Two‐Orders‐of‐Magnitude Enhancement of Photoinitiation Activity via a Simple Surface Engineering of Metal Nanoclusters

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(23)

Published: March 26, 2024

Abstract Development of high‐performance photoinitiator is the key to enhance printing speed, structure resolution and product quality in 3D laser printing. Here, improve efficiency nanoprinting, we investigate underlying photochemistry gold silver nanocluster initiators under multiphoton excitation. Experimental results DFT calculations reveal high cleavage probability surface S−C bonds nanoclusters which generate multiple radicals. Based on this understanding, design several alkyl‐thiolated achieve a more than two‐orders‐of‐magnitude enhancement photoinitiation activity, as well significant improvement fabrication window. Overall, work for first time unveils detailed radical formation pathways activation substantially improves their sensitivity via engineering, pushes limit lithography.

Language: Английский

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Assemble–Disassemble–Reassemble Dynamics in Copper Nanocluster-Based Superstructures

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(18), P. 4880 - 4889

Published: April 29, 2024

Assembling metal nanoclusters (MNCs) to form superstructures generates exciting photophysical properties distinct from those of their discrete precursors. Controlling the assembly process MNCs and understanding assembly-disassembly dynamics can have implications in achieving reversible self-assembly MNCs. The formation self-assembled copper (CuNCs) as homogeneous underlying mechanisms governing such a remain unexplored. Smart molecular imprinting surface ligands establish forces necessary for superstructures. Herein, we report highly luminescent, ordered 4-phenylimidazole-2-thiol (4-PIT)-protected CuNCs with help l-ascorbic acid secondary ligand. Through comprehensive spectroscopic analysis, deciphered mechanism process, where role interligand H-bonding C-H-π interactions was established. Notably, efficient reversibility demonstrated by re-establishing regenerating morphological signatures.

Language: Английский

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Atomic Design of Copper Active Sites in Pristine Metal–Organic Coordination Compounds for Electrocatalytic Carbon Dioxide Reduction

Small Methods, Journal Year: 2024, Volume and Issue: 8(11)

Published: May 20, 2024

Abstract Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) has emerged as a promising and sustainable approach to cut emissions by converting greenhouse gas CO value‐added chemicals fuels. Metal–organic coordination compounds, especially the copper (Cu)‐based which feature well‐defined crystalline structures designable metal active sites, have attracted much research attention in electrocatalytic RR. Herein, recent advances of electrochemical RR on pristine Cu‐based compounds with different types Cu sites are reviewed. First, general pathways briefly introduced. Then highly efficient conversion various kinds (e.g., single‐Cu site, dimeric‐Cu multi‐Cu heterometallic site) is systematically discussed, along corresponding catalytic mechanisms. Finally, some existing challenges potential opportunities for this direction provided guide rational design metal–organic their practical application

Language: Английский

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Anomalous Structural Transformation of Cu(I) Clusters into Multifunctional CuAg Nanoclusters

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(36)

Published: May 23, 2024

Abstract We report an anomalous structural transformation of a Cu(I) cluster into two different types copper‐silver (CuAg) alloy nanoclusters. Different from previous reports, we demonstrate that under specifically designed reaction conditions, the Ag‐doping could induce substantial growth starting Cu 15 and Ag 13 20 nanocluster was obtained via unexpected insertion kernel inside Cu(I)‐S shell. demonstrates high activity to initiate photopolymerization previously hard‐to‐print inorganic polymers in 3D laser microprinting. Interestingly, slight modification condition leads formation another 18‐x x S (8≤x) templated by central 2− anion, which possesses unique electronic structure compared conventional template‐free CuAg Overall, this work unveils intriguing doping chemistry clusters, as well their capability create nanoclusters with unobtainable structures multifunctionality.

Language: Английский

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Applications of in-situ spectroscopic techniques towards CO2 electroreduction

Science China Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: June 6, 2024

Language: Английский

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