Lattice Distortion Broadens the eg Band of Co3O4 to Facilitate p-d Hybridization for Enhanced Electrochemical Nitrate Synthesis DOI
Jingxian Li, Jun Wang, Shiyu Wang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: March 26, 2025

The electrochemical nitrogen oxidation reaction (NOR) presents a sustainable pathway for nitrate synthesis under mild conditions; however, the process is hindered by inadequate adsorption and activation of N2 on electrocatalysts. In this study, we utilized Co3O4 as model catalyst engineered lattice distortions introducing oxygen vacancies, which expanded eg band active sites to enhance activation. modified achieved Faradaic efficiency 10.68% yield 58.80 μg·h-1·mgcat-1. Comprehensive experimental density functional theory (DFT) analyses demonstrated that these modifications resulted in shortened Co-N bond length an elongated N≡N bond, leading improved p-d hybridization between Co sites. Moreover, enhancements catalytic performance were also attributed electron transfer properties stemming from altered structure Co3O4. This work provides innovative design principles catalysts aimed at facilitating complex electrocatalytic reactions with multiple kinetics.

Language: Английский

The Electron‐Rich Interface Regulated MBene by S‐Bridge Guided to Enhance Nitrogen Fixation under Environmental Conditions DOI Open Access

Kun Cheng,

Shaobin Li,

Qingyu Cheng

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 15, 2024

Abstract The underutilization of active sites limits the performance enhancement 2D transition metal boride (MBene) in electrocatalytic nitrogen reduction reaction (NRR). Herein, a highly efficient NRR electrocatalyst with S atoms bridging Fe and Mo on surface MBene is successfully constructed by using an site electron optimization strategy, which increases charge density around enhances activation ability catalyst to N 2 molecules. It noteworthy that FeS ‐MBene demonstrates low intrinsic potential for (−0.2 V vs RHE). more favorable adsorption comparison hydrogen atoms, thereby it can effectively inhibit evolution (HER). Under −0.2 versus RHE, ammonia yield rate 37.13 ± 1.31 µg h −1 mg , FE 55.97 2.63%. Density functional theory (DFT) calculations demonstrate serves as . formation heterostructure transfer, resulting becoming electron‐rich state favor subsequent hydrogenation steps. This work offers significant insights into design utilization MBene‐based catalysts NRR.

Language: Английский

Citations

13
Regulating the Unsaturated Co Sites on MOF-74(Co) for Enhancing Photocatalytic N2 to NH3 Conversion DOI

Bing-Hua Ye,

Cheng Liu,

Yueling Chen

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

Language: Английский

Citations

0
Lattice Distortion Broadens the eg Band of Co3O4 to Facilitate p-d Hybridization for Enhanced Electrochemical Nitrate Synthesis DOI
Jingxian Li, Jun Wang, Shiyu Wang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: March 26, 2025

The electrochemical nitrogen oxidation reaction (NOR) presents a sustainable pathway for nitrate synthesis under mild conditions; however, the process is hindered by inadequate adsorption and activation of N2 on electrocatalysts. In this study, we utilized Co3O4 as model catalyst engineered lattice distortions introducing oxygen vacancies, which expanded eg band active sites to enhance activation. modified achieved Faradaic efficiency 10.68% yield 58.80 μg·h-1·mgcat-1. Comprehensive experimental density functional theory (DFT) analyses demonstrated that these modifications resulted in shortened Co-N bond length an elongated N≡N bond, leading improved p-d hybridization between Co sites. Moreover, enhancements catalytic performance were also attributed electron transfer properties stemming from altered structure Co3O4. This work provides innovative design principles catalysts aimed at facilitating complex electrocatalytic reactions with multiple kinetics.

Language: Английский

Citations

0