Accounts of Chemical Research最新文献

{"title":"Last Honors and Life Experiences of Bereaved Families in the Context of COVID-19 in Kashmir: A Qualitative Inquiry About Exclusion, Family Trauma, and Other Issues.","authors":"Tanveer Ahmad Khan, Abdul Mohsin, Sumiya Din, Shaista Qayum, Irfanullah Farooqi","doi":"10.1177/00302228221134205","DOIUrl":"10.1177/00302228221134205","url":null,"abstract":"<p><p>This study examined the changing character of the last honours of those who died of COVID-19 in Kashmir and the life experiences of the families of the deceased. A semi-structured interview schedule was used to collect information from 21 participants. Using qualitative data analysis approaches, five key themes were identified vis-à-vis the impact of COVID-19 on burial rituals and customs; effects on bereaved families, shades of grief, bereavement care, community response, and coping with loss. Based on examining the pandemic-induced changes related to customs and rituals around death, the study found that the bereaved family members were in danger of marginalization, economic burdens, psychological traumas, and overall reduced quality of life. This study would be a credible addition to the existing literature on death practices as there is a shortage of research on funeral rituals during the post-pandemic period in Kashmir.</p>","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":" ","pages":"361-382"},"PeriodicalIF":16.4,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9606636/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"42358876","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}

{"title":"Fluoroalkylacylsilanes as Novel Ambiphilic Donor–Acceptor Carbene Precursors","authors":"Xiao Shen","doi":"10.1021/acs.accounts.5c00136","DOIUrl":"https://doi.org/10.1021/acs.accounts.5c00136","url":null,"abstract":"Carbenes, as highly reactive intermediates, have emerged as pivotal tools in organic synthesis, catalysis, and materials science due to their versatile reactivity and broad applicability. Among the diverse classes of carbenes, donor–acceptor carbenes (DACs) have attracted significant attention owing to their unique electronic properties and exceptional reaction selectivity. The distinctive reactivity of DACs arises from the synergistic electronic interplay between electron-withdrawing and electron-donating groups attached to the carbene center, enabling a wide array of transformations. These attributes have established DACs as indispensable building blocks for constructing complex molecular architectures and achieving precise control over chemical transformation.","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"42 1","pages":""},"PeriodicalIF":18.3,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876175","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":"Tuning 3-D Nanomaterial Architectures Using Atomic Layer Deposition to Direct Solution Synthesis","authors":"Alondra M. Ortiz-Ortiz, Daniel O. Delgado Cornejo, Ashley R. Bielinski, Neil P. Dasgupta","doi":"10.1021/acs.accounts.5c00076","DOIUrl":"https://doi.org/10.1021/acs.accounts.5c00076","url":null,"abstract":"The ability to synthesize nanoarchitected materials with tunable geometries provides a means to control their functional properties, with applications in biological, environmental, and energy fields. To this end, various bottom-up and top-down synthesis processes have been developed. However, many of these processes require prepatterning or etching steps, making them challenging to scale-up to complex, nonplanar substrates. Furthermore, the ability to integrate nanomaterials into hierarchical arrays with precise control of feature spacing and orientation remains a challenge.","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"52 1","pages":""},"PeriodicalIF":18.3,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853294","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":"How to Achieve Hydrogenation/Hydrofunctionalization via Metal Hydride Complexes","authors":"Ju Peng, Ruopeng Bai, Yu Lan","doi":"10.1021/acs.accounts.5c00115","DOIUrl":"https://doi.org/10.1021/acs.accounts.5c00115","url":null,"abstract":"Metal hydride (M–H) complexes have garnered widespread attention in the synthesis of fine chemicals, materials, agrochemicals, and pharmaceuticals owing to the remarkable reactivity of the M–H bonds. Specifically, M–H complexes are active intermediates that catalyze hydrogen-transfer reactions, leading to efficient hydrogenation and hydrofunctionalization of C═C/C═X (X = O or N) bonds in unsaturated organic substrates for the formation of new carbon–hydrogen, carbon–carbon, and carbon–heteroatom bonds.","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"108 1","pages":""},"PeriodicalIF":18.3,"publicationDate":"2025-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853295","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":"Atomically Dispersed Metal Interfaces for Analytical Chemistry","authors":"Weiqing Xu, Yu Wu, Wenling Gu, Chengzhou Zhu","doi":"10.1021/acs.accounts.4c00845","DOIUrl":"https://doi.org/10.1021/acs.accounts.4c00845","url":null,"abstract":"Engineering sensing interfaces with functional nanomaterials have aroused great interest in constructing novel analytical platforms. The good catalytic abilities and physicochemical properties allow functional nanomaterials to perform catalytic signal transductions and synergistically amplify biorecognition events for efficient target analysis. However, further boosting their catalytic performances poses grand challenges in achieving more sensitive and selective sample assays. Besides, nanomaterials with abundant atomic compositions and complex structural characteristics bring about more difficulties in understanding the underlying mechanism of signal amplification. Atomically dispersed metal catalysts (ADMCs), as an emerging class of heterogeneous catalysts, feature support-stabilized isolated metal catalytic sites, showing maximum metal utilization and a strong metal–support interfacial interaction. These unique structural characteristics are akin to those of homogeneous catalysts, which have well-defined coordination structures between metal sites with synthetic or biological ligands. By integrating the advantages of heterogeneous and homogeneous catalysts, ADMCs present superior catalytic activity and specificity relative to the nanoparticles formed by the nonuniform aggregation of active sites. ADMC-enabled sensing platforms have been demonstrated to realize advanced applications in various fields. Notably, the easily tunable coordination structures of ADMCs bring more opportunities to improve their catalytic performance, further moving toward efficient signal transduction ability. Besides, by leveraging their inherent physicochemical properties and various detection strategies, ADMC-enabled sensing interfaces not only achieve enhanced signal transductions but also show diversified output models. Such superior functions allow ADMC-enabled sensing platforms to access the goal of high-performance detection of trace targets and making significant progress in analytical chemistry.","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"6 1","pages":""},"PeriodicalIF":18.3,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846547","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":"Photon Management Through Energy Transfer in Halide Perovskite Nanocrystal–Dye Hybrids: Singlet vs Triplet Tuning","authors":"Jishnudas Chakkamalayath, Akshaya Chemmangat, Jeffrey T. DuBose, Prashant V. Kamat","doi":"10.1021/acs.accounts.5c00097","DOIUrl":"https://doi.org/10.1021/acs.accounts.5c00097","url":null,"abstract":"Photoinduced energy and electron transfer processes offer a convenient way to convert light energy into electrical or chemical energy. These processes remain the basis of operation of thin film solar cells, light emitting and optoelectronic devices, and solar fuel generation. In many of these applications, semiconductor nanocrystals that absorb in the visible and near-infrared region are the building blocks that harvest photons and initiate energy or electron transfer to surface-bound chromophores. Such multifunctional aspects make it challenging to steer the energy transfer pathway selectively. Proper selection of the semiconductor nanocrystal donor requires consideration of the nanocrystal bandgap, along with the alignment of valence and conduction band energies relative to that of the acceptor, in order to achieve desired output of energy or electron transfer.","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"3 1","pages":""},"PeriodicalIF":18.3,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831989","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":"Mass Transport Based on Covalent Organic Frameworks","authors":"Jianwei Yang, Bo Wang, Xiao Feng","doi":"10.1021/acs.accounts.5c00086","DOIUrl":"https://doi.org/10.1021/acs.accounts.5c00086","url":null,"abstract":"Mass transport is fundamental to biological systems and industrial processes, governing chemical reactions, substance exchange, and energy conversion across various material scales. In biological systems, ion transport, such as proton migration through voltage-gated proton channels, regulates cellular potential, signaling, and metabolic balance. In industrial processes, transporting molecules through solid, liquid, or gas phases dictates reactant contact and diffusion rates, directly impacting reaction efficiency and conversion. Optimizing these processes necessitates the design of efficient interfaces or channels to enhance mass transport.","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"60 1","pages":""},"PeriodicalIF":18.3,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822424","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":"Identifying Lanthanide Energy Levels in Semiconductor Nanoparticles Enables Tailored Multicolor Emission through Rational Dopant Combinations","authors":"Gouranga H. Debnath, Prasun Mukherjee, David H. Waldeck","doi":"10.1021/acs.accounts.5c00116","DOIUrl":"https://doi.org/10.1021/acs.accounts.5c00116","url":null,"abstract":"The unique photon emission signatures of trivalent lanthanide cations (Ln³⁺, where Ln = Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, and Yb) enables multicolor emission from semiconductor nanoparticles (NPs) either through doping multiple Ln³⁺ ions of distinct identities or in combination with other elements for the creation of next-generation light emitting diodes (LEDs), lasers, sensors, imaging probes, and other optoelectronic devices. Although advancements have been made in synthetic strategies to dope Ln³⁺ in semiconductor NPs, the dopant(s) selection criteria have hinged largely on trial-and-error. This combinatorial approach is often guided by treating NP–dopant(s) energy transfer dynamics through the lens of spectral overlap. Over the past decade, however, we have demonstrated that the spectral outcomes correlate better with the placement of Ln³⁺ energy levels with respect to the band edges of the semiconductor, and oxide, host.","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"5 1","pages":""},"PeriodicalIF":18.3,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822512","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":"Vibronic Engineering for Quantum Functional Groups.","authors":"Haowen Zhou, Taras Khvorost, Anastassia N Alexandrova, Justin R Caram","doi":"10.1021/acs.accounts.4c00773","DOIUrl":"https://doi.org/10.1021/acs.accounts.4c00773","url":null,"abstract":"<p><p>ConspectusChemists have a firm understanding of the concept of a functional group: a small molecular moiety that confers properties (reactivity, solubility, and chemical recognition) onto a larger scaffold. Analogously, a quantum functional group (QFG) would act as an isolated \"quantum handle\" that could attach onto an extended molecule and enable quantum state preparation and measurement (SPAM). However, the complexity associated with molecular chemistry is often at odds with the requirements of nonthermal state preparation. The rest of the molecule acts as a local bath that leads to dephasing and loss of quantum information upon excitation and relaxation. Yet, there exists an enormous chemical space of potential chemical bonding motifs to design isolated QFGs. The goal of this Account is to explore the underlying chemical design principles for the optimization of QFG performance.For typical state preparation, an applied field is used to put the qubit into a specific known state (via optical cycling and laser cooling), where it can be manipulated or entangled with other species. That same field (or another) can be used to read out or report on the qubit state at the end of the operation. For example, in trapped ions/neutral atoms, state preparation is accomplished by pumping a specific transition using a narrowband laser. From there, further operations can be performed on the qubit via selective RF or laser excitation, and the state can be read out via fluorescence. However, extending this paradigm to molecular systems is highly challenging: molecules have many more degrees of freedom that can couple to the absorbed or emitted field. Overcoming this requires greatly limiting the number of these \"off-diagonal\" decay pathways through the judicious selection of the QFG and vibronic engineering of the molecular substrate.Our work has demonstrated that alkaline-earth (I) alkoxides (MOR) may meet the necessary requirements for efficient SPAM. In particular, we capitalize on the -OM (M = Ca, Sr) motif, which acts as a quantum handle that has been attached to a variety of aliphatic and aromatic hydrocarbons. The precise breakdown of the optical cycling property depends on familiar chemical concepts, including conjugation, conformer formation, electron-withdrawing abilities, and symmetry. In this Account, we review the recent efforts in the field to construct QFGs and codesign molecular scaffolds that can host them without destruction of their desired quantum properties. QFGs are explored as attachments to photoswitching scaffolds and mounted in pairs to larger hosts. A variety of physical phenomena relevant to the ability of these QFGs to function as qubits, from Fermi resonances to super radiance, have been explored. We thus began deriving the first set of rules for vibronic engineering toward the QFG functionality. Prospects toward increasing the number densities of these QFGs through molecular and material design are also presented.</p>","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":" ","pages":""},"PeriodicalIF":16.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143794006","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":"Vibronic Engineering for Quantum Functional Groups","authors":"Haowen Zhou,&nbsp;Taras Khvorost,&nbsp;Anastassia N. Alexandrova* and Justin R. Caram*,&nbsp;","doi":"10.1021/acs.accounts.4c0077310.1021/acs.accounts.4c00773","DOIUrl":"https://doi.org/10.1021/acs.accounts.4c00773https://doi.org/10.1021/acs.accounts.4c00773","url":null,"abstract":"<p >Chemists have a firm understanding of the concept of a functional group: a small molecular moiety that confers properties (reactivity, solubility, and chemical recognition) onto a larger scaffold. Analogously, a quantum functional group (QFG) would act as an isolated “quantum handle” that could attach onto an extended molecule and enable quantum state preparation and measurement (SPAM). However, the complexity associated with molecular chemistry is often at odds with the requirements of nonthermal state preparation. The rest of the molecule acts as a local bath that leads to dephasing and loss of quantum information upon excitation and relaxation. Yet, there exists an enormous chemical space of potential chemical bonding motifs to design isolated QFGs. The goal of this Account is to explore the underlying chemical design principles for the optimization of QFG performance.</p><p >For typical state preparation, an applied field is used to put the qubit into a specific known state (via optical cycling and laser cooling), where it can be manipulated or entangled with other species. That same field (or another) can be used to read out or report on the qubit state at the end of the operation. For example, in trapped ions/neutral atoms, state preparation is accomplished by pumping a specific transition using a narrowband laser. From there, further operations can be performed on the qubit via selective RF or laser excitation, and the state can be read out via fluorescence. However, extending this paradigm to molecular systems is highly challenging: molecules have many more degrees of freedom that can couple to the absorbed or emitted field. Overcoming this requires greatly limiting the number of these “off-diagonal” decay pathways through the judicious selection of the QFG and vibronic engineering of the molecular substrate.</p><p >Our work has demonstrated that alkaline-earth (I) alkoxides (MOR) may meet the necessary requirements for efficient SPAM. In particular, we capitalize on the −OM (M = Ca, Sr) motif, which acts as a quantum handle that has been attached to a variety of aliphatic and aromatic hydrocarbons. The precise breakdown of the optical cycling property depends on familiar chemical concepts, including conjugation, conformer formation, electron-withdrawing abilities, and symmetry. In this Account, we review the recent efforts in the field to construct QFGs and codesign molecular scaffolds that can host them without destruction of their desired quantum properties. QFGs are explored as attachments to photoswitching scaffolds and mounted in pairs to larger hosts. A variety of physical phenomena relevant to the ability of these QFGs to function as qubits, from Fermi resonances to super radiance, have been explored. We thus began deriving the first set of rules for vibronic engineering toward the QFG functionality. Prospects toward increasing the number densities of these QFGs through molecular and material design are also presented.</p>","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"58 8","pages":"1181–1191 1181–1191"},"PeriodicalIF":16.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827978","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}