Donald G. Truhlar, Chengyi Zhang, Ruihu Lu, Qi Sun, Yu Mao, Tilo Söhnel, Yan Zhao, Ziyun Wang
Finding catalysts that have both high activity and high stability presents a long-standing challenge. Since optimizing activity and stability are conflicting objectives, the best one can do is find the Pareto front that yields optimal tradeoffs between these features. On the Pareto front, there is a trade-off where a portion of catalytic activity must be sacrificed to gain further stability and vice versa. Here, we provide a method to optimize the front by designing a multi-objective genetic algorithm that combines machine learning, graph neural network calculations, and density functional calculations. The application considered is the oxygen evolution reaction catalyzed by high-entropy alloys. We find that the Pareto front generally contains alloys with diverse elements, but that enhancing stability inevitably inflicts a toll on activity. We compare the general conclusions of our work to a survey of 545 experiments.
{"title":"Finding the Pareto front for high-entropy-alloy catalysts","authors":"Donald G. Truhlar, Chengyi Zhang, Ruihu Lu, Qi Sun, Yu Mao, Tilo Söhnel, Yan Zhao, Ziyun Wang","doi":"10.1039/d5sc06100h","DOIUrl":"https://doi.org/10.1039/d5sc06100h","url":null,"abstract":"Finding catalysts that have both high activity and high stability presents a long-standing challenge. Since optimizing activity and stability are conflicting objectives, the best one can do is find the Pareto front that yields optimal tradeoffs between these features. On the Pareto front, there is a trade-off where a portion of catalytic activity must be sacrificed to gain further stability and vice versa. Here, we provide a method to optimize the front by designing a multi-objective genetic algorithm that combines machine learning, graph neural network calculations, and density functional calculations. The application considered is the oxygen evolution reaction catalyzed by high-entropy alloys. We find that the Pareto front generally contains alloys with diverse elements, but that enhancing stability inevitably inflicts a toll on activity. We compare the general conclusions of our work to a survey of 545 experiments.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"254 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947494","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}
Xinlei Ji, Keyi Zhou, My Ha Tran, Xi Chen, Ning Yan
Sustainable bioplastics have attracted considerable attention as alternatives to conventional petroleum-based plastics in response to growing concerns about resource depletion and environmental pollution. Natural biopolymers, such as starch, cellulose, and chitin/chitosan, are emerging as promising candidates for bioplastic production due to their widespread availability and biodegradability. This review conducts a comprehensive examination of recent advances in polymer-level structural engineering of natural biopolymers into bioplastics, with a focus on strategies that introduce intermolecular interactions, including permanent covalent bonds, dynamic covalent linkages, and noncovalent interactions, to reconstruct intrinsic hydrogen-bonded networks. This reconstruction provides the basis for converting natural biopolymers into bioplastics with permanent covalent, dynamic covalent, and physically crosslinked architectures, and the ways in which these architectures affect material properties, processability, and overall performance are systematically assessed. Additionally, the review discusses the direct utilization of raw lignocellulosic biomass as a potential approach to enhance the cost-effectiveness and scalability of bioplastic production. Finally, the challenges in developing high-performance bioplastics are examined, along with future perspectives for advancing bioplastics in alignment with circular economy principles and carbon neutrality objectives.
{"title":"Converting natural biopolymers to sustainable bioplastics via structure engineering","authors":"Xinlei Ji, Keyi Zhou, My Ha Tran, Xi Chen, Ning Yan","doi":"10.1039/d5sc07592k","DOIUrl":"https://doi.org/10.1039/d5sc07592k","url":null,"abstract":"Sustainable bioplastics have attracted considerable attention as alternatives to conventional petroleum-based plastics in response to growing concerns about resource depletion and environmental pollution. Natural biopolymers, such as starch, cellulose, and chitin/chitosan, are emerging as promising candidates for bioplastic production due to their widespread availability and biodegradability. This review conducts a comprehensive examination of recent advances in polymer-level structural engineering of natural biopolymers into bioplastics, with a focus on strategies that introduce intermolecular interactions, including permanent covalent bonds, dynamic covalent linkages, and noncovalent interactions, to reconstruct intrinsic hydrogen-bonded networks. This reconstruction provides the basis for converting natural biopolymers into bioplastics with permanent covalent, dynamic covalent, and physically crosslinked architectures, and the ways in which these architectures affect material properties, processability, and overall performance are systematically assessed. Additionally, the review discusses the direct utilization of raw lignocellulosic biomass as a potential approach to enhance the cost-effectiveness and scalability of bioplastic production. Finally, the challenges in developing high-performance bioplastics are examined, along with future perspectives for advancing bioplastics in alignment with circular economy principles and carbon neutrality objectives.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"9 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947496","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}
Manpreet Kaur, Evan F Chen, Jan Michael Salgado, Ruofei Cheng, Chao-Jun Li
Primarily found in the plants, 1-benzyltetrahydroisoquinoline (1-benzylTHIQ) alkaloids are a diverse class of N-heterocyclic natural products with biological activity against various infectious diseases and neurodegenerative pathologies. Traditionally, 1-benzylTHIQs are synthesized using commercially inaccessible pre-functionalized materials or hazardous organometallic reagents, making their synthesis challenging. Herein, we developed an environmentally benign synthetic strategy to synthesize 1-benzylTHIQs, which aligns with green chemistry principles. This method utilizes abundant, renewable aldehydes as sustainable alkyl carbanion equivalents, thereby eliminating the use of highly reactive or hazardous organometallic reagents. This reaction is catalyzed by ruthenium, using water as a greener solvent, eliminating the need for organic solvents, thereby reducing its environmental impact. Moreover, only N2 and H2O are produced as by-products, which minimizes waste generation. A diverse array of substituted 1-benzylTHIQs was synthesized, showing good functional group tolerance (without the need to protect the functional groups) and resulting in moderate to excellent yields. The sustainability of our method was further demonstrated through the synthesis of natural 1-benzylTHIQ-based alkaloids and late-stage functionalization of pharmacologically relevant molecules.
{"title":"A general aqueous synthetic strategy towards 1-benzylTHIQs enabled by umpolung hydrazone","authors":"Manpreet Kaur, Evan F Chen, Jan Michael Salgado, Ruofei Cheng, Chao-Jun Li","doi":"10.1039/d5sc08310a","DOIUrl":"https://doi.org/10.1039/d5sc08310a","url":null,"abstract":"Primarily found in the plants, 1-benzyltetrahydroisoquinoline (1-benzylTHIQ) alkaloids are a diverse class of N-heterocyclic natural products with biological activity against various infectious diseases and neurodegenerative pathologies. Traditionally, 1-benzylTHIQs are synthesized using commercially inaccessible pre-functionalized materials or hazardous organometallic reagents, making their synthesis challenging. Herein, we developed an environmentally benign synthetic strategy to synthesize 1-benzylTHIQs, which aligns with green chemistry principles. This method utilizes abundant, renewable aldehydes as sustainable alkyl carbanion equivalents, thereby eliminating the use of highly reactive or hazardous organometallic reagents. This reaction is catalyzed by ruthenium, using water as a greener solvent, eliminating the need for organic solvents, thereby reducing its environmental impact. Moreover, only N2 and H2O are produced as by-products, which minimizes waste generation. A diverse array of substituted 1-benzylTHIQs was synthesized, showing good functional group tolerance (without the need to protect the functional groups) and resulting in moderate to excellent yields. The sustainability of our method was further demonstrated through the synthesis of natural 1-benzylTHIQ-based alkaloids and late-stage functionalization of pharmacologically relevant molecules.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"24 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145937982","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}
Lin-bo Tang, Xian-Kai Fan, Kaixiong Xiang, Wei Zhou, Weina Deng, Hai Zhu, Liang Chen, Junchao Zheng, Han Chen
Ammonium (NH4+) ions as charge carriers have exposed tremendous potentials in aqueous batteries because of the rich resources, ultrafast reaction kinetics, and negligible dendrite risks. However, the choices for cathode materials have encountered relatively low capacities in aqueous ammonium ions batteries (AAIBs). Herein, the double tunnel NH4+ ions insertion behaviors with hydrogen bond building-breaking in rutile-phase VO2 (R-VO2) microspheres were revealed for the first time and the capacity contribution forms were confirmed to be dominated by surface-control according to kinetic analysis and density functional theory (DFT) calculations. Those commensal composite microspheres with R-VO2 and carbon nanotubes (R-VO2/CNTs) were acquired to comprehensively promote the capacity, rate performance, and cycling stability for R-VO2 microspheres. In addition, R-VO2/CNTs composite microspheres exhibited the distinguished capacity (950 mAh g-1) within -1.3-0.8 V under 0.05 A g-1, which was maintained at 170 mAh g-1 under 5 A g-1, and achieved an eminent capacity retention of 113% at 5000th cycle and 0-0.4 V. To explore the practical application, a full cell was constructed by coupling R-VO2/CNTs composite microspheres cathode with a urea-perylene diimide polymer (UP) anode. An excellent capacity (130 mAh g-1) with imperceptible capacity decay following 2500 cycles at 1 A g-1 was achieved within the 0-0.9 V pragmatic voltage range. In brief, R-VO2/CNTs composite microspheres have been demonstrated the potential application for sustainable energy storage in AAIBs.
铵离子作为电荷载体，由于其资源丰富、反应速度快、枝晶风险小等优点，在水性电池中显示出巨大的应用潜力。然而，正极材料的选择在水铵离子电池（AAIBs）中遇到了相对较低的容量。通过动力学分析和密度泛函理论（DFT）计算，首次揭示了金红石相VO2 （R-VO2）微球中具有氢键建立-断裂的双隧道NH4+离子插入行为，并证实了容量贡献形式以表面控制为主。为了全面提高R-VO2微球的容量、速率性能和循环稳定性，获得了与R-VO2和碳纳米管共生的复合微球（R-VO2/CNTs）。此外，R-VO2/CNTs复合微球在0.05 A g-1下-1.3-0.8 V范围内具有950 mAh g-1的优异容量，在5 A g-1下可保持170 mAh g-1，在0-0.4 V和5000次循环时可保持113%的优异容量。为了探索其实际应用，采用R-VO2/CNTs复合微球阴极与尿素-苝酰亚胺聚合物（UP）阳极耦合的方法构建了全电池。在0-0.9 V实用电压范围内，在1 A g-1下进行2500次循环后，实现了优异的容量（130 mAh g-1）和难以察觉的容量衰减。简而言之，R-VO2/CNTs复合微球已被证明在AAIBs中具有可持续储能的潜在应用。
{"title":"Coupling abundant active sites and Ultra-short ion diffusion path: R-VO 2 /carbon nanotubes composite microspheres boosted high performance aqueous ammonium-ion batteries","authors":"Lin-bo Tang, Xian-Kai Fan, Kaixiong Xiang, Wei Zhou, Weina Deng, Hai Zhu, Liang Chen, Junchao Zheng, Han Chen","doi":"10.1039/d5sc08747c","DOIUrl":"https://doi.org/10.1039/d5sc08747c","url":null,"abstract":"Ammonium (NH4+) ions as charge carriers have exposed tremendous potentials in aqueous batteries because of the rich resources, ultrafast reaction kinetics, and negligible dendrite risks. However, the choices for cathode materials have encountered relatively low capacities in aqueous ammonium ions batteries (AAIBs). Herein, the double tunnel NH4+ ions insertion behaviors with hydrogen bond building-breaking in rutile-phase VO2 (R-VO2) microspheres were revealed for the first time and the capacity contribution forms were confirmed to be dominated by surface-control according to kinetic analysis and density functional theory (DFT) calculations. Those commensal composite microspheres with R-VO2 and carbon nanotubes (R-VO2/CNTs) were acquired to comprehensively promote the capacity, rate performance, and cycling stability for R-VO2 microspheres. In addition, R-VO2/CNTs composite microspheres exhibited the distinguished capacity (950 mAh g-1) within -1.3-0.8 V under 0.05 A g-1, which was maintained at 170 mAh g-1 under 5 A g-1, and achieved an eminent capacity retention of 113% at 5000th cycle and 0-0.4 V. To explore the practical application, a full cell was constructed by coupling R-VO2/CNTs composite microspheres cathode with a urea-perylene diimide polymer (UP) anode. An excellent capacity (130 mAh g-1) with imperceptible capacity decay following 2500 cycles at 1 A g-1 was achieved within the 0-0.9 V pragmatic voltage range. In brief, R-VO2/CNTs composite microspheres have been demonstrated the potential application for sustainable energy storage in AAIBs.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"3 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145937983","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}
Zhaoming Wang, Guanghui Shi, Guanghui Wang, Man Wang, Feng Ding, Xiao Wang
Hard carbon (HC) has attracted considerable interest as a promising anode material for sodium-ion batteries (SIBs) due to its high specific capacity, excellent cycling stability, and cost-effectiveness. Nevertheless, the sodium storage mechanism in HC remains poorly understood owing to challenges in precisely characterizing its structural disorder, complexity, and intricate interatomic interactions. In this work, we investigate sodium storage behavior in HC anodes using a machine learning potential (MLP) integrated with a random forest-based sodium insertion site identification framework. The trained MLP accurately captures both the structural features of HC and the sodium insertion behavior. HC comprises an amorphous network of defects, edges, graphitic domains, and nanopores, primarily interconnected through sp/sp2/sp3-hybridized carbon bonds. For the first time, we simulate the continuous voltage profile associated with the stepwise sodium insertion during both the charging and overcharging states. This voltage profile reproduces experimental observations and disentangles the contributions of adsorption, intercalation, and pore filling, offering a pathway to elucidate the storage mechanisms across different systems and rationalize the discrepancies observed in experiments. During the overcharging stage, excessively short Na-Na distances enhance repulsion, leading to negative voltages. Besides, the formation of sodium clusters was observed, which poses a safety risk to the battery. Our findings demonstrate that machine learning-based simulations constitute a powerful and emerging approach for investigating sodium storage mechanisms and offer valuable guidance for the experimental optimization of HC anodes. Moreover, this strategy can be extended to other electrodes, electrolytes in SIBs, and even alternative battery systems.
{"title":"Unveiling sodium storage mechanisms in hard carbon via machine learning-driven simulations with accurate site occupation identification","authors":"Zhaoming Wang, Guanghui Shi, Guanghui Wang, Man Wang, Feng Ding, Xiao Wang","doi":"10.1039/d5sc07068f","DOIUrl":"https://doi.org/10.1039/d5sc07068f","url":null,"abstract":"Hard carbon (HC) has attracted considerable interest as a promising anode material for sodium-ion batteries (SIBs) due to its high specific capacity, excellent cycling stability, and cost-effectiveness. Nevertheless, the sodium storage mechanism in HC remains poorly understood owing to challenges in precisely characterizing its structural disorder, complexity, and intricate interatomic interactions. In this work, we investigate sodium storage behavior in HC anodes using a machine learning potential (MLP) integrated with a random forest-based sodium insertion site identification framework. The trained MLP accurately captures both the structural features of HC and the sodium insertion behavior. HC comprises an amorphous network of defects, edges, graphitic domains, and nanopores, primarily interconnected through sp/sp2/sp3-hybridized carbon bonds. For the first time, we simulate the continuous voltage profile associated with the stepwise sodium insertion during both the charging and overcharging states. This voltage profile reproduces experimental observations and disentangles the contributions of adsorption, intercalation, and pore filling, offering a pathway to elucidate the storage mechanisms across different systems and rationalize the discrepancies observed in experiments. During the overcharging stage, excessively short Na-Na distances enhance repulsion, leading to negative voltages. Besides, the formation of sodium clusters was observed, which poses a safety risk to the battery. Our findings demonstrate that machine learning-based simulations constitute a powerful and emerging approach for investigating sodium storage mechanisms and offer valuable guidance for the experimental optimization of HC anodes. Moreover, this strategy can be extended to other electrodes, electrolytes in SIBs, and even alternative battery systems.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"46 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145920456","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}
Achieving simultaneously ultrabright and narrowband organic afterglow emission remains a formidable challenge because enhancing one property often compromises the other. Herein, we report a low-frequency vibronic coupling strategy to design intrinsic narrowband organic afterglow materials that combine high brightness with long lifetimes. Through molecular engineering of coronene, introduction of aroyl and ethoxy substituents breaks molecular symmetry, enhances intersystem crossing, and preserves a localized triplet state with a small radiative rate constant. The optimized coronene derivative doped into dimethyl isophthalate (DMI) exhibits a phosphorescence efficiency of 17.5%, a lifetime of 3.19 s, and a narrow full width at half maximum (FWHM) of 24.2 nm under ambient conditions. Deuteration further increases the lifetime to 5.11 s and phosphorescence efficiency to 20.2%, achieving one of the brightest (73 cd/m2 at ~0.2 s) and narrowband organic afterglow emissions to date. Theoretical simulations attribute the narrowband emission to dominant low-frequency vibronic coupling in the coronene derivative system, offering mechanistic insights into spectral narrowing. This work establishes a new paradigm for molecular design of ultrabright narrowband afterglow materials, paving the way for their applications in illumination, anticounterfeiting, and information encryption.
{"title":"Ultrabright and narrowband organic afterglow achieved by molecular engineering of coronene","authors":"Yuanyuan Chen, Yue Zhang, Guoyi Wu, Ting Luo, Jialiang Jiang, Tengyue Wang, Xiaoya Guo, Kaka Zhang","doi":"10.1039/d5sc08966b","DOIUrl":"https://doi.org/10.1039/d5sc08966b","url":null,"abstract":"Achieving simultaneously ultrabright and narrowband organic afterglow emission remains a formidable challenge because enhancing one property often compromises the other. Herein, we report a low-frequency vibronic coupling strategy to design intrinsic narrowband organic afterglow materials that combine high brightness with long lifetimes. Through molecular engineering of coronene, introduction of aroyl and ethoxy substituents breaks molecular symmetry, enhances intersystem crossing, and preserves a localized triplet state with a small radiative rate constant. The optimized coronene derivative doped into dimethyl isophthalate (DMI) exhibits a phosphorescence efficiency of 17.5%, a lifetime of 3.19 s, and a narrow full width at half maximum (FWHM) of 24.2 nm under ambient conditions. Deuteration further increases the lifetime to 5.11 s and phosphorescence efficiency to 20.2%, achieving one of the brightest (73 cd/m2 at ~0.2 s) and narrowband organic afterglow emissions to date. Theoretical simulations attribute the narrowband emission to dominant low-frequency vibronic coupling in the coronene derivative system, offering mechanistic insights into spectral narrowing. This work establishes a new paradigm for molecular design of ultrabright narrowband afterglow materials, paving the way for their applications in illumination, anticounterfeiting, and information encryption.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"6 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947557","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}
Constanze Schultz, Paul Mike Jordan, Philipp Dahlke, Zehra Tuğçe Gür Maz, Erden Banoğlu, Tobias Meyer-Zedler, Michael Schmitt, Oliver Werz, Juergen Popp
The nitrile (–CN) functional group is a versatile pharmacophore motif that also serves as an intrinsic, bioorthogonal Raman tag in the silent wavenumber region (1800–2700 cm−1). Here, we exploit this dual functionality to track the potent nitrile-containing 5-lipoxygenase-activating protein (FLAP) antagonist BRP-685 in primary human macrophages using label-free spontaneous and stimulated Raman scattering. This approach enables direct intracellular localization at biologically relevant, low micromolar concentrations without chemical modification or external labels. Quantitative Raman imaging reveals that BRP-685 preferentially accumulates in lipid droplets, distinct from its membrane-bound target site at the nuclear envelope/endoplasmic reticulum. Multiplexed analysis with an alkyne-tagged lipid analog uncovers a unique distribution pattern, suggesting that lipid droplets act as intracellular reservoirs for highly lipophilic drugs.
{"title":"Unveiling the molecular dynamics of a nitrile-containing 5-lipoxygenase-activating protein antagonist in primary macrophages through Raman spectroscopy","authors":"Constanze Schultz, Paul Mike Jordan, Philipp Dahlke, Zehra Tuğçe Gür Maz, Erden Banoğlu, Tobias Meyer-Zedler, Michael Schmitt, Oliver Werz, Juergen Popp","doi":"10.1039/d5sc09493c","DOIUrl":"https://doi.org/10.1039/d5sc09493c","url":null,"abstract":"The nitrile (–C<img alt=\"[triple bond, length as m-dash]\" border=\"0\" src=\"https://www.rsc.org/images/entities/char_e002.gif\"/>N) functional group is a versatile pharmacophore motif that also serves as an intrinsic, bioorthogonal Raman tag in the silent wavenumber region (1800–2700 cm<small><sup>−1</sup></small>). Here, we exploit this dual functionality to track the potent nitrile-containing 5-lipoxygenase-activating protein (FLAP) antagonist BRP-685 in primary human macrophages using label-free spontaneous and stimulated Raman scattering. This approach enables direct intracellular localization at biologically relevant, low micromolar concentrations without chemical modification or external labels. Quantitative Raman imaging reveals that BRP-685 preferentially accumulates in lipid droplets, distinct from its membrane-bound target site at the nuclear envelope/endoplasmic reticulum. Multiplexed analysis with an alkyne-tagged lipid analog uncovers a unique distribution pattern, suggesting that lipid droplets act as intracellular reservoirs for highly lipophilic drugs.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"2 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145920457","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}
Biomolecular assemblies with non-centrosymmetric structures exhibit piezoelectric response toward bionanotechnology.Yet, the piezoelectricity of monosaccharide self-assembled materials has not been reported. Herein, for the first time, we have systematically investigated the piezoelectric properties of fourteen natural monosaccharide-based supramolecular materials toward energy harvesting and information transmission. Hydroxyl number and orientation determined the supramolecular arrangements and piezoelectricity of monosaccharide assemblies. Density functional theory (DFT) calculation revealed the maximum piezoelectric coefficients of monosaccharide assemblies ranged from 6 to 13.7 pC/N, in which a-D-Gal assemblies exhibited a higher value. The a-D-Gal assemblies-based piezoelectric device produced opencircuit voltage of 1.08 V under 55 N which lighted up an LED by charging a 0.1 μF capacitor for 1 minute, and reached a voltage of 32 V across the capacitor after 4 minutes of charging. The a-D-Gal assemblies-based composite film can associate with Morse code for information transmission, enabling the conversion of electrical signals into numbers, letters, and words. This work not only reports the piezoelectric properties of various monosaccharide self-assemblies and investigates the correlation between supramolecular structure and piezoelectric response, but also provides new ideas for the development of innovative green energy biomaterials and electronic information transmission media.
具有非中心对称结构的生物分子组件对生物纳米技术表现出压电响应。然而，单糖自组装材料的压电性尚未见报道。在此，我们首次系统地研究了14种天然单糖基超分子材料在能量收集和信息传输方面的压电特性。羟基的数目和取向决定了单糖组合的超分子排列和压电性。密度泛函理论（DFT）计算表明，单糖组装体的最大压电系数在6 ~ 13.7 pC/N之间，其中a- d - gal组装体具有较高的压电系数。基于a- d - gal组件的压电器件在55 N下产生1.08 V的电压，通过对0.1 μF的电容器充电1分钟点亮LED，充电4分钟后电容器两端电压达到32 V。基于a-D-Gal组装体的复合薄膜可以与莫尔斯电码相关联，用于信息传输，使电信号转换为数字、字母和单词。本工作不仅报道了各种单糖自组装体的压电特性，探讨了超分子结构与压电响应的关系，而且为创新绿色能源生物材料和电子信息传输介质的开发提供了新的思路。
{"title":"Natural monosaccharide-based piezoelectric supramolecular materials for energy harvesting and information transmission","authors":"Siying Chen, Junli Yang, Shuaijie Liu, Yehong Huo, Xin Cheng, Lingling Li, Wei Ji","doi":"10.1039/d5sc07918g","DOIUrl":"https://doi.org/10.1039/d5sc07918g","url":null,"abstract":"Biomolecular assemblies with non-centrosymmetric structures exhibit piezoelectric response toward bionanotechnology.Yet, the piezoelectricity of monosaccharide self-assembled materials has not been reported. Herein, for the first time, we have systematically investigated the piezoelectric properties of fourteen natural monosaccharide-based supramolecular materials toward energy harvesting and information transmission. Hydroxyl number and orientation determined the supramolecular arrangements and piezoelectricity of monosaccharide assemblies. Density functional theory (DFT) calculation revealed the maximum piezoelectric coefficients of monosaccharide assemblies ranged from 6 to 13.7 pC/N, in which a-D-Gal assemblies exhibited a higher value. The a-D-Gal assemblies-based piezoelectric device produced opencircuit voltage of 1.08 V under 55 N which lighted up an LED by charging a 0.1 μF capacitor for 1 minute, and reached a voltage of 32 V across the capacitor after 4 minutes of charging. The a-D-Gal assemblies-based composite film can associate with Morse code for information transmission, enabling the conversion of electrical signals into numbers, letters, and words. This work not only reports the piezoelectric properties of various monosaccharide self-assemblies and investigates the correlation between supramolecular structure and piezoelectric response, but also provides new ideas for the development of innovative green energy biomaterials and electronic information transmission media.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"263 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145920463","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}
Vladislav A. Voloshkin, Cecile Valsecchi, Florian Medina, Laurent Lefort, Mikko Muuronen, Matthieu Jouffroy, Steven P. Nolan
In this study, we synthesized a set of 21 N-heterocyclic carbene (NHC)Pd complexes and evaluated them in a benchmark reaction for Suzuki–Miyaura coupling under 12 different conditions, resulting in a high-quality dataset tailored for machine learning applications. We present a detailed analysis of the data, enabling a thorough assessement of the various parameters (ligand structure and reaction parameters) influencing the reaction yield. We used a new workflow to select descriptors for building linear regression models. The models achieved satisfactory performance in interpolation across all reaction conditions. To ensure these results were not artifacts, we critically examined our models, assessing features explainability, featurization strategies, the impact of train-test splits, and the influence of conformer sets. This work highlights key practical considerations for modeling catalytic activity using machine learning.
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![[triple bond, length as m-dash]](https://www.rsc.org/images/entities/char_e002.gif)
N) functional group is a versatile pharmacophore motif that also serves as an intrinsic, bioorthogonal Raman tag in the silent wavenumber region (1800–2700 cm−1). Here, we exploit this dual functionality to track the potent nitrile-containing 5-lipoxygenase-activating protein (FLAP) antagonist BRP-685 in primary human macrophages using label-free spontaneous and stimulated Raman scattering. This approach enables direct intracellular localization at biologically relevant, low micromolar concentrations without chemical modification or external labels. Quantitative Raman imaging reveals that BRP-685 preferentially accumulates in lipid droplets, distinct from its membrane-bound target site at the nuclear envelope/endoplasmic reticulum. Multiplexed analysis with an alkyne-tagged lipid analog uncovers a unique distribution pattern, suggesting that lipid droplets act as intracellular reservoirs for highly lipophilic drugs.
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