The Journal of Physical Chemistry Letters最新文献_第10页

Room-Temperature Decomposition of the Ethaline Deep Eutectic Solvent

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-17 DOI: 10.1021/acs.jpclett.4c03645

Julia H. Yang, Amanda Whai Shin Ooi, Zachary A. H. Goodwin, Yu Xie, Jingxuan Ding, Stefano Falletta, Ah-Hyung Alissa Park, Boris Kozinsky

{"title":"Room-Temperature Decomposition of the Ethaline Deep Eutectic Solvent","authors":"Julia H. Yang, Amanda Whai Shin Ooi, Zachary A. H. Goodwin, Yu Xie, Jingxuan Ding, Stefano Falletta, Ah-Hyung Alissa Park, Boris Kozinsky","doi":"10.1021/acs.jpclett.4c03645","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03645","url":null,"abstract":"Environmentally benign, nontoxic electrolytes with combinatorial design spaces are excellent candidates for green solvents, green leaching agents, and carbon capture sources. We examine ethaline, a 2:1 molar ratio of ethylene glycol and choline chloride. Despite its touted green credentials, we find partial decomposition of ethaline into toxic chloromethane and dimethylaminoethanol at room temperature, limiting its sustainable advantage. We experimentally characterize these decomposition products and computationally develop a general, quantum-chemically accurate workflow to understand its decomposition. We find that fluctuations in the hydrogen bonds bind chloride near reaction sites, initiating the reaction between choline cations and chloride anions. The strong hydrogen bonds formed in ethaline are resistant to thermal perturbations, entrapping Cl in high-energy states and promoting the uphill reaction. In the design of stable green solvents, we recommend detailed evaluation of the hydrogen-bonding potential energy landscape as a key consideration for generating stable solvent mixtures.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"55 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640890","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

Mimicking Real Catalysts: Model Stepped Nickel Surfaces in Furfural Catalysis─Insights into Adsorption, Reactivity, and Defect-Driven Conversion Pathways

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-17 DOI: 10.1021/acs.jpclett.5c00066

Sotirios Tsatsos, Georgios Kyriakou

{"title":"Mimicking Real Catalysts: Model Stepped Nickel Surfaces in Furfural Catalysis─Insights into Adsorption, Reactivity, and Defect-Driven Conversion Pathways","authors":"Sotirios Tsatsos, Georgios Kyriakou","doi":"10.1021/acs.jpclett.5c00066","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00066","url":null,"abstract":"The catalytic conversion of furanic compounds into renewable chemicals is essential for sustainable manufacturing. Here, we report a unique self-hydrogenation pathway of furfural to 2-methylfuran on Ni(119) surface, showing how steps and nickel carbides govern reaction selectivity. Thermal desorption and spectroscopic measurements reveal that furfural undergoes decarbonylation to furan on terraces, while step sites act as “hydrogen transfer pumps”, abstracting hydrogen from furfural and facilitating its diffusion to terrace-bound molecules, thereby promoting selective hydrogenation to 2-methylfuran. Moreover, the surface-bound hydrogen enhances hydrogenolysis, with product selectivity closely connected to hydrogen concentration. DFT calculations show a preference for the top step edges, where strong bonding and electron redistribution stabilize intermediates and promote catalytic transformations. We further demonstrate how these insights provide a framework for designing advanced catalysts through surface structure optimization. By linking model catalysts with real-world applications, this approach enables the development of efficient and selective catalysts tailored for biomass conversion.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"33 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635402","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

Two-Dimensional Zeolitic Imidazolate Framework Based Optoelectronic Synaptic Transistor

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-17 DOI: 10.1021/acs.jpclett.5c0000910.1021/acs.jpclett.5c00009

Ziqi Jia, Wenmin Zhong, Kui Zhou, Wei Zeng, Yan Li, Zihao Feng, Haozhe Xue, Pengfei Zhao, Xue Chen, Hongxiang Wang, Xingke Cai, Shuangmei Xue, Yongbiao Zhai, Ziyu Lv, Yan Yan, Meng Zhang, Xueqing Yang, Guanglong Ding*, Su-Ting Han, Chi-Ching Kuo* and Ye Zhou*,

{"title":"Two-Dimensional Zeolitic Imidazolate Framework Based Optoelectronic Synaptic Transistor","authors":"Ziqi Jia, Wenmin Zhong, Kui Zhou, Wei Zeng, Yan Li, Zihao Feng, Haozhe Xue, Pengfei Zhao, Xue Chen, Hongxiang Wang, Xingke Cai, Shuangmei Xue, Yongbiao Zhai, Ziyu Lv, Yan Yan, Meng Zhang, Xueqing Yang, Guanglong Ding*, Su-Ting Han, Chi-Ching Kuo* and Ye Zhou*, ","doi":"10.1021/acs.jpclett.5c0000910.1021/acs.jpclett.5c00009","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00009https://doi.org/10.1021/acs.jpclett.5c00009","url":null,"abstract":"Neuromorphic computing systems that integrate memory and computation offer a solution to the limitations of traditional von Neumann architectures. Optoelectronic synaptic transistors, responding to both optical and electrical signals, enable multifunctional operation with low power consumption. However, challenges such as short data retention and low processing efficiency remain. This study presents an optoelectronic synaptic transistor utilizing two-dimensional (2D) MoS2, 2D zeolitic imidazolate framework (ZIF) Zn2(bim)4, and gold (Au) nanoparticles (NPs) as semiconductor, tunneling layer, and floating gate materials, respectively. By adjusting the tunneling layer thickness, the charge-blocking capacity of Zn2(bim)4 is modulated, improving long-term data retention. The optoelectronic properties of MoS2 and the charge-trapping ability of Au NPs enable the transistor to mimic synaptic behaviors such as postsynaptic current (PSC), long-term potentiation (LTP), and transition from short-term to long-term memory (STM-LTM). This device can also be integrated into an artificial neural network (ANN) for smart healthcare applications, achieving 88.1% accuracy in electrocardiogram classification through optoelectronic dual-mode stimulation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 12","pages":"3012–3021 3012–3021"},"PeriodicalIF":4.8,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703860","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

Two-Dimensional Zeolitic Imidazolate Framework Based Optoelectronic Synaptic Transistor

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-17 DOI: 10.1021/acs.jpclett.5c00009

Ziqi Jia, Wenmin Zhong, Kui Zhou, Wei Zeng, Yan Li, Zihao Feng, Haozhe Xue, Pengfei Zhao, Xue Chen, Hongxiang Wang, Xingke Cai, Shuangmei Xue, Yongbiao Zhai, Ziyu Lv, Yan Yan, Meng Zhang, Xueqing Yang, Guanglong Ding, Su-Ting Han, Chi-Ching Kuo, Ye Zhou

{"title":"Two-Dimensional Zeolitic Imidazolate Framework Based Optoelectronic Synaptic Transistor","authors":"Ziqi Jia, Wenmin Zhong, Kui Zhou, Wei Zeng, Yan Li, Zihao Feng, Haozhe Xue, Pengfei Zhao, Xue Chen, Hongxiang Wang, Xingke Cai, Shuangmei Xue, Yongbiao Zhai, Ziyu Lv, Yan Yan, Meng Zhang, Xueqing Yang, Guanglong Ding, Su-Ting Han, Chi-Ching Kuo, Ye Zhou","doi":"10.1021/acs.jpclett.5c00009","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00009","url":null,"abstract":"Neuromorphic computing systems that integrate memory and computation offer a solution to the limitations of traditional von Neumann architectures. Optoelectronic synaptic transistors, responding to both optical and electrical signals, enable multifunctional operation with low power consumption. However, challenges such as short data retention and low processing efficiency remain. This study presents an optoelectronic synaptic transistor utilizing two-dimensional (2D) MoS2, 2D zeolitic imidazolate framework (ZIF) Zn2(bim)4, and gold (Au) nanoparticles (NPs) as semiconductor, tunneling layer, and floating gate materials, respectively. By adjusting the tunneling layer thickness, the charge-blocking capacity of Zn2(bim)4 is modulated, improving long-term data retention. The optoelectronic properties of MoS2 and the charge-trapping ability of Au NPs enable the transistor to mimic synaptic behaviors such as postsynaptic current (PSC), long-term potentiation (LTP), and transition from short-term to long-term memory (STM-LTM). This device can also be integrated into an artificial neural network (ANN) for smart healthcare applications, achieving 88.1% accuracy in electrocardiogram classification through optoelectronic dual-mode stimulation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"17 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635401","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

Mimicking Real Catalysts: Model Stepped Nickel Surfaces in Furfural Catalysis─Insights into Adsorption, Reactivity, and Defect-Driven Conversion Pathways

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-17 DOI: 10.1021/acs.jpclett.5c0006610.1021/acs.jpclett.5c00066

Sotirios Tsatsos, and , Georgios Kyriakou*,

{"title":"Mimicking Real Catalysts: Model Stepped Nickel Surfaces in Furfural Catalysis─Insights into Adsorption, Reactivity, and Defect-Driven Conversion Pathways","authors":"Sotirios Tsatsos,  and , Georgios Kyriakou*, ","doi":"10.1021/acs.jpclett.5c0006610.1021/acs.jpclett.5c00066","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00066https://doi.org/10.1021/acs.jpclett.5c00066","url":null,"abstract":"The catalytic conversion of furanic compounds into renewable chemicals is essential for sustainable manufacturing. Here, we report a unique self-hydrogenation pathway of furfural to 2-methylfuran on Ni(119) surface, showing how steps and nickel carbides govern reaction selectivity. Thermal desorption and spectroscopic measurements reveal that furfural undergoes decarbonylation to furan on terraces, while step sites act as “hydrogen transfer pumps”, abstracting hydrogen from furfural and facilitating its diffusion to terrace-bound molecules, thereby promoting selective hydrogenation to 2-methylfuran. Moreover, the surface-bound hydrogen enhances hydrogenolysis, with product selectivity closely connected to hydrogen concentration. DFT calculations show a preference for the top step edges, where strong bonding and electron redistribution stabilize intermediates and promote catalytic transformations. We further demonstrate how these insights provide a framework for designing advanced catalysts through surface structure optimization. By linking model catalysts with real-world applications, this approach enables the development of efficient and selective catalysts tailored for biomass conversion.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 12","pages":"3022–3033 3022–3033"},"PeriodicalIF":4.8,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.5c00066","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703857","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

Phase Separation of Binary Triptycenes by an Iodine Interlayer Film on a Ag(111) Surface

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-17 DOI: 10.1021/acs.jpclett.5c0033410.1021/acs.jpclett.5c00334

Peizhen Liu, Peichao Wang, Zichan Zheng, Hongchao Wang, Zhixin Hu* and Hong-Ying Gao*,

{"title":"Phase Separation of Binary Triptycenes by an Iodine Interlayer Film on a Ag(111) Surface","authors":"Peizhen Liu, Peichao Wang, Zichan Zheng, Hongchao Wang, Zhixin Hu* and Hong-Ying Gao*, ","doi":"10.1021/acs.jpclett.5c0033410.1021/acs.jpclett.5c00334","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00334https://doi.org/10.1021/acs.jpclett.5c00334","url":null,"abstract":"We report the self-assembly behaviors of two triptycenes (Trip-1 and Trip-2) on metal surfaces without and with an iodine passivation interlayer by combining scanning tunneling microscopy (STM) and density functional theory (DFT) studies. On the Ag(111) surface, Trip-1 molecules form islands through intermolecular aldehyde–aldehyde hydrogen bonding and π–π stacking of benzene rings. In contrast, Trip-2 molecules lie flat and dispersed on the surface. The introduction of Trip-2 molecules can break the ordered assembly of Trip-1. Trip-1 and Trip-2 molecules will be mixed in a disorderly manner. On the iodine-passivated Ag(111) surface, Trip-1 molecules form islands of long chains by intermolecular aldehyde–aldehyde hydrogen bonding. Trip-1 and Trip-2 molecules will automatically be separated, forming a self-assembled binary monolayer. These results show that the interface can adjust the mixture and separation of two structurally analogous triptycenes.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 12","pages":"3034–3038 3034–3038"},"PeriodicalIF":4.8,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703788","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

Nuclear Quantum Effects in Neutral Water Clusters at Finite Temperature: Structural Evolution from Two to Three Dimensions

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-17 DOI: 10.1021/acs.jpclett.5c0033610.1021/acs.jpclett.5c00336

Mengxu Li, Jiale Kong, Pengju Wang, Jinggang Lan*, Yan Su* and Jijun Zhao*,

{"title":"Nuclear Quantum Effects in Neutral Water Clusters at Finite Temperature: Structural Evolution from Two to Three Dimensions","authors":"Mengxu Li, Jiale Kong, Pengju Wang, Jinggang Lan*, Yan Su* and Jijun Zhao*, ","doi":"10.1021/acs.jpclett.5c0033610.1021/acs.jpclett.5c00336","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00336https://doi.org/10.1021/acs.jpclett.5c00336","url":null,"abstract":"Understanding the structure of bulk water presents a significant challenge due to its intricate hydrogen bond network and dynamic properties. Neutral water clusters, serving as fundamental building blocks, provide key insights into hydrogen bond configurations and intermolecular interactions, thereby establishing a critical foundation for elucidating the behavior of liquid water. In this study, state-of-the-art quantum simulations utilizing a many-body potential for water are employed to investigate the influence of nuclear quantum effects (NQEs) on the structural evolution of neutral water clusters (H2O)n (n = 2–10). For the pentamer at finite temperature, quantum simulations demonstrate that NQEs substantially facilitate the transition from two-dimensional (2D) to three-dimensional (3D) configurations. The population of 3D isomers is governed by a synergistic interplay among the effects of thermal fluctuates and NQEs. For water hexamers with fully 3D structures, the quantum simulations uncover a lower-energy pathway for structural evolution from a prism to a book structure via a cage-like intermediate―a pathway not observed in classical simulations. These findings highlight the crucial role of NQEs in the structural evolution of water clusters and provide a theoretical framework to explore the structure and dynamic properties of condensed-phase water.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 12","pages":"3004–3011 3004–3011"},"PeriodicalIF":4.8,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703786","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

Positive Aging in Quantum Dot Light-Emitting Diodes with Controllable Quantum Dot Assembly

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-16 DOI: 10.1021/acs.jpclett.5c0009410.1021/acs.jpclett.5c00094

Yueting Zheng, Chengyu Luo, Hailong Hu, Tailiang Guo and Fushan Li*,

引用次数: 0

Nuclear Quantum Effects and the Grotthuss Mechanism Dictate the pH of Liquid Water

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-16 DOI: 10.1021/acs.jpclett.5c00168

Saswata Dasgupta, Giuseppe Cassone, Francesco Paesani

{"title":"Nuclear Quantum Effects and the Grotthuss Mechanism Dictate the pH of Liquid Water","authors":"Saswata Dasgupta, Giuseppe Cassone, Francesco Paesani","doi":"10.1021/acs.jpclett.5c00168","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00168","url":null,"abstract":"Water’s ability to autoionize into hydronium (H3O+) and hydroxide (OH–) ions dictates the acidity or basicity of aqueous solutions, influencing the reaction pathways of many chemical and biochemical processes. In this study, we determine the molecular mechanism of the autoionization process by leveraging both the computational efficiency of a deep neural network potential trained on highly accurate data calculated within density-corrected density functional theory and the ability of enhanced sampling techniques to ensure a comprehensive exploration of the underlying multidimensional free-energy landscape. By properly accounting for nuclear quantum effects, our simulations provide an accurate estimate of the autoionization constant of liquid water (pKw = 13.71 ± 0.16), offering a realistic molecular-level picture of the autoionization process and emphasizing its quantum-mechanical nature. Importantly, our simulations highlight the central role played by the Grotthuss mechanism in stabilizing solvent-separated ion pair configurations, revealing its profound impact on acid–base equilibria in aqueous environments.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"202 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635405","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

Positive Aging in Quantum Dot Light-Emitting Diodes with Controllable Quantum Dot Assembly

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-16 DOI: 10.1021/acs.jpclett.5c00094

Yueting Zheng, Chengyu Luo, Hailong Hu, Tailiang Guo, Fushan Li

引用次数: 0