Pub Date : 2024-03-21DOI: 10.1038/s41570-024-00585-3
Ling Huang, Gang Han
Photon upconversion is a method for harnessing high-energy excited states from low-energy photons. Such photons, particularly in the red and near-infrared wavelength ranges, can penetrate tissue deeply and undergo less competitive absorption in coloured reaction media, enhancing the efficiency of large-scale reactions and in vivo phototherapy. Among various upconversion methodologies, the organic-based triplet–triplet annihilation upconversion (TTA-UC) stands out — demonstrating high upconversion efficiencies, requiring low excitation power densities and featuring tunable absorption and emission wavelengths. These factors contribute to improved photochemical reactions for fields such as photoredox catalysis, photoactivation, 3D printing and immunotherapy. In this Review, we explore concepts and design principles of organic TTA-UC-mediated photochemical reactions, highlighting notable advancements in the field, as well as identify challenges and propose potential solutions. This Review sheds light on the potential of organic TTA-UC to advance beyond the traditional photochemical reactions and paves the way for research in various fields and clinical applications. Organic-based triplet–triplet annihilation upconversion-mediated photochemical reactions utilize low-energy photons to obtain high-energy excited states leading to notable advancements in photoredox catalysis, photoactivation, 3D printing and immunotherapy. Classifications, design principles, challenges and possible solutions are discussed in this Review.
{"title":"Triplet–triplet annihilation photon upconversion-mediated photochemical reactions","authors":"Ling Huang, Gang Han","doi":"10.1038/s41570-024-00585-3","DOIUrl":"10.1038/s41570-024-00585-3","url":null,"abstract":"Photon upconversion is a method for harnessing high-energy excited states from low-energy photons. Such photons, particularly in the red and near-infrared wavelength ranges, can penetrate tissue deeply and undergo less competitive absorption in coloured reaction media, enhancing the efficiency of large-scale reactions and in vivo phototherapy. Among various upconversion methodologies, the organic-based triplet–triplet annihilation upconversion (TTA-UC) stands out — demonstrating high upconversion efficiencies, requiring low excitation power densities and featuring tunable absorption and emission wavelengths. These factors contribute to improved photochemical reactions for fields such as photoredox catalysis, photoactivation, 3D printing and immunotherapy. In this Review, we explore concepts and design principles of organic TTA-UC-mediated photochemical reactions, highlighting notable advancements in the field, as well as identify challenges and propose potential solutions. This Review sheds light on the potential of organic TTA-UC to advance beyond the traditional photochemical reactions and paves the way for research in various fields and clinical applications. Organic-based triplet–triplet annihilation upconversion-mediated photochemical reactions utilize low-energy photons to obtain high-energy excited states leading to notable advancements in photoredox catalysis, photoactivation, 3D printing and immunotherapy. Classifications, design principles, challenges and possible solutions are discussed in this Review.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 4","pages":"238-255"},"PeriodicalIF":36.3,"publicationDate":"2024-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140184876","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 : 2024-03-21DOI: 10.1038/s41570-024-00594-2
Sarah Clapham, Peter J. Hotchkiss
The Chemical Weapons Convention has a unique Scientific Advisory Board that ensures it keeps pace with science, and its implementing body is prepared for future challenges. It is a model that could be usefully applied to other disarmament treaties.
{"title":"Robust scientific advisory mechanisms future-proof disarmament treaties","authors":"Sarah Clapham, Peter J. Hotchkiss","doi":"10.1038/s41570-024-00594-2","DOIUrl":"10.1038/s41570-024-00594-2","url":null,"abstract":"The Chemical Weapons Convention has a unique Scientific Advisory Board that ensures it keeps pace with science, and its implementing body is prepared for future challenges. It is a model that could be usefully applied to other disarmament treaties.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 4","pages":"231-233"},"PeriodicalIF":36.3,"publicationDate":"2024-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140184875","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 : 2024-03-18DOI: 10.1038/s41570-024-00592-4
Ana Koperniku, Nicholas A. Meanwell
Targeted covalent inhibitors (TCIs) can react irreversibly with lysine in kinases and other proteins. Small molecule TCIs can have both broad or specific lysine targeting whereas peptide- and protein-based TCIs were shown to provide high target specificity for lysines in shallow protein surfaces.
{"title":"Tying the knot with lysine","authors":"Ana Koperniku, Nicholas A. Meanwell","doi":"10.1038/s41570-024-00592-4","DOIUrl":"10.1038/s41570-024-00592-4","url":null,"abstract":"Targeted covalent inhibitors (TCIs) can react irreversibly with lysine in kinases and other proteins. Small molecule TCIs can have both broad or specific lysine targeting whereas peptide- and protein-based TCIs were shown to provide high target specificity for lysines in shallow protein surfaces.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 4","pages":"235-237"},"PeriodicalIF":36.3,"publicationDate":"2024-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140158549","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 : 2024-03-06DOI: 10.1038/s41570-024-00584-4
Sophie C. Patrick, Paul D. Beer, Jason J. Davis
Anion recognition is pertinent to a range of environmental, medicinal and industrial applications. Recent progress in the field has relied on advances in synthetic host design to afford a broad range of potent recognition motifs and novel supramolecular structures capable of effective binding both in solution and at derived molecular films. However, performance in aqueous media remains a critical challenge. Understanding the effects of bulk and local solvent on anion recognition by host scaffolds is imperative if effective and selective detection in real-world media is to be viable. This Review seeks to provide a framework within which these effects can be considered both experimentally and theoretically. We highlight proposed models for solvation effects on anion binding and discuss approaches to retain strong anion binding in highly competitive (polar) solvents. The synthetic design principles for exploiting the aforementioned solvent effects are explored. Anion recognition in competitive, aqueous media remains a critical challenge. Bulk and local solvation models for anion recognition events are herein explored, as well as targeted design approaches to retain strong anion binding in highly polar media.
{"title":"Solvent effects in anion recognition","authors":"Sophie C. Patrick, Paul D. Beer, Jason J. Davis","doi":"10.1038/s41570-024-00584-4","DOIUrl":"10.1038/s41570-024-00584-4","url":null,"abstract":"Anion recognition is pertinent to a range of environmental, medicinal and industrial applications. Recent progress in the field has relied on advances in synthetic host design to afford a broad range of potent recognition motifs and novel supramolecular structures capable of effective binding both in solution and at derived molecular films. However, performance in aqueous media remains a critical challenge. Understanding the effects of bulk and local solvent on anion recognition by host scaffolds is imperative if effective and selective detection in real-world media is to be viable. This Review seeks to provide a framework within which these effects can be considered both experimentally and theoretically. We highlight proposed models for solvation effects on anion binding and discuss approaches to retain strong anion binding in highly competitive (polar) solvents. The synthetic design principles for exploiting the aforementioned solvent effects are explored. Anion recognition in competitive, aqueous media remains a critical challenge. Bulk and local solvation models for anion recognition events are herein explored, as well as targeted design approaches to retain strong anion binding in highly polar media.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 4","pages":"256-276"},"PeriodicalIF":36.3,"publicationDate":"2024-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140049928","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 : 2024-03-04DOI: 10.1038/s41570-024-00586-2
Ella Sciamma-O’Brien, Thomas Drant, Nicholas Wogan
JWST collects vast amounts of information about exoplanets light years away from Earth. Back home, the measured optical constants of laboratory aerosols are critically input parameters in models to interpret the observational results.
{"title":"In an exoplanet atmosphere far, far away","authors":"Ella Sciamma-O’Brien, Thomas Drant, Nicholas Wogan","doi":"10.1038/s41570-024-00586-2","DOIUrl":"10.1038/s41570-024-00586-2","url":null,"abstract":"JWST collects vast amounts of information about exoplanets light years away from Earth. Back home, the measured optical constants of laboratory aerosols are critically input parameters in models to interpret the observational results.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 3","pages":"157-158"},"PeriodicalIF":36.3,"publicationDate":"2024-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140026526","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 : 2024-02-28DOI: 10.1038/s41570-024-00590-6
Alexander Rosu-Finsen
Semiconducting polymers require narrow molecular weight distributions for optimal efficiency. Synthesizing such polymers is no easy task, however a combined ultrasonication-assisted Stille polymerization reaction could be the solution to this problem.
{"title":"Pump up the ultrasound","authors":"Alexander Rosu-Finsen","doi":"10.1038/s41570-024-00590-6","DOIUrl":"10.1038/s41570-024-00590-6","url":null,"abstract":"Semiconducting polymers require narrow molecular weight distributions for optimal efficiency. Synthesizing such polymers is no easy task, however a combined ultrasonication-assisted Stille polymerization reaction could be the solution to this problem.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 3","pages":"156-156"},"PeriodicalIF":36.3,"publicationDate":"2024-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139990645","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 : 2024-02-26DOI: 10.1038/s41570-024-00588-0
Stephanie Greed
A metal templating approach can be used to generate homo- and heterointerlocked cage structures.
金属模板法可用于生成同互锁和异互锁笼状结构。
{"title":"Picking an inter-locked cage","authors":"Stephanie Greed","doi":"10.1038/s41570-024-00588-0","DOIUrl":"10.1038/s41570-024-00588-0","url":null,"abstract":"A metal templating approach can be used to generate homo- and heterointerlocked cage structures.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 3","pages":"155-155"},"PeriodicalIF":36.3,"publicationDate":"2024-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139967319","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 : 2024-02-23DOI: 10.1038/s41570-024-00578-2
Nikolaos Dimitratos, Gianvito Vilé, Stefania Albonetti, Fabrizio Cavani, Jhonatan Fiorio, Núria López, Liane M. Rossi, Robert Wojcieszak
Catalytic reactions involving molecular hydrogen are at the heart of many transformations in the chemical industry. Classically, hydrogenations are carried out on Pd, Pt, Ru or Ni catalysts. However, the use of supported Au catalysts has garnered attention in recent years owing to their exceptional selectivity in hydrogenation reactions. This is despite the limited understanding of the physicochemical aspects of hydrogen activation and reaction on Au surfaces. A rational design of new improved catalysts relies on making better use of the hydrogenating properties of Au. This Review analyses the strategies utilized to improve hydrogen–Au interactions, from addressing the importance of the Au particle size to exploring alternative mechanisms for H2 dissociation on Au cations and Au–ligand interfaces. These insights hold the potential to drive future applications of Au catalysis. Gold catalysts have attracted attention for their ability to activate hydrogen towards the hydrogenation of organic molecules. This Review explores strategies to enhance hydrogen–gold interactions to help design new efficient hydrogenation catalysts.
涉及分子氢的催化反应是化学工业中许多转化过程的核心。通常，氢化反应是在 Pd、Pt、Ru 或 Ni 催化剂上进行的。然而，近年来，由于支撑金催化剂在氢化反应中具有优异的选择性，其使用已引起人们的关注。尽管人们对金表面氢气活化和反应的物理化学方面了解有限，但这种催化剂的使用近年来仍备受关注。合理设计新的改良催化剂有赖于更好地利用金的氢化特性。本综述分析了用于改善氢-金相互作用的策略，从解决金颗粒尺寸的重要性到探索氢在金阳离子和金配体界面上解离的替代机制。这些见解有望推动金催化的未来应用。
{"title":"Strategies to improve hydrogen activation on gold catalysts","authors":"Nikolaos Dimitratos, Gianvito Vilé, Stefania Albonetti, Fabrizio Cavani, Jhonatan Fiorio, Núria López, Liane M. Rossi, Robert Wojcieszak","doi":"10.1038/s41570-024-00578-2","DOIUrl":"10.1038/s41570-024-00578-2","url":null,"abstract":"Catalytic reactions involving molecular hydrogen are at the heart of many transformations in the chemical industry. Classically, hydrogenations are carried out on Pd, Pt, Ru or Ni catalysts. However, the use of supported Au catalysts has garnered attention in recent years owing to their exceptional selectivity in hydrogenation reactions. This is despite the limited understanding of the physicochemical aspects of hydrogen activation and reaction on Au surfaces. A rational design of new improved catalysts relies on making better use of the hydrogenating properties of Au. This Review analyses the strategies utilized to improve hydrogen–Au interactions, from addressing the importance of the Au particle size to exploring alternative mechanisms for H2 dissociation on Au cations and Au–ligand interfaces. These insights hold the potential to drive future applications of Au catalysis. Gold catalysts have attracted attention for their ability to activate hydrogen towards the hydrogenation of organic molecules. This Review explores strategies to enhance hydrogen–gold interactions to help design new efficient hydrogenation catalysts.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 3","pages":"195-210"},"PeriodicalIF":36.3,"publicationDate":"2024-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139940300","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 : 2024-02-22DOI: 10.1038/s41570-024-00575-5
Ernest Pastor, Zan Lian, Lu Xia, David Ecija, José Ramón Galán-Mascarós, Sara Barja, Sixto Giménez, Jordi Arbiol, Núria López, F. Pelayo García de Arquer
The functions of electrochemical energy conversion and storage devices rely on the dynamic junction between a solid and a fluid: the electrochemical interface (EI). Many experimental techniques have been developed to probe the EI, but they provide only a partial picture. Building a full mechanistic understanding requires combining multiple probes, either successively or simultaneously. However, such combinations lead to important technical and theoretical challenges. In this Review, we focus on complementary optoelectronic probes and modelling to address the EI across different timescales and spatial scales — including mapping surface reconstruction, reactants and reaction modulators during operation. We discuss how combining these probes can facilitate a predictive design of the EI when closely integrated with theory. Electrochemical devices enable clean energy technologies such as hydrogen cells, batteries and solar fuels. Their design is hindered by incomplete information about the electrochemical interface during operation. Complementary optoelectronic probes offer a path to improved mechanistic insights into such interfaces.
电化学能量转换和存储设备的功能依赖于固体和流体之间的动态交界处：电化学界面（EI）。目前已开发出许多实验技术来探测电化学界面，但这些技术只能提供部分图像。要全面了解机理，需要将多种探针先后或同时结合起来。然而，这种组合会带来重要的技术和理论挑战。在本综述中，我们将重点介绍互补的光电探针和建模，以解决不同时间尺度和空间尺度上的电离层问题--包括绘制运行过程中的表面重构、反应物和反应调制器。我们将讨论如何将这些探针与理论紧密结合，以促进 EI 的预测性设计。
{"title":"Complementary probes for the electrochemical interface","authors":"Ernest Pastor, Zan Lian, Lu Xia, David Ecija, José Ramón Galán-Mascarós, Sara Barja, Sixto Giménez, Jordi Arbiol, Núria López, F. Pelayo García de Arquer","doi":"10.1038/s41570-024-00575-5","DOIUrl":"10.1038/s41570-024-00575-5","url":null,"abstract":"The functions of electrochemical energy conversion and storage devices rely on the dynamic junction between a solid and a fluid: the electrochemical interface (EI). Many experimental techniques have been developed to probe the EI, but they provide only a partial picture. Building a full mechanistic understanding requires combining multiple probes, either successively or simultaneously. However, such combinations lead to important technical and theoretical challenges. In this Review, we focus on complementary optoelectronic probes and modelling to address the EI across different timescales and spatial scales — including mapping surface reconstruction, reactants and reaction modulators during operation. We discuss how combining these probes can facilitate a predictive design of the EI when closely integrated with theory. Electrochemical devices enable clean energy technologies such as hydrogen cells, batteries and solar fuels. Their design is hindered by incomplete information about the electrochemical interface during operation. Complementary optoelectronic probes offer a path to improved mechanistic insights into such interfaces.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 3","pages":"159-178"},"PeriodicalIF":36.3,"publicationDate":"2024-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139924217","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 : 2024-02-22DOI: 10.1038/s41570-024-00579-1
Zhenguang Zhao, Shay Laps, Jacob S. Gichtin, Norman Metanis
The ability to construct a peptide or protein in a spatio-specific manner is of great interest for therapeutic and biochemical research. However, the various functional groups present in peptide sequences and the need to perform chemistry under mild and aqueous conditions make selective protein functionalization one of the greatest synthetic challenges. The fascinating paradox of selenium (Se) — being found in both toxic compounds and also harnessed by nature for essential biochemical processes — has inspired the recent exploration of selenium chemistry for site-selective functionalization of peptides and proteins. In this Review, we discuss such approaches, including metal-free and metal-catalysed transformations, as well as traceless chemical modifications. We report their advantages, limitations and applications, as well as future research avenues. The unique properties of selenium have been exploited in protein science. This Review highlights the recent applications of selenium chemistry in protein chemical synthesis, modification, folding, stabilization, the preparation of therapeutic proteins and more.
{"title":"Selenium chemistry for spatio-selective peptide and protein functionalization","authors":"Zhenguang Zhao, Shay Laps, Jacob S. Gichtin, Norman Metanis","doi":"10.1038/s41570-024-00579-1","DOIUrl":"10.1038/s41570-024-00579-1","url":null,"abstract":"The ability to construct a peptide or protein in a spatio-specific manner is of great interest for therapeutic and biochemical research. However, the various functional groups present in peptide sequences and the need to perform chemistry under mild and aqueous conditions make selective protein functionalization one of the greatest synthetic challenges. The fascinating paradox of selenium (Se) — being found in both toxic compounds and also harnessed by nature for essential biochemical processes — has inspired the recent exploration of selenium chemistry for site-selective functionalization of peptides and proteins. In this Review, we discuss such approaches, including metal-free and metal-catalysed transformations, as well as traceless chemical modifications. We report their advantages, limitations and applications, as well as future research avenues. The unique properties of selenium have been exploited in protein science. This Review highlights the recent applications of selenium chemistry in protein chemical synthesis, modification, folding, stabilization, the preparation of therapeutic proteins and more.","PeriodicalId":18849,"journal":{"name":"Nature reviews. Chemistry","volume":"8 3","pages":"211-229"},"PeriodicalIF":36.3,"publicationDate":"2024-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139932059","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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