Chemical ReviewsPub Date : 2024-11-06DOI: 10.1021/acs.chemrev.4c0037310.1021/acs.chemrev.4c00373
Vladimir Ladizhansky*, Ravi Shankar Palani, Michael Mardini and Robert G. Griffin*,
{"title":"Dipolar Recoupling in Rotating Solids","authors":"Vladimir Ladizhansky*, Ravi Shankar Palani, Michael Mardini and Robert G. Griffin*, ","doi":"10.1021/acs.chemrev.4c0037310.1021/acs.chemrev.4c00373","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00373https://doi.org/10.1021/acs.chemrev.4c00373","url":null,"abstract":"<p >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.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"124 22","pages":"12844–12917 12844–12917"},"PeriodicalIF":51.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713639","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}
Chemical ReviewsPub Date : 2024-11-06DOI: 10.1021/acs.chemrev.4c00373
Vladimir Ladizhansky, Ravi Shankar Palani, Michael Mardini, Robert G. Griffin
{"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}
Chemical ReviewsPub Date : 2024-11-05DOI: 10.1021/acs.chemrev.4c0036910.1021/acs.chemrev.4c00369
Guanglong Ding, Hang Li, JiYu Zhao, Kui Zhou, Yongbiao Zhai, Ziyu Lv, Meng Zhang, Yan Yan, Su-Ting Han and Ye Zhou*,
{"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 and Ye Zhou*, ","doi":"10.1021/acs.chemrev.4c0036910.1021/acs.chemrev.4c00369","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00369https://doi.org/10.1021/acs.chemrev.4c00369","url":null,"abstract":"<p >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.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"124 22","pages":"12738–12843 12738–12843"},"PeriodicalIF":51.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142719570","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}
Chemical ReviewsPub 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
{"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}
Chemical ReviewsPub Date : 2024-11-05DOI: 10.1021/acs.chemrev.4c00472
Sigitas Mikutis, Gonçalo J. L. Bernardes
{"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}
Chemical ReviewsPub Date : 2024-11-05DOI: 10.1021/acs.chemrev.4c0047210.1021/acs.chemrev.4c00472
Sigitas Mikutis*, and , Gonçalo J. L. Bernardes*,
{"title":"Technologies for Targeted RNA Degradation and Induced RNA Decay","authors":"Sigitas Mikutis*, and , Gonçalo J. L. Bernardes*, ","doi":"10.1021/acs.chemrev.4c0047210.1021/acs.chemrev.4c00472","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00472https://doi.org/10.1021/acs.chemrev.4c00472","url":null,"abstract":"<p >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.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"124 23","pages":"13301–13330 13301–13330"},"PeriodicalIF":51.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemrev.4c00472","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844131","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}
Chemical ReviewsPub 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
{"title":"Electrochemical and Non-Electrochemical Pathways in the Electrocatalytic Oxidation of Monosaccharides and Related Sugar Alcohols into Valuable Products","authors":"Matthijs P. J. M. van der Ham, Jordi Creus, Johannes H. Bitter, Marc T. M. Koper, Paolo P. Pescarmona","doi":"10.1021/acs.chemrev.4c00261","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00261","url":null,"abstract":"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.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"112 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556166","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}
Chemical ReviewsPub Date : 2024-10-31DOI: 10.1021/acs.chemrev.4c00438
Michele Stofella, Antonio Grimaldi, Jochem H. Smit, Jürgen Claesen, Emanuele Paci, Frank Sobott
{"title":"Computational Tools for Hydrogen–Deuterium Exchange Mass Spectrometry Data Analysis","authors":"Michele Stofella, Antonio Grimaldi, Jochem H. Smit, Jürgen Claesen, Emanuele Paci, Frank Sobott","doi":"10.1021/acs.chemrev.4c00438","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00438","url":null,"abstract":"Hydrogen–deuterium exchange (HDX) has become a pivotal method for investigating the structural and dynamic properties of proteins. The versatility and sensitivity of mass spectrometry (MS) made the technique the ideal companion for HDX, and today HDX-MS is addressing a growing number of applications in both academic research and industrial settings. The prolific generation of experimental data has spurred the concurrent development of numerous computational tools, designed to automate parts of the workflow while employing different strategies to achieve common objectives. Various computational methods are available to perform automated peptide searches and identification; different statistical tests have been implemented to quantify differences in the exchange pattern between two or more experimental conditions; alternative strategies have been developed to deconvolve and analyze peptides showing multimodal behavior; and different algorithms have been proposed to computationally increase the resolution of HDX-MS data, with the ultimate aim to provide information at the level of the single residue. This review delves into a comprehensive examination of the merits and drawbacks associated with the diverse strategies implemented by software tools for the analysis of HDX-MS data.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"30 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556459","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}
Chemical ReviewsPub Date : 2024-10-31DOI: 10.1021/acs.chemrev.4c00282
Mingrui Wang, Guanghui Zhang, Hao Wang, Zhiqun Wang, Yu Zhou, Xiaowa Nie, Ben Hang Yin, Chunshan Song, Xinwen Guo
{"title":"Understanding and Tuning the Effects of H2O on Catalytic CO and CO2 Hydrogenation","authors":"Mingrui Wang, Guanghui Zhang, Hao Wang, Zhiqun Wang, Yu Zhou, Xiaowa Nie, Ben Hang Yin, Chunshan Song, Xinwen Guo","doi":"10.1021/acs.chemrev.4c00282","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00282","url":null,"abstract":"Catalytic CO<sub><i>x</i></sub> (CO and CO<sub>2</sub>) hydrogenation to valued chemicals is one of the promising approaches to address challenges in energy, environment, and climate change. H<sub>2</sub>O is an inevitable side product in these reactions, where its existence and effect are often ignored. In fact, H<sub>2</sub>O significantly influences the catalytic active centers, reaction mechanism, and catalytic performance, preventing us from a definitive and deep understanding on the structure-performance relationship of the authentic catalysts. It is necessary, although challenging, to clarify its effect and provide practical strategies to tune the concentration and distribution of H<sub>2</sub>O to optimize its influence. In this review, we focus on how H<sub>2</sub>O in CO<sub><i>x</i></sub> hydrogenation induces the structural evolution of catalysts and assists in the catalytic processes, as well as efforts to understand the underlying mechanism. We summarize and discuss some representative tuning strategies for realizing the rapid removal or local enrichment of H<sub>2</sub>O around the catalysts, along with brief techno-economic analysis and life cycle assessment. These fundamental understandings and strategies are further extended to the reactions of CO and CO<sub>2</sub> reduction under an external field (light, electricity, and plasma). We also present suggestions and prospects for deciphering and controlling the effect of H<sub>2</sub>O in practical applications.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"126 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556112","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}
{"title":"Evolution of Copolymers of Epoxides and CO2: Catalysts, Monomers, Architectures, and Applications","authors":"Guan-Wen Yang, Rui Xie, Yao-Yao Zhang, Cheng-Kai Xu, Guang-Peng Wu","doi":"10.1021/acs.chemrev.4c00517","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00517","url":null,"abstract":"The copolymerization of CO<sub>2</sub> and epoxides presents a transformative approach to converting greenhouse gases into aliphatic polycarbonates (CO<sub>2</sub>-PCs), thereby reducing the polymer industry’s dependence on fossil resources. Over the past 50 years, a wide array of metallic catalysts, both heterogeneous and homogeneous, have been developed to achieve precise control over polymer selectivity, sequence, regio-, and stereoselectivity. This review details the evolution of metal-based catalysts, with a particular focus on the emergence of organoborane catalysts, and explores how these catalysts effectively address kinetic and thermodynamic challenges in CO<sub>2</sub>/epoxides copoly<sub>2</sub>merization. Advances in the synthesis of CO<sub>2</sub>-PCs with varied sequence and chain architectures through diverse polymerization protocols are examined, alongside the applications of functional CO<sub>2</sub>-PCs produced by incorporating different epoxides. The review also underscores the contributions of computational techniques to our understanding of copolymerization mechanisms and highlights recent advances in the closed-loop chemical recycling of CO<sub>2</sub>-sourced polycarbonates. Finally, the industrialization efforts of CO<sub>2</sub>-PCs are discussed, offering readers a comprehensive understanding of the evolution and future potential of epoxide copolymerization with CO<sub>2</sub>.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"6 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142489456","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}