Small, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 20, 2024
Atomically dispersed metal-nitrogen-carbon materials (AD-MNCs) are considered the most promising non-precious catalysts for oxygen reduction reaction (ORR), but it remains a major challenge simultaneously achieving high intrinsic activity, fast mass transport, and effective utilization of active sites within single catalyst. Here, an AD-MNCs consisting defect-rich Fe-N
Language: Английский
Advanced Materials, Journal Year: 2024, Volume and Issue: 36(33)
Published: June 25, 2024
Abstract Double‐atom catalysts (DACs) with asymmetric coordination are crucial for enhancing the benefits of electrochemical carbon dioxide reduction and advancing sustainable development, however, rational design DACs is still challenging. Herein, this work synthesizes atomically dispersed novel sulfur‐bridged Cu‐S‐Ni sites (named Cu‐S‐Ni/SNC), utilizing biomass wool keratin as precursor. The plentiful disulfide bonds in overcome limitations traditional gas‐phase S ligand etching process enable one‐step formation S‐bridged sites. X‐ray absorption spectroscopy (XAS) confirms existence bimetallic N 2 Cu‐S‐NiN moiety. In H‐cell, Cu‐S‐Ni/SNC shows high CO Faraday efficiency 98.1% at −0.65 V versus RHE. Benefiting from charge tuning effect between metal site bridged sulfur atoms, a large current density 550 mA cm −2 can be achieved −1.00 flow cell. Additionally, situ XAS, attenuated total reflection surface‐enhanced infrared (ATR‐SEIRAS), functional theory (DFT) calculations show Cu main adsorption dual‐regulated by Ni which enhances activation accelerates *COOH intermediates. This kind atom may open new pathways precision preparation performance regulation atomic materials toward energy applications.
Language: Английский
Citations
27
Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(14), P. 4847 - 4870
Published: Jan. 1, 2024
Based on the advancements in atomically dispersed multi-site catalysts for FZABs, this review discusses design methodologies to regulate performance of bifunctional oxygen electrocatalysts from electronic and geometric structures.
Language: Английский
Citations
23
Small, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 13, 2025
Abstract Single‐atom catalysts (SACs) are a class of with low dosage, cost, and the presence metal atom‐carrier interactions high catalytic activity, which considered to possess significant potential in field electrocatalysis. The most important aspect synthesis SACs is selection suitable carriers. Metal carbides, nitrides, or carbon‐nitrides (MXenes) widely used as new type 2D materials good electrical conductivity tunable surface properties. abundance functional groups vacancy defects on MXenes an ideal anchoring site for single atoms therefore regarded carrier single‐atom loading. In this work, preparation method MXenes, loading mode SACs, characterization catalysts, electrochemical performance described detail, some hot issues current research future directions also summarized. aim work promote development MXene‐based within realm With ongoing innovation, these expected be crucial energy conversion storage solutions.
Language: Английский
Citations
2
Advanced Materials, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 2, 2025
Abstract Catalysis remains a cornerstone of chemical research, with the active sites catalysts being crucial for their functionality. Identifying sites, particularly during reaction process, is elucidating relationship between catalyst's structure and its catalytic property. However, dynamic evolution within heterogeneous metal presents substantial challenge accurately pinpointing real sites. The advent in situ operando characterization techniques has illuminated path toward understanding changes offering robust scientific evidence to support rational design catalysts. There pressing need comprehensive review that systematically explores among single atoms, clusters, nanoparticles as utilizing techniques. This aims delineate effects various factors on nanoparticles. Moreover, several are elaborated emphases tracking linking them properties. Finally, it discusses challenges future perspectives identifying process advancing
Language: Английский
Citations
1
Journal of Materials Chemistry A, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
Significant functionalization of Fe 5 clusters with CuN 2 O single atom, compared 4 and FeN , in decreasing d-band center weakening the oxygen adsorption.
Language: Английский
Citations
1
Nano Research, Journal Year: 2024, Volume and Issue: unknown
Published: Sept. 3, 2024
Language: Английский
Citations
6
Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 497, P. 155005 - 155005
Published: Aug. 23, 2024
Language: Английский
Citations
5
Small, Journal Year: 2025, Volume and Issue: unknown
Published: March 21, 2025
The inherent sluggish kinetics of the conventional four-electron transfer pathway fundamentally limits oxygen reduction reaction (ORR) efficiency. While electronic structure modulation offers potential solutions, developing effective catalytic regulation strategies remains challenging due to elusive structure-activity correlations. In this study, Fe4 cluster sites are engineered with dual parallel electron channels that enable concurrent O─O bond cleavage and atom protonation. This unique configuration facilitates an optimized two-step double mechanism, significantly enhancing ORR kinetics. Synergistic Mn single sites, strategically positioned as reservoirs, substantially elevate density clusters while reinforcing Fe─N coordination bonds through charge redistribution. Remarkably, spatial at support periphery minimizes steric confinement effects, allowing simultaneous product desorption adsorption - a critical advantage for sustaining continuous cycles. Through combined experimental theoretical analyses, it is demonstrated dual-channel transport system effectively reduces activation barriers elementary steps accelerating fundamental study establishes new paradigm designing high-performance catalysts multi-site collaborative engineering optimization.
Language: Английский
Citations
0
Molecules, Journal Year: 2025, Volume and Issue: 30(7), P. 1505 - 1505
Published: March 28, 2025
The rational design of high-performance catalysts for the oxygen evolution reaction (OER) and reduction (ORR) is essential development clean renewable energy technologies, particularly in fuel cells metal-air batteries. Two-dimensional (2D) covalent organic frameworks (COFs) possess numerous hollow sites, which contribute to stable anchoring transition metal (TM) atoms become promising supports single atom (SACs). Herein, OER ORR catalytic performance a series SACs based on TQBQ-COFs were systematically investigated through density functional theory (DFT) calculations, with particular emphasis role coordination environment modulating activity. results reveal that Rh/TQBQ exhibits most effective performance, an overpotential 0.34 V, while Au/TQBQ demonstrates superior 0.50 V. A critical mechanistic insight lies distinct boundary TQBQ, perturb adsorption energetics intermediates, thereby circumventing conventional scaling relationships governing pathways. Furthermore, we established TM (Ead) as robust descriptor predicting activity, enabling streamlined screening strategy SAC design. This study emphasizes significance determining offers new perspective novel OER/ORR COFs-based SACs.
Language: Английский
Citations
0
Journal of Power Sources, Journal Year: 2025, Volume and Issue: 644, P. 237058 - 237058
Published: April 18, 2025
Language: Английский
Citations
0