Chemical Science, Journal Year: 2024, Volume and Issue: unknown
Published: Jan. 1, 2024
A sterically demanding ortho -CF 3 substituent defines not only the arrangement of ligands on a Ag 98 (2-CF PhCC) 48 Cl 4 nanocluster (Ag98) but also inter-cluster interactions. Ag98 shows excellent methanol tolerance in oxygen reduction reaction.
Language: Английский
The Journal of Physical Chemistry C, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 7, 2025
Intercluster reactions involving atomically precise noble metal nanoclusters (NCs) in solution, closely resembling between molecules, are important for exploring chemistry on the nanoscale. In present study, we conducted [Ag29(1,3-BDT)12]3– (1,3-BDT = 1,3-benzenedithiol) and center-doped [MAg24(2,4-DMBT)18]q− (q 1 M Ag, Au; q 2 Pd, Pt; 2,4-DMBT 2,4-dimethylbenzenethiol) NCs solution. For first time, report formation of stable dimers, formed two with mixed metal–ligand interfaces. The dimeric species were [MAg53–xBDT12DMBT18–y]3– (x ≥ 0 y 0), 16 electrons their valence shells. Here, dimers irrespective nature central atom NC, although compositions different depending atom. These solution ∼2 days. dithiol-protected [Ag29BDT12]3– part was more during fragmentation than monothiol-protected [MAg24DMBT18]q− part. UV/vis spectroscopic mass spectrometric analyses, along density functional theory calculations, used to understand dimers. Our work highlighted importance cluster interface stability dimer formed. Probing such intercluster can help us reaction mechanism greater detail.
Language: Английский
Citations
0
Rare Metals, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 16, 2025
Language: Английский
Citations
0
Nanoscale, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
This work achieved the manipulation of Pd dopant numbers in cluster framework based on two structurally comparable x Au 12 ( = 1, 2) nanoclusters.
Language: Английский
Citations
0
Inorganics, Journal Year: 2025, Volume and Issue: 13(3), P. 72 - 72
Published: Feb. 27, 2025
Chiral gold nanomaterials have promising applications in biomedicine, catalysis, optics and other fields. However, the complexity of their chiral sources has led to many challenges terms functional design controlled synthesis. In this paper, we systematically review development history Au nanomaterials; deeply analyze synthesis strategy, construction mechanism, performance optimization pathway; discuss formation mechanism light progress cutting-edge research look into future direction development. The aim is provide theoretical methodological support for controllable nanomaterials.
Language: Английский
Citations
0
Small, Journal Year: 2025, Volume and Issue: unknown
Published: March 23, 2025
An investigation combining neutron diffraction and DFT allows determining the most likely hydride migration pathway within icosahedral metal framework of [RhH2Ag19{S2P(OnPr)2}12] (RhH2Ag19). Starting from experimentally derived solid-state structures, a computational analysis is able to reveal an energetically favorable with maximum energy barrier 4.2 kcal mol-1. The two hydrides migrate simultaneously Rh@Ag12 core, traversing several positional isomers. This study expands understanding dynamics in nanoclusters provides critical insights into structural flexibility superatom framework. These findings have significant implications for hydrogen storage, catalysis, design advanced hydride-containing materials.
Language: Английский
Citations
0
Chemical Science, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
Surface ligands play an important role in dictating the structure and catalytic properties of metal nanoclusters. Recently, a novel class Au clusters protected by N-heterocyclic carbenes (NHCs) halogens has been synthesized; however, dynamic stability Au-NHCs/Au-halogen interface real electrochemical environments as well influence ligand layer on process remains obscure. Herein, we combined first-principles simulations with experiments to investigate metal-ligand interaction classical [Au13(NHCMe)9Cl3]2+ cluster its unique potential promote electrocatalytic CO2 reduction syngas. Our revealed facile shedding chlorine from surface Au13 core upon biasing, more negative applied potential, faster kinetics Au-Cl bond cleavage. By contrast, Au-NHC is highly stable, indicating greater Au-C bonds over under conditions. Interestingly, exposed icosahedral dechlorinated [Au13(NHCMe)9Cl2]3+ capable efficiently catalyzing generate CO H2 comparable barriers wide range, showcasing strong for syngas formation. predictions are further corroborated experimental data, where X-ray photoelectron spectroscopy (XPS) verified halogen stripping acid or neutral media, activated demonstrated enhanced efficacy formation : ratio approximately 0.8 1.2 across broad range -0.50 -1.20 V. This work reveals exciting frontier understanding etching dynamics NHC-protected nanoclusters, particularly, preference production first time gold-based which distinctive previously reported nanoclusters that mainly produce CO.
Language: Английский
Citations
0
Nanoscale Horizons, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
The latest developments in thiolate-protected metal nanoclusters important electrocatalytic applications, such as hydrogen evolution, oxygen reduction and CO 2 reactions, are briefly reviewed this work.
Language: Английский
Citations
0
Dalton Transactions, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
This review covers atomically precise metal nanocluster-based photocatalysts for hydrogen production, focusing on their unique structures, strong light harvesting abilities, and charge-transfer mechanisms.
Language: Английский
Citations
0
The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(25), P. 10317 - 10323
Published: June 7, 2024
There exist numerous challenges in hydrogen generation, storage, and transportation. Ammonia has been attractive as an efficient carrier by virtue of its high specific density. Designing outstanding catalysts for converting NH3 through the ammonia oxidation reaction (AOR) is significant. Because synergistic effects resulting from interactions between metal support, it believed that support significant improving catalyst's activity. Owing to this, activity small Mn (M = Pt, Ir; n 3, 4) clusters supported CeO2(111) surfaces was theoretically explored. The Mn/CeO2(111) kinetically exhibit G–M mechanism rather than N + mechanism. In addition, we determined range operating onset potentials over effective AOR. Using Sabatier analysis, also predicted Pt3/CeO2(111) most active catalyst
Language: Английский
Citations
3
Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(34)
Published: June 7, 2024
Abstract Owing to the significant attention directed toward alloy metal nanoclusters, it is crucial explore relationship between their structures and performance during electrocatalytic CO 2 reduction reaction (eCO RR) discover potential synergistic effects for design of novel functional nanoclusters. However, a lack suitable analogs makes this investigation challenging. In study, we synthesized well‐defined pair structural analogs, [Au 8 Cu 1 (SAdm) 4 (Dppm) 3 Cl] 2+ Ag ( Au , respectively), characterized them. Single‐crystal X‐ray diffraction analysis revealed that M (M=Cu/Ag) consists tetrahedral core capped by three (Dppm)Au staples, one (SR) staple, lone SR ligand, terminal Cl ligand. were doped at same site in which has rarely been reported. exhibited significantly higher Faradaic efficiency (FE ; ~82.2 %) eCO RR than ~33.1 %). Density theory calculations demonstrated *COOH key intermediate CO. The formation on more thermodynamically stable shows smaller *CO energy promotes . We believe offer template in‐depth structure‐property correlations atomic level.
Language: Английский
Citations
2