Synthesis, Structural Characterization, and Electronic Structure Analysis of F2-type Superatomic Molecules DOI

Manman Zhou,

Chuanjun Zhou,

Shuang Chen

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 28, 2024

The investigation of bonding interactions between superatoms continues to be a largely unexplored area study. In this study, we present the synthesis and characterization two F2-type superatomic molecules [Au2Ag25(C7H4NOS)13(DPPB)3] [Au9Ag18(C5H4NS)11(DPPM)5]2+ (Au2Ag25 Au9Ag18 for short, respectively). overall structures were confirmed via X-ray crystallography, revealing horizontal expansion biicosahedral Au2Ag21 yielding vertical Au8Ag15 [Au9Ag18(C5H4NS)11(DPPM)5]2+. Furthermore, their electronic elucidated through density functional theory (DFT) calculations. Spectroscopic analysis absorption characteristics, in conjunction with Tamm–Dancoff approximation DFT (TDA-DFT) calculations, revealed that Au2Ag21(+9) Au8Ag15(+9) cores analogues F2 molecule configuration.

Language: Английский

Efficient Electrocatalytic Semi‐Hydrogenation of Alkynes by Interfacial Engineering of Atomically Precise Silver Nanoclusters DOI Open Access
Zhipu Zhang, Rongrong Yin, Ziyang Song

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 6, 2025

Owing to its green energy and hydrogen sources, electrocatalytic semi-hydrogenation of alkynes is an attractive alternative for industrial alkene production. However, broad application hindered by low selectivity Faradaic efficiency (FE) due side reactions like over-hydrogenation alkanes. Here, we demonstrate that atomically precise Ag25(MHA)18 nanoclusters (NCs) can electrocatalyze alkyne with 98 % conversion, 99 selectivity, 85 FE, in a substrate pool. This achieved engineering the local environment at catalytically active sites. We leverage amphiphilic MHA (6-mercaptohexanoic acid) ligands pre-concentrate water molecules near ligand-layer/Ag25 interface. Long-chain disrupt hydrogen-bond network interface, high negative charge Ag25 attract weakly hydrogen-bonded through counterions promote generation (H*), while enzyme-like catalytic pockets on surface NCs facilitate adsorption terminal via σ-bonding Ag atoms. Density functional theory calculations confirmed preference model further revealed facile release product alkene. work not only exemplifies interface strategy control sites optimized activity selectivity.

Language: Английский

Citations

0
Atomic-level insights into the synergistic effect between ligands on electrochemical CO2 reduction: based on Au7Ag8 series nanoclusters DOI

Along Ma,

Yuansheng Li,

Yang Zuo

et al.

Rare Metals, Journal Year: 2025, Volume and Issue: unknown

Published: March 21, 2025

Language: Английский

Citations

0
Phosphine-induced conversion from Au36 to Au32 for constructing high-performance CO2RR catalyst DOI
Jian‐Sheng Ye,

Yali Dai,

Wenjun Liu

et al.

Dalton Transactions, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

A monophosphine-mediated structural modification strategy is performed to convert Au 36 into 32 nanoclusters and boost the eCO 2 RR performance.

Language: Английский

Citations

0
Poisoning Electrocatalytic CO2 Conversion to CO by Adding a μ4-S Atom on Au60 Nanocluster DOI
Yining Chen, Shuguang Wang,

Yan Sun

et al.

ACS Materials Letters, Journal Year: 2025, Volume and Issue: unknown, P. 2366 - 2373

Published: May 22, 2025

Language: Английский

Citations

0
Highly Selective Methanol Synthesis Using Electrochemical CO2 Reduction with Defect‐Engineered Cu58 Nanoclusters DOI Creative Commons
Sourav Biswas, Tomoya Tanaka, Haohong Song

et al.

Small Science, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 28, 2024

Atomically precise copper nanoclusters (Cu NCs) exhibit significant potential as catalysts for the electrocatalytic reduction of CO 2 . However, range products achievable with these NCs has been somewhat constrained. This study presents an innovative design strategy to enhance catalytic activity Cu by engineering their active sites. These sites are formed here introducing defects on cubic through partial dislocation atoms at vertices, which creates surface ligand vacancies. further refines internal cationic geometry altering cuprophilic interactions, leading distinct modifications in edges and vertices geometry. unique Cu(I) atom arrangements within cluster effectively influence product specificity during electrochemical reduction. Density functional theory calculations correlate enhanced selectivity CH 3 OH [Cu 58 H 20 (SPr) 36 (PPh ) 7 ] 2+ (Pr = NC increased reactivity edge binding CHO intermediates, compared 8 (SEt) 6 (Et NCs. Thus, this work underscores tailored structural designs atomically nanocatalysts directing toward unconventional products.

Language: Английский

Citations

1
Asymmetric Charge Distribution in Atomically Precise Metal Nanoclusters for Boosted CO2 Reduction Catalysis DOI Open Access
Yuanxin Du,

Pei Wang,

Yi Fang

et al.

ChemSusChem, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 30, 2024

Recently, atomically precise metal nanoclusters (NCs) have been widely applied in CO

Language: Английский

Citations

0
Synthesis, Structural Characterization, and Electronic Structure Analysis of F2-type Superatomic Molecules DOI

Manman Zhou,

Chuanjun Zhou,

Shuang Chen

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 28, 2024

The investigation of bonding interactions between superatoms continues to be a largely unexplored area study. In this study, we present the synthesis and characterization two F2-type superatomic molecules [Au2Ag25(C7H4NOS)13(DPPB)3] [Au9Ag18(C5H4NS)11(DPPM)5]2+ (Au2Ag25 Au9Ag18 for short, respectively). overall structures were confirmed via X-ray crystallography, revealing horizontal expansion biicosahedral Au2Ag21 yielding vertical Au8Ag15 [Au9Ag18(C5H4NS)11(DPPM)5]2+. Furthermore, their electronic elucidated through density functional theory (DFT) calculations. Spectroscopic analysis absorption characteristics, in conjunction with Tamm–Dancoff approximation DFT (TDA-DFT) calculations, revealed that Au2Ag21(+9) Au8Ag15(+9) cores analogues F2 molecule configuration.

Language: Английский

Citations

0