{"title":"SERS microscopy as a tool for comprehensive biochemical characterization in complex samples.","authors":"Janina Kneipp, Stephan Seifert, Florian Gärber","doi":"10.1039/d4cs00460d","DOIUrl":"https://doi.org/10.1039/d4cs00460d","url":null,"abstract":"<p><p>Surface enhanced Raman scattering (SERS) spectra of biomaterials such as cells or tissues can be used to obtain biochemical information from nanoscopic volumes in these heterogeneous samples. This tutorial review discusses the factors that determine the outcome of a SERS experiment in complex bioorganic samples. They are related to the SERS process itself, the possibility to selectively probe certain regions or constituents of a sample, and the retrieval of the vibrational information in order to identify molecules and their interaction. After introducing basic aspects of SERS experiments in the context of biocompatible environments, spectroscopy in typical microscopic settings is exemplified, including the possibilities to combine SERS with other linear and non-linear microscopic tools, and to exploit approaches that improve lateral and temporal resolution. In particular the great variation of data in a SERS experiment calls for robust data analysis tools. Approaches will be introduced that have been originally developed in the field of bioinformatics for the application to omics data and that show specific potential in the analysis of SERS data. They include the use of simulated data and machine learning tools that can yield chemical information beyond achieving spectral classification.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":40.4,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453769","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}
Saudagar Dongare, Muhammad Zeeshan, Ahmet Safa Aydogdu, Ruth Dikki, Samira F Kurtoğlu-Öztulum, Oguz Kagan Coskun, Miguel Muñoz, Avishek Banerjee, Manu Gautam, R Dominic Ross, Jared S Stanley, Rowan S Brower, Baleeswaraiah Muchharla, Robert L Sacci, Jesús M Velázquez, Bijandra Kumar, Jenny Y Yang, Christopher Hahn, Seda Keskin, Carlos G Morales-Guio, Alper Uzun, Joshua M Spurgeon, Burcu Gurkan
{"title":"Reactive capture and electrochemical conversion of CO<sub>2</sub> with ionic liquids and deep eutectic solvents.","authors":"Saudagar Dongare, Muhammad Zeeshan, Ahmet Safa Aydogdu, Ruth Dikki, Samira F Kurtoğlu-Öztulum, Oguz Kagan Coskun, Miguel Muñoz, Avishek Banerjee, Manu Gautam, R Dominic Ross, Jared S Stanley, Rowan S Brower, Baleeswaraiah Muchharla, Robert L Sacci, Jesús M Velázquez, Bijandra Kumar, Jenny Y Yang, Christopher Hahn, Seda Keskin, Carlos G Morales-Guio, Alper Uzun, Joshua M Spurgeon, Burcu Gurkan","doi":"10.1039/d4cs00390j","DOIUrl":"https://doi.org/10.1039/d4cs00390j","url":null,"abstract":"<p><p>Ionic liquids (ILs) and deep eutectic solvents (DESs) have tremendous potential for reactive capture and conversion (RCC) of CO<sub>2</sub> due to their wide electrochemical stability window, low volatility, and high CO<sub>2</sub> solubility. There is environmental and economic interest in the direct utilization of the captured CO<sub>2</sub> using electrified and modular processes that forgo the thermal- or pressure-swing regeneration steps to concentrate CO<sub>2</sub>, eliminating the need to compress, transport, or store the gas. The conventional electrochemical conversion of CO<sub>2</sub> with aqueous electrolytes presents limited CO<sub>2</sub> solubility and high energy requirement to achieve industrially relevant products. Additionally, aqueous systems have competitive hydrogen evolution. In the past decade, there has been significant progress toward the design of ILs and DESs, and their composites to separate CO<sub>2</sub> from dilute streams. In parallel, but not necessarily in synergy, there have been studies focused on a few select ILs and DESs for electrochemical reduction of CO<sub>2</sub>, often diluting them with aqueous or non-aqueous solvents. The resulting electrode-electrolyte interfaces present a complex speciation for RCC. In this review, we describe how the ILs and DESs are tuned for RCC and specifically address the CO<sub>2</sub> chemisorption and electroreduction mechanisms. Critical bulk and interfacial properties of ILs and DESs are discussed in the context of RCC, and the potential of these electrolytes are presented through a techno-economic evaluation.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":40.4,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141441815","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}
Silin Xu, Kai-Cheng Yan, Zhi-Hong Xu, Yuan Wang, Tony D James
{"title":"Fluorescent probes for targeting the Golgi apparatus: design strategies and applications.","authors":"Silin Xu, Kai-Cheng Yan, Zhi-Hong Xu, Yuan Wang, Tony D James","doi":"10.1039/d3cs00171g","DOIUrl":"https://doi.org/10.1039/d3cs00171g","url":null,"abstract":"<p><p>The Golgi apparatus is an essential organelle constructed by the stacking of flattened vesicles, that is widely distributed in eukaryotic cells and is dynamically regulated during cell cycles. It is a central station which is responsible for collecting, processing, sorting, transporting, and secreting some important proteins/enzymes from the endoplasmic reticulum to intra- and extra-cellular destinations. Golgi-specific fluorescent probes provide powerful non-invasive tools for the real-time and <i>in situ</i> visualization of the temporal and spatial fluctuations of bioactive species. Over recent years, more and more Golgi-targeting probes have been developed, which are essential for the evaluation of diseases including cancer. However, when compared with systems that target other important organelles (<i>e.g.</i> lysosomes and mitochondria), Golgi-targeting strategies are still in their infancy, therefore it is important to develop more Golgi-targeting probes. This review systematically summarizes the currently reported Golgi-specific fluorescent probes, and highlights the design strategies, mechanisms, and biological uses of these probes, we have structured the review based on the different targeting groups. In addition, we highlight the future challenges and opportunities in the development of Golgi-specific imaging agents and therapeutic systems.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":40.4,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141430958","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":"Metal-catalyzed Markovnikov-type selective hydrofunctionalization of terminal alkynes.","authors":"Jieping Chen, Wen-Ting Wei, Zhuocheng Li, Zhan Lu","doi":"10.1039/d4cs00167b","DOIUrl":"https://doi.org/10.1039/d4cs00167b","url":null,"abstract":"<p><p>Metal-catalyzed highly Markovnikov-type selective hydrofunctionalization of terminal alkynes provides a straightforward and atom-economical route to access 1,1-disubstituted alkenes, which have a wide range of applications in organic synthesis. However, the highly Markovnikov-type selective transformations are challenging due to the electronic and steric effects during the addition process. With the development of metal-catalyzed organic synthesis, different metal catalysts have been developed to solve this challenge, especially for platinum group metal catalysts. In this perspective, we review homogeneous metal-catalyzed Markovnikov-type selective hydrofunctionalization of terminal alkynes according to the classified element types as well as reaction mechanisms. Future avenues for investigation are also presented to help expand this exciting field.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":40.4,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141430959","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":"Recent advances in zinc-ion dehydration strategies for optimized Zn-metal batteries.","authors":"Haoyu Li, Sijie Li, Ruilin Hou, Yuan Rao, Shaohua Guo, Zhi Chang, Haoshen Zhou","doi":"10.1039/d4cs00343h","DOIUrl":"https://doi.org/10.1039/d4cs00343h","url":null,"abstract":"<p><p>Aqueous Zn-metal batteries have attracted increasing interest for large-scale energy storage owing to their outstanding merits in terms of safety, cost and production. However, they constantly suffer from inadequate energy density and poor cycling stability due to the presence of zinc ions in the fully hydrated solvation state. Thus, designing the dehydrated solvation structure of zinc ions can effectively address the current drawbacks of aqueous Zn-metal batteries. In this case, considering the lack of studies focused on strategies for the dehydration of zinc ions, herein, we present a systematic and comprehensive review to deepen the understanding of zinc-ion solvation regulation. Two fundamental design principles of component regulation and pre-desolvation are summarized in terms of solvation environment formation and interfacial desolvation behavior. Subsequently, specific strategy based distinct principles are carefully discussed, including preparation methods, working mechanisms, analysis approaches and performance improvements. Finally, we present a general summary of the issues addressed using zinc-ion dehydration strategies, and four critical aspects to promote zinc-ion solvation regulation are presented as an outlook, involving updating (de)solvation theories, revealing interfacial evolution, enhancing analysis techniques and developing functional materials. We believe that this review will not only stimulate more creativity in optimizing aqueous electrolytes but also provide valuable insights into designing other battery systems.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":40.4,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141430960","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":"Renewable biomass-based aerogels: from structural design to functional regulation.","authors":"Linfeng Chen, Xiaoxiao Yu, Mengyue Gao, Chengjian Xu, Junyan Zhang, Xinhai Zhang, Meifang Zhu, Yanhua Cheng","doi":"10.1039/d3cs01014g","DOIUrl":"https://doi.org/10.1039/d3cs01014g","url":null,"abstract":"<p><p>Global population growth and industrialization have exacerbated the nonrenewable energy crises and environmental issues, thereby stimulating an enormous demand for producing environmentally friendly materials. Typically, biomass-based aerogels (BAs), which are mainly composed of biomass materials, show great application prospects in various fields because of their exceptional properties such as biocompatibility, degradability, and renewability. To improve the performance of BAs to meet the usage requirements of different scenarios, a large number of innovative works in the past few decades have emphasized the importance of micro-structural design in regulating macroscopic functions. Inspired by the ubiquitous random or regularly arranged structures of materials in nature ranging from micro to meso and macro scales, constructing different microstructures often corresponds to completely different functions even with similar biomolecular compositions. This review focuses on the preparation process, design concepts, regulation methods, and the synergistic combination of chemical compositions and microstructures of BAs with different porous structures from the perspective of gel skeleton and pore structure. It not only comprehensively introduces the effect of various microstructures on the physical properties of BAs, but also analyzes their potential applications in the corresponding fields of thermal management, water treatment, atmospheric water harvesting, CO<sub>2</sub> absorption, energy storage and conversion, electromagnetic interference (EMI) shielding, biological applications, <i>etc.</i> Finally, we provide our perspectives regarding the challenges and future opportunities of BAs. Overall, our goal is to provide researchers with a thorough understanding of the relationship between the microstructures and properties of BAs, supported by a comprehensive analysis of the available data.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":46.2,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416704","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":"The development of catalysts and auxiliaries for the synthesis of covalent organic frameworks.","authors":"Wei Zhao, Qiang Zhu, Xiaofeng Wu, Dan Zhao","doi":"10.1039/d3cs00908d","DOIUrl":"https://doi.org/10.1039/d3cs00908d","url":null,"abstract":"<p><p>Covalent organic frameworks (COFs) have recently seen significant advancements. Large quantities of structurally & functionally oriented COFs with a wide range of applications, such as gas adsorption, catalysis, separation, and drug delivery, have been explored. Recent achievements in this field are primarily focused on advancing synthetic methodologies, with catalysts playing a crucial role in achieving highly crystalline COF materials, particularly those featuring novel linkages and chemistry. A series of reviews have already been published over the last decade, covering the fundamentals, synthesis, and applications of COFs. However, despite the pivotal role that catalysts and auxiliaries play in forming COF materials and adjusting their properties (<i>e.g.</i>, crystallinity, porosity, stability, and morphology), limited attention has been devoted to these essential components. In this Critical Review, we mainly focus on the state-of-the-art progress of catalysts and auxiliaries applied to the synthesis of COFs. The catalysts include four categories: acid catalysts, base catalysts, transition-metal catalysts, and other catalysts. The auxiliaries, such as modulators, oxygen, and surfactants, are discussed as well. This is then followed by the description of several specific applications derived from the utilization of catalysts and auxiliaries. Lastly, a perspective on the major challenges and opportunities associated with catalysts and auxiliaries is provided.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":46.2,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416639","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":"Chemistries and materials for atmospheric water harvesting.","authors":"Chuxin Lei, Weixin Guan, Yaxuan Zhao, Guihua Yu","doi":"10.1039/d4cs00423j","DOIUrl":"https://doi.org/10.1039/d4cs00423j","url":null,"abstract":"<p><p>Atmospheric water harvesting (AWH) is recognized as a crucial strategy to address the global challenge of water scarcity by tapping into the vast reserves of atmospheric moisture for potable water supply. Within this domain, sorbents lie in the core of AWH technologies as they possess broad adaptability across a wide spectrum of humidity levels, underpinned by the cyclic sorption and desorption processes of sorbents, necessitating a multi-scale viewpoint regarding the rational material and chemical selection and design. This Invited Review delves into the essential sorption mechanisms observed across various classes of sorbent systems, emphasizing the water-sorbent interactions and the progression of water networks. A special focus is placed on the insights derived from isotherm profiles, which elucidate sorbent structures and sorption dynamics. From these foundational principles, we derive material and chemical design guidelines and identify key tuning factors from a structural-functional perspective across multiple material systems, addressing their fundamental chemistries and unique attributes. The review further navigates through system-level design considerations to optimize water production efficiency. This review aims to equip researchers in the field of AWH with a thorough understanding of the water-sorbent interactions, material design principles, and system-level considerations essential for advancing this technology.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":46.2,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416703","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}
Xiaowen Sun, Rafael B Araujo, Egon Campos Dos Santos, Yuanhua Sang, Hong Liu, Xiaowen Yu
{"title":"Advancing electrocatalytic reactions through mapping key intermediates to active sites <i>via</i> descriptors.","authors":"Xiaowen Sun, Rafael B Araujo, Egon Campos Dos Santos, Yuanhua Sang, Hong Liu, Xiaowen Yu","doi":"10.1039/d3cs01130e","DOIUrl":"https://doi.org/10.1039/d3cs01130e","url":null,"abstract":"<p><p>Descriptors play a crucial role in electrocatalysis as they can provide valuable insights into the electrochemical performance of energy conversion and storage processes. They allow for the understanding of different catalytic activities and enable the prediction of better catalysts without relying on the time-consuming trial-and-error approaches. Hence, this comprehensive review focuses on highlighting the significant advancements in commonly used descriptors for critical electrocatalytic reactions. First, the fundamental reaction processes and key intermediates involved in several electrocatalytic reactions are summarized. Subsequently, three types of descriptors are classified and introduced based on different reactions and catalysts. These include d-band center descriptors, readily accessible intrinsic property descriptors, and spin-related descriptors, all of which contribute to a profound understanding of catalytic behavior. Furthermore, multi-type descriptors that collectively determine the catalytic performance are also summarized. Finally, we discuss the future of descriptors, envisioning their potential to integrate multiple factors, broaden application scopes, and synergize with artificial intelligence for more efficient catalyst design and discovery.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":46.2,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416702","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}
Junzhi Ye, Deepika Gaur, Chenjia Mi, Zijian Chen, Iago López Fernández, Haitao Zhao, Yitong Dong, Lakshminarayana Polavarapu, Robert L Z Hoye
{"title":"Strongly-confined colloidal lead-halide perovskite quantum dots: from synthesis to applications.","authors":"Junzhi Ye, Deepika Gaur, Chenjia Mi, Zijian Chen, Iago López Fernández, Haitao Zhao, Yitong Dong, Lakshminarayana Polavarapu, Robert L Z Hoye","doi":"10.1039/d4cs00077c","DOIUrl":"https://doi.org/10.1039/d4cs00077c","url":null,"abstract":"<p><p>Colloidal semiconductor nanocrystals enable the realization and exploitation of quantum phenomena in a controlled manner, and can be scaled up for commercial uses. These materials have become important for a wide range of applications, from ultrahigh definition displays, to solar cells, quantum computing, bioimaging, optical communications, and many more. Over the last decade, lead-halide perovskite nanocrystals have rapidly gained prominence as efficient semiconductors. Although the majority of studies have focused on large nanocrystals in the weak- to intermediate-confinement regime, quantum dots (QDs) in the strongly-confined regime (with sizes smaller than the Bohr diameter, which ranges from 4-12 nm for lead-halide perovskites) offer unique opportunities, including polarized light emission and color-pure, stable luminescence in the region that is unattainable by perovskites with single-halide compositions. In this tutorial review, we bring together the latest insights into this emerging and rapidly growing area, focusing on the synthesis, steady-state optical properties (including exciton fine-structure splitting), and transient kinetics (including hot carrier cooling) of strongly-confined perovskite QDs. We also discuss recent advances in their applications, including single photon emission for quantum technologies, as well as light-emitting diodes. We finish with our perspectives on future challenges and opportunities for strongly-confined QDs, particularly around improving the control over monodispersity and stability, important fundamental questions on the photophysics, and paths forward to improve the performance of perovskite QDs in light-emitting diodes.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":null,"pages":null},"PeriodicalIF":46.2,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416705","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}