Engineering Asymmetric Electronic Structure of Co─N─C Single‐Atomic Sites Toward Excellent Electrochemical H₂O₂ Production and Biomass Upgrading

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract To advance electrochemical H 2 O production and unravel catalytic mechanisms, the precise structural coordination of single‐atomic M‐N‐C electrocatalysts is urgently required. Herein, Co─N 5 site with an asymmetric electronic configuration constructed to boost two‐electron oxygen reduction reaction (2e − ORR) compared symmetric 4 , effectively overcoming trade‐off between activity selectivity in production. Both experimental theoretical analyses demonstrate that breaking symmetry sites promotes activation molecules moderates adsorption key *OOH intermediate by disrupting linear scaling relationship for intermediates adsorption. This modulation enables efficient H₂O₂ its effective retention subsequent applications. As a proof concept, achieves rate as high 16.1 mol g cat −1 h flow cell, outperforming most recently reported counterparts. Furthermore, coupling 2e ORR oxidation cellulose‐derived carbohydrates accomplishes formic acid yields (84.1% from glucose 62.0%–92.1% other substrates), underpinning sustainable electro‐refinery biomass valorization at ambient conditions. By elucidating intrinsic 2e⁻ asymmetry sites, this work paves way high‐performance electrosynthesis.

Language: Английский

---

Engineering Asymmetric Electronic Structure of Co─N─C Single‐Atomic Sites Toward Excellent Electrochemical H₂O₂ Production and Biomass Upgrading

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract To advance electrochemical H 2 O production and unravel catalytic mechanisms, the precise structural coordination of single‐atomic M‐N‐C electrocatalysts is urgently required. Herein, Co─N 5 site with an asymmetric electronic configuration constructed to boost two‐electron oxygen reduction reaction (2e − ORR) compared symmetric 4 , effectively overcoming trade‐off between activity selectivity in production. Both experimental theoretical analyses demonstrate that breaking symmetry sites promotes activation molecules moderates adsorption key *OOH intermediate by disrupting linear scaling relationship for intermediates adsorption. This modulation enables efficient H₂O₂ its effective retention subsequent applications. As a proof concept, achieves rate as high 16.1 mol g cat −1 h flow cell, outperforming most recently reported counterparts. Furthermore, coupling 2e ORR oxidation cellulose‐derived carbohydrates accomplishes formic acid yields (84.1% from glucose 62.0%–92.1% other substrates), underpinning sustainable electro‐refinery biomass valorization at ambient conditions. By elucidating intrinsic 2e⁻ asymmetry sites, this work paves way high‐performance electrosynthesis.

Language: Английский

---

Tuning the Formation Kinetics of *OOH Intermediate with Hollow Bowl-Like Carbon by Pulsed Electroreduction for Enhanced H₂O₂ Production

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: March 28, 2025

The electrochemical synthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction (2e- ORR) is a promising alternative to conventional anthraquinone method. However, due local alkalinization near catalyst surface, restricted replenishment and insufficient activated water molecule supply limit formation key *OOH intermediate. Herein, pulsed electrocatalysis approach based on structurally optimized S/N/O tridoped hollow carbon bowl has been proposed overcome this challenge. In an H-type electrolytic cell, method achieves superior H2O2 yield rate 55.6 mg h-1 mgcat.-1, approximately 1.6 times higher than potentiostatic (34.2 mgcat.-1), while maintaining Faradaic efficiency above 94.6%. situ characterizations, finite element simulations, density functional theory analyses unveil that application potentials mitigates OH- concentration, enhances activation proton generation, facilitates production within bowl-like structure. These effects synergistically accelerate kinetics intermediate by efficient generation *O2 *H2O intermediates, leading yields. This work develops strategy tune catalytic environments for diverse applications.

Language: Английский

---

Spent coffee ground-derived hydrochar: An ecologically compatible material for solar-driven H2O2 production and wastewater purification

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: unknown, P. 137371 - 137371

Published: March 1, 2025

Language: Английский

---

XANES-EXAFS spectroscopy for discerning and retrieval of atomic and coordination states of a diverse single-metal-atomic structures

Materials Chemistry and Physics, Journal Year: 2025, Volume and Issue: unknown, P. 130837 - 130837

Published: April 1, 2025

Language: Английский

---

Charge Redistribution of Mo-Incorporated Fe2Ni2N Customizes Potential-Determining Step for Highly Selective Electroreduction of Nitrobenzene to Azoxybenzene

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125358 - 125358

Published: April 1, 2025

Language: Английский

---

Breaking Planar Constraints: Curvature-Tailored Co-N-C Electrocatalysts for High-Efficiency Proton Exchange Membrane H2O2 Production

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125454 - 125454

Published: May 1, 2025

Language: Английский

---