Electrochemistry of Atomically Precise Metal Nanoclusters.

Abstract:
Thiolate-protected metal nanoparticles containing a few to few hundred metal atoms are interesting materials exhibiting unique physicochemical properties. They encompass the bulk-to-molecule transition region, where discrete electronic states emerge and electronic band energetics yield to quantum confinement effects. Recent progresses in the synthesis and characterization of ultrasmall gold nanoparticles have opened up new avenues for the isolation of extremely monodispersed nanoparticles with atomically precision. These nanoparticles are also called nanoclusters to distinguish them from other regular metal nanoparticles with core diameter >2 nm. These nanoclusters are typically identified by their actual molecular formulas; prominent among these are Au25(SR)18, Au38(SR)24, and Au102(SR)44, where SR is organothiolate. A number of single crystal structures of these nanoclusters have been disclosed. Researchers have effectively utilized density functional theory (DFT) calculations to predict their atomic and electronic structures, as well as their physicochemical properties. The atomically precise metal nanoclusters have been the focus of recent studies owing to their novel size-specific electrochemical, optical, and catalytic properties. In this Account, we highlight recent advances in electrochemistry of atomically precise metal nanoclusters and their applications in electrocatalysis and electrochemical sensing. Compared with gold nanoclusters, much less progress has been made in the electrochemical studies of other metal nanoclusters, and thus, we mainly focus on the electrochemistry and electrochemical applications of gold-based nanoclusters. Voltammetry has been extremely powerful in investigating the electronic structure of metal nanoclusters, especially near HOMO and LUMO levels. A sizable opening of HOMO-LUMO gap observed for Au25(SR)18 gradually decreases with increasing nanocluster size, which is in line with the change in the optical gap. Heteroatom-doping has been a powerful strategy to modify the optical and electrochemical properties of metal nanoclusters at the atomic level. While the superatom theory predicts 8-electron configuration for [Au25(SR)18]- and many doped nanoclusters thereof, Pt- and Pd-doped [PtAu24(SR)18]0 and [PdAu24(SR)18]0 nanoclusters show dramatically different electronic structures, as manifested in their optical spectra and voltammograms, suggesting the occurrence of the Jahn-Teller distortion in these doped nanoclusters. Furthermore, metal-doping may alter their surface binding properties, as well as redox potentials. Metal nanoclusters offer great potential for attaining high activity and selectivity in their electrocatalytic applications. The well-defined core-shell structure of a metal nanocluster is of special advantage because the core and shell can be independently engineered to exhibit suitable binding properties and redox potentials. We discuss recent progress made in electrocatalysis based upon metal nanoclusters tailored for water splitting, CO2 conversion, and electrochemical sensing. A well-defined model nanocatalyst is absolutely necessary to reveal the detailed mechanism of electrocatalysis and thereby to lead to the development of a new efficient electrocatalyst. We envision that atomically controlled metal nanoclusters will enable us to systematically optimize the electrochemical and surface properties suitable for electrocatalysis, thus providing a powerful platform for the discovery of finely tuned nanocatalysts.
Author Listing： Kyuju Kwak;Dongil Lee
Volume： 52 1
Pages： \n 12-22\n
DOI： 10.1021/acs.accounts.8b00379
Language： English
Journal： Accounts of chemical research

ACCOUNTS OF CHEMICAL RESEARCH

Acc. Chem. Res.

影响因子：16.4 是否综述期刊：是 是否OA：否 是否预警：不在预警名单内 发行时间：1968 ISSN：0001-4842 发刊频率：Monthly 收录数据库：SCIE/Scopus收录 出版国家/地区：UNITED STATES 出版社：American Chemical Society

期刊介绍

Accounts of Chemical Research 主要发表化学和生物化学领域内关于基础研究和应用的短小精悍、具有作者团队自己研究特色的述评文章，或者前瞻性观点。这些短综述都是基于作者自己实验室的过往研究，以便向读者完整介绍研究项目。期刊收录研究方向：化学，化学综合Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Visit the Accounts Special Issues page for listings, descriptions, and TOC's of all special issues.Beginning in 2008, Accounts of Chemical Research replaced their traditional article abstract with an article "Conspectus." These new entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article’s discoverability by search engines and the exposure for the research.

化学研究报告提供了简短，简洁和关键的文章，提供了化学和生物化学所有领域的基础研究和应用的易于阅读的概述。此外，《化学研究报告》还出版了专门针对异常活动和意义的单一问题的特刊。访问帐户特殊问题页面以获取所有特殊问题的列表，描述和目录。从2008年开始，化学研究帐户用文章 “Conspectus” 代替了传统的文章摘要。这些新条目概述了这项研究，使读者可以更仔细地了解文章的内容和意义。通过提供对文章内容的更详细描述，Conspectus增强了搜索引擎对文章的可发现性和对研究的了解。

年发文量 311
国人发稿量 102
国人发文占比 32.8%
自引率 0.6%
平均录取率 极难
平均审稿周期 一般,3-6周
版面费 -
偏重研究方向 化学-化学综合
期刊官网 https://pubs.acs.org/journal/achre4
投稿链接 https://acs.manuscriptcentral.com/acs

质量指标占比

研究类文章占比 OA被引用占比 撤稿占比 出版后修正文章占比
0.00% 12.32% 0.00% 0.90%

相关指数

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《2019年中国科学院文献情报中心期刊分区表升级版（试行）》首次将社会科学引文数据库（SSCI）期刊纳入到分区评估中。升级版分区表（试行）设置了包括自然科学和社会科学在内的18个大类学科。基础版和升级版（试行）将过渡共存三年时间，推测在此期间各大高校和科研院所仍可能会以基础版为考核参考标准。 提示：中科院分区官方微信公众号“fenqubiao”仅提供基础版数据查询，暂无升级版数据，请注意区分。

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