IF 8.7

JACS Au Pub Date : 2025-07-30 DOI: 10.1021/jacsau.5c00713

Jiahui Wang*, Arash Nikoubashman, Young C. Kim and Jeetain Mittal*,

{"title":"Controlling Multicomponent Condensate Morphology via Additive-Modulated Interactions","authors":"Jiahui Wang*, Arash Nikoubashman, Young C. Kim and Jeetain Mittal*, ","doi":"10.1021/jacsau.5c00713","DOIUrl":"https://doi.org/10.1021/jacsau.5c00713","url":null,"abstract":"The morphology of biomolecular condensates plays a critical role in regulating intracellular organization and function by enabling both spatial and temporal control over biochemical processes. Recent studies have shown that small-molecule cosolutes can not only modulate phase separation but also influence condensate morphology. However, the mechanistic understanding of how small molecules regulate condensate structure remains limited. In this study, we employ coarse-grained molecular dynamics simulations to investigate how the morphology of two-component condensates can be modulated through the introduction of additional small-molecule cosolutes. By systematically varying the interaction strengths between the small molecules and the macromolecular components, we observe morphological transitions between, e.g., core–shell and dewetted structures. To rationalize these transitions, we calculate second virial coefficients in the presence of the small molecules, providing a molecular-level framework to capture shifts in effective homotypic and heterotypic interactions. We further investigate the role of stoichiometry between the small molecules and macromolecules, demonstrating that stoichiometry and interaction strength jointly determine the condensate morphology by altering the relative interaction strengths among components. Additionally, we show that fully mixed two-component condensates can undergo transitions to microphase-separated morphologies, such as core–shell or dewetted, upon small molecule introduction. Together, these findings reveal that condensate morphology can be rationally tuned through interaction- and stoichiometry-dependent mechanisms, offering molecular-scale insights into how small-molecule cosolutes modulate condensate structure.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"4064–4072"},"PeriodicalIF":8.7,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00713","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892621","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Superconductivity in Electrochemically Intercalated R/S-CTA–SnSe2 by Using Chiral Piezoelectric Precursors 手性压电前驱体在电化学插层R/ S-CTA-SnSe2中的超导性

IF 8.7

JACS Au Pub Date : 2025-07-29 DOI: 10.1021/jacsau.5c00739

Hui-Peng Lv, Yong Ai, Wei Hu, Yuqin Susan Xiong, Yan-Ran Weng, Xian-Jiang Song, Yan Qin, Wei-Qiang Liao and Ren-Gen Xiong*,

{"title":"Superconductivity in Electrochemically Intercalated R/S-CTA–SnSe2 by Using Chiral Piezoelectric Precursors","authors":"Hui-Peng Lv, Yong Ai, Wei Hu, Yuqin Susan Xiong, Yan-Ran Weng, Xian-Jiang Song, Yan Qin, Wei-Qiang Liao and Ren-Gen Xiong*, ","doi":"10.1021/jacsau.5c00739","DOIUrl":"https://doi.org/10.1021/jacsau.5c00739","url":null,"abstract":"Molecule intercalation has shown distinct advantages in modulating the superconducting properties of 2D materials. Chiral molecule intercalation provides a strategy for tuning electronic properties, while this approach has been limited to a few 2D materials such as TaS2 and TiS2. Although extensive research on 2D SnSe2 exists, chiral molecule intercalation in SnSe2 remains unexplored. Herein, we report the first successful electrochemical intercalation of chiral CTA cations (CTA = 3-chloro-2-hydroxypropyltrimethylammonium) into SnSe2 by using piezoelectric R/S-CTA-Cl with a large piezoelectric coefficient of approximately 24 pm/V as the precursors, leading to the formation of superconductors R/S-CTA–SnSe2. Characterization techniques, including powder X-ray diffraction, Raman spectroscopy, and circular dichroism spectroscopy, confirm a significant lattice expansion in SnSe2 and the successful intercalation of chiral CTA cations, while polar R/S-CTA-Cl does not endow R/S-CTA–SnSe2 with piezoelectric/ferroelectric properties. Magnetic susceptibility and electrical transport measurements reveal that the intercalated R/S-CTA–SnSe2 materials exhibit a superconducting transition at around 5 K. Notably, the distinct out-of-plane and in-plane upper critical magnetic fields demonstrate the 2D nature of the intercalated compounds. This work highlights an approach for designing and tailoring superconducting materials through chiral cation intercalation and opens avenues for further exploration of chiral effects in superconductors.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"4086–4093"},"PeriodicalIF":8.7,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00739","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892596","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cellulose Proton Conductor: Both Sulfonic Acid and Hydrophobic Group Functionalization Enable High Proton Conductivity. 纤维素质子导体：磺酸和疏水性基团功能化使质子具有高导电性。

IF 8.7

JACS Au Pub Date : 2025-07-29 eCollection Date: 2025-09-22 DOI: 10.1021/jacsau.5c00547

Junpei Miyake

{"title":"Cellulose Proton Conductor: Both Sulfonic Acid and Hydrophobic Group Functionalization Enable High Proton Conductivity.","authors":"Junpei Miyake","doi":"10.1021/jacsau.5c00547","DOIUrl":"10.1021/jacsau.5c00547","url":null,"abstract":"Proton exchange membranes (PEMs), Nafion as a representative, are one of the key materials for energy-converting devices such as fuel cells, water electrolyzers, and redox flow batteries. Recently, environmental concerns regarding perfluoro compounds (e.g., PFAS) have been issues; thus, synthesis of PEMs with mitigated environmental impact is highly demanded. In this paper, we describe that a one-pot synthesis from cellulose provides highly proton conductive cellulose-based PEMs (SC-1) very effectively. The SC-1 with ion exchange capacity ranging from 1.07-1.49 mmol g-1 was successfully prepared by controlling the feed molar ratio of the reactants. 1H NMR spectra, titration, and elemental analysis supported the successful synthesis of SC-1 with a high purity and well-defined structure. Consequently, our synthetic method provided SC-1 with a high degree of substitution (1.87-2.48), which was advantageous for membrane properties. For example, the maximum H+ conductivity of the SC-1 membranes exceeded 140 mS cm-1 (in water at 60 °C) with a suppressed water uptake value (69%), which is one of the best performances among cellulose-based PEMs. The SC-1 membranes also showed good acid resistivity in 2 M H2SO4 at 30 °C for 24 h.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 9","pages":"4165-4169"},"PeriodicalIF":8.7,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12458048/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145152409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Generating New Coordination Compounds via Multireference Simulations, Genetic Algorithms, and Machine Learning: The Case of Co(II) and Dy(III) Molecular Magnets 通过多参考模拟、遗传算法和机器学习生成新的配位化合物：Co（II）和Dy（III）分子磁体的案例

IF 8.7

JACS Au Pub Date : 2025-07-29 DOI: 10.1021/jacsau.5c00502

Lion Frangoulis, Zahra Khatibi, Lorenzo A. Mariano and Alessandro Lunghi*,

{"title":"Generating New Coordination Compounds via Multireference Simulations, Genetic Algorithms, and Machine Learning: The Case of Co(II) and Dy(III) Molecular Magnets","authors":"Lion Frangoulis, Zahra Khatibi, Lorenzo A. Mariano and Alessandro Lunghi*, ","doi":"10.1021/jacsau.5c00502","DOIUrl":"https://doi.org/10.1021/jacsau.5c00502","url":null,"abstract":"The design of coordination compounds with target properties often requires years of continuous feedback loop between theory, simulations, and experiments. In the case of magnetic molecules, this conventional strategy has indeed led to the breakthrough of single-molecule magnets with working temperatures above liquid nitrogen’s boiling point, but at significant costs in terms of resources and time. Here, we propose a computational strategy capable of accelerating the discovery of new coordination compounds with the desired electronic and magnetic properties. Our approach is based on a combination of high-throughput multireference ab initio methods, genetic algorithms, and machine learning. While genetic algorithms allow for an intelligent sampling of the vast chemical space available, machine learning reduces the computational cost by prescreening molecular properties in advance of their accurate and automated multireference ab initio characterization. Importantly, the presented framework is able to generate novel organic ligands and explore chemical motifs beyond those available in pre-existing structural databases. We showcase the power of this approach by automatically generating new Co(II) and Dy(III) mononuclear coordination compounds with record magnetic properties in a fraction of the time required by either experiments or brute-force ab initio approaches. In the case of Dy compounds, simulations uncover new nontrivial chemical strategies toward pentagonal bipyramidal complexes with record-breaking values of magnetic anisotropy.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"3808–3821"},"PeriodicalIF":8.7,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00502","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892620","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Recyclable Whole-Cell Biotransformation System for the Direct Hydroxylation of Propane Catalyzed by a Robust Intracellular Wild-Type Cytochrome P450BM3 Activated by Decoy Molecules. 可回收的全细胞生物转化系统，用于丙烷的直接羟基化，由诱饵分子激活的细胞内野生型细胞色素P450BM3催化。

IF 8.7

JACS Au Pub Date : 2025-07-29 eCollection Date: 2025-09-22 DOI: 10.1021/jacsau.5c00453

Yuki Sugai, Masayuki Karasawa, Osami Shoji

引用次数: 0

Beyond Surface-Localized Reaction Paradigm: Intramacropore-Confined Thermal-Field-Driven Photothermal Reactivity Leap 超越表面局部反应范式：大孔内受限热场驱动的光热反应性飞跃

IF 8.7

JACS Au Pub Date : 2025-07-29 DOI: 10.1021/jacsau.5c00515

Leitao Zhang*, Yu Zhang, Chaofan Xu, Xinjian Li, Yu Bao, Wenyuan Sun, Xiang Li, Yutong Zhao, Qiuli Cheng, Wenlan Wu, Keke Zhang and Junbo Li*,

{"title":"Beyond Surface-Localized Reaction Paradigm: Intramacropore-Confined Thermal-Field-Driven Photothermal Reactivity Leap","authors":"Leitao Zhang*, Yu Zhang, Chaofan Xu, Xinjian Li, Yu Bao, Wenyuan Sun, Xiang Li, Yutong Zhao, Qiuli Cheng, Wenlan Wu, Keke Zhang and Junbo Li*, ","doi":"10.1021/jacsau.5c00515","DOIUrl":"https://doi.org/10.1021/jacsau.5c00515","url":null,"abstract":"Although photothermal reactions have gained extensive attention, their surface-localized nature─where heat concentrates on nanoscale surfaces─leads to suboptimal chemical reactivity. This study establishes an intrapore-confined thermal-field-driven reaction paradigm with unprecedented photothermal reactivity, through investigations of photothermal Congo Red (CR) pyrolysis in three-dimensional ordered macroporous carbon (OMC) versus nonmacroporous solid carbon (SC). Two model systems are constructed: (1) intrapore-confined configuration: fluorine–cerium nanodomains with ultrahigh CR adsorption capacity are anchored onto macroporous walls to achieve uniform CR distribution in OMC; (2) surface-localized pathway: CR is blended on the external surface of SC, decoupling intrapore confinement and surface localization mechanisms. The intrapore-confined system demonstrates transformative advantages: near-complete CR pyrolysis (>99.00 vs 39.89%), a 27.73-fold increase in rate constants (4.00 vs 0.14%/s), and a 30.71-fold enhancement in energy efficiency. Finite element analysis reveals an intrapore-confined thermal field within OMC due to its low thermal conductivity. Characterized by an inward-increasing temperature gradient, this field overcomes surface-localized limitations by reconstructing the temperature distribution, forming effective reaction driving forces. This work transcends conventional understanding of photothermal mechanisms and highlights macroporous architecture as a critical design principle for advanced photothermal materials.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 8","pages":"3822–3832"},"PeriodicalIF":8.7,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/jacsau.5c00515","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892554","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

IF 8.5

JACS Au Pub Date : 2025-07-28

Ryotaro Yoneyama, Naoya Morikawa, Ryota Ushiyama, Tomoya Maruyama, Reiko Sato, Mamiko Tsugane, Masahiro Takinoue and Hiroaki Suzuki*,

引用次数: 0

IF 8.5

JACS Au Pub Date : 2025-07-28

Julio C. Vieyto-Nuñez, Marco Campanile, Joel Mieres-Perez, Lena Ostermeier, Caitlyn Agar, Luigi Petraccone, Pompea Del Vecchio, Rosario Oliva*, Roland Winter* and Elsa Sanchez-Garcia*,

引用次数: 0

IF 8.5

JACS Au Pub Date : 2025-07-28

Jing Xie, Yi Zeng, Ziqi Sun, Jiawang Liu, Chen Zhang, Yue Wang, Wenyu Sun, Jiahui Wang, Duanyun Cao*, Qing Guo* and Jing Guo*,

引用次数: 0

IF 8.5

JACS Au Pub Date : 2025-07-28

Léon Escomel, Laure Vendier, David Gatineau, Florian Molton, Carole Duboc, Marcello Gennari* and Antoine Simonneau*,

引用次数: 0

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