Recent research has focused on the heavy-atom effect in organic luminescent materials, especially in multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters. Traditional strategies involve directly conjugating heavy atoms to the chromophore, which often broadens the emission spectrum. This study explores an unconventional approach using the through-space heavy-atom effect, positioning heavy-atom moieties with nonconjugated short-range interaction with the chromophore. This method successfully demonstrates the “intramolecular external heavy-atom effect” proposed in the 1970s in cutting-edge high-efficiency emissive materials. Comparative analysis of these emitters confirms the spatial heavy-atom effect, maintaining the spectroscopic properties of MR chromophore while significantly improving external quantum efficiency in organic light-emitting diodes (OLEDs). These emitters also mitigate efficiency roll-off, showcasing the potential of spatial interactions to enhance MR-TADF materials for OLED applications.
{"title":"Enhancing multi-resonance thermally activated delayed fluorescence emission via through-space heavy-atom effect","authors":"Qi Zheng, Yang-Kun Qu, Peng Zuo, Hai-Tian Yuan, Yue-Jian Yang, Yu-Chen Qiu, Liang-Sheng Liao, Dong-Ying Zhou, Zuo-Quan Jiang","doi":"10.1016/j.chempr.2024.10.020","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.020","url":null,"abstract":"Recent research has focused on the heavy-atom effect in organic luminescent materials, especially in multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters. Traditional strategies involve directly conjugating heavy atoms to the chromophore, which often broadens the emission spectrum. This study explores an unconventional approach using the through-space heavy-atom effect, positioning heavy-atom moieties with nonconjugated short-range interaction with the chromophore. This method successfully demonstrates the “intramolecular external heavy-atom effect” proposed in the 1970s in cutting-edge high-efficiency emissive materials. Comparative analysis of these emitters confirms the spatial heavy-atom effect, maintaining the spectroscopic properties of MR chromophore while significantly improving external quantum efficiency in organic light-emitting diodes (OLEDs). These emitters also mitigate efficiency roll-off, showcasing the potential of spatial interactions to enhance MR-TADF materials for OLED applications.","PeriodicalId":268,"journal":{"name":"Chem","volume":"13 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610117","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}
Pub Date : 2024-11-14DOI: 10.1016/j.chempr.2024.08.005
Hao Wu , Yiyao Wang , Shiyuan Sui , Gongming Chen , Lei Wang , Jiaxin Yang , Junbiao Chang , Dachang Bai
β-Lactams are privileged and appealing motifs in medicinal chemistry. Herein, we report enantioselective desymmetrization and parallel kinetic resolution of aminocyclopropanes for the synthesis of chiral β-lactams through Rh(I)-catalyzed asymmetric C–C bond activation. The chiral Rh(I) catalyzed C–C bond cleavage of aminocyclopropanes first and then underwent β-hydride elimination to generate π-allylic hydridorhodium(III) intermediates, which could be trapped by tethered alkyne units, and gave various strained chiral β-lactams with excellent regio- and enantioselectivity (90%–99% ee). Moreover, parallel kinetic resolution was realized when using unsymmetrical aminocyclopropanes with pre-existing C2-stereocenters through C–C bond activation, delivering two types of β-lactams in one pot with excellent enantiomeric excesses. Notably, these systems achieve complete atom and step economy. The obtained enantioenriched β-lactams exhibit the capability to undergo a variety of stereospecific transformations. Theoretical calculations reveal the origin of enantioselectivity and support the alkyne unit insertion to allylic Rh(III) –C bond mechanisms.
{"title":"Enantioselective desymmetrization and parallel kinetic resolution of cyclopropanes via C–C activation: Synthesis of chiral β-lactams","authors":"Hao Wu , Yiyao Wang , Shiyuan Sui , Gongming Chen , Lei Wang , Jiaxin Yang , Junbiao Chang , Dachang Bai","doi":"10.1016/j.chempr.2024.08.005","DOIUrl":"10.1016/j.chempr.2024.08.005","url":null,"abstract":"<div><div>β-Lactams are privileged and appealing motifs in medicinal chemistry. Herein, we report enantioselective desymmetrization and parallel kinetic resolution of aminocyclopropanes for the synthesis of chiral β-lactams through Rh(I)-catalyzed asymmetric C–C bond activation. The chiral Rh(I) catalyzed C–C bond cleavage of aminocyclopropanes first and then underwent β-hydride elimination to generate π-allylic hydridorhodium(III) intermediates, which could be trapped by tethered alkyne units, and gave various strained chiral β-lactams with excellent <em>regio</em>- and enantioselectivity (90%–99% ee). Moreover, parallel kinetic resolution was realized when using unsymmetrical aminocyclopropanes with pre-existing C2-stereocenters through C–C bond activation, delivering two types of β-lactams in one pot with excellent enantiomeric excesses. Notably, these systems achieve complete atom and step economy. The obtained enantioenriched β-lactams exhibit the capability to undergo a variety of stereospecific transformations. Theoretical calculations reveal the origin of enantioselectivity and support the alkyne unit insertion to allylic Rh(III) –C bond mechanisms.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3503-3516"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138191","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}
Pub Date : 2024-11-14DOI: 10.1016/j.chempr.2024.10.015
Sagnik Chakrabarti , Liviu M. Mirica
Zinc and manganese are the reductants of choice for nickel-catalyzed cross-electrophile coupling (XEC), but their exact redox potentials are unknown in organic solvents. In a recent report from Stahl and colleagues in Nature Chemistry, these potentials have been measured for the first time and their implications on model XEC reactions have been discussed.
{"title":"Quantifying zinc and manganese reduction potentials in organic solvents","authors":"Sagnik Chakrabarti , Liviu M. Mirica","doi":"10.1016/j.chempr.2024.10.015","DOIUrl":"10.1016/j.chempr.2024.10.015","url":null,"abstract":"<div><div>Zinc and manganese are the reductants of choice for nickel-catalyzed cross-electrophile coupling (XEC), but their exact redox potentials are unknown in organic solvents. In a recent report from Stahl and colleagues in <em>Nature Chemistry</em>, these potentials have been measured for the first time and their implications on model XEC reactions have been discussed.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3273-3275"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142562009","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}
Pub Date : 2024-11-14DOI: 10.1016/j.chempr.2024.06.012
Mingfeng Li , Clement Kim Soon Ho , Ivan Keng Wee On , Vincent Gandon , Ye Zhu
Cavitands have emerged as privileged architectures in supramolecular chemistry. Nonetheless, achieving structural diversity and tunability through heterofunctionalization along the rims of macrocycles has remained a formidable challenge. As a rudimental example, stepwise conversion of C4v-symmetric scaffolds to inherently chiral ABCD patterns is synthetically impractical owing to the low theoretical yields (0.8%) and the need for chromatographic enantioseparation.
Herein, we report a catalytic desymmetrization strategy to access inherently chiral cavitands. Through engineering ionic chiral palladium catalysts, diverse functionalities, including aryl, alkenyl, alkynyl, and amino groups, can be installed on the large rims with high site- and stereoselectivity. An adaptable stepwise protocol has been established to furnish designer ABCD-type cavitands in accordance with the choreography of coupling partners. Experimental and computational studies reveal synergistic electrostatic steering and electrostatic catalysis by the ionic catalyst–substrate interactions.
{"title":"Inherently chiral resorcinarene cavitands through ionic catalyst-controlled cross-coupling","authors":"Mingfeng Li , Clement Kim Soon Ho , Ivan Keng Wee On , Vincent Gandon , Ye Zhu","doi":"10.1016/j.chempr.2024.06.012","DOIUrl":"10.1016/j.chempr.2024.06.012","url":null,"abstract":"<div><div>Cavitands have emerged as privileged architectures in supramolecular chemistry. Nonetheless, achieving structural diversity and tunability through heterofunctionalization along the rims of macrocycles has remained a formidable challenge. As a rudimental example, stepwise conversion of <em>C</em><sub>4v</sub>-symmetric scaffolds to inherently chiral ABCD patterns is synthetically impractical owing to the low theoretical yields (0.8%) and the need for chromatographic enantioseparation.</div><div>Herein, we report a catalytic desymmetrization strategy to access inherently chiral cavitands. Through engineering ionic chiral palladium catalysts, diverse functionalities, including aryl, alkenyl, alkynyl, and amino groups, can be installed on the large rims with high site- and stereoselectivity. An adaptable stepwise protocol has been established to furnish designer ABCD-type cavitands in accordance with the choreography of coupling partners. Experimental and computational studies reveal synergistic electrostatic steering and electrostatic catalysis by the ionic catalyst–substrate interactions.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3323-3341"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141546260","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}
Pub Date : 2024-11-14DOI: 10.1016/j.chempr.2024.09.008
Yiwei Gong , Jan Langwald , Florian F. Mulks
Recent advances in the isolation of masked gem-carbodications have shown that such species may be more accessible than we thought. This perspective article summarizes the milestones of the last 140 years of research and aims to point the way toward the isolation of species containing true four-valence-electron carbon. Currently, strong mesomeric donation or coordination by donor ligands is used to stabilize such dications. Achieving true localization of both charges on a single atom will require smart combinations of inductive donation, hyperconjugation, and steric hindrance.
{"title":"On the road to isolable geminal carbodications","authors":"Yiwei Gong , Jan Langwald , Florian F. Mulks","doi":"10.1016/j.chempr.2024.09.008","DOIUrl":"10.1016/j.chempr.2024.09.008","url":null,"abstract":"<div><div>Recent advances in the isolation of masked <em>gem</em>-carbodications have shown that such species may be more accessible than we thought. This perspective article summarizes the milestones of the last 140 years of research and aims to point the way toward the isolation of species containing true four-valence-electron carbon. Currently, strong mesomeric donation or coordination by donor ligands is used to stabilize such dications. Achieving true localization of both charges on a single atom will require smart combinations of inductive donation, hyperconjugation, and steric hindrance.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3294-3308"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398096","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}
Pub Date : 2024-11-14DOI: 10.1016/j.chempr.2024.10.017
Niklas Sülzner
Despite the long-lasting research on proton transfer as a fundamental chemical reaction, not all details regarding its precise mechanism have been revealed. Particularly, a complete spectroscopic and kinetic characterization of all intermediates remains challenging. In the September issue of Cell Reports Physical Science, Lee et al. identify a transient Eigen complex and determine the molecularity of each elementary step.
尽管对质子转移这一基本化学反应的研究持续了很长时间，但有关其精确机理的所有细节仍未得到揭示。特别是，对所有中间产物进行完整的光谱和动力学表征仍然具有挑战性。在 9 月份的《细胞报告-物理科学》（Cell Reports Physical Science）杂志上，Lee 等人确定了一个瞬态 Eigen 复合物，并确定了每个基本步骤的分子性。
{"title":"New light on proton transfer: Spectral and kinetic signature of a transient Eigen complex","authors":"Niklas Sülzner","doi":"10.1016/j.chempr.2024.10.017","DOIUrl":"10.1016/j.chempr.2024.10.017","url":null,"abstract":"<div><div>Despite the long-lasting research on proton transfer as a fundamental chemical reaction, not all details regarding its precise mechanism have been revealed. Particularly, a complete spectroscopic and kinetic characterization of all intermediates remains challenging. In the September issue of <em>Cell Reports Physical Science</em>, Lee et al. identify a transient Eigen complex and determine the molecularity of each elementary step.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3276-3278"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580548","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}
Pub Date : 2024-11-14DOI: 10.1016/j.chempr.2024.06.033
Subhayan Chakraborty , Han P.Q. Nguyen , Junichi Usuba , Ji Yong Choi , Zhenhuan Sun , Cijil Raju , Gustavo Sigelmann , Qianfeng Qiu , Sungwon Cho , Stephanie M. Tenney , Katherine E. Shulenberger , Klaus Schmidt-Rohr , Jihye Park , Grace G.D. Han
We introduce donor-acceptor substituted anthracenes as effective molecular solar thermal energy storage compounds that operate exclusively in the solid state. The donor-acceptor anthracenes undergo a visible light-induced [4+4] cycloaddition reaction, producing metastable cycloadducts—dianthracenes with quaternary carbons—and storing photon energy. The triggered cycloreversion of dianthracenes to anthracenes discharges the stored energy as heat in the order of 100 kJ/mol (200 J/g). The series of compounds displays remarkable self-heating, or cascading heat release, upon the initial triggering. Such self-activated energy release is enabled by the large energy storage in dianthracenes, low activation energy for their thermal reversion, and effective heat transfer to unreacted molecules in the solid state. This process mirroring the self-ignition of fossil fuels opens up opportunities to use dianthracenes as effective and renewable solid-state fuels that can release energy rapidly and completely upon initial activation.
{"title":"Self-activated energy release cascade from anthracene-based solid-state molecular solar thermal energy storage systems","authors":"Subhayan Chakraborty , Han P.Q. Nguyen , Junichi Usuba , Ji Yong Choi , Zhenhuan Sun , Cijil Raju , Gustavo Sigelmann , Qianfeng Qiu , Sungwon Cho , Stephanie M. Tenney , Katherine E. Shulenberger , Klaus Schmidt-Rohr , Jihye Park , Grace G.D. Han","doi":"10.1016/j.chempr.2024.06.033","DOIUrl":"10.1016/j.chempr.2024.06.033","url":null,"abstract":"<div><div>We introduce donor-acceptor substituted anthracenes as effective molecular solar thermal energy storage compounds that operate exclusively in the solid state. The donor-acceptor anthracenes undergo a visible light-induced [4+4] cycloaddition reaction, producing metastable cycloadducts—dianthracenes with quaternary carbons—and storing photon energy. The triggered cycloreversion of dianthracenes to anthracenes discharges the stored energy as heat in the order of 100 kJ/mol (200 J/g). The series of compounds displays remarkable self-heating, or cascading heat release, upon the initial triggering. Such self-activated energy release is enabled by the large energy storage in dianthracenes, low activation energy for their thermal reversion, and effective heat transfer to unreacted molecules in the solid state. This process mirroring the self-ignition of fossil fuels opens up opportunities to use dianthracenes as effective and renewable solid-state fuels that can release energy rapidly and completely upon initial activation.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3309-3322"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141746613","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}
Pub Date : 2024-11-14DOI: 10.1016/j.chempr.2024.08.003
Andrew R. Bortz , John M. Bennett , Rudi Fasan
Natural products have historically represented a major source of therapeutics and small-molecule probes for interrogating biological systems. Here, we describe the design and implementation of P450-mediated chemoenzymatic diversity-oriented synthesis (CeDOS), a strategy in which selective, regiodivergent P450-catalyzed oxyfunctionalizations are leveraged as key steps for enabling the skeletal rearrangement and diversification of a parent compound. Using this strategy and plant-derived parthenolide as the parent molecule, a structurally diverse library of over 50 unprecedented natural-product-like scaffolds was generated via divergent chemoenzymatic routes. Importantly, several members of this CeDOS library were found to exhibit notable cytotoxicity against human cancer cells as well as diversified anticancer activity profiles. This work demonstrates the power of CeDOS as a strategy for directing the construction and discovery of novel bioactive molecules, and it offers a blueprint for the broader application of this approach toward the creation and exploration of natural-product-like chemical libraries.
{"title":"A skeletally diverse library of bioactive natural-product-like compounds enabled by late-stage P450-catalyzed oxyfunctionalization","authors":"Andrew R. Bortz , John M. Bennett , Rudi Fasan","doi":"10.1016/j.chempr.2024.08.003","DOIUrl":"10.1016/j.chempr.2024.08.003","url":null,"abstract":"<div><div>Natural products have historically represented a major source of therapeutics and small-molecule probes for interrogating biological systems. Here, we describe the design and implementation of P450-mediated chemoenzymatic diversity-oriented synthesis (CeDOS), a strategy in which selective, regiodivergent P450-catalyzed oxyfunctionalizations are leveraged as key steps for enabling the skeletal rearrangement and diversification of a parent compound. Using this strategy and plant-derived parthenolide as the parent molecule, a structurally diverse library of over 50 unprecedented natural-product-like scaffolds was generated via divergent chemoenzymatic routes. Importantly, several members of this CeDOS library were found to exhibit notable cytotoxicity against human cancer cells as well as diversified anticancer activity profiles. This work demonstrates the power of CeDOS as a strategy for directing the construction and discovery of novel bioactive molecules, and it offers a blueprint for the broader application of this approach toward the creation and exploration of natural-product-like chemical libraries.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3488-3502"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138190","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}
Pub Date : 2024-11-14DOI: 10.1016/j.chempr.2024.07.025
Erin C. Day , Supraja S. Chittari , Keila C. Cunha , Roy J. Zhao , James N. Dodds , Delaney C. Davis , Erin S. Baker , Rebecca B. Berlow , Joan-Emma Shea , Rishikesh U. Kulkarni , Abigail S. Knight
Understanding how a macromolecule’s primary sequence governs its conformational landscape is crucial for elucidating its function, yet these design principles are still emerging for macromolecules with intrinsic disorder. Herein, we introduce a high-throughput workflow that implements a practical colorimetric conformational assay, introduces a semi-automated sequencing protocol using matrix-assisted laser desorption/ionization and tandem mass spectrometry (MALDI-MS/MS), and develops a generalizable sequence-structure algorithm. Using a model system of 20mer peptidomimetics containing polar glycine and hydrophobic N-butylglycine residues, we identified nine classifications of conformational disorder and isolated 122 unique sequences across varied compositions and conformations. Conformational distributions of three compositionally identical library sequences were corroborated through atomistic simulations and ion mobility spectrometry coupled with liquid chromatography. A data-driven strategy was developed using existing sequence variables and data-derived “motifs” to inform a machine-learning algorithm toward conformation prediction. This multifaceted approach enhances our understanding of sequence-conformation relationships and offers a powerful tool for accelerating the discovery of materials with conformational control.
{"title":"A high-throughput workflow to analyze sequence-conformation relationships and explore hydrophobic patterning in disordered peptoids","authors":"Erin C. Day , Supraja S. Chittari , Keila C. Cunha , Roy J. Zhao , James N. Dodds , Delaney C. Davis , Erin S. Baker , Rebecca B. Berlow , Joan-Emma Shea , Rishikesh U. Kulkarni , Abigail S. Knight","doi":"10.1016/j.chempr.2024.07.025","DOIUrl":"10.1016/j.chempr.2024.07.025","url":null,"abstract":"<div><div>Understanding how a macromolecule’s primary sequence governs its conformational landscape is crucial for elucidating its function, yet these design principles are still emerging for macromolecules with intrinsic disorder. Herein, we introduce a high-throughput workflow that implements a practical colorimetric conformational assay, introduces a semi-automated sequencing protocol using matrix-assisted laser desorption/ionization and tandem mass spectrometry (MALDI-MS/MS), and develops a generalizable sequence-structure algorithm. Using a model system of 20mer peptidomimetics containing polar glycine and hydrophobic <em>N</em>-butylglycine residues, we identified nine classifications of conformational disorder and isolated 122 unique sequences across varied compositions and conformations. Conformational distributions of three compositionally identical library sequences were corroborated through atomistic simulations and ion mobility spectrometry coupled with liquid chromatography. A data-driven strategy was developed using existing sequence variables and data-derived “motifs” to inform a machine-learning algorithm toward conformation prediction. This multifaceted approach enhances our understanding of sequence-conformation relationships and offers a powerful tool for accelerating the discovery of materials with conformational control.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3444-3458"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142142935","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}
The study of different forms of nanocellulose is a fast-growing field with many advantages. As a biobased polymer, it holds strong promise to replace petrochemical solid supports that need to be phased out. While there are already a plethora of nanocellulose applications, e.g., in the fields of material science, engineering, and water treatment, there is a surprising lack of reports concerning their applications in catalysis and organic chemistry. A crucial property of nanocellulose is its well-defined surface structure, which enables surface modifications to reach useful solid-supported catalysts and reagents. In this perspective, we explore the use of unmodified and modified variants of nanocellulose in organic chemistry. We further propose that the use of mechanochemistry could be a future application to increase the activity and eliminate the requirement for aqueous media due to nanocellulose’s dispersion issues.
{"title":"Nanocellulose: New horizons in organic chemistry and beyond","authors":"Sayad Doobary , Varvara Apostolopoulou-Kalkavoura , Aji P. Mathew , Berit Olofsson","doi":"10.1016/j.chempr.2024.09.007","DOIUrl":"10.1016/j.chempr.2024.09.007","url":null,"abstract":"<div><div>The study of different forms of nanocellulose is a fast-growing field with many advantages. As a biobased polymer, it holds strong promise to replace petrochemical solid supports that need to be phased out. While there are already a plethora of nanocellulose applications, e.g., in the fields of material science, engineering, and water treatment, there is a surprising lack of reports concerning their applications in catalysis and organic chemistry. A crucial property of nanocellulose is its well-defined surface structure, which enables surface modifications to reach useful solid-supported catalysts and reagents. In this perspective, we explore the use of unmodified and modified variants of nanocellulose in organic chemistry. We further propose that the use of mechanochemistry could be a future application to increase the activity and eliminate the requirement for aqueous media due to nanocellulose’s dispersion issues.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3279-3293"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142405506","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}
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