Atomically dispersed multi-site catalysts: bifunctional oxygen electrocatalysts boost flexible zinc–air battery performance

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

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Bimetallic Single-Atom Catalysts for Water Splitting

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

Published: Sept. 25, 2024

Abstract Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead global transition fossil fuel-independent society. The field of catalysis been revolutionized by single-atom catalysts (SACs), which exhibit unique and intricate interactions between atomically dispersed metal atoms their supports. Recently, bimetallic SACs (bimSACs) have garnered significant attention for leveraging synergistic functions two ions coordinated on appropriately designed BimSACs offer an avenue rich metal–metal metal–support cooperativity, potentially addressing current limitations in effectively furnishing transformations involve synchronous proton–electron exchanges, substrate activation reversible redox cycles, simultaneous multi-electron transfer, regulation spin states, tuning electronic properties, cyclic states low energies. This review aims encapsulate growing advancements bimSACs, emphasis pivotal role generation via splitting. We subsequently delve into advanced experimental methodologies elaborate characterization SACs, elucidate discuss local coordination environment. Overall, we present comprehensive discussion deployment bimSACs both evolution reaction oxygen reaction, half-reactions electrolysis process.

Language: Английский

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Manipulating the Electronic Properties of an Fe Single Atom Catalyst via Secondary Coordination Sphere Engineering to Provide Enhanced Oxygen Electrocatalytic Activity in Zinc‐Air Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(44)

Published: Sept. 16, 2024

Abstract Oxygen reduction and evolution reactions are two key processes in electrochemical energy conversion technologies. Synthesis of nonprecious metal, carbon‐based electrocatalysts with high oxygen bifunctional activity stability is a crucial, yet challenging step to achieving conversion. Here, an approach address this issue: synthesis atomically dispersed Fe electrocatalyst (Fe 1 /NCP) over porous, defect‐containing nitrogen‐doped carbon support, described. Through incorporation phosphorus atom into the second coordination sphere iron, durability boundaries catalyst pushed unprecedented level alkaline environments, such as those found zinc‐air battery. The rationale delicately incorporate P heteroatoms defects close central metal sites (FeN 4 ‐OH) order break local symmetry electronic distribution. This enables suitable binding strength oxygenated intermediates. In situ characterizations theoretical studies demonstrate that these synergetic interactions responsible for stability. These intrinsic advantages /NCP enable potential gap mere 0.65 V power density 263.8 mW cm −2 when incorporated findings underscore importance design principles access high‐performance green

Language: Английский

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Regulation of d‐Orbital Electron in Fe‐N₄ by High‐Entropy Atomic Clusters for Highly Active and Durable Oxygen Reduction Reaction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(46)

Published: June 19, 2024

Abstract Simultaneously improving activity and stability is a crucial yet challenge in the development of metallic single‐atom‐based catalysts. In current work, novel approach introduced to address this issue by combining post‐adsorption secondary pyrolysis techniques create synergistic catalytic system, which single atoms (SAs) Fe sites played NC matrix (Fe─NC) are coupled with high‐entropy atomic clusters (HEACs). Theoretical calculations reveal that incorporation HEACs lead rehybridization 3d orbital configuration Fe‐N 4 , helps balance adsorption/desorption energy oxygenated intermediates. situ spectroscopy further reveals rate‐limiting step OH * desorption on HEAC/Fe─NC oxygen reduction reaction (ORR) more facile compared Fe─NC, implying higher ORR activity. Moreover, effect diffusion activation barriers entropy contributes structural HEAC/Fe─NC, resulting remarkable durability. Consequently, unique catalyst exhibits half‐wave potentials 0.927 0.828 V an aqueous solution KOH (0.1 m ) HClO ), respectively, along excellent The findings propose strategy for modulating electronic structure SAs catalysts enhancing their through strong interactions between HEACs.

Language: Английский

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Principles of coordination structure design of single-atom catalysts in electrocatalytic oxygen reduction reaction

Rare Metals, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 3, 2025

Language: Английский

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Facile Microwave Synthesis of Kilogram‐Scale Electrocatalysts with Nanocarbons Bridged Cobalt Active Sites for Enhanced Oxygen Electrocatalysis

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

Published: March 30, 2025

Abstract Oxygen reductions and evolution reactions (ORR/OER) are pivotal electrochemical processes in fuel cells metal‐air batteries, yet the rapid, large‐scale production of efficient ORR/OER electrocatalysts remains challenging. Herein, a groundbreaking microwave‐synthesis strategy is presented that enables rapid facile preparation kilogram‐scale electrocatalysts. The unique microwave irradiation generates instantaneous thermal energy, facilitating formation nano‐carbon bridges interconnect high‐density active sites comprising cobalt single atoms nanoparticles. This innovative architectural configuration significantly enhances kinetics electron/mass transfer maximizing accessibility sites. optimized carbon‐bridged catalyst (CBCo‐800) demonstrates commendable half‐wave potential ( E 1/2 ) 0.86 V versus RHE minimal overpotential difference (Δ 0.696 V. Furthermore, lab‐assembled zinc‐air battery utilizing CBCo‐800 achieved great specific capacity 794 mAh g −1 sustained over 650 h, outperforming commercial Pt/C RuO 2 catalysts. Density functional theory (DFT) calculations elucidate nanocarbon bridge between dual‐active boosts oxygen activation optimizes adsorption/desorption dynamics *OH/*OOH intermediates, thereby lowering energy barriers for ORR/OER. study offers solution producing site materials, also establishes robust platform mass high‐performance

Language: Английский

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The unique Co2Mn1N8 structure enhances peroxymonosulfate activation and singlet oxygen generation through a localized electric field

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 162674 - 162674

Published: April 1, 2025

Language: Английский

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Metal-organic-framework-derived dual-atom catalysts: from synthesis to electrocatalytic applications

Materials Science and Engineering R Reports, Journal Year: 2024, Volume and Issue: 162, P. 100886 - 100886

Published: Nov. 23, 2024

Language: Английский

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Synergistic Effect of Electrocatalyst for Enhanced Oxygen Reduction Reaction: Low Pt-Loaded CuPt Alloy Nanoparticles Supported on N-Doped Hierarchical Porous Carbon

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(11), P. 13893 - 13902

Published: March 11, 2024

It is challenging to synthesize oxygen reduction reaction (ORR) electrocatalysts that are highly efficient, affordable, and stable for use in proton exchange membrane fuel cells. To address this challenge, we developed a low platinum-loading (only 6.68% wt) ORR catalyst (PtCu1-NC), comprising CuPt nanoparticles (average size: 1.51 nm) supported on the N-doped carbon substrates. PtCu1-NC possesses high specific surface area of 662 m2 g–1 hierarchical porous structure, facilitating efficient mass transfer. The synergistic effect from introduced copper electron nitrogen modify electronic structure platinum, effectively accelerating enhancing stability. Density functional theory calculations demonstrate catalytic mechanism further verify effect. Electrochemical assessments indicate exhibits activity 5.3 5.6 times higher, respectively, than commercial Pt/C. half-wave potential 27 mV more positive electrochemical active value 104.3 g–1, surpassing Approximately 78% current retained after 10,000 s chronoamperometry measurement. These results highlight effectiveness alloying improving performance.

Language: Английский

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Regulating Local Electron Distribution of Cu Electrocatalyst via Boron Doping for Boosting Rapid Absorption and Conversion of Nitrate to Ammonia

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(48)

Published: Oct. 15, 2024

Abstract The electrochemical reduction of nitrate to ammonia (NO 3 RR) is an effective route synthesis with the characteristics low energy input. However, complex multi‐electron/proton transfer pathways associated this reaction may trigger accumulation competitive by‐products. Herein, boron (B)‐doped Cu electrode (denoted as B–Cu 2 O/Cu/CP) “all‐in‐one” catalyst prepared by one‐step electrodeposition strategy. Caused B doping, charge redistribution and local coordination environment O/Cu species are modulated, resulting in exposure active sites on O/Cu/CP catalyst. In‐situ Fourier transform infrared spectroscopy theoretical investigations demonstrate that both O modulated can effectively enhance adsorption NO − facilitate conversion intermediate by‐products, thus promoting direct NH . Consequently, a remarkable Faradaic efficiency 92.74% be obtained minimal It expected work, based heterogeneous will open maneuverable versatile way for design catalysts.

Language: Английский

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