Tailoring the Chemisorption Manner of Fe d‐Band Center with La2O3 for Enhanced Oxygen Reduction in Anion Exchange Membrane Fuel Cells DOI
Tongfei Li, Luping Zhang, Li Zhang

и другие.

Advanced Functional Materials, Год журнала: 2023, Номер 34(9)

Опубликована: Ноя. 27, 2023

Abstract Engineering the electronic configuration and intermediates adsorption behaviors of high‐performance non‐noble‐metal‐based catalysts for sluggish oxygen reduction reaction (ORR) kinetics at cathode is highly imperative development anion exchange membrane fuel cells (AEMFCs), yet remains an enormous challenge. Herein, a rare‐earth metal oxide engineering tactic through formation Fe 3 O 4 /La 2 heterostructures in N,O‐doped carbon nanospheres (Fe @N,O‐CNSs) efficient electrocatalysis reported. The theoretical calculations reveal that interfacial bonds formed by La─O─Fe heterogeneous interface effectively optimize structure d‐band center relative to Fermi level, which results significant barriers rate‐limiting steps during ORR. modulation chemisorption enables @N,O‐CNSs outstanding ORR performance improved stability, with significantly higher half‐wave potential value (0.88 V). More impressively, this integrated catalyst delivers remarkable power density 148.7 mW cm −2 practical AEMFC operating conditions, along negligible degradation over 100 h using H ‐air atmosphere, than commercial Pt/C‐coupled electrodes. presented here are believed provide guidelines fabricating AEMFCs electrocatalysts terms heterointerface strong coupling effect induced oxides.

Язык: Английский

Terbium-induced cobalt valence-band narrowing boosts electrocatalytic oxygen reduction DOI

Xuan Wang,

Juan Zhang, Pu Wang

и другие.

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 5500 - 5512

Опубликована: Янв. 1, 2023

Tb 2 O 3 endows Co 3d with a narrow band and appropriate location via 3d–O 2p–Tb 4f gradient orbital coupling to efficiently enhance the oxygen reduction reaction.

Язык: Английский

Процитировано

81

High-coordination Fe–N4SP single-atom catalysts via the multi-shell synergistic effect for the enhanced oxygen reduction reaction of rechargeable Zn–air battery cathodes DOI
Jiaqi Liu,

Weibin Chen,

Shuang Yuan

и другие.

Energy & Environmental Science, Год журнала: 2023, Номер 17(1), С. 249 - 259

Опубликована: Ноя. 16, 2023

Novel Fe single-atom catalysts with highly coordinated Fe–N 4 SP structures were designed via the multi-coordination-shell synergistic effect. The optimization of enhances their ORR activity in alkaline/acidic media towards rechargeable Zn–air batteries.

Язык: Английский

Процитировано

75

Modulating Coordination of Iron Atom Clusters on N,P,S Triply‐Doped Hollow Carbon Support towards Enhanced Electrocatalytic Oxygen Reduction DOI
Xingmei Guo, Jing Shi, Ming Li

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(49)

Опубликована: Окт. 24, 2023

Constructing atom-clusters (ACs) with in situ modulation of coordination environment and simultaneously hollowing carbon support are critical yet challenging for improving electrocatalytic efficiency atomically dispersed catalysts (ADCs). Herein, a general diffusion-controlled strategy based on spatial confining Kirkendall effect is proposed to construct metallic ACs N,P,S triply-doped hollow matrix (MACs /NPS-HC, M=Mn, Fe, Co, Ni, Cu). Thereinto, FeACs /NPS-HC the best catalytic activity oxygen reduction reaction (ORR) thoroughly investigated. Unlike benchmark sample symmetrical N-surrounded iron single-atoms N-doped (FeSAs /N-C), comprises bi-/tri-atomic Fe centers engineered S/N coordination. Theoretical calculation reveals that proper gathering could mildly delocalize electron distribution optimize free energy pathways ORR. In addition, triple doping structure further regulate local allow sufficient exposure active sites, resulting more enhanced ORR kinetics /NPS-HC. The zinc-air battery assembled as cathodic catalyst exhibits all-round superiority Pt/C most Fe-based ADCs. This work provides an exemplary method establishing atomic-cluster S-dominated hollowed matrix, which paves new avenue fabrication optimization advanced

Язык: Английский

Процитировано

74

Carbon-based electrocatalysts for rechargeable Zn–air batteries: design concepts, recent progress and future perspectives DOI

Xiaohong Zou,

Mingcong Tang, Qian Lü

и другие.

Energy & Environmental Science, Год журнала: 2023, Номер 17(2), С. 386 - 424

Опубликована: Ноя. 22, 2023

This review provides an in-depth discussion of the carbon-based electrocatalysts for rechargeable Zn–air batteries from design strategies, research progress, and future perspectives.

Язык: Английский

Процитировано

70

Modulating Electronic Structures of Iron Clusters through Orbital Rehybridization by Adjacent Single Copper Sites for Efficient Oxygen Reduction DOI Open Access

Chunhong Qi,

Haoyu Yang, Ziqi Sun

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(39)

Опубликована: Июль 24, 2023

The atom-cluster interaction has recently been exploited as an effective way to increase the performance of metal-nitrogen-carbon catalysts for oxygen reduction reaction (ORR). However, rational design such and understanding their structure-property correlations remain a great challenge. Herein, we demonstrate that introduction adjacent metal (M)-N4 single atoms (SAs) could significantly improve ORR well-screened Fe atomic cluster (AC) catalyst by combining density functional theory (DFT) calculations experimental analysis. DFT studies suggest Cu-N4 SAs act modulator assist O2 adsorption cleavage O-O bond on AC active center, well optimize release OH* intermediates accelerate whole kinetic. depositing with nitrogen doped mesoporous carbon nanosheet are then constructed through universal interfacial monomicelles assembly strategy. Consistent theoretical predictions, resultant exhibits outstanding half-wave potential 0.92 eV in alkali 0.80 acid, high power 214.8 mW cm-2 zinc air battery. This work provides novel strategy precisely tuning atomically dispersed poly-metallic centers electrocatalysis.

Язык: Английский

Процитировано

54

Electronic structure regulation of the Fe-based single-atom catalysts for oxygen electrocatalysis DOI
Xiaochen Wang,

Zhiwen Kang,

Dan Wang

и другие.

Nano Energy, Год журнала: 2024, Номер 121, С. 109268 - 109268

Опубликована: Янв. 9, 2024

Язык: Английский

Процитировано

46

An overview of silicon-air batteries: Principle, current state and future perspectives DOI
Sujuan Hu, Ziyu Wang, Junjie Wang

и другие.

Coordination Chemistry Reviews, Год журнала: 2024, Номер 517, С. 216045 - 216045

Опубликована: Июль 1, 2024

Язык: Английский

Процитировано

41

Surface Engineered Single‐atom Systems for Energy Conversion DOI

Yutang Yu,

Zijian Zhu, Hongwei Huang

и другие.

Advanced Materials, Год журнала: 2024, Номер 36(16)

Опубликована: Янв. 10, 2024

Abstract Single‐atom catalysts (SACs) are demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs still early stages of conversion, problems like agglomeration low conversion efficiency hampering their practical applications. Substantial research focus on support modifications, which vital SAC stability due intimate relationship between atoms support. In this review, category supports variety surface engineering strategies employed SA systems summarized, including site (heteroatom doping, vacancy introducing, groups grafting, coordination tunning) structure (size/morphology control, cocatalyst deposition, facet engineering, crystallinity control). Also, merits single‐atom systematically introduced. Highlights comprehensive summary discussions utilization surface‐engineered diversified applications photocatalysis, electrocatalysis, thermocatalysis, devices. At end potential obstacles using field discussed. This review aims guide rational design manipulation target‐specific capitalizing characteristic benefits engineering.

Язык: Английский

Процитировано

29

Construction of Fe Nanoclusters/Nanoparticles to Engineer FeN4 Sites on Multichannel Porous Carbon Fibers for Boosting Oxygen Reduction Reaction DOI
Zhe Wang, Zhe Lü, Qitong Ye

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер 34(23)

Опубликована: Янв. 15, 2024

Abstract Fe–N–C catalysts are emerging as promising alternatives to Pt‐based for the oxygen reduction reaction (ORR), while they still suffer from sluggish kinetics due discontented binding affinity between Fe‐N 4 sites and oxygen‐containing intermediates, unsatisfactory stability. Herein, a flexible multichannel carbon fiber membrane immobilized with atomically dispersed neighboring Fe nanoclusters/nanoparticles (FeN ‐Fe NCP @MCF) is synthesized. The optimized geometric electronic structures of atomic brought by adjacent hierarchically porous structure matrix endow FeN @MCF outstanding ORR activity stability, considerably outperforming its counterpart only commercial Pt/C catalyst. Liquid solid‐state zinc–air batteries employing both exhibit durability. Theoretical calculation reveals that nanoclusters can trigger remarkable electron redistribution modulate hybridization central 3 d O 2 p orbitals, facilitating activation molecules optimizing adsorption capacity intermediates on sites, thus accelerating kinetic. This work offers an effective approach constructing coupling have single atoms coexisting efficient catalysis.

Язык: Английский

Процитировано

29

3D Hierarchical MOF-Derived Defect-Rich NiFe Spinel Ferrite as a Highly Efficient Electrocatalyst for Oxygen Redox Reactions in Zinc–Air Batteries DOI Creative Commons
Mohan Gopalakrishnan, Wathanyu Kao‐ian, Meena Rittiruam

и другие.

ACS Applied Materials & Interfaces, Год журнала: 2024, Номер 16(9), С. 11537 - 11551

Опубликована: Фев. 16, 2024

The strategy of defect engineering is increasingly recognized for its pivotal role in modulating the electronic structure, thereby significantly improving electrocatalytic performance materials. In this study, we present defect-enriched nickel and iron oxides as highly active cost-effective electrocatalysts, denoted Ni0.6Fe2.4O4@NC, derived from NiFe-based metal–organic frameworks (MOFs) oxygen reduction reactions (ORR) evolution (OER). XANES EXAFS confirm that crystals have a distorted structure metal vacancies. cation defect-rich Ni0.6Fe2.4O4@NC electrocatalyst exhibits exceptional ORR OER activities (ΔE = 0.68 V). Mechanistic pathways electrochemical are studied by DFT calculations. Furthermore, rechargeable zinc–air battery (RZAB) using catalyst demonstrates peak power density 187 mW cm–2 remarkable long-term cycling stability. flexible solid-state ZAB 66 cm–2. proposed structural design allows rational delocalization NiFe spinel ferrite attached to ultrathin N-doped graphitic carbon sheets order enhance site availability facilitate mass electron transport.

Язык: Английский

Процитировано

28