IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.09.020

Aramballi J. Savyasachi , Oxana Kotova , Ena T. Luis , Amy D. Lynes , Shaun Mills , Sandra A. Bright , Gavin J. McManus , Matthias E. Möbius , D. Clive Williams , Robert Pal , John J. Boland , Thorfinnur Gunnlaugsson

{"title":"Exerting control of self-assembly pathways via morphological switching and patterning in amino-acid-based benzene-1,3,5-tricarboxamide conjugates","authors":"Aramballi J. Savyasachi , Oxana Kotova , Ena T. Luis , Amy D. Lynes , Shaun Mills , Sandra A. Bright , Gavin J. McManus , Matthias E. Möbius , D. Clive Williams , Robert Pal , John J. Boland , Thorfinnur Gunnlaugsson","doi":"10.1016/j.chempr.2024.09.020","DOIUrl":"10.1016/j.chempr.2024.09.020","url":null,"abstract":"<div><div>Small structural changes to benzene-1,3,5-tricarboxamide (BTA) dictate its self-assembly behavior and morphological outcome. Functionalization with an α-amino acid close to the BTA core, which also possesses a terminal terpyridine (tpy) unit, led to a robust gel in the case of glycine, whereas monodisperse, solid microspheres formed in the case of alanine, phenylalanine, and leucine. The self-assembly pathways of the chiral and achiral BTAs are orthogonal and both microspheres and gel fibers independently assemble in the same medium. Further hierarchical self-assembly results upon addition of lanthanide ions (i.e., Eu(III) and Tb(III) that emit at long wavelengths with long excited-state lifetimes) that crosslink the microspheres through coordination, whereas coordination within the gel led to a change in morphology toward microspheres, as well as the formation of hierarchical superstructures. The chirality of the BTA influences helicity of the assembly and the resulting enantiomeric conformation around the lanthanides, evidenced by circularly polarized luminescence.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102321"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439928","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Hydrogen-bond catalysis in biomass valorization 生物质增值中的氢键催化

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.11.002

Yingchuan Zhang , George W. Huber , Zhengxiao Guo

{"title":"Hydrogen-bond catalysis in biomass valorization","authors":"Yingchuan Zhang , George W. Huber , Zhengxiao Guo","doi":"10.1016/j.chempr.2024.11.002","DOIUrl":"10.1016/j.chempr.2024.11.002","url":null,"abstract":"<div><div>As a biomimetic concept of enzymatic catalysis, hydrogen-bond catalysis (HBC) leverages H-bond-inducing atomic sites or functional groups in catalysts to regulate substrate binding and transition states so as to enable highly efficient and (stereo)selective organic reactions. However, it has rarely been employed in catalytic biomass valorization toward renewable fuels and value-added chemicals until recently. This perspective aims to highlight the opportunities offered by HBC to promote effective transformations of biomass-derived oxygenates. The concept and characterization approaches of HBC strategies are first introduced, followed by a critical overview of HBC-involved reactions, catalyst structures, and dynamic interfaces between biomass substrates and catalysts. Particular attention is paid to binding configurations and adsorption energetics for which engineered H-bonds can tune bond cleavage/formation and promote desirable reaction pathways in association with intrinsic catalytic sites (e.g., Lewis/Brønsted acid sites, metal active sites, and photogenerated charges) and therefore enable biomass valorization in more efficient and sustainable manners.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102364"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825653","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

Producing economically viable renewable diesel by upgrading organic solid waste with natural gas

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102459

Ali Omidkar, Avinash Alagumalai, Razieh Es’haghian, Hua Song

引用次数: 0

Rolling-circle-amplification-based DNA-enzyme nanostructure for immobilization and functionalization of enzymes 用于酶固定化和功能化的基于滚动圈扩增技术的 DNA 酶纳米结构

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.10.002

Dongsheng Mao , Wenxing Li , Xueliang Liu , Jingqi Chen , Dali Wei , Lei Luo , Qianqin Yuan , Yu Yang , Xiaoli Zhu , Weihong Tan

{"title":"Rolling-circle-amplification-based DNA-enzyme nanostructure for immobilization and functionalization of enzymes","authors":"Dongsheng Mao , Wenxing Li , Xueliang Liu , Jingqi Chen , Dali Wei , Lei Luo , Qianqin Yuan , Yu Yang , Xiaoli Zhu , Weihong Tan","doi":"10.1016/j.chempr.2024.10.002","DOIUrl":"10.1016/j.chempr.2024.10.002","url":null,"abstract":"<div><div>Enzymes with ingenious structures and diverse functions are crucial for biomedical applications but face challenges like instability, limited targetability, and delivery complexity. We developed core-shell DNA-enzyme conjugates using rolling circle amplification (RCA), creating RCA-based DNA-enzyme nanostructure (RCA-DEN) for efficient enzyme immobilization and functionalization. RCA-DEN, characterized by densely packed nucleic acids and negligible disruption of enzyme activity, increases the stability of enzymes and nucleic acids while reducing technical difficulties, making it a versatile platform for diverse biomedical applications. This approach facilitates the modular customization of enzymes and the incorporation of functionalities such as aptamers and DNAzymes. The efficacy of RCA-DEN has been demonstrated in several areas, including selective catalysis, cascade catalysis, dynamic monitoring of intracellular chemical processes, and synergistic therapeutic interventions against tumors. Overall, this work provides a new perspective on enzyme immobilization and functionalization, paving the way for broader biomedical applications of enzymes.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102335"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142536375","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

Exploring enzymatic degradation, reinforcement, recycling, and upcycling of poly(ester)-poly(urethane) with movable crosslinks 探索具有可移动交联的聚（酯）-聚（氨基甲酸乙酯）的酶降解、加固、回收和再循环

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.09.026

Jiaxiong Liu , Ryohei Ikura , Kenji Yamaoka , Akihide Sugawara , Yuya Takahashi , Bunsho Kure , Naomi Takenaka , Junsu Park , Hiroshi Uyama , Yoshinori Takashima

{"title":"Exploring enzymatic degradation, reinforcement, recycling, and upcycling of poly(ester)-poly(urethane) with movable crosslinks","authors":"Jiaxiong Liu , Ryohei Ikura , Kenji Yamaoka , Akihide Sugawara , Yuya Takahashi , Bunsho Kure , Naomi Takenaka , Junsu Park , Hiroshi Uyama , Yoshinori Takashima","doi":"10.1016/j.chempr.2024.09.026","DOIUrl":"10.1016/j.chempr.2024.09.026","url":null,"abstract":"<div><div>Enzymes are highly efficient, chemoselective, and sustainable biocatalysts, standing out as eco-friendly tools to advance the circular plastics economy. Herein, we explored enzymatic reactions of poly(<em>ε</em>-caprolactone)-poly(urethane) (PCL-PUs) in organic solvent under different reaction conditions using Novozym 435 (immobilized lipase) as the enzyme. PCL-PUs with triacetylated γ-cyclodextrin (TAcγCD)-based movable crosslinks (PCL-γCD-PU) not only exhibited excellent mechanical properties due to effective energy dissipation, but also efficient enzymatic degradation that was optimized for increases in TAcγCD content. Under reaction time control, molecular weight and mechanical properties of PCL-γCD-PU were enhanced by a novel enzymatic reinforcement strategy. Without sorting, the degraded products are versatile resources that can be enzymatically closed-loop recycled by switching reaction concentration or enzymatically upcycled into value-added polymers by mixing with selective substrates. The facile polymer structure design combined with enzymatic reactions is expected to provide a broad approach for toughening various polymeric materials and advancing their development as sustainable resources.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102327"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142536378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Producing economically viable renewable diesel by upgrading organic solid waste with natural gas 将有机固体废物转化为天然气，生产经济上可行的可再生柴油

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.102389

Ali Omidkar , Avinash Alagumalai , Razieh Es’haghian , Hua Song

引用次数: 0

Biomass waste valorization: Ambient synthesis of reduced graphene oxide 生物质废物价值化：还原氧化石墨烯的常温合成

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102443

Xin Jiang , Yunyan Qiu

引用次数: 0

Morphological-transition-induced motion

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102454

Xianbao Li , Qi Li , Junbai Li

引用次数: 0

Electrocatalysis enables polyvinyl chloride functionalization

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102435

Yuanbo Liu , Haohong Duan

引用次数: 0

Terahertz-Raman spectroscopy for in situ benchtop monitoring of changes to extended, supramolecular structure in milling mechanochemistry 太赫兹-拉曼光谱法用于原位台式监测研磨机械化学中扩展超分子结构的变化

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.09.018

Tristan H. Borchers , Filip Topić , Mihails Arhangelskis , Michael Ferguson , Cameron B. Lennox , Patrick A. Julien , Tomislav Friščić

{"title":"Terahertz-Raman spectroscopy for in situ benchtop monitoring of changes to extended, supramolecular structure in milling mechanochemistry","authors":"Tristan H. Borchers , Filip Topić , Mihails Arhangelskis , Michael Ferguson , Cameron B. Lennox , Patrick A. Julien , Tomislav Friščić","doi":"10.1016/j.chempr.2024.09.018","DOIUrl":"10.1016/j.chempr.2024.09.018","url":null,"abstract":"<div><div>Low-frequency Raman, also known as terahertz-Raman (THz-Raman), spectroscopy offers a laboratory benchtop-based alternative to synchrotron X-ray diffraction for real-time, <em>in situ</em> monitoring of ball-milling mechanochemical reactions. Although direct monitoring of the long-range structure of materials during mechanochemical reactions is generally challenging by conventional Raman spectroscopy, and typically requires synchrotron X-ray diffraction, here we use THz-Raman spectroscopy to monitor mechanosynthesis of cocrystals, stoichiomorphs, and polymorphs, detect multi-step sequences, and discover solid-state phases in systems difficult to differentiate using fingerprint-region Raman spectroscopy—all through real-time observation of changes in lattice vibrational models. The methodology is augmented by periodic density functional theory (DFT), which enables structural interpretation of spectroscopic changes, notably the identification of THz-Raman bands associated with halogen bond transformations. Simultaneous monitoring of mechanochemical processes in both the fingerprint and low-frequency Raman regions enables real-time observation of changes to extended as well as molecular structure during milling, in a single laboratory benchtop experiment, without synchrotron radiation.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102319"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142489464","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Chem最新文献