Elucidation of the mechanistic origin of spin-state-dependent P-doped Fe single-atom catalysts for the oxidation of organic pollutants through peroxymonosulfate activation

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 341, С. 123289 - 123289

Опубликована: Сен. 14, 2023

Язык: Английский

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Tailoring the coordination environment of double-atom catalysts to boost electrocatalytic nitrogen reduction: a first-principles study

Nanoscale, Год журнала: 2023, Номер 15(39), С. 16056 - 16067

Опубликована: Янв. 1, 2023

Tailoring the coordination environment is an effective strategy to modulate electronic structure and catalytic activity of atomically dispersed transition-metal (TM) catalysts, which has been widely investigated for single-atom catalysts but received less attention emerging double-atom (DACs). Herein, based on first-principles calculations, taking commonly studied N-coordinated graphene-based DACs as references, we explored effect engineering behaviors towards electrocatalytic nitrogen reduction reaction (NRR), realized through replacing one N atom by B or O form B, O, co-coordinated DACs. We found that co-coordination could significantly strengthen N2 adsorption alter pattern TM dimer active center, greatly facilitates activation. Moreover, DACs, linear scaling relationship between binding strengths key intermediates can be attenuated. Consequently, Mn2 exhibiting ultralow limiting potential -0.27 V, climb peak volcano. In addition, experimental feasibility this DAC system was also identified. Overall, benefiting from effect, chemical performance NRR boosted. This phenomena understood adjusted center due changes its microenvironment, affects strength (pattern) pathways, leading enhanced selectivity. work highlights importance in developing other important reactions.

Язык: Английский

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Electronic structure regulation of the Fe-based single-atom catalysts for oxygen electrocatalysis

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

Опубликована: Янв. 9, 2024

Язык: Английский

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Substantial Impact of Spin State Evolution in OER/ORR Catalyzed by Fe–N–C

ACS Catalysis, Год журнала: 2024, Номер 14(9), С. 6816 - 6826

Опубликована: Апрель 18, 2024

The Fe-embedded N-doped graphene (Fe–N–C) is the most representative single atom catalyst (SAC) that has shown great potentiality in electrocatalysis, such as oxygen reduction reaction (ORR) and evolution (OER). However, active moiety of Fe–N–C still elusive due to contradictory experimental results. Moreover, early simulations mainly focus on thermodynamic potential adsorbates, while effect spin multiplicity receives little attention. To explore role we employ constant-potential density functional theory (DFT) systematically study structural high-spin (HS) intermediate-spin (IS) FeN4 site (marked by FeN4HS/IS) OER ORR processes. With consideration multiplicity, our simulation shows spontaneous oxidation from Fe(II)N4IS Fe(III)N4HS at U = 0.4 V versus SHE. Further indicates FeN4IS undergoes a sequential adsorption *OH *OOH along with increase, which leads state transition IS HS. According free energy analysis, FeN4HS*OOH confirmed be practical centers OER, FeN4HS*OH are assigned center low high overpotentials. predicted activity agrees situ X-ray absorption near-edge spectroscopy (XANES) 57Fe Mössbauer measurement Xiao et al. [Microporous Framework Induced Synthesis Single-Atom Dispersed Fe-NC Acidic Catalyst its In Situ Reduced Fe-N4 Active Site Identification Revealed X-Ray Absorption Spectroscopy. ACS Catal. 2018, 8, 2824–2832]. Based geometry orbital bond length Fe–N coordination number Fe found have significant impact d splitting thus induce turnover HS/IS stability OER/ORR intermediates. Our brings comprehensive insights into Fe–N–C, reveals significance electrocatalysis benefits further theoretical design SACs perspective effects.

Язык: Английский

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Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction

Electrochemical Energy Reviews, Год журнала: 2024, Номер 7(1)

Опубликована: Июнь 5, 2024

Язык: Английский

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Tuning the local coordination environment of single-atom catalysts for enhanced electrocatalytic activity

EnergyChem, Год журнала: 2024, Номер 6(2), С. 100119 - 100119

Опубликована: Фев. 17, 2024

Язык: Английский

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Structure–Activity Relationships in Oxygen Electrocatalysis

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 30, 2024

Abstract Oxygen electrocatalysis, as the pivotal circle of many green energy technologies, sets off a worldwide research boom in full swing, while its large kinetic obstacles require remarkable catalysts to break through. Here, based on summarizing reaction mechanisms and situ characterizations, structure–activity relationships oxygen electrocatalysts are emphatically overviewed, including influence geometric morphology chemical structures electrocatalytic performances. Subsequently, experimental/theoretical is combined with device applications comprehensively summarize cutting‐edge according various material categories. Finally, future challenges forecasted from perspective catalyst development applications, favoring researchers promote industrialization electrocatalysis at an early date.

Язык: Английский

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Atomically Dispersed Dual-Metal ORR Catalyst with Hierarchical Porous Structure for Zn–Air Batteries

ACS Applied Materials & Interfaces, Год журнала: 2024, Номер 16(10), С. 12398 - 12406

Опубликована: Фев. 27, 2024

The metal-nitrogen-carbon (M-N-C)-based catalysts are promising to replace PGM (platinum group metal) accelerate oxygen reduction reaction due their excellent electrocatalytic performance. However, the inferior intrinsic activity and poor active site density confining further improvement in Modulating electronic structure reasonably designing pore widely acknowledged effective strategies boost of M-N-C catalysts. it is a great challenge form abundant pores regulate via facile method. Herein, hierarchical, porous dual-atom catalyst FeNi-NPC-1000 has been architectured by Na

Язык: Английский

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Wood-derived Fe cluster-reinforced asymmetric single-atom catalysts and weather-resistant organohydrogel for wide-temperature flexible Zn–air batteries

Energy & Environmental Science, Год журнала: 2024, Номер 17(13), С. 4746 - 4757

Опубликована: Янв. 1, 2024

All wood-based wide-temperature flexible Zn–air battery.

Язык: Английский

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Sulfur‐Tuned Main‐Group Sb−N−C Catalysts for Selective 2‐Electron and 4‐Electron Oxygen Reduction

Advanced Materials, Год журнала: 2024, Номер 36(27)

Опубликована: Апрель 15, 2024

The selective oxygen reduction reaction (ORR) is important for various energy conversion processes such as the fuel cells and metal-air batteries 4e

Язык: Английский

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