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Annual review of physical chemistry最新文献

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Cascaded Biocatalysis and Bioelectrocatalysis: Overview and Recent Advances. 级联生物催化和生物电催化:综述和最新进展。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-01-27 DOI: 10.1146/annurev-physchem-090519-050109
Yoo Seok Lee, Koun Lim, Shelley D Minteer
{"title":"Cascaded Biocatalysis and Bioelectrocatalysis: Overview and Recent Advances.","authors":"Yoo Seok Lee,&nbsp;Koun Lim,&nbsp;Shelley D Minteer","doi":"10.1146/annurev-physchem-090519-050109","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090519-050109","url":null,"abstract":"<p><p>Enzyme cascades are plentiful in nature, but they also have potential in artificial applications due to the possibility of using the target substrate in biofuel cells, electrosynthesis, and biosensors. Cascade reactions from enzymes or hybrid bioorganic catalyst systems exhibit extended substrate range, reaction depth, and increased overall performance. This review addresses the strategies of cascade biocatalysis and bioelectrocatalysis for (<i>a</i>) CO<sub>2</sub> fixation, (<i>b</i>) high value-added product formation, (<i>c</i>) sustainable energy sources via deep oxidation, and (<i>d</i>) cascaded electrochemical enzymatic biosensors. These recent updates in the field provide fundamental concepts, designs of artificial electrocatalytic oxidation-reduction pathways (using a flexible setup involving organic catalysts and engineered enzymes), and advances in hybrid cascaded sensors for sensitive analyte detection.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38872099","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}
引用次数: 16
Vibronic and Environmental Effects in Simulations of Optical Spectroscopy. 光谱学模拟中的振动和环境效应。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-01-04 DOI: 10.1146/annurev-physchem-090419-051350
Tim J Zuehlsdorff, Sapana V Shedge, Shao-Yu Lu, Hanbo Hong, Vincent P Aguirre, Liang Shi, Christine M Isborn
{"title":"Vibronic and Environmental Effects in Simulations of Optical Spectroscopy.","authors":"Tim J Zuehlsdorff,&nbsp;Sapana V Shedge,&nbsp;Shao-Yu Lu,&nbsp;Hanbo Hong,&nbsp;Vincent P Aguirre,&nbsp;Liang Shi,&nbsp;Christine M Isborn","doi":"10.1146/annurev-physchem-090419-051350","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090419-051350","url":null,"abstract":"<p><p>Including both environmental and vibronic effects is important for accurate simulation of optical spectra, but combining these effects remains computationally challenging. We outline two approaches that consider both the explicit atomistic environment and the vibronic transitions. Both phenomena are responsible for spectral shapes in linear spectroscopy and the electronic evolution measured in nonlinear spectroscopy. The first approach utilizes snapshots of chromophore-environment configurations for which chromophore normal modes are determined. We outline various approximations for this static approach that assumes harmonic potentials and ignores dynamic system-environment coupling. The second approach obtains excitation energies for a series of time-correlated snapshots. This dynamic approach relies on the accurate truncation of the cumulant expansion but treats the dynamics of the chromophore and the environment on equal footing. Both approaches show significant potential for making strides toward more accurate optical spectroscopy simulations of complex condensed phase systems.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39126539","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}
引用次数: 22
Modeling Spin-Crossover Dynamics. 自旋交叉动力学建模。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-02-09 DOI: 10.1146/annurev-physchem-101419-012625
Saikat Mukherjee, Dmitry A Fedorov, Sergey A Varganov
{"title":"Modeling Spin-Crossover Dynamics.","authors":"Saikat Mukherjee,&nbsp;Dmitry A Fedorov,&nbsp;Sergey A Varganov","doi":"10.1146/annurev-physchem-101419-012625","DOIUrl":"https://doi.org/10.1146/annurev-physchem-101419-012625","url":null,"abstract":"<p><p>In this article, we review nonadiabatic molecular dynamics (NAMD) methods for modeling spin-crossover transitions. First, we discuss different representations of electronic states employed in the grid-based and direct NAMD simulations. The nature of interstate couplings in different representations is highlighted, with the main focus on nonadiabatic and spin-orbit couplings. Second, we describe three NAMD methods that have been used to simulate spin-crossover dynamics, including trajectory surface hopping, ab initio multiple spawning, and multiconfiguration time-dependent Hartree. Some aspects of employing different electronic structure methods to obtain information about potential energy surfaces and interstate couplings for NAMD simulations are also discussed. Third, representative applications of NAMD to spin crossovers in molecular systems of different sizes and complexities are highlighted. Finally, we pose several fundamental questions related to spin-dependent processes. These questions should be possible to address with future methodological developments in NAMD.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25348858","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}
引用次数: 15
Electrochemical Tip-Enhanced Raman Spectroscopy: An In Situ Nanospectroscopy for Electrochemistry. 电化学尖端增强拉曼光谱:电化学的原位纳米光谱。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-05-01 DOI: 10.1146/annurev-physchem-061020-053442
Sheng-Chao Huang, Yi-Fan Bao, Si-Si Wu, Teng-Xiang Huang, Matthew M Sartin, Xiang Wang, Bin Ren
{"title":"Electrochemical Tip-Enhanced Raman Spectroscopy: An In Situ Nanospectroscopy for Electrochemistry.","authors":"Sheng-Chao Huang,&nbsp;Yi-Fan Bao,&nbsp;Si-Si Wu,&nbsp;Teng-Xiang Huang,&nbsp;Matthew M Sartin,&nbsp;Xiang Wang,&nbsp;Bin Ren","doi":"10.1146/annurev-physchem-061020-053442","DOIUrl":"https://doi.org/10.1146/annurev-physchem-061020-053442","url":null,"abstract":"<p><p>Revealing the intrinsic relationships between the structure, properties, and performance of the electrochemical interface is a long-term goal in the electrochemistry and surface science communities because it could facilitate the rational design of electrochemical devices. Achieving this goal requires in situ characterization techniques that provide rich chemical information and high spatial resolution. Electrochemical tip-enhanced Raman spectroscopy (EC-TERS), which provides molecular fingerprint information with nanometer-scale spatial resolution, is a promising technique for achieving this goal. Since the first demonstration of this technique in 2015, EC-TERS has been developed for characterizing various electrochemical processes at the nanoscale and molecular level. Here, we review the development of EC-TERS over the past 5 years. We discuss progress in addressing the technical challenges, including optimizing the EC-TERS setup and solving tip-related issues, and provide experimental guidelines. We also survey the important applications of EC-TERS for probing molecular protonation, molecular adsorption, electrochemical reactions, and photoelectrochemical reactions. Finally, we discuss the opportunities and challenges in the future development of this young technique.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38782809","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}
引用次数: 11
Control of Chemical Reaction Pathways by Light-Matter Coupling. 光-物质耦合对化学反应途径的控制。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-01-22 DOI: 10.1146/annurev-physchem-090519-045502
Dinumol Devasia, Ankita Das, Varun Mohan, Prashant K Jain
{"title":"Control of Chemical Reaction Pathways by Light-Matter Coupling.","authors":"Dinumol Devasia,&nbsp;Ankita Das,&nbsp;Varun Mohan,&nbsp;Prashant K Jain","doi":"10.1146/annurev-physchem-090519-045502","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090519-045502","url":null,"abstract":"<p><p>Because plasmonic metal nanostructures combine strong light absorption with catalytically active surfaces, they have become platforms for the light-assisted catalysis of chemical reactions. The enhancement of reaction rates by plasmonic excitation has been extensively discussed. This review focuses on a less discussed aspect: the induction of new reaction pathways by light excitation. Through commentary on seminal reports, we describe the principles behind the optical modulation of chemical reactivity and selectivity on plasmonic metal nanostructures. Central to these phenomena are excited charge carriers generated by plasmonic excitation, which modify the energy landscape available to surface reactive species and unlock pathways not conventionally available in thermal catalysis. Photogenerated carriers can trigger bond dissociation or desorption in an adsorbate-selective manner, drive charge transfer and multielectron redox reactions, and generate radical intermediates. Through one or more of these mechanisms, a specific pathway becomes favored under light. By improved control over these mechanisms, light-assisted catalysis can be transformational for chemical synthesis and energy conversion.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38848220","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}
引用次数: 23
Droplet Interfacial Tensions and Phase Transitions Measured in Microfluidic Channels. 微流体通道中液滴界面张力和相变的测量。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-02-19 DOI: 10.1146/annurev-physchem-090419-105522
Priyatanu Roy, Shihao Liu, Cari S Dutcher
{"title":"Droplet Interfacial Tensions and Phase Transitions Measured in Microfluidic Channels.","authors":"Priyatanu Roy,&nbsp;Shihao Liu,&nbsp;Cari S Dutcher","doi":"10.1146/annurev-physchem-090419-105522","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090419-105522","url":null,"abstract":"<p><p>Measurements of droplet phase and interfacial tension (IFT) are important in the fields of atmospheric aerosols and emulsion science. Bulk macroscale property measurements with similar constituents cannot capture the effect of microscopic length scales and highly curved surfaces on the transport characteristics and heterogeneous chemistry typical in these applications. Instead, microscale droplet measurements ensure properties are measured at the relevant length scale. With recent advances in microfluidics, customized multiphase fluid flows can be created in channels for the manipulation and observation of microscale droplets in an enclosed setting without the need for large and expensive control systems. In this review, we discuss the applications of different physical principles at the microscale and corresponding microfluidic approaches for the measurement of droplet phase state, viscosity, and IFT.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25386244","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}
引用次数: 20
In Situ Surface-Enhanced Raman Spectroscopy Characterization of Electrocatalysis with Different Nanostructures. 不同纳米结构电催化的原位表面增强拉曼光谱表征。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-01-20 DOI: 10.1146/annurev-physchem-090519-034645
Bao-Ying Wen, Qing-Qi Chen, Petar M Radjenovic, Jin-Chao Dong, Zhong-Qun Tian, Jian-Feng Li
{"title":"In Situ Surface-Enhanced Raman Spectroscopy Characterization of Electrocatalysis with Different Nanostructures.","authors":"Bao-Ying Wen,&nbsp;Qing-Qi Chen,&nbsp;Petar M Radjenovic,&nbsp;Jin-Chao Dong,&nbsp;Zhong-Qun Tian,&nbsp;Jian-Feng Li","doi":"10.1146/annurev-physchem-090519-034645","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090519-034645","url":null,"abstract":"<p><p>As energy demands increase, electrocatalysis serves as a vital tool in energy conversion. Elucidating electrocatalytic mechanisms using in situ spectroscopic characterization techniques can provide experimental guidance for preparing high-efficiency electrocatalysts. Surface-enhanced Raman spectroscopy (SERS) can provide rich spectral information for ultratrace surface species and is extremely well suited to studying their activity. To improve the material and morphological universalities, researchers have employed different kinds of nanostructures that have played important roles in the development of SERS technologies. Different strategies, such as so-called borrowing enhancement from shell-isolated modes and shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS)-satellite structures, have been proposed to obtain highly effective Raman enhancement, and these methods make it possible to apply SERS to various electrocatalytic systems. Here, we discuss the development of SERS technology, focusing on its applications in different electrocatalytic reactions (such as oxygen reduction reactions) and at different nanostructure surfaces, and give a brief outlook on its development.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38842056","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}
引用次数: 20
First-Principles Simulations of Biological Molecules Subjected to Ionizing Radiation. 电离辐射下生物分子的第一性原理模拟。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 DOI: 10.1146/annurev-physchem-101419-013639
Karwan Ali Omar, Karim Hasnaoui, Aurélien de la Lande
{"title":"First-Principles Simulations of Biological Molecules Subjected to Ionizing Radiation.","authors":"Karwan Ali Omar,&nbsp;Karim Hasnaoui,&nbsp;Aurélien de la Lande","doi":"10.1146/annurev-physchem-101419-013639","DOIUrl":"https://doi.org/10.1146/annurev-physchem-101419-013639","url":null,"abstract":"<p><p>Ionizing rays cause damage to genomes, proteins, and signaling pathways that normally regulate cell activity, with harmful consequences such as accelerated aging, tumors, and cancers but also with beneficial effects in the context of radiotherapies. While the great pace of research in the twentieth century led to the identification of the molecular mechanisms for chemical lesions on the building blocks of biomacromolecules, the last two decades have brought renewed questions, for example, regarding the formation of clustered damage or the rich chemistry involving the secondary electrons produced by radiolysis. Radiation chemistry is now meeting attosecond science, providing extraordinary opportunities to unravel the very first stages of biological matter radiolysis. This review provides an overview of the recent progress made in this direction, focusing mainly on the atto- to femto- to picosecond timescales. We review promising applications of time-dependent density functional theory in this context.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38899064","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}
引用次数: 12
Optical Properties and Excited-State Dynamics of Atomically Precise Gold Nanoclusters. 原子精密金纳米团簇的光学性质和激发态动力学。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2020-12-09 DOI: 10.1146/annurev-physchem-090419-104921
Meng Zhou, Rongchao Jin
{"title":"Optical Properties and Excited-State Dynamics of Atomically Precise Gold Nanoclusters.","authors":"Meng Zhou,&nbsp;Rongchao Jin","doi":"10.1146/annurev-physchem-090419-104921","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090419-104921","url":null,"abstract":"<p><p>Understanding the excited-state dynamics of nanomaterials is essential to their applications in photoenergy storage and conversion. This review summarizes recent progress in the excited-state dynamics of atomically precise gold (Au) nanoclusters (NCs). We first discuss the electronic structure and typical relaxation pathways of Au NCs from subpicoseconds to microseconds. Unlike plasmonic Au nanoparticles, in which collective electron excitation dominates, Au NCs show single-electron transitions and molecule-like exciton dynamics. The size-, shape-, structure-, and composition-dependent dynamics in Au NCs are further discussed in detail. For small-sized Au NCs, strong quantum confinement effects give rise to relaxation dynamics that is significantly dependent on atomic packing, shape, and heteroatom doping. For relatively larger-sized Au NCs, strong size dependence can be observed in exciton and electron dynamics. We also discuss the origin of coherent oscillations and their roles in excited-state relaxation. Finally, we provide our perspective on future directions in this area.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1146/annurev-physchem-090419-104921","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38694057","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}
引用次数: 27
α-Crystallins in the Vertebrate Eye Lens: Complex Oligomers and Molecular Chaperones. 脊椎动物眼球晶状体中的α-晶体蛋白：复杂的低聚物和分子伴侣。
IF 14.7 1区 化学
Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2020-12-15 DOI: 10.1146/annurev-physchem-090419-121428
Marc A Sprague-Piercy, Megan A Rocha, Ashley O Kwok, Rachel W Martin
{"title":"α-Crystallins in the Vertebrate Eye Lens: Complex Oligomers and Molecular Chaperones.","authors":"Marc A Sprague-Piercy, Megan A Rocha, Ashley O Kwok, Rachel W Martin","doi":"10.1146/annurev-physchem-090419-121428","DOIUrl":"10.1146/annurev-physchem-090419-121428","url":null,"abstract":"<p><p>α-Crystallins are small heat-shock proteins that act as holdase chaperones. In humans, αA-crystallin is expressed only in the eye lens, while αB-crystallin is found in many tissues. α-Crystallins have a central domain flanked by flexible extensions and form dynamic, heterogeneous oligomers. Structural models show that both the C- and N-terminal extensions are important for controlling oligomerization through domain swapping. α-Crystallin prevents aggregation of damaged β- and γ-crystallins by binding to the client protein using a variety of binding modes. α-Crystallin chaperone activity can be compromised by mutation or posttranslational modifications, leading to protein aggregation and cataract. Because of their high solubility and their ability to form large, functional oligomers, α-crystallins are particularly amenable to structure determination by solid-state nuclear magnetic resonance (NMR) and solution NMR, as well as cryo-electron microscopy.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":null,"pages":null},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8062273/pdf/nihms-1628487.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38713564","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}
引用次数: 0
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