Catalase-like Fe Nanoparticles and Single Atoms Catalysts with Boosted Activity and Stability of Oxygen Reduction for Pesticide Detection DOI

Peipei Zong,

Lei Jiao, Ruimin Li

et al.

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(24), P. 10021 - 10027

Published: June 6, 2024

Although oxygen reduction reaction (ORR) as an effective signal amplification strategy has been extensively investigated for the improvement of sensitivity electrochemical sensors, their activity and stability are still a great challenge. Herein, single-atom Fe (FeSA) nanoparticles (FeNP) on nitrogen-doped carbon (FeSA/FeNP) catalysts demonstrate highly active stable ORR performance, thus achieving sensitive sensing organophosphorus pesticides (OPs). Experimental investigations indicate that FeNP in FeSA/FeNP can improve by adjusting electronic structure FeSA sites. Besides, owing to excellent catalase-like activity, rapidly consume situ generated H2O2 process avoid leakage sites, thereby improving ORR. Utilizing performance FeSA/FeNP, sensor OPs is established based thiocholine-induced poison demonstrating satisfactory stability. This work provides new insight into design high sensing.

Language: Английский

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

Xiaohong Zou,

Mingcong Tang, Qian Lü

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(2), P. 386 - 424

Published: Nov. 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.

Language: Английский

Citations

71

Optimizing Integrated‐Loss Capacities via Asymmetric Electronic Environments for Highly Efficient Electromagnetic Wave Absorption DOI
Panbo Liu, Shuyun Zheng,

Zizhuang He

et al.

Small, Journal Year: 2024, Volume and Issue: 20(43)

Published: July 2, 2024

Asymmetric electronic environments based on microscopic-scale perspective have injected infinite vitality in understanding the intrinsic mechanism of polarization loss for electromagnetic (EM) wave absorption, but still exists a significant challenge. Herein, Zn single-atoms (SAs), structural defects, and Co nanoclusters are simultaneously implanted into bimetallic metal-organic framework derivatives via two-step dual coordination-pyrolysis process. Theoretical simulations experimental results reveal that coupling interactions between SAs defects delocalize symmetric generate additional dipole without sacrificing conduction owing to compensation carbon nanotubes. Moreover, with large nanocurvatures induce strong interfacial electric field, activate superiority heterointerfaces promote polarization. Benefiting from aforementioned merits, resultant deliver an optimal reflection -58.9 dB effective absorption bandwidth is 5.2 GHz. These findings provide innovative insight clarifying microscopic asymmetric electron viewpoint inspire generalized modulation engineering optimizing EM absorption.

Language: Английский

Citations

53

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

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(23)

Published: Jan. 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.

Language: Английский

Citations

30

Synergy of Ni Nanoclusters and Single Atom Site: Size Effect on the Performance of Electrochemical CO2 Reduction Reaction and Rechargeable Zn−CO2 Batteries DOI

Kanghua Miao,

Jundi Qin,

Jun Yang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(33)

Published: April 18, 2024

Abstract The design of bifunctional electrocatalysts toward reduction reaction carbon dioxide (ECO 2 RR) and oxygen evolution (OER) in aqueous rechargeable Zn─CO batteries (ZABs) still poses a significant challenge. Herein, Ni clusters (Ni x ) 0.5 0.8 nm diameter coupled with single site (Ni−N 4 −C), denoted as Ni−N /Ni 5 8 , respectively, are synthesized the size effect nanoclusters studied. exhibits an ≈100% Faradaic efficiency ( FE CO ECO RR for from −0.4 to −0.8 V versus reversible hydrogen electrode, superior that −C = 55.0%) 80.0%). OER performance or comparable commercial RuO but outperform −C. Theoretical calculation indicates * COOH intermediates bond synergistically atom site, promoting activation reducing energy barrier potential determining step RR. Such is strongly size‐dependent larger result too strong binding intermediates, impede formation CO. As cathode electrocatalyst alkaline ZABs, peak power density 11.7 mW cm −2 cycling durability over 1200 cycles 420 h.

Language: Английский

Citations

29

Recent Design Strategies for M‐N‐C Single‐Atom Catalysts in Oxygen Reduction: An Entropy Increase Perspective DOI
Wei Yan, Wenmiao Chen, Yanli Chen

et al.

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

Asymmetric Coordination Regulating D‐Orbital Spin‐Electron Filling in Single‐Atom Iron Catalyst for Efficient Oxygen Reduction DOI
Yizhe Li, Hao Sun,

Longtao Ren

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(28)

Published: May 9, 2024

The single-atom Fe-N-C catalyst has shown great promise for the oxygen reduction reaction (ORR), yet intrinsic activity is not satisfactory. There a pressing need to gain deeper understanding of charge configuration and develop rational modulation strategies. Herein, we have prepared Fe with co-coordination N O (denoted as Fe-N/O-C) adjacent defect, proposing strategy optimize d-orbital spin-electron filling sites by fine-tuning first coordination shell. Fe-N/O-C exhibits significantly better ORR compared its counterpart commercial Pt/C, much more positive half-wave potential (0.927 V) higher kinetic current density. Moreover, using catalyst, Zn-air battery proton exchange membrane fuel cell achieve peak power densities up 490 1179 mW cm

Language: Английский

Citations

22

Spatially Axial Boron Coordinated Single‐Atom Nanozymes with Boosted Multi‐Enzymatic Performances for Periodontitis Treatment DOI
Wendong Liu,

Enyu Shi,

Hao Wu

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: May 3, 2024

Abstract Single‐atom nanozymes (SAzymes) have made significant strides in antibacterial treatment but fall short as natural enzyme and drug replacements due to limited catalytic performance. Here, a rational strategy is presented for incorporating spatially axial boron (B) ligands effectively modulate the local coordination environment of planar Fe─N 4 motifs (Fe─B/N─C SAzymes). With electronic modulation, Fe─B/N─C SAzymes exhibit significantly enhanced oxidase‐, peroxidase‐, catalase‐like activities. Theoretical calculations highlight that B adjust charge distribution around active center, which facilitates heterolysis H 2 O desorption , resulting accelerated decomposition. Furthermore, intrinsic photothermal effect enhances multienzyme‐like activities, rapidly generating abundant reactive oxygen species (ROS), achieving chemodynamic/photothermal synergistic therapy impressive disinfection against periodontal‐related pathogenic bacteria. These findings offer distinctive viewpoint optimizing with ligand enhance their performance effectiveness periodontitis therapy.

Language: Английский

Citations

20

Electronic Structure Modulation in N, P, S Tri‐Doped Nanofibers with Interpenetrated Pores for Enhanced Oxygen Reduction Reaction DOI Open Access
Xiaoxue Xu, Hongliang Wu, Yan Yan

et al.

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

Published: Jan. 16, 2025

Abstract Multi‐heteroatom‐doped metal‐free carbons with well‐tailored electronic structures are regarded as promising oxygen reduction reaction (ORR) catalysts. However, their active sites often hindered by the carbon matrix, resulting in reduced catalytic activity. Herein, nitrogen, phosphorus, and sulfur tri‐doped hollow hierarchical porous nanofibers (NPS‐HPCNFs) interpenetrated pores synthesized using a facile coaxial electrospinning method. The distinctive steric confinement induced created positive microenvironment for ORR. As result, resultant NPS‐HPCNF catalyst exhibits half‐wave potential ( E 1/2 ) of 0.86 V (vs. RHE) superb long‐term stability 0.1 m KOH. Furthermore, zinc‐air battery (ZAB) assembled achieves great peak power density 210 mW cm −2 superior specific capacity 795 mAh g −1 , outperforming commercial Pt/C candidate. In addition, functional theory (DFT) calculations reveal that synergistic effect N, P, S tri‐doping combined defect effectively regulated structure significantly enhanced * OOH adsorption, thus accelerating ORR process. Therefore, abundant represent eco‐friendly alternative to state‐of‐the‐art electrocatalysts various electrochemical energy applications.

Language: Английский

Citations

2

Accelerated proton-coupled electron transfer kinetics of iron phthalocyanine for oxygen reduction via heteropoly blue clusters DOI

Lingzhe Meng,

Shuwen Niu, Zhengyu Wei

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125080 - 125080

Published: Jan. 1, 2025

Language: Английский

Citations

2

Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction DOI
Tong Liu,

Yudan Chen,

Airong Xu

et al.

Science China Chemistry, Journal Year: 2024, Volume and Issue: 67(4), P. 1352 - 1359

Published: Jan. 15, 2024

Language: Английский

Citations

14