ACS Publications最新文献_第3页

High Efficiency Shear-Driven Nanofluidic System for Energy Conversion/Harvesting. 用于能量转换/收集的高效剪切驱动纳米流体系统。

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2024-11-14 Epub Date: 2024-11-04 DOI: 10.1021/acs.jpcb.4c06142

Le Zhou, Yanguang Zhou, Zhigang Li

{"title":"High Efficiency Shear-Driven Nanofluidic System for Energy Conversion/Harvesting.","authors":"Le Zhou, Yanguang Zhou, Zhigang Li","doi":"10.1021/acs.jpcb.4c06142","DOIUrl":"10.1021/acs.jpcb.4c06142","url":null,"abstract":"In this work, we propose a shear-driven nanofluidic system for energy harvesting/conversion. The system consists of a nanochannel formed by two parallel walls, where the lower wall is negatively charged, while the upper wall is neutral. The motion of the upper wall caused by a shear force drives the solution in the fluidic system to move, which generates an ionic current due to the migration of excess cations in the system. Molecular dynamics simulations demonstrate that the efficiency of the system is affected by the wall charge density, shearing stress, channel height, and binding energy of the walls. The effects of these factors on the efficiency are studied. In particular, it is shown that a high binding energy for the upper wall (e.g., hydrophilic wall) can reduce the flow slip at the upper wall and effectively transfer energy from the wall to the fluid. For the lower wall, a low binding energy, which corresponds to a hydrophobic wall, can reduce the friction at the wall, enhance the flow velocity, and improve the energy conversion efficiency. By varying these parameters, it is found that the maximum energy conversion efficiency of the system reaches 65.8%, which is the highest compared with previous systems. The underlying mechanisms are explained using the slip length at the walls, wall velocity, and charge density profiles. The system proposed in this work provides insights into the design of nanofluidic systems for energy harvesting/conversion.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142566366","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 Modular Approach to Tuning Emissive N-Quinolyl Through-Space Charge Transfer States Using sp³-Scaffolds. 利用 sp3 支架调谐发射性 N-喹啉基通空电荷转移态的模块化方法。

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2024-11-14 Epub Date: 2024-11-04 DOI: 10.1021/acs.jpcb.4c05220

Joseph O Watson, Ruth M Pollard, Mark T Sims, Marc K Etherington, Jonathan P Knowles

引用次数: 0

Gas Phase Reactions of Pristine and Single-Atom-Doped Copper and Silver Clusters: Probing Size-Dependent Stability and Novel Superatoms. 原始和单原子掺杂铜银簇的气相反应：探索尺寸稳定性和新型超原子。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-14 Epub Date: 2024-11-06 DOI: 10.1021/acs.jpclett.4c02582

Qiuying Du, Zhixun Luo, Xiaopeng Xing, Jijun Zhao

{"title":"Gas Phase Reactions of Pristine and Single-Atom-Doped Copper and Silver Clusters: Probing Size-Dependent Stability and Novel Superatoms.","authors":"Qiuying Du, Zhixun Luo, Xiaopeng Xing, Jijun Zhao","doi":"10.1021/acs.jpclett.4c02582","DOIUrl":"10.1021/acs.jpclett.4c02582","url":null,"abstract":"Gas phase reactions have been a subject of research interest, enabling reliable strategies to explore the stability and reactivity of metal clusters as well as to probe novel superatoms that form the building blocks to assemble new materials with tailored properties. Coinage metal clusters have attracted great research attention due to their simple electronic shell structures and rich photochemical and catalytic properties at relatively low cost. This perspective focuses on the recent progress made in studying the gas phase reactions of undamaged and single-atom-doped Cun±,0 and Agn±,0 clusters with O2, CO, and NO molecules. It covers various aspects, such as reaction mechanisms, relationships between structure and activity, control of reactivity by changing cluster size and composition, and the identification of novel superatoms (Cu18-, Ag13-, Ag17-, and Ag15O+). Lastly, we provide a detailed account of the obstacles and prospective avenues for future research in order to establish a connection between these findings and nanocluster systems that have practical applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581021","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

Neural Thermodynamic Integration: Free Energies from Energy-Based Diffusion Models. 神经热力学集成：基于能量的扩散模型的自由能

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-14 Epub Date: 2024-11-06 DOI: 10.1021/acs.jpclett.4c01958

Bálint Máté, François Fleuret, Tristan Bereau

引用次数: 0

Probing Aromaticity with Supersonic Jet Spectroscopy: A Case Study on Furan, Thiophene, and Selenophene. 利用超音速喷射光谱探测芳香性：呋喃、噻吩和硒吩案例研究。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-14 Epub Date: 2024-11-07 DOI: 10.1021/acs.jpclett.4c02791

Akshay Kumar Sahu, Anant Ram Satpathi, Saiprakash Rout, Pranay Mohanty, Laxmipriya Dash, Himansu S Biswal

{"title":"Probing Aromaticity with Supersonic Jet Spectroscopy: A Case Study on Furan, Thiophene, and Selenophene.","authors":"Akshay Kumar Sahu, Anant Ram Satpathi, Saiprakash Rout, Pranay Mohanty, Laxmipriya Dash, Himansu S Biswal","doi":"10.1021/acs.jpclett.4c02791","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02791","url":null,"abstract":"Aromaticity is a century-old concept that is even introduced in high school textbooks. However, the determination of the order of aromaticity of molecules as simple as furan, thiophene, and selenophene is still challenging. This work describes how different theoretical and experimental methods posit different aromaticity orders. To benchmark the theoretical results and arrive at a conclusion, mass-selective electronic and vibrational spectroscopy of these five-membered heterocycles under isolated supersonic-jet-cooled conditions was necessary. Since the aromaticity order can be unveiled from the magnitude of the electron density in the ring, we used hydrogen bonding as a probe. The experimental results revealed that selenophene forms the strongest π-hydrogen bond, suggesting that selenophene is the most aromatic, followed by thiophene and furan. It is concluded that gauge-including magnetically induced currents (GIMIC) and relative 1H and 13C NMR chemical shifts are better parameters to determine the aromaticity order in a similar class of molecules.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142602156","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

Developing Stapled Aptamers with a Constrained Conformation for Osteogenesis Imperfect Therapeutics. 开发用于骨不连治疗的具有受限构象的钉合体。

IF 6.8 1区医学

Journal of Medicinal Chemistry Pub Date : 2024-11-14 Epub Date: 2024-10-29 DOI: 10.1021/acs.jmedchem.4c01293

Gubu Amu, Ge Zhang, Nannan Jing, Yuan Ma

{"title":"Developing Stapled Aptamers with a Constrained Conformation for Osteogenesis Imperfect Therapeutics.","authors":"Gubu Amu, Ge Zhang, Nannan Jing, Yuan Ma","doi":"10.1021/acs.jmedchem.4c01293","DOIUrl":"10.1021/acs.jmedchem.4c01293","url":null,"abstract":"Despite the extensive development of aptamers in basic research, only a limited number have successfully progressed to clinical trials. This limitation is primarily attributed to the inherent instability of aptamers' conformation, resulting in low affinity, poor serum stability, and inconsistent potency, posing a significant challenge to their stabilization. Herein, we established a feasible strategy to develop staple aptamers using the predicted binding conformations and titration cross-linking (TTC) method. Through this strategy, we successfully synthesized various stapled sclerostin aptamers with over 70% yield. Importantly, we demonstrated that stapled aptamers significantly enhanced their affinity (approximately 20-fold) and serum stability (negligible degradation within 32 h). Moreover, in an osteogenesis imperfecta mouse model (Col1a2+/G610C mice), the stapled aptamer (named c-0127OA) exhibited a potent antagonistic effect on sclerostin, leading to enhanced anabolic bone anabolic potential. Collectively, our established stapling strategy is effective in stabilizing aptamers' conformation, with c-0127OA emerging as a promising therapeutic candidate for osteogenesis imperfecta.","PeriodicalId":46,"journal":{"name":"Journal of Medicinal Chemistry","volume":null,"pages":null},"PeriodicalIF":6.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520341","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Discovery of MD-265: A Potent MDM2 Degrader That Achieves Complete Tumor Regression and Improves Long-Term Survival of Mice with Leukemia. 发现 MD-265：一种强效 MDM2 降解剂，可实现肿瘤完全消退并改善白血病小鼠的长期生存。

IF 6.8 1区医学

Journal of Medicinal Chemistry Pub Date : 2024-11-14 Epub Date: 2024-10-31 DOI: 10.1021/acs.jmedchem.4c01818

Angelo Aguilar, Jiuling Yang, Yangbing Li, Donna McEachern, Liyue Huang, Stevenchoukry Razzouk, Shaomeng Wang

引用次数: 0

Development of Neural Network Potentials for Studying Chemical Behaviors of La³⁺/Nd³⁺ Ions in Molten LiCl-KCl-CsCl in Combination with Raman Spectroscopy. 开发结合拉曼光谱研究熔融 LiCl-KCl-CsCl 中 La3+/Nd3+ 离子化学行为的神经网络潜能。

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2024-11-14 Epub Date: 2024-11-01 DOI: 10.1021/acs.jpcb.4c04750

Yi-Zhi Han, Yi-Chuan Liu, Jian-Hui Lan, Ya-Lan Liu, Cong-Zhi Wang, Qun-Yan Wu, Xiang-Dong Ding, Xue Liu, Anastasia O Khudorozhkova, Michael V Laptev, Yury P Zaikov, Wei-Qun Shi

{"title":"Development of Neural Network Potentials for Studying Chemical Behaviors of La3+/Nd3+ Ions in Molten LiCl-KCl-CsCl in Combination with Raman Spectroscopy.","authors":"Yi-Zhi Han, Yi-Chuan Liu, Jian-Hui Lan, Ya-Lan Liu, Cong-Zhi Wang, Qun-Yan Wu, Xiang-Dong Ding, Xue Liu, Anastasia O Khudorozhkova, Michael V Laptev, Yury P Zaikov, Wei-Qun Shi","doi":"10.1021/acs.jpcb.4c04750","DOIUrl":"10.1021/acs.jpcb.4c04750","url":null,"abstract":"The chemistry of molten salts has attracted great research interest owing to their wide applications in diverse fields. In the pyrochemical reprocessing of spent nuclear fuel or molten salt nuclear reactors, lanthanide elements as the principal fission products bring about changes in the composition and properties of molten salts. Herein, we report a comprehensive study on the coordination chemistry of the representative trivalent lanthanide ions (La3+/Nd3+) in LiCl-KCl-CsCl using a multiscale strategy combining Raman spectroscopy, deep learning, and large-scale molecular dynamics (MD) simulations. The neural network potential (NNP)-based MD and Raman spectroscopy studies revealed that La3+/Nd3+ ions prefer to form persistent octahedron complexes with the six-coordinated species as the dominant species at high temperatures. Compared to LaCl63-, NdCl63- shows higher stability with obviously longer lifetimes in LiCl-KCl-CsCl, as confirmed by the observed stronger interaction of Nd3+-Cl- pairs. The total and partial structure factors further indicated the formation of a more stable network structure in LiCl-KCl-CsCl containing NdCl3. Besides, the temperature exerts a larger influence on the local structures of the La3+ species compared to the Nd3+ analogues. According to the potential mean force calculations, the bond dissociation energies follow the order Ln-Cl > Li-Cl > K-Cl > Cs-Cl in LiCl-KCl-CsCl-LnCl3. The NNP-based large-scale MD simulations have been verified to be an efficient and powerful way in molten salt chemistry research.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556665","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

Medium-Range Structural Order as the Driver of Activated Dynamics and Complexity Reduction in Glass-Forming Liquids. 中程结构秩序是玻璃态液体活化动力学和复杂性降低的驱动力

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2024-11-14 Epub Date: 2024-10-31 DOI: 10.1021/acs.jpcb.4c05488

Baicheng Mei, Kenneth S Schweizer

{"title":"Medium-Range Structural Order as the Driver of Activated Dynamics and Complexity Reduction in Glass-Forming Liquids.","authors":"Baicheng Mei, Kenneth S Schweizer","doi":"10.1021/acs.jpcb.4c05488","DOIUrl":"10.1021/acs.jpcb.4c05488","url":null,"abstract":"We analyze in depth the Elastically Collective Nonlinear Langevin Equation theory of activated dynamics in metastable liquids to establish that the predicted inter-relationships between the alpha relaxation time, local cage and collective elastic barriers, dynamic localization length, and shear modulus are causally related within the theory to the medium range order (MRO) static correlation length. The latter grows exponentially with density for metastable hard sphere fluids and as a nonuniversal inverse power law with temperature for supercooled liquids under isobaric conditions. The physical origin of predicted connections between the alpha time and other metrics of cage order and the thermodynamic inverse dimensionless compressibility is fully established. It is discovered that although kinetic constraints from the real space first coordination shell are important for the alpha time, they are of secondary importance compared to the consequences of the more universal MRO correlations in both the modestly and deeply metastable regimes. This understanding sheds new light on the theoretical basis for, and prior successes of, the predictive mapping of chemically complex thermal liquids to effective hard sphere fluids based on matching their dimensionless compressibilities, a scheme we call \"complexity reduction\". In essence, the latter is equivalent to the physical requirement that the thermal liquid MRO correlation equals that of its effective hard sphere analog. The mapping alone is shown to provide a remarkable level of quantitative predictive power for the glass transition temperature Tg of 21 molecular and polymer liquids. Predictions for the chemically specific absolute magnitude and growth with cooling of the MRO correlation length are obtained and lie in the window of 2-6 nm at Tg. Dynamic heterogeneity, elastic facilitation, and beyond pair structure issues are briefly discussed. Future opportunities to theoretically analyze the equilibrated deep glass regime are outlined.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556669","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

Modulation of the Chirality and Dynamics of Self-Assembled Nanocellulose-Chiral C-Dot Film for Chiral Sensing Applications. 用于手性传感应用的自组装纳米纤维素-手性 C 点薄膜的手性和动力学调制。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-14 Epub Date: 2024-11-04 DOI: 10.1021/acs.jpclett.4c02564

Sapna Waghmare, Umarfaruk S Sayyad, Arunavo Chatterjee, Somen Mondal

{"title":"Modulation of the Chirality and Dynamics of Self-Assembled Nanocellulose-Chiral C-Dot Film for Chiral Sensing Applications.","authors":"Sapna Waghmare, Umarfaruk S Sayyad, Arunavo Chatterjee, Somen Mondal","doi":"10.1021/acs.jpclett.4c02564","DOIUrl":"10.1021/acs.jpclett.4c02564","url":null,"abstract":"The detection and sensing of chirality using chiral biomaterials are growing areas of research in advanced bioelectronics. As a result, chiral-controlled biomaterials are crucial for advancing current technologies in chiral sensing applications within biosystems. A chiral carbon dot (C-dot) modulated self-assembled emissive cellulose nanocrystal (CNC) film is developed where the chirality of the CNC film can be tempered between left-handed and right-handed chirality after being doped with chiral L/D-C-dots in CNCs (C-dot-CNC film), transferring the chirality from C-dots to CNCs. The interaction between C-dots, CNCs, and carrier dynamics is investigated using a variety of steady-state and time-resolved PL spectroscopy techniques. The chiral C-dot enhanced the protonic conductivity across the CNC via the formation of hydrogen bonds with its surface functional groups and water molecules. Further, the chiral CNC-C-dots photoelectrodes demonstrate an excellent ability to distinguish between left-handed and right-handed small molecules. These findings on the underlying mechanism of spin selectivity between chiral CNC-C-dot and chiral ligand hold promise for the development of efficient chiral-sensing electronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142566367","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