Unraveling volcano trend in OER of metal–organic frameworks with asymmetric configuration through energy band engineering

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 353, С. 124089 - 124089

Опубликована: Апрель 17, 2024

Язык: Английский

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Asymmetric Coordination Regulating D‐Orbital Spin‐Electron Filling in Single‐Atom Iron Catalyst for Efficient Oxygen Reduction

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(28)

Опубликована: Май 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

Язык: Английский

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Mo2N nanoclusters and FeMo dual atomic active sites confined in N-doped hollow carbon nanocages for synergistic improvement in oxygen reduction and Zn-air battery

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 160442 - 160442

Опубликована: Фев. 1, 2025

Язык: Английский

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Metal-organic frameworks-based single-atom catalysts: From synthesis to sustainable electrocatalytic systems

Materials Today Chemistry, Год журнала: 2024, Номер 37, С. 102035 - 102035

Опубликована: Март 29, 2024

Язык: Английский

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Boron in the Second Coordination Sphere of Fe Single Atom Boosts the Oxygen Reduction Reaction

ACS Applied Materials & Interfaces, Год журнала: 2024, Номер 16(13), С. 16224 - 16231

Опубликована: Март 21, 2024

Metal single atoms coordinated with four nitrogen (M1N4) are regarded as tremendously promising catalysts for the electrocatalytic oxygen reduction reaction (ORR). Nevertheless, strong bond intensity between metal center and O atom in oxygen-containing intermediates significantly limits ORR activity of M1N4. Herein, catalytically active B is successfully introduced into second coordination sphere Fe (Fe1N4-B-C) to realize alternative binding thus facilitate activity. Compared pristine Fe1N4 catalyst, synthesized Fe1N4-B-C catalyst exhibits improved catalytic capability a half-wave potential (E1/2) 0.80 V kinetic current density (JK) 5.32 mA cm–2 acid electrolyte. Moreover, an alkaline electrolyte, displays remarkable E1/2 0.87 JK 8.94 at 0.85 V, outperforming commercial Pt/C. Notably, mechanistic study has revealed that shell which avoids direct bonding Fe–O. The moderate force intermediate, flattens energy diagram thereby improves performance. Therefore, this offers novel strategy tailoring performance by tuning single-atom catalyst.

Язык: Английский

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Exposure engineering of active sites of Co-N-C for efficient oxygen reduction reaction

Chemical Engineering Journal, Год журнала: 2025, Номер 505, С. 159449 - 159449

Опубликована: Янв. 9, 2025

Язык: Английский

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

Rare Metals, Год журнала: 2025, Номер unknown

Опубликована: Фев. 3, 2025

Язык: Английский

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Oxygen Reduction Reaction Catalysts for Zinc‐Air Batteries Featuring Single Cobalt Atoms in a Nitrogen‐Doped 3D‐Interconnected Porous Graphene Framework

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 15, 2025

Abstract Single‐atom catalysts (SACs) with high activity and efficient atom utilization for oxygen reduction reactions (ORRs) are imperative rechargeable Zinc‐air batteries (ZABs). However, it is still a prominent challenge to construct noble‐metal‐free SAC low cost but efficiency. Herein, novel nitrogen‐doped graphene (NrGO) based SAC, immobilized atomically dispersed single cobalt (Co) atoms (Co‐NrGO‐SAC), reported ORRs. In this 3D NrGO, the Co‐N 4 sites endow high‐efficiency ORR activity, 3D‐interconnected porous architectures of NrGOs guarantee numberous active accessibility. Compared commercial Pt/C catalyst (≈5.8 mA cm −2 ), as‐prepared Co‐NrGO‐SACs presents considerable limiting current density ≈5.9 , half‐wave potential ≈0.84 V, onset ≈1.05 as well superior methanol resistance. Particularly, ZABs deliver remarkable power (≈240 mW super durability over 233 h at 5 outperforming noble‐metal‐based benchmarks. This work provides an effective noble‐metal free carbon‐based nano‐engineering superdurable ZABs.

Язык: Английский

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A Review on Single Site Catalysts for Electrochemical CO₂ Reduction

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 18, 2025

Abstract Single site catalysts (SSCs), characterized by high atomic utilization and well‐defined active sites, exhibit significant potential in the field of CO 2 electroreduction (CO RR). Typically, SSCs tend to a 2‐electron transfer reaction RR, there remain challenges achieving efficient conversion above 2‐electrons (methane (CH 4 ) multicarbon products(C 2+ ). Therefore, systematic review is crucial summarize recent advancements single electrocatalysts their structure‐activity relationship. The discussion begins with state‐of‐the‐art characterization techniques SSCs. Then influence central atoms, coordination environments, support metal‐support interactions on catalytic performance discussed detail. Subsequently, regulation strategies improve activity selectivity CH C products are discussed. Furthermore, dynamic evolution metal sites true nature during RR also addressed. Finally, associated for product formation analyzed.

Язык: Английский

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Asymmetric Coordination Regulating D‐Orbital Spin‐Electron Filling in Single‐Atom Iron Catalyst for Efficient Oxygen Reduction

Angewandte Chemie, Год журнала: 2024, Номер 136(28)

Опубликована: Май 9, 2024

Abstract 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 −2 , respectively. Theoretical studies in situ electrochemical Raman spectroscopy reveal that undergoes redistribution negative shifting d‐band center Fe−N−C, thus optimizing adsorption free energy intermediates. This work demonstrates feasibility introducing an asymmetric shell catalysts provides new optimization direction their practical application.

Язык: Английский

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