MacromoleculesPub Date : 2024-08-29DOI: 10.1021/acs.chemrev.3c0093810.1021/acs.chemrev.3c00938
Wei Niu*, and , Jiantao Guo*,
{"title":"Cellular Site-Specific Incorporation of Noncanonical Amino Acids in Synthetic Biology","authors":"Wei Niu*, and , Jiantao Guo*, ","doi":"10.1021/acs.chemrev.3c0093810.1021/acs.chemrev.3c00938","DOIUrl":"https://doi.org/10.1021/acs.chemrev.3c00938https://doi.org/10.1021/acs.chemrev.3c00938","url":null,"abstract":"<p >Over the past two decades, genetic code expansion (GCE)-enabled methods for incorporating noncanonical amino acids (ncAAs) into proteins have significantly advanced the field of synthetic biology while also reaping substantial benefits from it. On one hand, they provide synthetic biologists with a powerful toolkit to enhance and diversify biological designs beyond natural constraints. Conversely, synthetic biology has not only propelled the development of ncAA incorporation through sophisticated tools and innovative strategies but also broadened its potential applications across various fields. This Review delves into the methodological advancements and primary applications of site-specific cellular incorporation of ncAAs in synthetic biology. The topics encompass expanding the genetic code through noncanonical codon addition, creating semiautonomous and autonomous organisms, designing regulatory elements, and manipulating and extending peptide natural product biosynthetic pathways. The Review concludes by examining the ongoing challenges and future prospects of GCE-enabled ncAA incorporation in synthetic biology and highlighting opportunities for further advancements in this rapidly evolving field.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"124 18","pages":"10577–10617 10577–10617"},"PeriodicalIF":51.4,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142318192","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}
MacromoleculesPub Date : 2024-08-29DOI: 10.1021/acs.chemrev.4c00073
Peng Chen, Yun Xiao, Shunde Li, Xiaohan Jia, Deying Luo, Wei Zhang, Henry J. Snaith, Qihuang Gong, Rui Zhu
{"title":"The Promise and Challenges of Inverted Perovskite Solar Cells","authors":"Peng Chen, Yun Xiao, Shunde Li, Xiaohan Jia, Deying Luo, Wei Zhang, Henry J. Snaith, Qihuang Gong, Rui Zhu","doi":"10.1021/acs.chemrev.4c00073","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00073","url":null,"abstract":"Recently, there has been an extensive focus on inverted perovskite solar cells (PSCs) with a p-i-n architecture due to their attractive advantages, such as exceptional stability, high efficiency, low cost, low-temperature processing, and compatibility with tandem architectures, leading to a surge in their development. Single-junction and perovskite-silicon tandem solar cells (TSCs) with an inverted architecture have achieved certified PCEs of 26.15% and 33.9% respectively, showing great promise for commercial applications. To expedite real-world applications, it is crucial to investigate the key challenges for further performance enhancement. We first introduce representative methods, such as composition engineering, additive engineering, solvent engineering, processing engineering, innovation of charge transporting layers, and interface engineering, for fabricating high-efficiency and stable inverted PSCs. We then delve into the reasons behind the excellent stability of inverted PSCs. Subsequently, we review recent advances in TSCs with inverted PSCs, including perovskite-Si TSCs, all-perovskite TSCs, and perovskite-organic TSCs. To achieve final commercial deployment, we present efforts related to scaling up, harvesting indoor light, economic assessment, and reducing environmental impacts. Lastly, we discuss the potential and challenges of inverted PSCs in the future.","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"39 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142090483","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}
MacromoleculesPub Date : 2024-08-29DOI: 10.1021/acs.chemrev.4c00306
Daniel T. Infield, Miranda E. Schene, Jason D. Galpin, Christopher A. Ahern
{"title":"Genetic Code Expansion for Mechanistic Studies in Ion Channels: An (Un)natural Union of Chemistry and Biology","authors":"Daniel T. Infield, Miranda E. Schene, Jason D. Galpin, Christopher A. Ahern","doi":"10.1021/acs.chemrev.4c00306","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00306","url":null,"abstract":"Ion channels play central roles in biology and human health by catalyzing the transmembrane flow of electrical charge. These proteins are ideal targets for genetic code expansion (GCE) methods because it is feasible to measure ion channel activity from miniscule amounts of protein and to analyze the resulting data via rigorous, established biophysical methods. In an ideal scenario, the encoding of synthetic, noncanonical amino acids via GCE allows the experimenter to ask questions inaccessible to traditional methods. For this reason, GCE has been successfully applied to a variety of ligand- and voltage-gated channels wherein extensive structural, functional, and pharmacological data exist. Here, we provide a comprehensive summary of GCE as applied to ion channels. We begin with an overview of the methods used to encode noncanonical amino acids in channels and then describe mechanistic studies wherein GCE was used for photochemistry (cross-linking; caged amino acids) and atomic mutagenesis (isosteric manipulation of charge and aromaticity; backbone mutation). Lastly, we cover recent advances in the encoding of fluorescent amino acids for the real-time study of protein conformational dynamics.","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"14 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142101801","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}
MacromoleculesPub Date : 2024-08-29DOI: 10.1021/acs.chemrev.3c00938
Wei Niu, Jiantao Guo
{"title":"Cellular Site-Specific Incorporation of Noncanonical Amino Acids in Synthetic Biology","authors":"Wei Niu, Jiantao Guo","doi":"10.1021/acs.chemrev.3c00938","DOIUrl":"https://doi.org/10.1021/acs.chemrev.3c00938","url":null,"abstract":"Over the past two decades, genetic code expansion (GCE)-enabled methods for incorporating noncanonical amino acids (ncAAs) into proteins have significantly advanced the field of synthetic biology while also reaping substantial benefits from it. On one hand, they provide synthetic biologists with a powerful toolkit to enhance and diversify biological designs beyond natural constraints. Conversely, synthetic biology has not only propelled the development of ncAA incorporation through sophisticated tools and innovative strategies but also broadened its potential applications across various fields. This Review delves into the methodological advancements and primary applications of site-specific cellular incorporation of ncAAs in synthetic biology. The topics encompass expanding the genetic code through noncanonical codon addition, creating semiautonomous and autonomous organisms, designing regulatory elements, and manipulating and extending peptide natural product biosynthetic pathways. The Review concludes by examining the ongoing challenges and future prospects of GCE-enabled ncAA incorporation in synthetic biology and highlighting opportunities for further advancements in this rapidly evolving field.","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"130 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142090482","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}
MacromoleculesPub Date : 2024-08-29DOI: 10.1021/acs.chemrev.4c0030610.1021/acs.chemrev.4c00306
Daniel T. Infield, Miranda E. Schene, Jason D. Galpin and Christopher A. Ahern*,
{"title":"Genetic Code Expansion for Mechanistic Studies in Ion Channels: An (Un)natural Union of Chemistry and Biology","authors":"Daniel T. Infield, Miranda E. Schene, Jason D. Galpin and Christopher A. Ahern*, ","doi":"10.1021/acs.chemrev.4c0030610.1021/acs.chemrev.4c00306","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00306https://doi.org/10.1021/acs.chemrev.4c00306","url":null,"abstract":"<p >Ion channels play central roles in biology and human health by catalyzing the transmembrane flow of electrical charge. These proteins are ideal targets for genetic code expansion (GCE) methods because it is feasible to measure ion channel activity from miniscule amounts of protein and to analyze the resulting data via rigorous, established biophysical methods. In an ideal scenario, the encoding of synthetic, noncanonical amino acids via GCE allows the experimenter to ask questions inaccessible to traditional methods. For this reason, GCE has been successfully applied to a variety of ligand- and voltage-gated channels wherein extensive structural, functional, and pharmacological data exist. Here, we provide a comprehensive summary of GCE as applied to ion channels. We begin with an overview of the methods used to encode noncanonical amino acids in channels and then describe mechanistic studies wherein GCE was used for photochemistry (cross-linking; caged amino acids) and atomic mutagenesis (isosteric manipulation of charge and aromaticity; backbone mutation). Lastly, we cover recent advances in the encoding of fluorescent amino acids for the real-time study of protein conformational dynamics.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"124 20","pages":"11523–11543 11523–11543"},"PeriodicalIF":51.4,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemrev.4c00306","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550647","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}
MacromoleculesPub Date : 2024-08-28Epub Date: 2024-07-23DOI: 10.1021/acs.chemrev.3c00937
Soumyabrata Roy, Antony Joseph, Xiang Zhang, Sohini Bhattacharyya, Anand B Puthirath, Abhijit Biswas, Chandra Sekhar Tiwary, Robert Vajtai, Pulickel M Ajayan
{"title":"Engineered Two-Dimensional Transition Metal Dichalcogenides for Energy Conversion and Storage.","authors":"Soumyabrata Roy, Antony Joseph, Xiang Zhang, Sohini Bhattacharyya, Anand B Puthirath, Abhijit Biswas, Chandra Sekhar Tiwary, Robert Vajtai, Pulickel M Ajayan","doi":"10.1021/acs.chemrev.3c00937","DOIUrl":"10.1021/acs.chemrev.3c00937","url":null,"abstract":"<p><p>Designing efficient and cost-effective materials is pivotal to solving the key scientific and technological challenges at the interface of energy, environment, and sustainability for achieving NetZero. Two-dimensional transition metal dichalcogenides (2D TMDs) represent a unique class of materials that have catered to a myriad of energy conversion and storage (ECS) applications. Their uniqueness arises from their ultra-thin nature, high fractions of atoms residing on surfaces, rich chemical compositions featuring diverse metals and chalcogens, and remarkable tunability across multiple length scales. Specifically, the rich electronic/electrical, optical, and thermal properties of 2D TMDs have been widely exploited for electrochemical energy conversion (e.g., electrocatalytic water splitting), and storage (e.g., anodes in alkali ion batteries and supercapacitors), photocatalysis, photovoltaic devices, and thermoelectric applications. Furthermore, their properties and performances can be greatly boosted by judicious structural and chemical tuning through phase, size, composition, defect, dopant, topological, and heterostructure engineering. The challenge, however, is to design and control such engineering levers, optimally and specifically, to maximize performance outcomes for targeted applications. In this review we discuss, highlight, and provide insights on the significant advancements and ongoing research directions in the design and engineering approaches of 2D TMDs for improving their performance and potential in ECS applications.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":" ","pages":"9376-9456"},"PeriodicalIF":51.4,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141746682","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}
MacromoleculesPub Date : 2024-08-28DOI: 10.1021/acs.chemrev.4c00049
Xuemei Fu, Wen Cheng, Guanxiang Wan, Zijie Yang, Benjamin C. K. Tee
{"title":"Toward an AI Era: Advances in Electronic Skins","authors":"Xuemei Fu, Wen Cheng, Guanxiang Wan, Zijie Yang, Benjamin C. K. Tee","doi":"10.1021/acs.chemrev.4c00049","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00049","url":null,"abstract":"Electronic skins (e-skins) have seen intense research and rapid development in the past two decades. To mimic the capabilities of human skin, a multitude of flexible/stretchable sensors that detect physiological and environmental signals have been designed and integrated into functional systems. Recently, researchers have increasingly deployed machine learning and other artificial intelligence (AI) technologies to mimic the human neural system for the processing and analysis of sensory data collected by e-skins. Integrating AI has the potential to enable advanced applications in robotics, healthcare, and human–machine interfaces but also presents challenges such as data diversity and AI model robustness. In this review, we first summarize the functions and features of e-skins, followed by feature extraction of sensory data and different AI models. Next, we discuss the utilization of AI in the design of e-skin sensors and address the key topic of AI implementation in data processing and analysis of e-skins to accomplish a range of different tasks. Subsequently, we explore hardware-layer in-skin intelligence before concluding with an analysis of the challenges and opportunities in the various aspects of AI-enabled e-skins.","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"57 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142090484","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}
MacromoleculesPub Date : 2024-08-28DOI: 10.1021/acs.chemrev.4c0004910.1021/acs.chemrev.4c00049
Xuemei Fu, Wen Cheng, Guanxiang Wan, Zijie Yang and Benjamin C. K. Tee*,
{"title":"Toward an AI Era: Advances in Electronic Skins","authors":"Xuemei Fu, Wen Cheng, Guanxiang Wan, Zijie Yang and Benjamin C. K. Tee*, ","doi":"10.1021/acs.chemrev.4c0004910.1021/acs.chemrev.4c00049","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00049https://doi.org/10.1021/acs.chemrev.4c00049","url":null,"abstract":"<p >Electronic skins (e-skins) have seen intense research and rapid development in the past two decades. To mimic the capabilities of human skin, a multitude of flexible/stretchable sensors that detect physiological and environmental signals have been designed and integrated into functional systems. Recently, researchers have increasingly deployed machine learning and other artificial intelligence (AI) technologies to mimic the human neural system for the processing and analysis of sensory data collected by e-skins. Integrating AI has the potential to enable advanced applications in robotics, healthcare, and human–machine interfaces but also presents challenges such as data diversity and AI model robustness. In this review, we first summarize the functions and features of e-skins, followed by feature extraction of sensory data and different AI models. Next, we discuss the utilization of AI in the design of e-skin sensors and address the key topic of AI implementation in data processing and analysis of e-skins to accomplish a range of different tasks. Subsequently, we explore hardware-layer in-skin intelligence before concluding with an analysis of the challenges and opportunities in the various aspects of AI-enabled e-skins.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"124 17","pages":"9899–9948 9899–9948"},"PeriodicalIF":51.4,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161456","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}
MacromoleculesPub Date : 2024-08-28Epub Date: 2024-08-13DOI: 10.1021/acs.chemrev.3c00892
Maidileyvis C Cabello, Gen Chen, Michael J Melville, Rokia Osman, G Dinesh Kumar, Dylan W Domaille, Alexander R Lippert
{"title":"Ex Tenebris Lux: Illuminating Reactive Oxygen and Nitrogen Species with Small Molecule Probes.","authors":"Maidileyvis C Cabello, Gen Chen, Michael J Melville, Rokia Osman, G Dinesh Kumar, Dylan W Domaille, Alexander R Lippert","doi":"10.1021/acs.chemrev.3c00892","DOIUrl":"10.1021/acs.chemrev.3c00892","url":null,"abstract":"<p><p>Reactive oxygen and nitrogen species are small reactive molecules derived from elements in the air─oxygen and nitrogen. They are produced in biological systems to mediate fundamental aspects of cellular signaling but must be very tightly balanced to prevent indiscriminate damage to biological molecules. Small molecule probes can transmute the specific nature of each reactive oxygen and nitrogen species into an observable luminescent signal (or even an acoustic wave) to offer sensitive and selective imaging in living cells and whole animals. This review focuses specifically on small molecule probes for superoxide, hydrogen peroxide, hypochlorite, nitric oxide, and peroxynitrite that provide a luminescent or photoacoustic signal. Important background information on general photophysical phenomena, common probe designs, mechanisms, and imaging modalities will be provided, and then, probes for each analyte will be thoroughly evaluated. A discussion of the successes of the field will be presented, followed by recommendations for improvement and a future outlook of emerging trends. Our objectives are to provide an informative, useful, and thorough field guide to small molecule probes for reactive oxygen and nitrogen species as well as important context to compare the ecosystem of chemistries and molecular scaffolds that has manifested within the field.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":" ","pages":"9225-9375"},"PeriodicalIF":51.4,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141974416","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}
MacromoleculesPub Date : 2024-08-28Epub Date: 2024-07-22DOI: 10.1021/acs.chemrev.4c00071
Yifan Yuan, Ranjan Kumar Patel, Suvo Banik, Tadesse Billo Reta, Ravindra Singh Bisht, Dillon D Fong, Subramanian K R S Sankaranarayanan, Shriram Ramanathan
{"title":"Proton Conducting Neuromorphic Materials and Devices.","authors":"Yifan Yuan, Ranjan Kumar Patel, Suvo Banik, Tadesse Billo Reta, Ravindra Singh Bisht, Dillon D Fong, Subramanian K R S Sankaranarayanan, Shriram Ramanathan","doi":"10.1021/acs.chemrev.4c00071","DOIUrl":"10.1021/acs.chemrev.4c00071","url":null,"abstract":"<p><p>Neuromorphic computing and artificial intelligence hardware generally aims to emulate features found in biological neural circuit components and to enable the development of energy-efficient machines. In the biological brain, ionic currents and temporal concentration gradients control information flow and storage. It is therefore of interest to examine materials and devices for neuromorphic computing wherein ionic and electronic currents can propagate. Protons being mobile under an external electric field offers a compelling avenue for facilitating biological functionalities in artificial synapses and neurons. In this review, we first highlight the interesting biological analog of protons as neurotransmitters in various animals. We then discuss the experimental approaches and mechanisms of proton doping in various classes of inorganic and organic proton-conducting materials for the advancement of neuromorphic architectures. Since hydrogen is among the lightest of elements, characterization in a solid matrix requires advanced techniques. We review powerful synchrotron-based spectroscopic techniques for characterizing hydrogen doping in various materials as well as complementary scattering techniques to detect hydrogen. First-principles calculations are then discussed as they help provide an understanding of proton migration and electronic structure modification. Outstanding scientific challenges to further our understanding of proton doping and its use in emerging neuromorphic electronics are pointed out.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":" ","pages":"9733-9784"},"PeriodicalIF":51.4,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141746683","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}