IF 23.5 1区化学

Chem Pub Date : 2025-05-28 DOI: 10.1016/j.chempr.2025.102597

Dihao Wang, Dvir Harris, Chern Chuang, Graham P. Schmidt, Olivia C. Fiebig, Gabriela S. Schlau-Cohen

{"title":"Robust light-harvesting properties upon low-light acclimation in purple bacteria","authors":"Dihao Wang, Dvir Harris, Chern Chuang, Graham P. Schmidt, Olivia C. Fiebig, Gabriela S. Schlau-Cohen","doi":"10.1016/j.chempr.2025.102597","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102597","url":null,"abstract":"Purple bacteria convert solar energy into biochemical energy with high quantum efficiency across diverse environments. Under low light, many species increase the number of antenna complexes and replace their primary light-harvesting complex 2 (LH2) with a blue-shifted variant, LH3. The structural basis of the blue shift and its influence on the dynamics of solar energy conversion have remained unclear. Here, we integrated cryogenic electron microscopy, ultrafast spectroscopy, and quantum dynamics simulations to compare LH2 and LH3 from Rhodoblastus acidophilus strain 7750. Our analyses revealed that hydrogen bonding dynamically tunes the transition energy, introducing a previously unreported excitation energy equilibrium between bacteriochlorophyll rings in LH3. This energy redistribution opened new inter-complex pathways, enabling 68% faster energy transport to maintain high conversion efficiency even with the larger antenna. Collectively, these results establish structural modifications as a tunable knob to optimize both absorption and transport for robust light harvesting under fluctuating conditions.","PeriodicalId":268,"journal":{"name":"Chem","volume":"50 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144154179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Designing generative dissipative networks for programming complex temporal dynamics and functions 设计生成耗散网络规划复杂的时间动态和函数

IF 23.5 1区化学

Chem Pub Date : 2025-05-27 DOI: 10.1016/j.chempr.2025.102593

Xiarui Wang, Shan Wang, Liang Yue, Weihong Tan

{"title":"Designing generative dissipative networks for programming complex temporal dynamics and functions","authors":"Xiarui Wang, Shan Wang, Liang Yue, Weihong Tan","doi":"10.1016/j.chempr.2025.102593","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102593","url":null,"abstract":"Complex temporal dynamics orchestrated by natural networks are essential for cellular functions. Replicating these dynamics in simplified synthetic networks could elucidate underlying mechanisms, facilitating the creation of life-like systems. Herein, we introduce a versatile, modular, and programmable framework for constructing hierarchical and multifunctional generative dissipative networks (GDNs) capable of producing complex temporal dynamics. This framework involves two types of modules. Generative modules produce fuels, and dissipative modules consume these fuels to activate transient signals. By integrating multiple modules, hierarchical GDNs with diverse compositions, sizes, connections, and topologies were constructed to produce controllable complex temporal dynamics, like precise pulse-multiphase control, pulse-repetition frequency modulation, and programmed timing of multiple pulses. These dynamics stem from coordination among heterogeneous modules and competition among homogeneous modules, as corroborated by kinetic modeling. Furthermore, GDNs offer a robust platform for programming autonomous temporal functions, exemplified by GDN-mediated temporal programming of RNA transcription and DNA condensate dynamics.","PeriodicalId":268,"journal":{"name":"Chem","volume":"56 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144145616","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Rate-limiting regimes in photochemical H2 generation by complexes of colloidal CdS nanorods and hydrogenase 胶体CdS纳米棒与氢化酶配合物光化学制氢的限速机制

IF 23.5 1区化学

Chem Pub Date : 2025-05-23 DOI: 10.1016/j.chempr.2025.102594

Helena R. Keller, James K. Utterback, Hayden Hamby, Carolyn E. Lubner, David W. Mulder, Paul W. King, Gordana Dukovic

{"title":"Rate-limiting regimes in photochemical H2 generation by complexes of colloidal CdS nanorods and hydrogenase","authors":"Helena R. Keller, James K. Utterback, Hayden Hamby, Carolyn E. Lubner, David W. Mulder, Paul W. King, Gordana Dukovic","doi":"10.1016/j.chempr.2025.102594","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102594","url":null,"abstract":"Driving redox enzyme catalysis with photoexcited semiconductor nanocrystals is a compelling approach for chemical conversion. We examined how the interplay of the many chemical steps involved determines the rates of photochemical H2 production with complexes of colloidal CdS nanorods and an [FeFe]-hydrogenase. We elucidated the roles of three critical and previously elusive processes—scavenging of photoexcited holes from nanorods, back-electron transfer, and H2 oxidation. Kinetic Monte Carlo simulations and fitting to experimental data revealed that hole transfer becomes the rate-limiting step at high illumination intensities. Comparisons of simulations to experimental H2 production showed that both back-electron transfer and H2 oxidation play an efficiency-limiting role at high catalyst loadings. This work provides guiding principles for tuning experimental parameters to minimize energy-wasting pathways and optimize photochemical product formation. More broadly, we demonstrate how critical but elusive chemical steps in photochemical reactions can be probed with a combination of experiments and simulations.","PeriodicalId":268,"journal":{"name":"Chem","volume":"4 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144122861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Central-to-axial chirality transfer to construct atropisomeric isothiazoles 从中心到轴向手性转移构建异噻唑

IF 23.5 1区化学

Chem Pub Date : 2025-05-19 DOI: 10.1016/j.chempr.2025.102592

Yasu Chen, Tongkun Wang, Ziqiang Wang, Chen Zhu

引用次数: 0

Bioluminescence-activated proximity labeling for spatial multi-omics 生物发光激活的空间多组学接近标记

IF 23.5 1区化学

Chem Pub Date : 2025-05-19 DOI: 10.1016/j.chempr.2025.102595

Ruixiang Wang, Yuxin Fang, Youyue Hu, Yanjun Liu, Peng R. Chen, Peng Zou

引用次数: 0

Synthesis and assembly strategy of electroactive biomaterials and systems for soft tissue engineering applications 用于软组织工程的电活性生物材料和系统的合成与装配策略

IF 23.5 1区化学

Chem Pub Date : 2025-05-19 DOI: 10.1016/j.chempr.2025.102596

Dong Yang, Yi Hu, Shuai Liu, Wenhui Yang, Xi Ren, Yanbing Li, Feng Xu, Min Gong, Yunlong Zhao, Xiaozhong Qiu, Honghao Hou

{"title":"Synthesis and assembly strategy of electroactive biomaterials and systems for soft tissue engineering applications","authors":"Dong Yang, Yi Hu, Shuai Liu, Wenhui Yang, Xi Ren, Yanbing Li, Feng Xu, Min Gong, Yunlong Zhao, Xiaozhong Qiu, Honghao Hou","doi":"10.1016/j.chempr.2025.102596","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102596","url":null,"abstract":"Soft tissue injuries are a common issue affecting human health, and the extent and duration of injuries often constrain the healing process. Electroactive biomaterials have become a key medium for tissue regeneration by modulating cellular behavior, but a systematic evaluation of their potential and challenges is still limited. This review comprehensively explores electroactive biomaterials, focusing on their chemical synthesis, assembly processes, application potential, challenges faced, and future directions. First, this work elaborates on the unique and innovative features of electroactive biomaterials’ chemical synthesis and preparation techniques. Subsequently, the principles of electroactive devices and their interactions with biological tissues are described to optimize tissue repair. Finally, the application prospects of electrical stimulation technology in soft tissue engineering are explored, emphasizing its role in cell and tissue regeneration and its clinical potential. In conclusion, this review provides theoretical and practical insights into the development and application of electroactive biomaterials.","PeriodicalId":268,"journal":{"name":"Chem","volume":"121 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Electrochemical sequencing of sequence-defined ferrocene-containing oligourethanes 序列定义的含二茂铁低聚脲的电化学测序

IF 23.5 1区化学

Chem Pub Date : 2025-05-16 DOI: 10.1016/j.chempr.2025.102571

Bipin Pandey, Bharadwaj Muralidharan, Tianmu Ma, Akshi Pant, Matthew Onorato, Kenneth A. Johnson, Ananth Dodabalapur, Praveen Pasupathy, Eric V. Anslyn

{"title":"Electrochemical sequencing of sequence-defined ferrocene-containing oligourethanes","authors":"Bipin Pandey, Bharadwaj Muralidharan, Tianmu Ma, Akshi Pant, Matthew Onorato, Kenneth A. Johnson, Ananth Dodabalapur, Praveen Pasupathy, Eric V. Anslyn","doi":"10.1016/j.chempr.2025.102571","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102571","url":null,"abstract":"The growing demand for data storage has driven research into alternative storage media. Although DNA has proven effective, synthetic sequence-defined polymers (SDPs) offer tailored information-encoding potential. Despite advances in SDP chemodiversity, sequencing methods remain limited, primarily relying on tandem mass spectrometry. To address this, we developed an electrochemical sequencing technique for sequence-defined oligourethanes (SDOs), incorporating four ferrocene-based monomers. Our method combines controlled chain-end degradation with differential pulse voltammetry (DPV) to yield unique voltammograms specific to each sequence. Coupled with kinetic modeling and principal component analysis (PCA), this approach enables accurate sequence identification. We automated this process with a Python program that decodes sequences by comparing experimental DPV data to predicted profiles and thereby successfully demonstrated the encoding and decoding of an 11-character password. The technique expands the toolbox for sequencing SDPs and opens new possibilities for molecular data storage.","PeriodicalId":268,"journal":{"name":"Chem","volume":"6 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Intermittent electrolysis enabling the enhanced efficiency and stability for nitrate reduction 间歇电解提高了硝酸还原的效率和稳定性

IF 23.5 1区化学

Chem Pub Date : 2025-05-13 DOI: 10.1016/j.chempr.2025.102591

Limin Wu, Libing Zhang, Jiaqi Feng, Shunhan Jia, Ruhan Wang, Xinning Song, Xiaodong Ma, Qinggong Zhu, Xinchen Kang, Qingli Qian, Xiaofu Sun, Buxing Han

{"title":"Intermittent electrolysis enabling the enhanced efficiency and stability for nitrate reduction","authors":"Limin Wu, Libing Zhang, Jiaqi Feng, Shunhan Jia, Ruhan Wang, Xinning Song, Xiaodong Ma, Qinggong Zhu, Xinchen Kang, Qingli Qian, Xiaofu Sun, Buxing Han","doi":"10.1016/j.chempr.2025.102591","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102591","url":null,"abstract":"Catalyst deactivation is a common issue in catalysis, which restricts its practical applications. Nitrate electroreduction using copper (Cu) catalysts offers an eco-friendly NH3 production route. However, the NH3 selectivity and activity decline significantly due to Cu surface reconstruction and compositional changes during electrolysis. Herein, an intermittent reduction strategy is proposed to maintain high efficiency and stability of Cu2O for NO3− to NH3 through applying an alternating on/off electrolysis. The high Faradaic efficiency (FE) (≥90%) and current density (≥110 mA cm−2) were maintained at least 200 h, which improved the cycle stability by 40 times compared with relay electrolysis. Detailed experimental studies and theoretical calculations manifest that the composition and structure of Cu catalyst could be recovered periodically via intermittent electrolysis, which facilitated NO3− adsorption, moderated ∗NO2 coverage, and balanced ∗H production/consumption, leading to high selectivity toward NH3 in long-term electrolysis. Further investigation showed that this strategy could also be extended to other Cu-based catalysts.","PeriodicalId":268,"journal":{"name":"Chem","volume":"124 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940494","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Scalable templated fabrication of Cu-based MOF on textiles for simultaneous sensing, filtration, and detoxification of SO2 可扩展模板制造的cu基MOF在纺织品上的同时传感，过滤和脱毒的二氧化硫

IF 23.5 1区化学

Chem Pub Date : 2025-05-12 DOI: 10.1016/j.chempr.2025.102580

Zhuoran Zhong, Patrick Damacet, Elí Sánchez-González, Aileen M. Eagleton, Nataliia Vereshchuk, Ravint Wongratanaphisan, Jamison T. Anderson, Sofia Goncalves, Gregory W. Peterson, Brandon Blount, Susanna Monti, Giovanni Barcaro, Ilich A. Ibarra, Katherine A. Mirica

{"title":"Scalable templated fabrication of Cu-based MOF on textiles for simultaneous sensing, filtration, and detoxification of SO2","authors":"Zhuoran Zhong, Patrick Damacet, Elí Sánchez-González, Aileen M. Eagleton, Nataliia Vereshchuk, Ravint Wongratanaphisan, Jamison T. Anderson, Sofia Goncalves, Gregory W. Peterson, Brandon Blount, Susanna Monti, Giovanni Barcaro, Ilich A. Ibarra, Katherine A. Mirica","doi":"10.1016/j.chempr.2025.102580","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102580","url":null,"abstract":"This paper describes the scalable fabrication of smart electronic textiles (e-textiles) capable of simultaneous sensing, filtration, and detoxification of sulfur dioxide (SO2). The templated method converts pre-deposited copper metal into copper hydroxide, followed by conversion into a copper-based hexahydroxytriphenylene metal-organic framework (MOF) (Cu3(HHTP)2), to afford a large-area (10 × 10 cm2) conductive coating (sheet resistance = 0.1–0.3 MΩ). The resulting e-textiles achieve sensing (theoretical limit of detection [LOD] of 0.43 ppm), filtration (adsorption uptake of 1.9 and 0.83 mmol g−1 for MOF powder and MOF/textile, respectively, at 1 bar and 298 K), and detoxification (redox conversion of SO2 gas into solid sulfate) due to the selective material-analyte interactions. This scalable method for generating e-textiles is a promising approach for the fabrication of smart membrane materials with multifunctional performance characteristics.","PeriodicalId":268,"journal":{"name":"Chem","volume":"26 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933564","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Phase behavior and pathway-selective oligomerization driven by amino acid side-chain recognition 氨基酸侧链识别驱动的相行为和途径选择性寡聚化

IF 23.5 1区化学

Chem Pub Date : 2025-05-12 DOI: 10.1016/j.chempr.2025.102589

Kun Dai, Lenard Saile, Mahesh D. Pol, Arti Sharma, Thejus Pramod, Charalampos G. Pappas

{"title":"Phase behavior and pathway-selective oligomerization driven by amino acid side-chain recognition","authors":"Kun Dai, Lenard Saile, Mahesh D. Pol, Arti Sharma, Thejus Pramod, Charalampos G. Pappas","doi":"10.1016/j.chempr.2025.102589","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102589","url":null,"abstract":"Within living systems, DNA-encoded information is translated into proteins through a precise process involving amino acid activation, recognition, and biocatalytic acyl transfer reactions. This process raises a fundamental question: what essential ingredients are required for amino acid side-chain recognition and assembly in the absence of enzymatic machinery? In this study, we demonstrate abiotic acyl transfer reactions from aminoacyl phosphate esters, synthetic analogs of biological aminoacyl adenylates, to amino esters, which serve as mimics of tRNA esters. The coupling of amino acid oligomerization to acyl transfer reaction cycles drives selective assembly of amino acid derivatives, recognizing aromatic side chains. Liquid-liquid phase separation creates selective microenvironments that enhance specificity and direct oligomerization. Notably, droplets formed by aromatic amino acids maintain specificity even in the presence of competing species. These findings suggest that amino acid-based compartments sustain chemical processes without biological templates, offering a minimal model of compartmentalization from simple activated monomers.","PeriodicalId":268,"journal":{"name":"Chem","volume":"3 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

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