Steering the oxygen reduction reaction pathways of N-carbon hollow spheres by heteroatom doping

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 327, P. 122470 - 122470

Published: Feb. 13, 2023

Language: Английский

---

A Fe Single Atom Seed‐Mediated Strategy Toward Fe₃C/FeNC Catalysts with Outstanding Bifunctional ORR/OER Activities

Advanced Science, Journal Year: 2023, Volume and Issue: 10(22)

Published: May 31, 2023

The discovery of low-cost and high-performance bifunctional oxygen electrocatalysts is vital to the future commercialization rechargeable zinc-air batteries (ZABs). Herein, a Fe single atom seed-mediated strategy reported for fabrication Fe3 C species closely surrounded by FeN4 C active sites with strong electronic interactions built between them more importantly, creating optimized coordination environment, via subtly adjusting their ratio, favorable adsorption energies intermediates formed during reduction reaction (ORR) evolution (OER). Concretely, voltage difference (ΔE) ORR half-wave OER potential at current density 10 mA cm-2 compositionally-optimized FeNC/Fe3 C-op electrocatalyst only 0.668 V, endowing itself one best OER/ORR benchmarks. As demo, ZABs assembled as air cathode deliver remarkable specific capacity (818.1 mAh gZn-1 ) power (1013.9 mWh ), along excellent long-term durability (>450 h). This work extends methodology modulate activity atomic site, undoubtedly inspiring wide explorations on precise design electrocatalysts.

Language: Английский

---

Co single atoms and Co nanoparticle relay electrocatalyst for rechargeable zinc air batteries

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 319, P. 121905 - 121905

Published: Aug. 27, 2022

Language: Английский

---

Engineering d-band center of FeN4 moieties for efficient oxygen reduction reaction electrocatalysts

Energy storage materials, Journal Year: 2023, Volume and Issue: 59, P. 102764 - 102764

Published: April 6, 2023

Atomically-dispersed FeN4 moieties are emerging as low-cost electrocatalysts for oxygen reduction reaction (ORR), which can be applied in fuel cells and metal-air batteries. Whereas, the unsatisfactory position of d-band center from metal sites offered by affects adsorption-desorption behaviors oxygenated intermediates, further impeding improvement their ORR performances. Herein, we report a well-designed diatomic Fe/Zn-CNHC catalyst on microporous hollow support. This strategy drives Fe upward, thus making active more favorable stable during kinetic processes. The material exhibits an excellent activity with half-wave potential 0.91 V stability (insignificant attenuation after 5,000 cycles), surpassing commercial Pt/C many other single-atom catalysts. DFT calculations indicate that tuning effect Zn d-orbital electron distribution facilitates stretching cleavage Fe-O, accelerating rate-determining step. work presents simple to fabricate well-defined coordination inspires future research developing new syntheses control electrocatalysts.

Language: Английский

---

Importance of broken geometric symmetry of single-atom Pt sites for efficient electrocatalysis

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 3, 2023

Platinum single-atom catalysts hold promise as a new frontier in heterogeneous electrocatalysis. However, the exact chemical nature of active Pt sites is highly elusive, arousing many hypotheses to compensate for significant discrepancies between experiments and theories. Here, we identify stabilization low-coordinated

Language: Английский

---

The operation active sites of O₂ reduction to H₂O₂ over ZnO

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(8), P. 3526 - 3533

Published: Jan. 1, 2023

ZnO@ZnO 2 shows ∼100% 2e − ORR selectivity in neutral media and a rate of 5.47 mol g cat −1 h an FE 95.5% bulk H O production. The situ growth ZnO on restructures the operation active sites to facilitate superior activity.

Language: Английский

---

Single atom catalysts for use in the selective production of hydrogen peroxide via two-electron oxygen reduction reaction: Mechanism, activity, and structure optimization

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 337, P. 122987 - 122987

Published: June 12, 2023

Language: Английский

---

Dual and Triple Atom Electrocatalysts for Energy Conversion (CO₂RR, NRR, ORR, OER, and HER): Synthesis, Characterization, and Activity Evaluation

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(2), P. 1121 - 1145

Published: Jan. 8, 2024

Dual and triple atom catalysts (DACs TACs) are an emerging field of heterogeneous catalysis research. They share properties with single (SACs), such as maximizing dispersion metals the ability to circumvent traditional scaling relations that limit extended surfaces. DACs TACs additionally provide adjacent sites necessary for certain reaction mechanisms add tunability electronic structure binding energies. are, however, inherently difficult selectively synthesize characterize. Characterization activity evaluation prone misinterpretation, adding confusion already complex field. In this review, we investigate current progress important electrochemical reactions in energy conversion storage. We further discuss future synthesis methods focus on common pitfalls characterization evaluation.

Language: Английский

---

Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production

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

Published: Jan. 2, 2024

Abstract Direct electrosynthesis of hydrogen peroxide (H 2 O ) via the two-electron oxygen reduction reaction presents a burgeoning alternative to conventional energy-intensive anthraquinone process for on-site applications. Nevertheless, its adoption is currently hindered by inferior H selectivity and diminished yield induced consecutive or Fenton reactions. Herein, guided theoretical calculations, we endeavor overcome this challenge activating main-group Pb single-atom catalyst local micro-environment engineering strategy employing sulfur super-coordinated structure. The catalyst, synthesized using carbon dot-assisted pyrolysis technique, displays an industrial current density reaching 400 mA cm −2 elevated accumulated concentrations (1358 mM) with remarkable Faradaic efficiencies. Both experimental results simulations elucidate that S super-coordination directs fraction electrons from sites coordinated atoms, consequently optimizing *OOH binding energy augmenting 2e − activity. This work unveils novel avenues mitigating production-depletion in through rational design catalysts.

Language: Английский

---

An overview of silicon-air batteries: Principle, current state and future perspectives

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 517, P. 216045 - 216045

Published: July 1, 2024

Language: Английский

---