Selective oxygen reduction reaction: mechanism understanding, catalyst design and practical application

Chemical Science, Journal Year: 2024, Volume and Issue: 15(29), P. 11188 - 11228

Published: Jan. 1, 2024

The oxygen reduction reaction (ORR) is a key component for many clean energy technologies and other industrial processes. However, the low selectivity sluggish kinetics of ORR catalysts have hampered conversion efficiency real application these new mentioned before. Recently, tremendous efforts been made in mechanism understanding, electrocatalyst development system design. Here, comprehensive critical review provided to present recent advances field electrocatalytic ORR. two-electron four-electron transfer catalytic mechanisms evaluation parameters are discussed first. Then, up-to-date synthetic strategies

Language: Английский

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Accelerated O2 adsorption and stabilized *OOH for electrocatalytic H2O2 production

Journal of Material Science and Technology, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Language: Английский

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f‐p‐d Gradient Orbital Coupling Induced Spin State Enhancement of Atomic Fe Sites for Efficient and Stable Oxygen Reduction Reaction

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

Published: Feb. 21, 2025

Abstract Advancing energy conversion technologies requires cost‐efficient electrocatalysts for the oxygen reduction reaction (ORR). Iron phthalocyanine (FePc) emerges as a scalable and economical ORR electrocatalyst. However, Fe–N 4 configuration in FePc still falls short of satisfied activity stability under electrocatalytic conditions. Here, an effective f‐p‐d (Eu–O–Fe) gradient orbital coupling strategy is introduced by integrating with Eu 2 O 3 (FePc/Eu ) to enhance spin state performance Fe center through precisely designed, synthetic approach. The Eu─O bond promotes electron delocalization shifts from low‐spin intermediate‐spin, increasing e g​ occupancy. This modification optimizes adsorption oxygen‐containing intermediates lowers barrier. Notably, increased accelerates charge transfer releasing more unpaired electrons, improving kinetics. Furthermore, f‐band serves buffer layer compensation during ORR, further stabilizing covalency electronic atomic boosting durability. one‐batch synthesis produces exceeding 300 g FePc/Eu , achieving half‐wave potential 0.931 V (vs RHE) at cost less than 1/15 commercial Pt/C. It demonstrates exceptional aluminum–air batteries, highlighting its significant application potential.

Language: Английский

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High‐Density Accessible Iron Single‐Atom Catalyst for Durable and Temperature‐Adaptive Laminated Zinc‐Air Batteries

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

Published: Feb. 7, 2025

Abstract Designing single‐atom catalysts (SACs) with high density of accessible sites by improving metal loading and utilization is a promising strategy to boost the catalytic activity, but remains challenging. Herein, site (SD) iron SAC (D‐Fe‐N/C) 11.8 wt.% Fe‐loading reported. The in situ scanning electrochemical microscopy technique attests that active SD D‐Fe‐N/C reach as 1.01 × 10 21 g −1 79.8%, respectively. Therefore, demonstrates superior oxygen reduction reaction (ORR) activity terms half‐wave potential 0.918 V turnover frequency 0.41 e s . excellent ORR property also demonstrated liquid zinc‐air batteries (ZABs), which exhibit peak power 306.1 mW cm −2 an ultra‐long cycling stability over 1200 h. Moreover, solid‐state laminated ZABs prepared presetting air flow layer show specific capacity 818.8 mA h , 520 h, wide temperature‐adaptive from −40 60 °C. This work not only offers possibilities metal‐loading for exploring efficient SACs, provides strategies device structure design toward advanced ZABs.

Language: Английский

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Boosting Oxygen Reduction Reaction Performance of Fe Single‐Atom Catalysts Via Precise Control of the Coordination Environment

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

Published: March 3, 2025

Abstract Fe single‐atom on N‐doped carbon (FeN‐C) catalysts emerge as promising alternatives to commercial Pt/C for the oxygen reduction reaction. Heterogeneous atom doping is proposed be effective modulating catalyst performance. Despite this, relationship between fine coordination structure of doped atoms and catalytic activity central metal site remains poorly understood. Herein, with S in either first shell (FeSN–C) or second (FeN–SC) active are synthesized compare effects different structure. FeN–SC exhibits prominent performance a half‐wave potential 0.92 V rotating disk electrode peak power density 251 mW cm −2 zinc–air battery. Theoretical studies reveal that effectively modulates electronic charge transfer at center. Compared directly coordinated within shell, located more optimizing adsorption desorption energy barriers oxygen‐containing intermediates sites. This study provides new strategy adjust by engineering multilayer center catalyst.

Language: Английский

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Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 31, 2025

Designing asymmetrical structures is an effective strategy to optimize metallic catalysts for electrochemical carbon dioxide reduction reactions. Herein, we demonstrate a transient pulsed discharge method instantaneously constructing graphene-aerogel supports asymmetric copper nanocluster catalysts. This process induces the convergence of atoms decomposed by chloride onto graphene originating from intense current pulse and high temperature. The exhibit atomic electronic due lattice distortion oxygen doping clusters. In reaction, selectivity activity ethanol production are enhanced structure abundance active sites on catalysts, achieving Faradaic efficiency 75.3% 90.5% multicarbon products at −1.1 V vs. reversible hydrogen electrode. Moreover, strong interactions between nanoclusters support confer notable long-term stability. We elucidate key reaction intermediates mechanisms Cu4O-Cu/C2O1 moieties through in situ testing density functional theory calculations. study provides innovative approach balancing stability asymmetric-structure energy conversion. Asymmetric show promise CO2 catalytic reduction. Here, authors develop prepare graphene-aerogel-supported Cu that enhance conversion into products.

Language: Английский

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Atomically dispersed bimetallic single-atom Cu, Fe/NC as pH-universal ORR electrocatalyst

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160400 - 160400

Published: Feb. 1, 2025

Language: Английский

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Recent advances in the development of single atom catalysts for oxygen evolution reaction

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 82, P. 1081 - 1100

Published: Aug. 9, 2024

Language: Английский

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Main-group element-boosted oxygen electrocatalysis of Cu-N-C sites for zinc-air battery with cycling over 5000 h

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Sept. 27, 2024

Language: Английский

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Constructing electron-enriched Co tetrahedral sites to promote oxygen electrocatalysis in rechargeable zinc-air batteries

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 359, P. 124468 - 124468

Published: Aug. 4, 2024

Language: Английский

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