in the Retinal Chromophore and Ion-Conducting Pathway of an Anion Channelrhodopsin GtACR1","authors":"Keisei Shibata*, Yuma Kawasaki, Shunki Takaramoto, Masaya Watanabe, Masahiro Fukuda, Ryohei Ono, Hideaki E. Kato, Hidefumi Akiyama and Keiichi Inoue*, ","doi":"10.1021/acs.jpclett.5c0100810.1021/acs.jpclett.5c01008","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01008https://doi.org/10.1021/acs.jpclett.5c01008","url":null,"abstract":"Guillardia theta anion-conducting channelrhodopsin 1 (GtACR1) is a light-gated anion channel and is widely used as a representative optogenetic tool for neuronal silencing. However, its gating mechanism is unclear due to the lack of insight into its structural changes and kinetics. Here, we measured the structural changes in the retinal chromophore of GtACR1 throughout its photocycle using time-resolved resonance Raman spectroscopy. Moreover, we investigated the rate-limiting factors of the gating through transient absorption spectroscopy and laser patch clamp electrophysiology. Our results provided the following understanding: the retinal chromophore keeps planar structure even in the open state. The ion-conducting pathway extends to the retinal Schiff base (RSB) as the channel opens. The channel closes in a two-step process, rate-limited by the RSB deprotonation and reprotonation. These findings reveal that the gating mechanism of GtACR1 differs markedly from that of a cation channelrhodopsin C1C2 and contribute to the development of next-generation optogenetic tools.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 24","pages":"6234–6241 6234–6241"},"PeriodicalIF":4.8,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312373","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

Overcoming the Cathode-Derived Li2CO3 Product by Incorporation of CO2 Capture to Boost Li-CO2 Battery Performance 利用二氧化碳捕获技术克服阴极衍生Li2CO3产物，提高锂-二氧化碳电池性能

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-12 DOI: 10.1021/acs.jpclett.5c01141

Yuheng Wang, Xuyang Chen, Ya Mao, Ying Luo, Baoyu Sun, Quansheng Zhang, Jingying Xie

{"title":"Overcoming the Cathode-Derived Li2CO3 Product by Incorporation of CO2 Capture to Boost Li-CO2 Battery Performance","authors":"Yuheng Wang, Xuyang Chen, Ya Mao, Ying Luo, Baoyu Sun, Quansheng Zhang, Jingying Xie","doi":"10.1021/acs.jpclett.5c01141","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01141","url":null,"abstract":"The development of highly efficient catalysts is critical for the lithium-carbon dioxide (Li-CO2) battery. However, the random deposition of lithium carbonate (Li2CO3) on cathodic active sites leads to catalyst poisoning and severely restricts the discharge capacity. Here, we introduce tetraethylenepentamine (TEPA), an amine-rich redox mediator integrated into the electrolyte, to mediate the CO2 reduction and evolution reactions (CO2RR/CO2ER) through a coupled cation-electron transfer mechanism. The multiple amine groups in TEPA regulate the adsorption and decomposition of reaction intermediates, thereby suppressing catalyst deactivation, mitigating voltage polarization, and enabling high discharge capacities up to ∼3984 mAh g–1. Notably, a reversible capacity of 1991 mAh g–1 is maintained even at −20 °C, and the Li-CO2 battery using TEPA demonstrates stable cycling over 100 cycles. This work provides a robust strategy to overcome cathode passivation and unlocks the potential of redox-mediating molecules to promote reversible electrochemistry in metal air batteries.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"20 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144269439","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