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

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

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Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Окт. 13, 2023

Abstract Single-atom catalysts (SACs) have garnered increasingly growing attention in renewable energy scenarios, especially electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability. The intensive efforts towards the rational design synthesis SACs with versatile local configurations significantly accelerated development efficient sustainable electrocatalysts for a wide range electrochemical applications. As an emergent coordination avenue, intentionally breaking planar symmetry by adding ligands axial direction metal single atoms offers novel approach tuning both geometric structures, thereby enhancing electrocatalytic performance at active sites. In this review, we briefly outline burgeoning research topic axially coordinated provide comprehensive summary recent advances synthetic strategies Besides, challenges outlooks field also been emphasized. present review provides in-depth understanding SACs, which could bring new perspectives solutions fine regulation structures catering high-performing electrocatalysis.

Язык: Английский

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Electrochemical CO2 reduction coupled with alternative oxidation reactions: Electrocatalysts, electrolytes, and electrolyzers

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 341, С. 123291 - 123291

Опубликована: Сен. 16, 2023

Язык: Английский

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Dual-axial engineering on atomically dispersed catalysts for ultrastable oxygen reduction in acidic and alkaline solutions

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(6)

Опубликована: Янв. 30, 2024

Atomically dispersed catalysts are a promising alternative to platinum group metal for catalyzing the oxygen reduction reaction (ORR), while limited durability during electrocatalytic process severely restricts their practical application. Here, we report an atomically Co-doped carbon−nitrogen bilayer catalyst with unique dual-axial Co–C bonds (denoted as Co/DACN) by smart phenyl-carbon-induced strategy, realizing highly efficient ORR in both alkaline and acidic media. The corresponding half-wave potential is up 0.85 0.77 V (vs. reversible hydrogen electrode (RHE)) 0.5 M H 2 SO 4 0.1 KOH, respectively, representing best activity among all non-noble reported date. Impressively, Zn–air battery (ZAB) equipped Co/DACN cathode achieves outstanding after 1,688 h operation at 10 mA cm −2 high current density (154.2 ) peak power (210.1 mW ). Density functional theory calculations reveal that cross-linking Co−C of significantly enhance stability also facilitate 4e − pathway forming joint electron pool due improved interlayer mobility. We believe axial engineering opens broad avenue develop high-performance heterogeneous electrocatalysts advanced energy conversion storage.

Язык: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Год журнала: 2024, Номер 11(33)

Опубликована: Июль 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Язык: Английский

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Regulating the Electronic Configuration of Ni Sites by Breaking Symmetry of Ni‐Porphyrin to Facilitate CO₂ Photocatalytic Reduction

Advanced Functional Materials, Год журнала: 2024, Номер 34(25)

Опубликована: Фев. 10, 2024

Abstract Adapting the coordination environment to influence electronic configuration of active sites represents an efficient approach for improving photocatalytic performance CO 2 reduction reaction (CO RR) but how execute it precisely remains challenging. Herein, heteroatom‐substitution in Ni‐porphyrin break symmetry Ni center is proposed be effective solution. Based on this, two symmetry‐breaking Ni‐porphyrins, namely Ni(Cl)ON 3 Por and Ni(Cl)SN , are designed successfully prepared. By theoretical calculation, found that efficiently regulates d orbital energy levels center. Furthermore, experimental findings jointly revealed Ni‐porphyrins facilitates generation highly reactive I species during catalytic process, effectively stabilizing reducing barrier formation key * COOH intermediate. As a result, gave production rates 24.7 38.8 mmol g −1 h as well selectivity toward 94.0% 96.4%, respectively, outperforming symmetric NiN 4 rate 6.6 82.8%). These offer microscopic insights into modulate activity by tuning rational design competent catalyst RR photocatalysis.

Язык: Английский

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Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO₂RR

ACS Catalysis, Год журнала: 2024, Номер 14(11), С. 8889 - 8898

Опубликована: Май 24, 2024

The formation of dual-atom catalysts or heteroatom ligand modulation is the most promising strategy for optimizing single–atom (SACs) more efficient conversion CO2 to valuable chemicals. However, ligands introduced into dual-atomic sites are expected but still under-explored. In this study, a Fe–Ni pair electrocatalyst with N– and S–coordination in porous carbon nanosheets was conceptually predicted electrocatalytic reduction CO (CO2RR). contrast SACs traditional diatomic (DACs), joined can balance cooperative activities Fe Ni sites, making adsorption configuration bidentate at both sites. This regulation leads substantial change CO* from facilitating desorption boosting CO2RR. Experimental results demonstrate that obtained FeNi–NSC catalyst achieves high selectivity Faradaic efficiencies 96.1%, remarkable activity turnover frequency 6526.9 h–1 −1.0 V, which were over 4.5 2.5 times those single work gives us insight designing highly effective guided by theoretical calculation.

Язык: Английский

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MOF‐derived Carbon‐Based Materials for Energy‐Related Applications

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Abstract New carbon‐based materials (CMs) are recommended as attractively active due to their diverse nanostructures and unique electron transport pathways, demonstrating great potential for highly efficient energy storage applications, electrocatalysis, beyond. Among these newly reported CMs, metal–organic framework (MOF)‐derived CMs have achieved impressive development momentum based on high specific surface areas, tunable porosity, flexible structural‐functional integration. However, obstacles regarding the integrity of porous structures, complexity preparation processes, precise control components hinder regulation interface engineering in CMs. In this context, review systematically summarizes latest advances tailored types, processing strategies, energy‐related applications MOF‐derived focuses structure‐activity relationship metal‐free carbon, metal‐doped metallide‐doped carbon. Particularly, intrinsic correlation evolutionary behavior between synergistic interaction micro/nanostructures species with electrochemical performances emphasized. Finally, insights perspectives relevant research presented, future prospects challenges discussed, providing valuable guidance boost high‐performance electrodes a broader range application fields.

Язык: Английский

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Engineering Electronic Structure of Nitrogen‐Carbon Sites by sp³‐Hybridized Carbon and Incorporating Chlorine to Boost Oxygen Reduction Activity

Angewandte Chemie International Edition, Год журнала: 2023, Номер 63(1)

Опубликована: Ноя. 30, 2023

Development of efficient and easy-to-prepare low-cost oxygen reaction electrocatalysts is essential for widespread application rechargeable Zn-air batteries (ZABs). Herein, we mixed NaCl ZIF-8 by simple physical milling pyrolysis to obtain a metal-free porous electrocatalyst doped with Cl (mf-pClNC). The mf-pClNC exhibits good reduction (ORR) activity (E1/2 =0.91 V vs. RHE) high stability in alkaline electrolyte, exceeding most the reported transition metal carbon-based being comparable commercial Pt/C electrocatalysts. Likewise, also shows state-of-the-art ORR acidic electrolyte. From experimental theoretical calculations, better likely originated from fact that introduced promotes increase sp3 -hybridized carbon, while carbon together modify electronic structure N-adjacent carbons, as active sites, molten-salt etching provides abundant paths transport electrons/protons. Furthermore, liquid ZAB using cathode fulfilling performance peak power density 276.88 mW cm-2 . Flexible quasi-solid-state constructed an exciting both at low, room temperatures.

Язык: Английский

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Ultrathin, Cationic Covalent Organic Nanosheets for Enhanced CO₂ Electroreduction to Methanol

Advanced Materials, Год журнала: 2023, Номер 36(17)

Опубликована: Ноя. 7, 2023

Metalloporphyrins and metallophthalocyanines emerge as popular building blocks to develop covalent organic nanosheets (CONs) for CO

Язык: Английский

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