Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 497, P. 155005 - 155005
Published: Aug. 23, 2024
Language: Английский
Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)
Published: April 9, 2024
The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the reduction reaction (ORR) kinetics. Herein, a new approach for boosting inherent ORR activity atomically dispersed Fe-N-C matrix is represented by implanting Fe atomic clusters nearby. as-prepared catalyst delivers excellent half-wave potentials 0.78 0.90 V in acidic alkaline solutions, respectively. decent can also be validated from high-performance rechargeable Zn-air battery. experiments density functional theory calculations reveal that electron spin-state monodispersed active transferred low spin (LS, t
Language: Английский
Citations
102
Advanced Materials, Journal Year: 2024, Volume and Issue: 36(19)
Published: Feb. 12, 2024
Abstract Dual‐metal center catalysts (DMCs) have shown the ability to enhance oxygen reduction reaction (ORR) owing their distinctive structural configurations. However, precise modulation of electronic structure and in‐depth understanding synergistic mechanisms between dual metal sites DMCs at atomic level remain challenging. Herein, mimicking ferredoxin, Fe‐based (Fe 2 N 6 ‐S) are strategically designed fabricated, in which additional Fe S synchronously installed near serve as “dual modulators” for coarse‐ fine‐tuning modulation, respectively. The as‐prepared ‐S catalyst exhibits enhanced ORR activity outstanding Zinc‐air (Zn–air) battery performance compared conventional single site catalysts. theoretical experimental results reveal that introducing second creates a adsorption alters O configuration effectively activates O─O bond, while effect downward shift d‐band center, facilitating release OH*. Additionally, local engineering heteroatom further facilitates formation rate‐determining step OOH*, thus accelerating kinetics.
Language: Английский
Citations
47
Advanced Materials, Journal Year: 2024, Volume and Issue: 36(32)
Published: May 29, 2024
Demetalation caused by the electrochemical dissolution of metallic Fe atoms is a major challenge for practical application Fe─N─C catalysts. Herein, an efficient single Mn active site constructed to improve strength Fe─N bond, inhibiting demetalation effect Fe─N─C. acts as electron donor inducing more delocalized electrons reduce oxidation state increasing density, thereby enhancing bond and Fe. The oxygen reduction reaction pathway dissociation Fe─Mn dual sites can overcome high energy barriers direct O─O modulate electronic states
Language: Английский
Citations
38
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(12)
Published: Jan. 29, 2024
Abstract Authentic surface structures under reaction conditions determine the activity and selectivity of electrocatalysts, therefore, knowledge structure‐activity relationship can facilitate design efficient catalyst for specific reactivity requirements. However, understanding between a more realistic active its performance is challenging due to complicated interface microenvironment in electrocatalysis. Herein, we proposed standard research paradigm effectively decipher electrocatalysis, which exemplified CO 2 electroreduction over SnO . The practice has aided discovering authentic/resting states (Sn layer) accountable electrochemical reduction (CO RR) electrocatalytic conditions, then corroborated subsequent RR experiments with different morphologies (nanorods, nanoparticles, nanosheets) combination situ characterizations. This methodology further extended providing helpful insights into catalytic structures. It believed that our also applicable other systems, meantime, decreases discrepancy theory experiments, accelerates achieve sustainable energy conversion.
Language: Английский
Citations
31
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)
Published: March 18, 2024
Abstract Recently, a diverse array of novel metal‐nitrogen‐carbon (M‐N‐C) single‐atom catalysts (SACs) have rapidly evolve, particularly in the realm oxygen reduction reaction (ORR). Despite plethora proposed design and improvement strategies for SACs, comprehensive review systematically compiling components M‐N‐C from unified perspective is notably absent. For first time, thorough examination each component conducted, focusing on entropy increase active sites SACs. single M‐N 4 whole system, an implies elevated degree disorder chaos. Broadly, entropy‐increasing modification M (single mental sites) guest groups entails augmentation chaos, with most effective co‐catalytic synergy achieved by establishing multiple through “cocktail effect”. Concerning N (nitrogen other heteroatoms) C (carbon supports), induces heightened disorder, symmetry breaking more likely to drive toward adsorbing molecules attain equilibrium symmetric structure. All these innovative led remarkable ORR activity stability offer guiding criterion future preparation
Language: Английский
Citations
27
Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(29), P. 20323 - 20332
Published: July 12, 2024
Addressing the sluggish kinetics in alkaline hydrogen oxidation reaction (HOR) is a pivotal yet challenging step toward commercialization of anion-exchange membrane fuel cells (AEMFCs). Here, we have successfully immobilized indium (In) atoms an orderly fashion into platinum (Pt) nanoparticles supported by reduced graphene oxide (denoted as O-Pt
Language: Английский
Citations
18
Advanced Materials, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 11, 2025
Abstract Exploiting robust and high‐efficiency electrocatalysts for sluggish oxygen reduction reaction (ORR) is essential proton exchange membrane fuel cells (PEMFCs) toward long‐term operation practical applications, yet remains challenging. Herein, the ordered PtCo intermetallic reported with a Pt‐rich shell loaded on highly graphitized carbon carrier (O‐PtCo@GCoNC) prepared by an impregnation annealing strategy. Systematic X‐ray spectroscopic, operando electrochemical techniques theoretical calculations reveal that thanks to synergistic interaction of core–shell structure tailor‐made Pt electronic configuration carbon, O‐PtCo@GCoNC exhibits significantly enhanced activity stability ORR. Crucially, delivers much‐enhanced mass 0.83 A mg −1 at 0.9 V versus reversible hydrogen electrode (RHE) in 0.1 m HClO 4 , which only drops 26.5% after 70 000 cycles (0.6–1.0 vs RHE), 10.8% 10 (1.0–1.5 apparently overmatching Pt/C (0.19 73.7%, 63.1%). Moreover, employed as cathode catalyst H 2 /air PEMFC achieves superb peak power density (1.04 W cm −2 2.06 ), outperforming (0.86 1.79 ). The cell voltage loss 0.8 28 mV 30 cycles, outstripping United States Department Energy 2025 target.
Language: Английский
Citations
2
Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 27 - 48
Published: Nov. 10, 2023
The “charge–spin–coordination” relationship was introduced into Fe functional units (Fe-FUs) in multiple forms to comprehensively analyze their activity sources and degradation mechanisms during the ORR process.
Language: Английский
Citations
32
Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 486, P. 150088 - 150088
Published: March 3, 2024
Language: Английский
Citations
12
ACS Nano, Journal Year: 2024, Volume and Issue: 18(17), P. 11474 - 11486
Published: April 18, 2024
Cobalt-nitrogen-carbon (Co-N-C) catalysts with a CoN
Language: Английский
Citations
12