Edge‐Rich Graphene Nanomesh Thermally Self‐Exfoliated From Metal‐Organic Frameworks for Boosting CO2 Electroreduction DOI

Mingxu Liu,

Yunhui Xie, Fulai Liu

et al.

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

Published: May 15, 2025

Abstract Atomic‐level metal sites at the edges of graphene‐like carbon supports are considered more active for CO 2 electrocatalysis than those in‐plane. However, creating high‐density edge‐dominating sites, particularly in a simple, scalable, and self‐templated fashion, presents significant challenge. Herein, MOF‐mediated self‐exfoliation strategy is reported to preferentially integrate edge‐type FeN 4 onto ultrathin edge‐rich N‐doped graphene nanomesh (e‐Fe‐NGM). Theoretical calculations, finite element method (FEM) simulations, together with series situ spectro‐electrochemical experiments corroborate that can not only optimize electronic structure catalysts, facilitating formation * COOH desorption CO, but also effectively induce strong local electrostatic field, promoting interfacial H O supply thereby accelerating protonation process . Thus‐prepared e‐Fe‐NGM delivers remarkable Faraday efficiency (FE) above 98% over an ultra‐wide potential window 500 mV high turnover frequency 6648 h −1 , much superior controlled sample dominant plane‐type sites. Moreover, this self‐exfoliated, non‐catalyzed approach readily scalable be used produce large‐size industrial levels.

Language: Английский

Dual‐reaction pathway engineering via anode‐driven methanol oxidation for efficient electrocatalytic ammonia production DOI
Yuzhe Zhang, Lu Chen,

Xiaoqing Yan

et al.

AIChE Journal, Journal Year: 2025, Volume and Issue: unknown

Published: April 21, 2025

Abstract Replacing the anodic oxygen evolution reaction with selective methanol oxidation to formic acid offers a promising route enhance paired electrochemical ammonia synthesis. However, inherent kinetic and thermodynamic disparities between cathodic reduction present significant challenges in achieving optimal system performance. Herein, we propose dual‐reaction strategy employing bifunctional Au/CoOOH nanocomposite catalysts, simultaneous NH 3 production (34.15 g) synthesis (69.65 after 24 h at 2.6 V cell voltage. Density functional theory (DFT) calculations further reveal that loading Co‐based catalysts its hybridization Au nanoparticles can effectively tune electronic configuration of Co‐O sites poison their strong adsorption capacity intermediate products, lowering energy barrier alter pathway. This work provides an atomic‐level design principle for coupled systems, demonstrating better efficiency, while co‐producing high‐value chemicals scalable green

Language: Английский

Citations

0
Enhancing the hydrogen spillover effect of Pt/SiC by regulating the hydrogen diffusion pathway for cinnamaldehyde hydrogenation DOI

Ji‐Xiao Zhao,

Xinchao Liu, Qingmin Hu

et al.

Applied Surface Science, Journal Year: 2025, Volume and Issue: unknown, P. 163403 - 163403

Published: May 1, 2025

Language: Английский

Citations

0
Advances in the Structure–Activity Relationship of Electrocatalytic C–N Coupling: From Nanocatalysis to Single Metal Site Catalysis DOI

Yinchao Yao,

Zhiyi Sun,

Tiesong Li

et al.

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

Published: May 14, 2025

C-N coupling is crucial for constructing amides and amines involves various fields, including medicine, chemical industries, agriculture, energy. With the rapid development of electrocatalytic continuous improvement catalytic performance, this field has aroused extensive research interest. A comprehensive review urgently needed to summarize structure-activity relationship, key challenges, future directions. This provides a concise overview recent advancements from nanocatalysis single metal site catalysis reactions. We mechanisms using different nitrogen sources further analyze influences active centers coordination environments on thereby elucidating relationship. Moreover, we discuss dynamic structural evolution sites during reaction. Finally, present current challenges perspectives in field. aims provide valuable insights into advanced nano/single catalysts reactions along with deeper understanding mechanisms.

Language: Английский

Citations

0
Edge‐Rich Graphene Nanomesh Thermally Self‐Exfoliated From Metal‐Organic Frameworks for Boosting CO2 Electroreduction DOI

Mingxu Liu,

Yunhui Xie, Fulai Liu

et al.

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

Published: May 15, 2025

Abstract Atomic‐level metal sites at the edges of graphene‐like carbon supports are considered more active for CO 2 electrocatalysis than those in‐plane. However, creating high‐density edge‐dominating sites, particularly in a simple, scalable, and self‐templated fashion, presents significant challenge. Herein, MOF‐mediated self‐exfoliation strategy is reported to preferentially integrate edge‐type FeN 4 onto ultrathin edge‐rich N‐doped graphene nanomesh (e‐Fe‐NGM). Theoretical calculations, finite element method (FEM) simulations, together with series situ spectro‐electrochemical experiments corroborate that can not only optimize electronic structure catalysts, facilitating formation * COOH desorption CO, but also effectively induce strong local electrostatic field, promoting interfacial H O supply thereby accelerating protonation process . Thus‐prepared e‐Fe‐NGM delivers remarkable Faraday efficiency (FE) above 98% over an ultra‐wide potential window 500 mV high turnover frequency 6648 h −1 , much superior controlled sample dominant plane‐type sites. Moreover, this self‐exfoliated, non‐catalyzed approach readily scalable be used produce large‐size industrial levels.

Language: Английский

Citations

0