Spin‐Selective Coupling in Mott–Schottky Er₂O₃‐Co Boosts Electrocatalytic Oxygen Reduction

Small Methods, Год журнала: 2023, Номер 7(7)

Опубликована: Апрель 8, 2023

Abstract Alkaline oxygen reduction reaction (ORR) is critical to electrochemical energy conversion technology, yet the rational breaking of thermodynamic inhibition for ORR through spin regulation remains a challenge. Herein, Mott–Schottky catalyst consisting Er 2 O 3 ‐Co particles uniformly implanted into carbon nanofibers (Er ‐Co/CNF) designed enhancing via spin‐selective coupling. The optimized ‐Co/CNF affords high half‐wave potential (0.835 V vs reversible hydrogen electrode, RHE) and onset (0.989 RHE ) surpassing individual Co/CNF /CNF. Theoretical calculations reveal introduction optimizes electronic structure Co Er(4f)‐O(2p)‐Co(3d) gradient orbital coupling, resulting in significantly enhanced performance. Through induced spin‐up hole 3d states endows Er‐O‐Co unit active site with coupling channel electron transition. This favors decrease gap potential‐limiting step, thus achieving theoretical limiting 0.77 ‐Co. Moreover, practicability as an air‐cathode also demonstrated Zn‐air batteries. work believed provide, new perspectives design efficient electrocatalysts by engineering rare‐earth oxides.

Язык: Английский

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Dual template-induced construction of three-dimensional porous SiO2/NC/Co-CNTs heterostructure with highly dispersed active sites for efficient oxygen evolution reaction

Tungsten, Год журнала: 2023, Номер 6(3), С. 585 - 595

Опубликована: Дек. 6, 2023

Язык: Английский

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Unified ORR mechanism criteria via charge–spin–coordination of Fe functional units

Energy & Environmental Science, Год журнала: 2023, Номер 17(1), С. 27 - 48

Опубликована: Ноя. 10, 2023

The “charge–spin–coordination” relationship was introduced into Fe functional units (Fe-FUs) in multiple forms to comprehensively analyze their activity sources and degradation mechanisms during the ORR process.

Язык: Английский

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In Situ Electrochemical Restructuring B‐Doped Metal–Organic Frameworks as Efficient OER Electrocatalysts for Stable Anion Exchange Membrane Water Electrolysis

Small, Год журнала: 2023, Номер 20(22)

Опубликована: Дек. 28, 2023

Abstract Metal organic frameworks (MOFs) are promising as effective electrocatalysts toward oxygen evolution reaction (OER). However, the origin of OER activity for MOF‐based is still unclear because their structure reconstruction during electrocatalysis process. Here, a novel MOF (B‐MOF‐Zn‐Co) with spherical superstructure developed by hydrothermal treatment zeolitic imidazolate framework‐Zn, Co (ZIF‐Zn‐Co) using boric acid. The resultant B‐MOF‐Zn‐Co shows high low overpotential 362 mV at 100 mA cm −2 . Remarkably, displays excellent stability only 3.6% voltage delay over 300 h in alkaline electrolyte. Surprisingly, thoroughly transforms into B‐doped CoOOH (B‐CoOOH) electrolysis process, which served actual active material electrocatalytic performance. newly‐formed B‐CoOOH possesses lower energy barrier potential‐determining step (PDS) OOH * formation compared CoOOH, benefiting activity. More importantly, based anion exchange membrane water electrolytic cell (AEMWE) demonstrates continuously durable operation stable current density 200 h, illustrating its potential application practice electrolysis. This work offers an situ electrochemical strategy development and AEMWE.

Язык: Английский

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Advances in polymer electrolytes for solid-state zinc–air batteries

Materials Chemistry Frontiers, Год журнала: 2023, Номер 7(18), С. 3994 - 4018

Опубликована: Янв. 1, 2023

Schematic illustration of the main research characteristics polymer electrolytes for solid-state zinc–air batteries.

Язык: Английский

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Noble metal-free N-doped carbon-based electrocatalysts for air electrode of rechargeable zinc-air battery

Science China Materials, Год журнала: 2023, Номер 66(8), С. 2953 - 3003

Опубликована: Июль 6, 2023

Язык: Английский

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Carbon-based nanoarrays embedded with Ce-doped ultrasmall Co2P nanoparticles enable efficient electrooxidation of 5-hydroxymethylfurfural coupled with hydrogen production

Science China Chemistry, Год журнала: 2023, Номер 66(7), С. 2141 - 2152

Опубликована: Июнь 20, 2023

Язык: Английский

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Revealing the Synergistic Enhancement Effect of Dual Metal RuFe(Co) Sites for Bifunctional Oxygen Catalysis

ACS Materials Letters, Год журнала: 2023, Номер 5(6), С. 1656 - 1664

Опубликована: Май 5, 2023

Modifying the geometric and electronic structures of metal–N–C single-atom catalysts to improve their catalytic activities is quite desirable challenging. Here, theoretical analysis experiment indicate inherent synergistic effect dual metal sites in N-doped carbon for bifunctional ORR OER. Specifically, introducing Ru generate RuFe–N–C or RuCo–N–C double-atom (DACs) can significantly enhance ORR/OER Fe(Co) sites, exceeding equivalent single Fe(Co)–N–C Ru–N–C. Investigations a series RuM–N–C DACs reveal that intriguing results from modified charge density d-band center by combining two optimized atoms, which affects adsorption energies intermediates activity. Based on these guidelines, synthesized using bimetal MOF as precursor, it exhibits exceptional alkaline media with small ΔE 0.63 V, outperforming Fe–N–C, Ru–N–C, even commercial Pt/C-RuO2.

Язык: Английский

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Regulating atomic Fe/Cu dual sites with unsymmetrical Fe-N6 and Cu-N1S2 coordination for promoting bifunctional oxygen electrocatalysis in advanced zinc-air batteries

Energy storage materials, Год журнала: 2024, Номер 68, С. 103342 - 103342

Опубликована: Март 11, 2024

Язык: Английский

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Hexavalent Chromium Reduction Mediated by Interfacial Electron Transfer over the Co@NC Nanosheet-Assembled Microflowers

Inorganic Chemistry, Год журнала: 2024, Номер 63(9), С. 4214 - 4223

Опубликована: Фев. 20, 2024

The reductive transformation of Cr(VI) into Cr(III) mediated by formic acid with efficient, stable, and cost-effective catalysts is a promising strategy for remediating contamination. Herein, we report the facile construction uniform Co@NC nanosheet-assembled microflowers reduction Cr(VI). Both experimental results density functional theory (DFT) calculations reveal vital role intensive interfacial electronic interaction between Co nanoparticles N-doped carbon layer in facilitating anchoring dispersion within framework. electron transfer from to NC contributes Cr2O72– ions, promoting subsequent H-transfer reaction. A Langmuir–Hinshelwood kinetic model has been established catalyzed CNCF2 (pyrolyzed at 700 °C), which shows superior reaction performance. This study provides delicately design well-assembled heterostructures rich interfaces strong interactions series applications environmental/thermal catalysis.

Язык: Английский

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