Periodic Single‐Metal Site Catalysts: Creating Homogeneous and Ordered Atomic‐Precision Structures DOI
Tianyu Zhang, Dingsheng Wang, Junfeng Liu

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(41)

Published: Aug. 16, 2024

Abstract Heterogeneous single‐metal‐site catalysts (SMSCs), often referred to as single‐atom (SACs), demonstrate promising catalytic activity, selectivity, and stability across a wide spectrum of reactions due their rationally designed microenvironments encompassing coordination geometry, binding ligands, electronic configurations. However, the inherent disorderliness SMSCs at both atomic scale nanoscale poses challenges in deciphering working principles establishing correlations between performances SMSCs. The rearrangement randomly dispersed single metals into homogeneous atomic‐precisely structured periodic single‐metal site (PSMSCs) not only simplifies chaos systems but also unveils new opportunities for manipulating performance gaining profound insights reaction mechanisms. Moreover, synergistic effects adjacent integration arrangement further broaden industrial application scope This perspective offers comprehensive overview recent advancements outlines prospective avenues research design characterizations PSMSCs, while acknowledging formidable encountered prospects that lie ahead.

Language: Английский

Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries DOI

Xiaotian Guo,

Hengyue Xu,

Yijian Tang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 31, 2024

Abstract Aqueous zinc–iodine batteries (AZIBs) are highly appealing for energy requirements owing to their safety, cost‐effectiveness, and scalability. However, the inadequate redox kinetics severe shuttling effect of polyiodide ions impede commercial viability. Herein, several Zn‐MOF‐derived porous carbon materials designed, further preparation iron–doped (Fe–N–C, M9) with varied Fe doping contents is optimized based on a facile self‐assembly/carbonization approach. M9, atomic coordinated nitrogen atoms, employed as an efficient cathode host AZIBs. Functional modifications hosts involving species levels investigated. The adsorption tests, in situ Raman spectroscopy, UV–vis results demonstrate capability charge‐discharge mechanism iodine species. Furthermore, experimental findings theoretical analyses have proven that conversion enhanced through physicochemical confinement effect. This study offers basic principles strategic design single‐atom dispersed high‐performance Flexible soft–pack battery wearable microbattery applications also implications future long‐life aqueous designs.

Language: Английский

Citations

53

Designing Electronic Structures of Multiscale Helical Converters for Tailored Ultrabroad Electromagnetic Absorption DOI Creative Commons

Zhaobo Feng,

Chongbo Liu, Xin Li

et al.

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 17(1)

Published: Sept. 26, 2024

Abstract Atomic-scale doping strategies and structure design play pivotal roles in tailoring the electronic physicochemical property of electromagnetic wave absorption (EMWA) materials. However, relationship between configuration (EM) loss mechanism has remained elusive. Herein, drawing inspiration from DNA transcription process, we report successful synthesis novel situ Mn/N co-doped helical carbon nanotubes with ultrabroad EMWA capability. Theoretical calculation EM simulation confirm that orbital coupling spin polarization Mn–N 4 –C configuration, along cross generated by structure, endow converters enhanced loss. As a result, HMC-8 demonstrates outstanding performance, achieving minimum reflection −63.13 dB at an ultralow thickness 1.29 mm. Through precise tuning graphite domain size, HMC-7 achieves effective bandwidth (EAB) 6.08 GHz 2.02 mm thickness. Furthermore, constructing macroscale gradient metamaterials enables ultrabroadband EAB 12.16 only 5.00 mm, maximum radar section reduction value reaching 36.4 m 2 . This innovative approach not advances understanding metal–nonmetal co-doping but also realizes broadband EMWA, thus contributing to development mechanisms applications.

Language: Английский

Citations

40

Fe/Cu diatomic sites dispersed on nitrogen-doped mesoporous carbon for the boosted oxygen reduction reaction in Mg-air and Zn-air batteries DOI

Weicheng Zhang,

Bowen Feng,

Le Huang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124450 - 124450

Published: July 27, 2024

Language: Английский

Citations

34

Spin effect in dual-atom catalysts for electrocatalysis DOI Creative Commons

Xiaoqin Xu,

Jingqi Guan

Chemical Science, Journal Year: 2024, Volume and Issue: 15(36), P. 14585 - 14607

Published: Jan. 1, 2024

The development of high-efficiency atomic-level catalysts for energy-conversion and -storage technologies is crucial to address energy shortages. spin states diatomic (DACs) are closely tied their catalytic activity. Adjusting the DACs' active centers can directly modify occupancy d-orbitals, thereby influencing bonding strength between metal sites intermediates as well transfer during electro reactions. Herein, we discuss various techniques characterizing atomic strategies modulating center states. Next, outline recent progress in study effects DACs oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), electrocatalytic nitrogen/nitrate (eNRR/NO

Language: Английский

Citations

29

Recent advances on support materials for enhanced Pt-based catalysts: applications in oxygen reduction reactions for electrochemical energy storage DOI Creative Commons
Feng Zhan, Lingyun Huang, Yue Luo

et al.

Journal of Materials Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 15, 2025

Abstract As the demand for sustainable energy solutions grows, developing efficient conversion and storage technologies, such as fuel cells metal-air batteries, is vital. Oxygen Reduction Reaction (ORR) a significant limitation in electrochemical systems due to its slower kinetics. Although Pt-based catalysts are commonly used address this challenge, their high cost suboptimal performance remain obstacles further development. This review offers comprehensive overview of advanced support materials aimed at improving efficiency, durability, cost-effectiveness catalysts. By examining range materials, including mesoporous carbon, graphene, carbon nanotubes, metal oxides, clarifies relationship between structural properties these supports influence on ORR performance. Additionally, it discusses fundamental characteristics practical applications cells, explores potential future directions optimizing advance technologies. Future research could focus nano-engineering composite material development unlock full catalysts, significantly enhancing economic viability applications.

Language: Английский

Citations

4

f‐p‐d Gradient Orbital Coupling Induced Spin State Enhancement of Atomic Fe Sites for Efficient and Stable Oxygen Reduction Reaction DOI Creative Commons
Ruiqi Cheng,

Xiaoqian He,

Min Jiang

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 21, 2025

Abstract Advancing energy conversion technologies requires cost‐efficient electrocatalysts for the oxygen reduction reaction (ORR). Iron phthalocyanine (FePc) emerges as a scalable and economical ORR electrocatalyst. However, Fe–N 4 configuration in FePc still falls short of satisfied activity stability under electrocatalytic conditions. Here, an effective f‐p‐d (Eu–O–Fe) gradient orbital coupling strategy is introduced by integrating with Eu 2 O 3 (FePc/Eu ) to enhance spin state performance Fe center through precisely designed, synthetic approach. The Eu─O bond promotes electron delocalization shifts from low‐spin intermediate‐spin, increasing e g​ occupancy. This modification optimizes adsorption oxygen‐containing intermediates lowers barrier. Notably, increased accelerates charge transfer releasing more unpaired electrons, improving kinetics. Furthermore, f‐band serves buffer layer compensation during ORR, further stabilizing covalency electronic atomic boosting durability. one‐batch synthesis produces exceeding 300 g FePc/Eu , achieving half‐wave potential 0.931 V (vs RHE) at cost less than 1/15 commercial Pt/C. It demonstrates exceptional aluminum–air batteries, highlighting its significant application potential.

Language: Английский

Citations

4

Boosting Oxygen Reduction Reaction Performance of Fe Single‐Atom Catalysts Via Precise Control of the Coordination Environment DOI Open Access
Shiyu Zhang,

Buwei Sun,

Kang Liao

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

Abstract Fe single‐atom on N‐doped carbon (FeN‐C) catalysts emerge as promising alternatives to commercial Pt/C for the oxygen reduction reaction. Heterogeneous atom doping is proposed be effective modulating catalyst performance. Despite this, relationship between fine coordination structure of doped atoms and catalytic activity central metal site remains poorly understood. Herein, with S in either first shell (FeSN–C) or second (FeN–SC) active are synthesized compare effects different structure. FeN–SC exhibits prominent performance a half‐wave potential 0.92 V rotating disk electrode peak power density 251 mW cm −2 zinc–air battery. Theoretical studies reveal that effectively modulates electronic charge transfer at center. Compared directly coordinated within shell, located more optimizing adsorption desorption energy barriers oxygen‐containing intermediates sites. This study provides new strategy adjust by engineering multilayer center catalyst.

Language: Английский

Citations

3

Reversible Angle Distortion-Dependent Electrochemical CO2 Reduction on Cobalt Phthalocyanine DOI
Bingbao Mei, Jianing Mao,

Zhaofeng Liang

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 7, 2025

Deducing the local electronic and atomic structural changes in active sites during electrochemical carbon dioxide reduction is essential for elucidating intrinsic mechanisms developing highly catalysts that are stable a long duration. Herein, utilizing operando valence-to-core X-ray emission spectroscopy high energy-resolution fluorescence detected absorption near-edge structure, combined with spectroscopic calculations, structure evolutions of model cobalt phthalocyanine (CoPc) were quantitatively elucidated. Under real reaction conditions, CoPc undergoes reversible angle distortion while maintaining constant metal-ligand bond length, causing energy levels split d orbitals electron density molecular orbitals. The further influences interactions among ligands, intermediates, metal centers. change CO Faraday efficiency was also determined, demonstrating robustness. demonstrated findings serve as an important contribution to determine structure-performance relationship which enlightens rational design atomically dispersed site activity emphasize capabilities resolution toward analyzing metal-implanted N-doped catalysts.

Language: Английский

Citations

2

CeO2 Boosted Fe‐N5 Electrocatalyst via Relay Catalysis for Modulating Oxygen Reduction Reaction in Al‐Air Batteries DOI Open Access
Yumeng Zhang, Fei He, Yijun Gao

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

Abstract Atomically dispersed iron‐nitrogen‐carbon (Fe‐N‐C) catalysts have demonstrated promising oxygen reduction reaction (ORR) activity. It poses a formidable challenge to simultaneously optimize the adsorption energies of multiple intermediates at single active site. In addition, lack long‐term stability remains significant problem due unavoidable 2‐electron by‐product hydrogen peroxide (H 2 O ). Here, sites are achieved modulate energy while removing by growing second site CeO nanoparticles in situ on surface hollow‐structured Fe‐N 5 , thus improving efficiency and /CeO . Density functional theory (DFT) calculations employed probe into synergistic catalytic interaction between proposing relay mechanism underlying enhanced Furthermore, catalyst is ability scavenge inhibit its destructive effects Additionally, liquid Al – air batteries equipped with display higher power density. This work proffers an innovative vista for conception refinement multi‐active‐site excellent performance prolonged lifespan.

Language: Английский

Citations

2

Cation-induced interface electric field redistribution and molecular orbital coupling in Co-FeS/MoS2 for boosting electrocatalytic overall water splitting DOI

Jipeng Dong,

Bohan An,

Weilong Liu

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 498, P. 155102 - 155102

Published: Aug. 28, 2024

Language: Английский

Citations

15