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Article
Chemistry, Multidisciplinary
Megalamane Siddaramappa Bootharaju et al.
Summary: This study presents the synthesis and crystal structure of selenolated Au-Ag core-shell nanoclusters, which exhibit enhanced stability and near-infrared-II photoluminescence due to the gold core modifying the overall electronic structure. The nanoclusters also show strong interactions with oxygen vacancies of TiO2, facilitating interfacial charge transfer for efficient photocatalysis. The Au12Ag32/TiO2 demonstrates remarkable solar H-2 production, approximately 6.2 and 37.8 times higher than Ag-44/TiO2 and TiO2, respectively, with good stability and recyclability.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Rhone Brocha P. Silalahi et al.
Summary: The first hydride-containing 2-electron palladium/copper alloys, PdHCu11 and PdHCu12, were synthesized. X-ray diffraction reveals that the PdHCu11 and PdHCu12 kernels consist of a central PdH unit encapsulated within a vertex-missing Cu-11 cuboctahedron and complete Cu-12 cuboctahedron, respectively. PdHCu11 shows excellent HER activity, with an onset potential of -0.05 V (at 10 mA cm(-2)) and consistent HER activity during 1000 cycles in 0.5 M H2SO4.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Kosuke Sakamoto et al.
Summary: Partially thiolated atomically precise Au cluster catalysts were developed by controlled calcination of presynthesized thiolate-protected Au clusters on a porous carbon support. The partially thiolated Au25 cluster catalysts exhibited comparable catalytic activity to that of the thiolate-free Au25 cluster for benzyl alcohol oxidation, but higher durability. These catalysts are promising model catalysts with both high activity and durability.
Article
Nanoscience & Nanotechnology
Jun Zha et al.
Summary: In this study, surface site specific antigalvanic replacement with remaining composition/structure and surface replacement-dependent selectivity in the electrocatalytic reduction of CO2 was achieved for the first time. Density functional theory calculations explained the catalysis selectivity switch induced by replacing Ag with Cu and the facilitation of C2 production by Cu replacement. Furthermore, CO2 electroreduction to C2 on well-defined metal nanoclusters was reported for the first time in this study.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Li Tang et al.
Summary: In this study, the synthesis and characterization of a gold cluster complex [Au-7(PPh3)(7)H-5](SbF6)(2), which decomposed to [Au-8(PPh3)(7)](2+) upon exposure to light, were reported. The valence state of Au-I and H- was verified through various experimental techniques. These two nanoclusters exhibited different selectivities in the electrocatalytic CO2 reduction reaction (CO2RR), with Au7H52+ showing 98.2% selectivity for H2 and Au-8(2+) showing 73.5% selectivity for CO. Further calculations showed that the H- ligand inhibited the CO2RR process compared to the electron-donor H.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Zong-Jie Guan et al.
Summary: We report the structures, stability, and catalytic properties of two Ag-21 nanoclusters with different electronic structures and an identical icosahedral kernel. These clusters exhibit superior stability under ambient conditions and one of them shows higher activity as a catalyst in a reduction reaction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Viveka K. Kulkarni et al.
Summary: Researchers have successfully synthesized a previously unseen N-heterocyclic carbene-stabilized hydrido gold nanocluster and demonstrated its catalytic activity in the electrocatalytic reduction of CO2.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Ze-Hua Gao et al.
Summary: In this study, a heteroleptic gold trihydride nanocluster was synthesized and found to have high catalytic activity and stability for electrochemical reduction of CO2 to CO. The hydride coordinated gold sites were identified as the active centers for the catalytic reaction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Guocheng Deng et al.
Summary: Atomically monodisperse nanostructured materials have significant importance in unraveling catalytic relationships. In this study, the synthesis and structure of a copper-containing alloy nanocluster were reported, which showed excellent catalytic activity and stability in the electrochemical CO2 reduction reaction. Density functional theory calculations revealed the mechanism behind the formation of efficient active sites.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Xu Liu et al.
Summary: In this study, Pt atoms were successfully doped into Au nanoclusters, and it was found that asymmetrical doping of one Pt atom increased energy and led to the loss of one valence electron, while symmetrical doping of two Pt atoms narrowed the energy gap and reduced two valence electrons. The different combinations of these doped nanoclusters exhibited varying CO2 electroreduction activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Arunachalam Sagadevan et al.
Summary: This study introduces a copper nanocluster-based catalyst that enables C-N bond-forming reactions of aryl chlorides under visible-light irradiation, showing good reaction yields.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Jia Dong et al.
Summary: This study reports the synthesis of a new undecagold cluster with a bidentate phosphine ligand. The cluster can undergo hydroauration reaction with alkynes containing electronwithdrawing groups, forming key gold-alkenyl semihydrogenation intermediates, which can be selectively converted to Z-alkenes under acidic conditions. By isolating and characterizing the intermediates, atomic-level insights into the active sites and mechanisms of semihydrogenation reactions catalyzed by gold-based nanomaterials are provided.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Shengli Zhuang et al.
Summary: This study proposes the concept of single-atom-kernelled nanoclusters and synthesizes a Pd-based trimetal nanocluster with a single-Ag atom-kernel using an alloying strategy. The nanoclusters with single-silver atom kernels exhibit higher activity and selectivity compared to the bimetal precursor nanoclusters. The single atoms in the kernel have significant influence on catalytic performance by affecting the electronic configuration.
Article
Chemistry, Multidisciplinary
Dan Yang et al.
Summary: This Review focuses on the recent progress in CO2RRs catalyzed by atomically precise metal nanoclusters, including gold, copper, and silver NCs. The influences of charge, ligand, surface structure, doping of Au NCs, and binders on the CO2RR are discussed in detail. Meanwhile the reaction mechanisms of CO2RRs including the active sites and the key reaction intermediates are also discussed. It is expected that progress in this research area could promote the development of metal NCs and CO2RRs.
Article
Chemistry, Multidisciplinary
Shengli Zhuang et al.
Summary: This study reports the successful synthesis of thiolated, reduced Pd nanoclusters and reveals their superior catalytic activity compared to other catalysts. The findings have important implications for understanding the influence of metal charge state and space structure on catalytic activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Hoeun Seong et al.
Summary: Atomically precise metal nanoclusters show promise as catalysts for electrochemical CO2 reduction reaction. A study found that Au25 nanoclusters have higher activity than Ag25 nanoclusters. Active-site engineering can significantly enhance the CO2 reduction activity of nanoclusters.
ACS ENERGY LETTERS
(2022)
Review
Chemistry, Multidisciplinary
Wenchuan Lai et al.
Summary: This review provides a comprehensive understanding of the energy efficiency (EE) in electrocatalytic CO2 reduction reaction (CO2RR). The fundamental principles and recent strategies for achieving high EE are discussed, with a focus on electrocatalysts and system design. The emerging integrated electrolysis is highlighted as a promising approach to enhance the EE and economic benefits of the CO2RR. Future research opportunities in this field are also outlined.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Rongchao Jin et al.
Summary: Researchers have successfully synthesized atomically precise metal nanoclusters with well-defined structures, opening up new opportunities for catalysis research. These atomically precise nanoclusters combine the characteristics of homogeneous catalysts and enzymes, holding significant potential for practical applications.
Article
Chemistry, Multidisciplinary
Lubing Qin et al.
Summary: This study reports the fabrication of a novel nanocluster Ag-15 and its electrocatalytic properties towards CO2 reduction, showcasing its self-assembly capability and high efficiency in converting CO2 to CO. The exposure of uncoordinated Ag atoms as catalytically active sites for CO formation is discussed, demonstrating promising potential for catalysis applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Site Li et al.
Summary: In this study, the surface modification of gold nanoclusters by Cd doping was found to significantly enhance the selectivity and activity for CO2 reduction reaction. The Cd-doped Au19Cd2 NC exhibited the highest CO2RR activity reported. Density-functional theory calculations revealed that Cd doping can boost the CO2RR performance by providing energetically feasible pathways and reducing the energy barrier for CO formation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Yaping Fang et al.
Summary: A designed Au4Cu4/CNT nanocluster system catalyzes the CuAAC reaction of terminal alkynes without alkyne deprotonation, unlike the classic mechanism involving a sigma,pi-alkynyl intermediate. DFT results confirmed the activation of HC CPh by pi-complexation with Au4Cu4. The specificity of Au4Cu4 involving synergy between Cu and Au was shown by the inactivity of internal alkynes under the same conditions for both Au-11/CNT and Cu-11/CNT catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Shang-Fu Yuan et al.
Summary: The first amidinate-protected gold nanocluster Au-28 has a compact core-shell structure of T symmetry, fully protected by bridging formamidinate ligands. It shows excellent catalytic performance for CO2 electroreduction with 96.5% FE. Superior stability is attributed to strong gold-ligand binding and geometric shell closure.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Hoeun Seong et al.
Summary: This study successfully identified active sites using gold nanoclusters as model catalysts in the electrochemical CO2 reduction reaction. The research showed that dethiolated Au sites are the active sites, and the CO2RR activity is determined by the number of active sites on the cluster surface.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Marco Neumaier et al.
Summary: The kinetics of intercluster metal atom exchange reactions between solvated clusters were studied using electrospray ionization mass spectrometry and computer-based modeling. The reactions involve both cluster monomers and dimers, with metal atom exchange occurring through transient dimers. The kinetic model contains generic reactions such as dimerization of monomers, metal atom exchange in transient dimers, and dissociation of dimers to monomers, with physically plausible rate constants supporting dimer-mediated metal atom exchange.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Review
Chemistry, Physical
Julia Linnemann et al.
Summary: Efforts in producing highly active, selective, and long-lived electrocatalysts by design are focused on understanding the relationship between material properties and catalytic performance. Surface characterization tools assess atomic scale information on electrocatalyst materials complexity, while electrochemical methodologies are less researched for this purpose. Complementary insights into electrocatalysis from other electrochemistry subareas may provide design strategies for improving mass transport and managing gas bubble release.
Article
Chemistry, Physical
Woojun Choi et al.
Summary: This study demonstrates controlled syngas production with different H-2/CO ratios on specifically formulated Au-25 and PtAu24 nanoclusters through electrochemical CO2 reduction reaction. Density functional theory calculations reveal that the conversion of CO2 to CO has lower reaction energy on Au-25 NCs compared to the hydrogen evolution reaction, leading to more CO production; while PtAu24 NCs are more favorable for H-2 production.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Sanghwa Lee et al.
Summary: Heteroatom-doped metal nanoclusters are synthesized by a metal-exchange strategy, leading to the discovery that Pt doping can significantly enhance the catalytic activity of Cu nanoclusters by around 300-fold. This synthetic approach has the potential to produce Ni-, Pd-, and Au-doped Cu nanoclusters, opening new avenues for studying their molecular structures and catalytic properties.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Yongnan Sun et al.
Summary: Research identified reaction sites of gold nanoclusters by selectively cleaving the Au-S or C-S bonds, showing that cleaving the C-S bonds creates open sulfur sites for CO2 reduction, while breaking the Au-S bonds favors H-2 evolution. Reactivities of these reaction sites can be further tailored by derivatizing ligands, showing promise in rational design of high-performance catalysts.
Review
Chemistry, Multidisciplinary
An Zhang et al.
Summary: Doping regulation is considered as an effective method to modulate the active sites of catalysts in electrocatalysis, especially in two-dimensional transition-metal compounds (TMCs) to optimize their electrocatalytic performance. This systematic overview highlights the impact of doping regulation on physicochemical properties of catalysts and their applications in various reactions, while also addressing the existing challenges and future perspectives in this promising field.
CHEMICAL SOCIETY REVIEWS
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Mina R. Narouz et al.
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Phil De Luna et al.
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Stephanie Nitopi et al.
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Zhouyang Yin et al.
TRENDS IN CHEMISTRY
(2019)
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Qiaofeng Yao et al.
ACCOUNTS OF CHEMICAL RESEARCH
(2018)
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Shuo Zhao et al.
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Juanzhu Yan et al.
NATIONAL SCIENCE REVIEW
(2018)
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ACCOUNTS OF CHEMICAL RESEARCH
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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Carlos G. Morales-Guio et al.
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INORGANIC CHEMISTRY
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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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