Hydrogen‐Bond‐Assisted Synthesis of Single‐Atom and Nanocluster Synergistic Sites for Enhanced Oxygen Reduction Reaction DOI

Xue Lu,

Fei Xiang,

Shaoyi Li

et al.

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

Published: April 27, 2025

Abstract Electrocatalysts combining metal single‐atom and nanocluster synergy are promising alternatives to platinum‐based catalysts for oxygen reduction reaction (ORR). However, controllable synthesis of such with high ORR performance remains challenging due atom aggregation into large nanoparticles. Here, a hydrogen‐bond network confinement approach construct Co Co‐N x ‐C moiety coexisting active sites on nitrogen‐doped porous carbon highly long‐term stable is reported. The optimized Co@Co‐N‐C catalyst exhibits half‐wave potential (E 1/2 ) 0.92 V versus RHE limiting current density (J L 6.02 mA cm −2 ORR, presenting 40 mV positive shift in E than the competitor highest J 15.7% improvement over most . enhanced catalytic originates from between moieties, which modulates electronic structure Co‐based improves electrochemically surface area. zinc‐air battery assembled delivers specific capacity 870 mAh g −1 maximum discharge power 210 mW , representing ≈52% Pt/C‐based devices. This hydrogen‐bond‐assisted strategy opens pathways designing high‐performing diversified fields beyond including water splitting, CO 2 reduction, nitrogen reduction.

Language: Английский

Constructing Pillar‐Layered Covalent Organic Frameworks via Metal–Ligand Coordination for Electrochemical CO2 Reduction DOI Open Access
Tianfu Yang,

Hongyin Hu,

Yan Wang

et al.

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

Published: Jan. 29, 2025

Abstract Growing global concerns over energy security and climate change have intensified efforts to develop sustainable strategies for electrochemical CO 2 reduction (eCO RR). Covalent Organic Frameworks (COFs) emerged as promising electrocatalysts eCO RR due their tunable structures, high surface areas, abundance of active sites. However, the performance 2D COFs is often limited by layer stacking, which restricts site exposure reduces selectivity. To overcome these challenges, a new class known pillar‐layered (PL‐COFs) developed featuring adjustable interlayer spacing 3D architecture. Characterization using PXRD, TEM, XPS, EIS confirmed successful integration pillar molecules, leads increased spacing, crystallinity, porosity. These structural advancements result in significantly improved activity selectivity ‐to‐CO conversion. Density functional theory simulations revealed that enhanced adsorption desorption contribute outstanding PL‐COF‐1, boasts largest spacing. This material achieved an impressive Faradaic efficiency 91.3% demonstrated significant current density, outperforming both original COF‐366‐Co PL‐COF‐2. findings highlight effectiveness pillaring strategy optimizing COF‐based electrocatalysts, paving way next‐generation materials

Language: Английский

Citations

0
Converging the Complementary Traits of Metal–Organic Frameworks and Covalent Organic Frameworks DOI Creative Commons
Riki Nakatani, Tsukasa Irie, Saikat Das

et al.

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

Published: March 27, 2025

Since their discovery, metal–organic frameworks (MOFs) and covalent organic (COFs) featuring permanent nanopores have transformed the landscape of porous materials, excelling as platforms for catalysis, gas separation, sensing thanks to exceptional surface areas, adjustable pore sizes, modular functionality. However, MOFs, while versatile, face stability challenges due coordination bonds, whereas COFs, although robust, lack metal sites, limiting catalytic activity, redox functionality, other metal-specific applications. To bridge these gaps, innovative such MCOFs, which incorporate ions into COF lattices; cluster frameworks, formed by assembling clusters networks; MOF–COF composites, integrate strengths both systems, emerged. This review explores synthesis design principles advanced showcasing applications unique advantages conferred composite nature. It provides insights future directions potential address key in materials science beyond.

Language: Английский

Citations

0
Controllable Regulation of Ligand Stacking in MOF Single‐Crystal: From F‐F to E‐F Stacking Mode for Efficient Photocatalysis DOI

Huaizhi Yang,

Xiaoke Li,

Susu Han

et al.

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

Published: April 15, 2025

Abstract Preparing single crystals of metal–organic frameworks (MOFs) is crucial for studying their semiconductor catalyst properties. In this study, Ni‐TBAPy‐EF (edge‐to‐face) are successfully synthesized in pure water the first time and an effective strategy proposed to promote efficient utilization photoexcited electrons by modulating stacking mode ligand MOFs. The C─H∙∙∙π interactions between ligands formation herringbone can withstand a wide range pH environments or organic reagents. Experimental results theoretical calculations corroborate that overlapping intermolecular orbitals enhance light absorption capacity charge transfer capability. hydrogen bonding microenvironment ligand‐metal (LMCT) electron MOFs ensured utilization. As result, exhibites excellent production (17.4 mmol g −1 h , λ ≥ 420 nm) high apparent quantum efficiency (AQE 9.16%) without co‐catalysts.

Language: Английский

Citations

0
Hydrogen‐Bond‐Assisted Synthesis of Single‐Atom and Nanocluster Synergistic Sites for Enhanced Oxygen Reduction Reaction DOI

Xue Lu,

Fei Xiang,

Shaoyi Li

et al.

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

Published: April 27, 2025

Abstract Electrocatalysts combining metal single‐atom and nanocluster synergy are promising alternatives to platinum‐based catalysts for oxygen reduction reaction (ORR). However, controllable synthesis of such with high ORR performance remains challenging due atom aggregation into large nanoparticles. Here, a hydrogen‐bond network confinement approach construct Co Co‐N x ‐C moiety coexisting active sites on nitrogen‐doped porous carbon highly long‐term stable is reported. The optimized Co@Co‐N‐C catalyst exhibits half‐wave potential (E 1/2 ) 0.92 V versus RHE limiting current density (J L 6.02 mA cm −2 ORR, presenting 40 mV positive shift in E than the competitor highest J 15.7% improvement over most . enhanced catalytic originates from between moieties, which modulates electronic structure Co‐based improves electrochemically surface area. zinc‐air battery assembled delivers specific capacity 870 mAh g −1 maximum discharge power 210 mW , representing ≈52% Pt/C‐based devices. This hydrogen‐bond‐assisted strategy opens pathways designing high‐performing diversified fields beyond including water splitting, CO 2 reduction, nitrogen reduction.

Language: Английский

Citations

0