Noncovalent interactions between a lone pair of electrons and π systems can be categorized into two types based on the nature of π systems. Lone pair−π(C═O) interactions with π systems of unsaturated, polarized bonds are primarily attributed to orbital interactions, whereas lone pair−π(Ar) interactions with π systems of aromatic functional groups result from electrostatic attractions (for electron-deficient aryls) or dispersion attractions and Pauli repulsions (for electron-rich/neutral aryls). Unlike well-established noncovalent interactions, lone pair−π interactions have been comparatively underappreciated or less used to influence reaction outcomes. This review emphasizes experimental and computational studies aimed at integrating lone pair−π interactions into the design of catalytic systems and utilizing these interactions to regulate the reactivity and selectivity of chemical transformations. The role of lone pair−π interactions is highlighted in the stabilization or destabilization of transition states and ground-state binding. Examples influenced by lone pair−π interactions with both unsaturated, polarized bonds and aromatic rings as π systems are included. At variance with previous reviews, the present review is not structured according to the physical origin of particular classes of lone pair−π interactions but is divided into chapters according to ways in which lone pair−π interactions affect kinetics and/or selectivity of reactions.
{"title":"Lone Pair−π Interactions in Organic Reactions","authors":"Yu Chen, Qianqian Zhen, Fan-Jie Meng, Peiyuan Yu, Chen Xu","doi":"10.1021/acs.chemrev.4c00516","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00516","url":null,"abstract":"Noncovalent interactions between a lone pair of electrons and π systems can be categorized into two types based on the nature of π systems. Lone pair−π(C═O) interactions with π systems of unsaturated, polarized bonds are primarily attributed to orbital interactions, whereas lone pair−π(Ar) interactions with π systems of aromatic functional groups result from electrostatic attractions (for electron-deficient aryls) or dispersion attractions and Pauli repulsions (for electron-rich/neutral aryls). Unlike well-established noncovalent interactions, lone pair−π interactions have been comparatively underappreciated or less used to influence reaction outcomes. This review emphasizes experimental and computational studies aimed at integrating lone pair−π interactions into the design of catalytic systems and utilizing these interactions to regulate the reactivity and selectivity of chemical transformations. The role of lone pair−π interactions is highlighted in the stabilization or destabilization of transition states and ground-state binding. Examples influenced by lone pair−π interactions with both unsaturated, polarized bonds and aromatic rings as π systems are included. At variance with previous reviews, the present review is not structured according to the physical origin of particular classes of lone pair−π interactions but is divided into chapters according to ways in which lone pair−π interactions affect kinetics and/or selectivity of reactions.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"72 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601604","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 : 2024-11-13Epub Date: 2024-10-28DOI: 10.1021/acs.chemrev.4c00275
Alan Costello, Alexander A Peterson, Pei-Hsin Chen, Rustam Bagirzadeh, David L Lanster, Ahmed H Badran
The genetic code is the foundation for all life. With few exceptions, the translation of nucleic acid messages into proteins follows conserved rules, which are defined by codons that specify each of the 20 proteinogenic amino acids. For decades, leading research groups have developed a catalogue of innovative approaches to extend nature's amino acid repertoire to include one or more noncanonical building blocks in a single protein. In this review, we summarize advances in the history of in vitro and in vivo genetic code expansion, and highlight recent innovations that increase the scope of biochemically accessible monomers and codons. We further summarize state-of-the-art knowledge in engineered cellular translation, as well as alterations to regulatory mechanisms that improve overall genetic code expansion. Finally, we distill existing limitations of these technologies into must-have improvements for the next generation of technologies, and speculate on future strategies that may be capable of overcoming current gaps in knowledge.
{"title":"Genetic Code Expansion History and Modern Innovations.","authors":"Alan Costello, Alexander A Peterson, Pei-Hsin Chen, Rustam Bagirzadeh, David L Lanster, Ahmed H Badran","doi":"10.1021/acs.chemrev.4c00275","DOIUrl":"10.1021/acs.chemrev.4c00275","url":null,"abstract":"<p><p>The genetic code is the foundation for all life. With few exceptions, the translation of nucleic acid messages into proteins follows conserved rules, which are defined by codons that specify each of the 20 proteinogenic amino acids. For decades, leading research groups have developed a catalogue of innovative approaches to extend nature's amino acid repertoire to include one or more noncanonical building blocks in a single protein. In this review, we summarize advances in the history of <i>in vitro</i> and <i>in vivo</i> genetic code expansion, and highlight recent innovations that increase the scope of biochemically accessible monomers and codons. We further summarize state-of-the-art knowledge in engineered cellular translation, as well as alterations to regulatory mechanisms that improve overall genetic code expansion. Finally, we distill existing limitations of these technologies into must-have improvements for the next generation of technologies, and speculate on future strategies that may be capable of overcoming current gaps in knowledge.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":" ","pages":"11962-12005"},"PeriodicalIF":51.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491101","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 : 2024-11-11DOI: 10.1021/acs.chemrev.3c00806
Christian M. Schott, Peter M. Schneider, Kun-Ting Song, Haiting Yu, Rainer Götz, Felix Haimerl, Elena Gubanova, Jian Zhou, Thorsten O. Schmidt, Qiwei Zhang, Vitaly Alexandrov, Aliaksandr S. Bandarenka
The electrical double layer (EDL) plays a central role in electrochemical energy systems, impacting charge transfer mechanisms and reaction rates. The fundamental importance of the EDL in interfacial electrochemistry has motivated researchers to develop theoretical and experimental approaches to assess EDL properties. In this contribution, we review recent progress in evaluating EDL characteristics such as the double-layer capacitance, highlighting some discrepancies between theory and experiment and discussing strategies for their reconciliation. We further discuss the merits and challenges of various experimental techniques and theoretical approaches having important implications for aqueous electrocatalysis. A strong emphasis is placed on the substantial impact of the electrode composition and structure and the electrolyte chemistry on the double-layer properties. In addition, we review the effects of temperature and pressure and compare solid–liquid interfaces to solid–solid interfaces.
{"title":"How to Assess and Predict Electrical Double Layer Properties. Implications for Electrocatalysis","authors":"Christian M. Schott, Peter M. Schneider, Kun-Ting Song, Haiting Yu, Rainer Götz, Felix Haimerl, Elena Gubanova, Jian Zhou, Thorsten O. Schmidt, Qiwei Zhang, Vitaly Alexandrov, Aliaksandr S. Bandarenka","doi":"10.1021/acs.chemrev.3c00806","DOIUrl":"https://doi.org/10.1021/acs.chemrev.3c00806","url":null,"abstract":"The electrical double layer (EDL) plays a central role in electrochemical energy systems, impacting charge transfer mechanisms and reaction rates. The fundamental importance of the EDL in interfacial electrochemistry has motivated researchers to develop theoretical and experimental approaches to assess EDL properties. In this contribution, we review recent progress in evaluating EDL characteristics such as the double-layer capacitance, highlighting some discrepancies between theory and experiment and discussing strategies for their reconciliation. We further discuss the merits and challenges of various experimental techniques and theoretical approaches having important implications for aqueous electrocatalysis. A strong emphasis is placed on the substantial impact of the electrode composition and structure and the electrolyte chemistry on the double-layer properties. In addition, we review the effects of temperature and pressure and compare solid–liquid interfaces to solid–solid interfaces.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"35 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598594","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 : 2024-11-07DOI: 10.1021/acs.chemrev.4c00417
Steven S. Cheng, Alison C. Mody, Christina M. Woo
O-Linked β-N-acetylglucosamine (O-GlcNAc) is an essential, dynamic monosaccharide post-translational modification (PTM) found on serine and threonine residues of thousands of nucleocytoplasmic proteins. The installation and removal of O-GlcNAc is controlled by a single pair of enzymes, O-GlcNAc transferase (OGT) and O-GlcNAcase (OGA), respectively. Since its discovery four decades ago, O-GlcNAc has been found on diverse classes of proteins, playing important functional roles in many cellular processes. Dysregulation of O-GlcNAc homeostasis has been implicated in the pathogenesis of disease, including neurodegeneration, X-linked intellectual disability (XLID), cancer, diabetes, and immunological disorders. These foundational studies of O-GlcNAc in disease biology have motivated efforts to target O-GlcNAc therapeutically, with multiple clinical candidates under evaluation. In this review, we describe the characterization and biochemistry of OGT and OGA, cellular O-GlcNAc regulation, development of OGT and OGA inhibitors, O-GlcNAc in pathophysiology, clinical progress of O-GlcNAc modulators, and emerging opportunities for targeting O-GlcNAc. This comprehensive resource should motivate further study into O-GlcNAc function and inspire strategies for therapeutic modulation of O-GlcNAc.
{"title":"Opportunities for Therapeutic Modulation of O-GlcNAc","authors":"Steven S. Cheng, Alison C. Mody, Christina M. Woo","doi":"10.1021/acs.chemrev.4c00417","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00417","url":null,"abstract":"<i>O</i>-Linked β-<i>N</i>-acetylglucosamine (O-GlcNAc) is an essential, dynamic monosaccharide post-translational modification (PTM) found on serine and threonine residues of thousands of nucleocytoplasmic proteins. The installation and removal of O-GlcNAc is controlled by a single pair of enzymes, O-GlcNAc transferase (OGT) and O-GlcNAcase (OGA), respectively. Since its discovery four decades ago, O-GlcNAc has been found on diverse classes of proteins, playing important functional roles in many cellular processes. Dysregulation of O-GlcNAc homeostasis has been implicated in the pathogenesis of disease, including neurodegeneration, X-linked intellectual disability (XLID), cancer, diabetes, and immunological disorders. These foundational studies of O-GlcNAc in disease biology have motivated efforts to target O-GlcNAc therapeutically, with multiple clinical candidates under evaluation. In this review, we describe the characterization and biochemistry of OGT and OGA, cellular O-GlcNAc regulation, development of OGT and OGA inhibitors, O-GlcNAc in pathophysiology, clinical progress of O-GlcNAc modulators, and emerging opportunities for targeting O-GlcNAc. This comprehensive resource should motivate further study into O-GlcNAc function and inspire strategies for therapeutic modulation of O-GlcNAc.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"9 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594515","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 : 2024-11-07DOI: 10.1021/acs.chemrev.4c00284
Moreno Wichert, Laura Guasch, Raphael M. Franzini
DNA-encoded library (DEL) technology is a powerful platform for the efficient identification of novel chemical matter in the early drug discovery process enabled by parallel screening of vast libraries of encoded small molecules through affinity selection and deep sequencing. While DEL selections provide rich data sets for computational drug discovery, the underlying technical factors influencing DEL data remain incompletely understood. This review systematically examines the key parameters affecting the chemical information in DEL data and their impact on hit triaging and machine learning integration. The need for rigorous data handling and interpretation is emphasized, with standardized methods being critical for the success of DEL-based approaches. Major challenges include the relationship between sequence counts and binding affinities, frequent hitters, and the influence of factors such as inhomogeneous library composition, DNA damage, and linkers on binding modes. Experimental artifacts, such as those caused by protein immobilization and screening matrix effects, further complicate data interpretation. Recent advancements in using machine learning to denoise DEL data and predict drug candidates are highlighted. This review offers practical guidance on adopting best practices for integrating robust methodologies, comprehensive data analysis, and computational tools to improve the accuracy and efficacy of DEL-driven hit discovery.
DNA 编码文库（DEL）技术是在早期药物发现过程中高效识别新型化学物质的强大平台，它通过亲和选择和深度测序对大量编码小分子文库进行平行筛选。虽然 DEL 筛选为计算药物发现提供了丰富的数据集，但人们对影响 DEL 数据的基本技术因素仍不甚了解。本综述系统地研究了影响 DEL 数据中化学信息的关键参数及其对命中分选和机器学习整合的影响。强调了严格处理和解释数据的必要性，标准化方法是基于 DEL 方法取得成功的关键。面临的主要挑战包括序列数与结合亲和力之间的关系、常中者以及非均质文库组成、DNA损伤和连接体等因素对结合模式的影响。蛋白质固定和筛选基质效应等造成的实验假象使数据解读更加复杂。本文重点介绍了利用机器学习对 DEL 数据进行去噪和预测候选药物的最新进展。本综述为采用最佳实践提供了实用指导，以整合稳健的方法学、全面的数据分析和计算工具，提高 DEL 驱动的新药发现的准确性和有效性。
{"title":"Challenges and Prospects of DNA-Encoded Library Data Interpretation","authors":"Moreno Wichert, Laura Guasch, Raphael M. Franzini","doi":"10.1021/acs.chemrev.4c00284","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00284","url":null,"abstract":"DNA-encoded library (DEL) technology is a powerful platform for the efficient identification of novel chemical matter in the early drug discovery process enabled by parallel screening of vast libraries of encoded small molecules through affinity selection and deep sequencing. While DEL selections provide rich data sets for computational drug discovery, the underlying technical factors influencing DEL data remain incompletely understood. This review systematically examines the key parameters affecting the chemical information in DEL data and their impact on hit triaging and machine learning integration. The need for rigorous data handling and interpretation is emphasized, with standardized methods being critical for the success of DEL-based approaches. Major challenges include the relationship between sequence counts and binding affinities, frequent hitters, and the influence of factors such as inhomogeneous library composition, DNA damage, and linkers on binding modes. Experimental artifacts, such as those caused by protein immobilization and screening matrix effects, further complicate data interpretation. Recent advancements in using machine learning to denoise DEL data and predict drug candidates are highlighted. This review offers practical guidance on adopting best practices for integrating robust methodologies, comprehensive data analysis, and computational tools to improve the accuracy and efficacy of DEL-driven hit discovery.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"144 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594544","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 : 2024-11-07DOI: 10.1021/acs.chemrev.4c00181
Chiara De Faveri, Jordan M. Mattheisen, Thomas P. Sakmar, Irene Coin
Methods rooted in chemical biology have contributed significantly to studies of integral membrane proteins. One recent key approach has been the application of genetic code expansion (GCE), which enables the site-specific incorporation of noncanonical amino acids (ncAAs) with defined chemical properties into proteins. Efficient GCE is challenging, especially for membrane proteins, which have specialized biogenesis and cell trafficking machinery and tend to be expressed at low levels in cell membranes. Many eukaryotic membrane proteins cannot be expressed functionally in E. coli and are most effectively studied in mammalian cell culture systems. Recent advances have facilitated broader applications of GCE for studies of membrane proteins. First, AARS/tRNA pairs have been engineered to function efficiently in mammalian cells. Second, bioorthogonal chemical reactions, including cell-friendly copper-free “click” chemistry, have enabled linkage of small-molecule probes such as fluorophores to membrane proteins in live cells. Finally, in concert with advances in GCE methodology, the variety of available ncAAs has increased dramatically, thus enabling the investigation of protein structure and dynamics by multidisciplinary biochemical and biophysical approaches. These developments are reviewed in the historical framework of the development of GCE technology with a focus on applications to studies of membrane proteins.
{"title":"Noncanonical Amino Acid Tools and Their Application to Membrane Protein Studies","authors":"Chiara De Faveri, Jordan M. Mattheisen, Thomas P. Sakmar, Irene Coin","doi":"10.1021/acs.chemrev.4c00181","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00181","url":null,"abstract":"Methods rooted in chemical biology have contributed significantly to studies of integral membrane proteins. One recent key approach has been the application of genetic code expansion (GCE), which enables the site-specific incorporation of noncanonical amino acids (ncAAs) with defined chemical properties into proteins. Efficient GCE is challenging, especially for membrane proteins, which have specialized biogenesis and cell trafficking machinery and tend to be expressed at low levels in cell membranes. Many eukaryotic membrane proteins cannot be expressed functionally in <i>E. coli</i> and are most effectively studied in mammalian cell culture systems. Recent advances have facilitated broader applications of GCE for studies of membrane proteins. First, AARS/tRNA pairs have been engineered to function efficiently in mammalian cells. Second, bioorthogonal chemical reactions, including cell-friendly copper-free “click” chemistry, have enabled linkage of small-molecule probes such as fluorophores to membrane proteins in live cells. Finally, in concert with advances in GCE methodology, the variety of available ncAAs has increased dramatically, thus enabling the investigation of protein structure and dynamics by multidisciplinary biochemical and biophysical approaches. These developments are reviewed in the historical framework of the development of GCE technology with a focus on applications to studies of membrane proteins.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"30 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598056","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 : 2024-11-06DOI: 10.1021/acs.chemrev.4c00373
Vladimir Ladizhansky, Ravi Shankar Palani, Michael Mardini, Robert G. Griffin
Magic angle spinning (MAS) nuclear magnetic resonance (NMR) has evolved significantly over the past three decades and established itself as a vital tool for the structural analysis of biological macromolecules and materials. This review delves into the development and application of dipolar recoupling techniques in MAS NMR, which are crucial for obtaining detailed structural and dynamic information. We discuss a variety of homonuclear and heteronuclear recoupling methods which are essential for measuring spatial restraints and explain in detail the spin dynamics that these sequences generate. We also explore recent developments in high spinning frequency MAS, proton detection, and dynamic nuclear polarization, underscoring their importance in advancing biomolecular NMR. Our aim is to provide a comprehensive account of contemporary dipolar recoupling methods, their principles, and their application to structural biology and materials, highlighting significant contributions to the field and emerging techniques that enhance resolution and sensitivity in MAS NMR spectroscopy.
魔角旋转核磁共振（MAS）在过去三十年中取得了长足发展，已成为生物大分子和材料结构分析的重要工具。本综述深入探讨了 MAS NMR 中双极性再偶联技术的发展和应用，这些技术对于获取详细的结构和动态信息至关重要。我们讨论了对测量空间限制至关重要的各种同核和异核再偶联方法，并详细解释了这些序列产生的自旋动力学。我们还探讨了高旋转频率 MAS、质子检测和动态核极化的最新发展，强调了它们在推动生物分子核磁共振方面的重要性。我们的目标是全面介绍当代偶极再偶联方法、其原理及其在结构生物学和材料中的应用，突出强调对该领域的重大贡献以及可提高 MAS NMR 光谱分辨率和灵敏度的新兴技术。
{"title":"Dipolar Recoupling in Rotating Solids","authors":"Vladimir Ladizhansky, Ravi Shankar Palani, Michael Mardini, Robert G. Griffin","doi":"10.1021/acs.chemrev.4c00373","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00373","url":null,"abstract":"Magic angle spinning (MAS) nuclear magnetic resonance (NMR) has evolved significantly over the past three decades and established itself as a vital tool for the structural analysis of biological macromolecules and materials. This review delves into the development and application of dipolar recoupling techniques in MAS NMR, which are crucial for obtaining detailed structural and dynamic information. We discuss a variety of homonuclear and heteronuclear recoupling methods which are essential for measuring spatial restraints and explain in detail the spin dynamics that these sequences generate. We also explore recent developments in high spinning frequency MAS, proton detection, and dynamic nuclear polarization, underscoring their importance in advancing biomolecular NMR. Our aim is to provide a comprehensive account of contemporary dipolar recoupling methods, their principles, and their application to structural biology and materials, highlighting significant contributions to the field and emerging techniques that enhance resolution and sensitivity in MAS NMR spectroscopy.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"91 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589021","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 : 2024-11-05DOI: 10.1021/acs.chemrev.4c00369
Guanglong Ding, Hang Li, JiYu Zhao, Kui Zhou, Yongbiao Zhai, Ziyu Lv, Meng Zhang, Yan Yan, Su-Ting Han, Ye Zhou
The quest to imbue machines with intelligence akin to that of humans, through the development of adaptable neuromorphic devices and the creation of artificial neural systems, has long stood as a pivotal goal in both scientific inquiry and industrial advancement. Recent advancements in flexible neuromorphic electronics primarily rely on nanomaterials and polymers owing to their inherent uniformity, superior mechanical and electrical capabilities, and versatile functionalities. However, this field is still in its nascent stage, necessitating continuous efforts in materials innovation and device/system design. Therefore, it is imperative to conduct an extensive and comprehensive analysis to summarize current progress. This review highlights the advancements and applications of flexible neuromorphics, involving inorganic nanomaterials (zero-/one-/two-dimensional, and heterostructure), carbon-based nanomaterials such as carbon nanotubes (CNTs) and graphene, and polymers. Additionally, a comprehensive comparison and summary of the structural compositions, design strategies, key performance, and significant applications of these devices are provided. Furthermore, the challenges and future directions pertaining to materials/devices/systems associated with flexible neuromorphics are also addressed. The aim of this review is to shed light on the rapidly growing field of flexible neuromorphics, attract experts from diverse disciplines (e.g., electronics, materials science, neurobiology), and foster further innovation for its accelerated development.
{"title":"Nanomaterials for Flexible Neuromorphics","authors":"Guanglong Ding, Hang Li, JiYu Zhao, Kui Zhou, Yongbiao Zhai, Ziyu Lv, Meng Zhang, Yan Yan, Su-Ting Han, Ye Zhou","doi":"10.1021/acs.chemrev.4c00369","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00369","url":null,"abstract":"The quest to imbue machines with intelligence akin to that of humans, through the development of adaptable neuromorphic devices and the creation of artificial neural systems, has long stood as a pivotal goal in both scientific inquiry and industrial advancement. Recent advancements in flexible neuromorphic electronics primarily rely on nanomaterials and polymers owing to their inherent uniformity, superior mechanical and electrical capabilities, and versatile functionalities. However, this field is still in its nascent stage, necessitating continuous efforts in materials innovation and device/system design. Therefore, it is imperative to conduct an extensive and comprehensive analysis to summarize current progress. This review highlights the advancements and applications of flexible neuromorphics, involving inorganic nanomaterials (zero-/one-/two-dimensional, and heterostructure), carbon-based nanomaterials such as carbon nanotubes (CNTs) and graphene, and polymers. Additionally, a comprehensive comparison and summary of the structural compositions, design strategies, key performance, and significant applications of these devices are provided. Furthermore, the challenges and future directions pertaining to materials/devices/systems associated with flexible neuromorphics are also addressed. The aim of this review is to shed light on the rapidly growing field of flexible neuromorphics, attract experts from diverse disciplines (e.g., electronics, materials science, neurobiology), and foster further innovation for its accelerated development.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"29 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580678","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 : 2024-11-05DOI: 10.1021/acs.chemrev.4c00472
Sigitas Mikutis, Gonçalo J. L. Bernardes
The vast majority of the human genome codes for RNA, but RNA-targeting therapeutics account for a small fraction of approved drugs. As such, there is great incentive to improve old and develop new approaches to RNA targeting. For many RNA targeting modalities, just binding is not sufficient to exert a therapeutic effect; thus, targeted RNA degradation and induced decay emerged as powerful approaches with a pronounced biological effect. This review covers the origins and advanced use cases of targeted RNA degrader technologies grouped by the nature of the targeting modality as well as by the mode of degradation. It covers both well-established methods and clinically successful platforms such as RNA interference, as well as emerging approaches such as recruitment of RNA quality control machinery, CRISPR, and direct targeted RNA degradation. We also share our thoughts on the biggest hurdles in this field, as well as possible ways to overcome them.
{"title":"Technologies for Targeted RNA Degradation and Induced RNA Decay","authors":"Sigitas Mikutis, Gonçalo J. L. Bernardes","doi":"10.1021/acs.chemrev.4c00472","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00472","url":null,"abstract":"The vast majority of the human genome codes for RNA, but RNA-targeting therapeutics account for a small fraction of approved drugs. As such, there is great incentive to improve old and develop new approaches to RNA targeting. For many RNA targeting modalities, just binding is not sufficient to exert a therapeutic effect; thus, targeted RNA degradation and induced decay emerged as powerful approaches with a pronounced biological effect. This review covers the origins and advanced use cases of targeted RNA degrader technologies grouped by the nature of the targeting modality as well as by the mode of degradation. It covers both well-established methods and clinically successful platforms such as RNA interference, as well as emerging approaches such as recruitment of RNA quality control machinery, CRISPR, and direct targeted RNA degradation. We also share our thoughts on the biggest hurdles in this field, as well as possible ways to overcome them.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"5 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580682","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 : 2024-10-31DOI: 10.1021/acs.chemrev.4c00261
Matthijs P. J. M. van der Ham, Jordi Creus, Johannes H. Bitter, Marc T. M. Koper, Paolo P. Pescarmona
In this contribution, we review the electrochemical upgrading of saccharides (e.g., glucose) and sugar alcohols (e.g., glycerol) on metal and metal-oxide electrodes by drawing conclusions on common trends and differences between these two important classes of biobased compounds. For this purpose, we critically review the literature on the electrocatalytic oxidation of saccharides and sugar alcohols, seeking trends in the effect of reaction conditions and electrocatalyst design on the selectivity for the oxidation of specific functional groups toward value-added compounds. Importantly, we highlight and discuss the competition between electrochemical and non-electrochemical pathways. This is a crucial and yet often neglected aspect that should be taken into account and optimized for achieving the efficient electrocatalytic conversion of monosaccharides and related sugar alcohols into valuable products, which is a target of growing interest in the context of the electrification of the chemical industry combined with the utilization of renewable feedstock.
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