ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 6852 - 6873
Published: April 12, 2025
Language: Английский
ACS Catalysis, Journal Year: 2023, Volume and Issue: 14(1), P. 45 - 55
Published: Dec. 9, 2023
The attention toward single-atom catalysts (SACs) for electrochemical processes is growing at an impressive pace. Electronic structure calculations play important role in this race by providing proposals of potentially relevant based on screening studies or the identification descriptors chemical activity. So far, almost all these predictions ignore a crucial aspect design catalyst: its stability. We propose simple yet general first-principles approach to predict stability SACs under working conditions pH and applied voltage. This construction thermodynamic cycle, where part information taken from experiment rest density functional theory (DFT) calculations. In particular, we make use formalism Pourbaix diagrams investigate reductive oxidative identify those that show pronounced tendency dissolve form other species. Applying procedure four transition metal atoms, Cr, Mn, Fe, Co, three supports, N-doped graphene, carbon nitride, covalent organic frameworks, key factor determining final binding energy free atom support. results several very good reactions are, fact, dramatically prone dissolution transformation species, suggesting every prediction SAC's catalytic activity should be accompanied parallel investigation
Language: Английский
Citations
43
Small, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 9, 2025
Abstract Single‐atom catalysts (SACs) are gathering significant attention in chemistry due to their unique properties, offering uniform active site distribution and enhanced selectivity. However, precise structure often remains unclear, with multiple models proposed the literature. Understanding coordination environment of at atomic level is crucial for explaining catalytic activity. Here, a comprehensive study SACs made carbon nitride (CN x ) containing isolated nickel atoms presented. Using combination synthesis techniques characterization methods including Fourier‐transform infrared spectroscopy, X‐ray absorption spectroscopy (XAS), density functional theory (DFT) calculations, local centers CN ‐supported investigated. These results challenge conventional structural propose new architecture that better aligns current experimental evidence. This serves as foundational step toward rational approach catalyst development can facilitate more design application these innovative catalysts.
Language: Английский
Citations
7
Physical Chemistry Chemical Physics, Journal Year: 2024, Volume and Issue: 26(14), P. 10746 - 10756
Published: Jan. 1, 2024
Impact of the adopted DFT functional on activation CO 2 a set single-atom catalysts.
Language: Английский
Citations
15
Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 511, P. 215870 - 215870
Published: April 21, 2024
Language: Английский
Citations
11
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(45)
Published: Aug. 13, 2024
Photocatalytic hydrogen production is one of the most valuable technologies in future energy system. Here, we designed a metal-covalent organic frameworks (MCOFs) with both small-sized metal clusters and nitrogen-rich ligands, named COF-Cu
Language: Английский
Citations
11
Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 516, P. 215961 - 215961
Published: May 29, 2024
Language: Английский
Citations
9
Advanced Materials, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 7, 2025
Abstract Metal single atoms (SA)‐support interactions inherently exhibit significant electrochemical activity, demonstrating potential in energy catalysis. However, leveraging these to modulate electronic properties and extend application fields is a formidable challenge, demanding in‐depth understanding quantitative control of atomic‐scale interactions. Herein, situ, off‐axis electron holography technique utilized directly visualize the between SAs graphene surface. These facilitate formation dispersed nanoscale regions with high charge density are highly sensitive external electromagnetic (EM) fields, resulting controllable dynamic relaxation processes for accumulation restoration. This leads customized dielectric relaxation, which difficult achieve current band engineering methods. Moreover, behaviors insensitive elevated temperatures, having characteristics distinct from those typical metallic or semiconducting materials. Based on results, programmable EM wave absorption achieved by developing library SA‐graphene materials precisely controlling SA‐support tailor their responses waves terms frequency intensity. advancement addresses anti‐EM interference requirements components, greatly enhancing development integrated circuits micro‐nano chips. Future efforts will concentrate manipulating atomic SA‐support, potentially revolutionizing nanoelectronics optoelectronics.
Language: Английский
Citations
1
Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 3, 2025
Abstract Single‐atom materials (SAMs) have garnered widespread attention due to their maximum utilization of active metal atoms for catalytic related applications. However, the facile preparation oxide with high single‐atom loading is still challenging. Herein, derivation highly tunable metal‐organic frameworks (MOFs) precursor found be a potential method Sn‐doped ZnO high‐performance chemiresistive sensing Specifically, Sn/Zn‐MOF‐L interdigitated lamellar morphology transferred from bimetallic Sn/Zn‐MOF‐B featuring microstructure and through solvent treatment. Utilizing finely MOF as precursor, nanosheet porous structure successfully constructed. The as‐prepared doped oxides show superior acetone performances, sensor based on 8% demonstrates an astonishing response value 213 ( R / g ) toward 10 ppm low detection limit 0.52 ppb. sensitivity attributed specific surface area distribution Sn sites, benefiting manipulation precursor. loaded considerable performance offers new perspective design application SAMs.
Language: Английский
Citations
1
Applied Surface Science, Journal Year: 2025, Volume and Issue: unknown, P. 162879 - 162879
Published: March 1, 2025
Language: Английский
Citations
1
Small, Journal Year: 2024, Volume and Issue: unknown
Published: April 26, 2024
Abstract A computational screening of Single Atom Catalysts (SACs) bound to titanium nitride (TiN) is presented, for the Hydrogen Evolution Reaction (HER), based on density functional theory. The role fundamental ingredients explored account a reliable SACs. Namely, formation H 2 ‐complexes besides classical * one impacts predicted HER activity, in line with previous studies other Also, results indicate that needs adopt self‐interaction‐corrected functionals. Finally, predicting an active catalyst little help without assessment its stability. Thus, it included theoretical framework analysis stability SACs working conditions pH and voltage. Once unconventional intermediates are considered self‐interaction corrected scheme, number potential good catalysts strongly reduced since i) some potentially not stable against dissolution ii) leads thermodynamic barriers. This study highlights importance including prediction new systems, such as intermediates, estimating SACs, adoption this interesting candidates deserving dedicated work.
Language: Английский
Citations
7