Pyrolytic Transformation of Zn-TAL Metal–Organic Framework into Hollow Zn–N–C Spheres for Improved Oxygen Reduction Reaction Catalysis DOI Creative Commons

Gulnara Yusibova,

John C. Douglin, Iuliia Vetik

et al.

ACS Omega, Journal Year: 2025, Volume and Issue: 10(15), P. 15280 - 15291

Published: April 12, 2025

Metal-organic frameworks (MOFs) are promising precursors for creating metal-nitrogen-carbon (M-N-C) electrocatalysts with high performance, though maintaining their structure during pyrolysis is challenging. This study examines the transformation of a Zn-based MOF into an M-N-C electrocatalyst, focusing on preservation carbon framework and prevention Zn aggregation pyrolysis. A highly porous Zn-N-C electrocatalyst derived from Zn-TAL (where TAL stands TalTech-UniTartu Alliance Laboratory) was synthesized via optimized pyrolysis, yielding notable electrocatalytic activity toward oxygen reduction reaction (ORR). Scanning electron microscopy (SEM) X-ray diffraction spectroscopy (XRD) analyses confirmed that preserved its integrity remained free metal aggregates, even at elevated temperatures. Rotating disc electrode (RDE) tests in alkaline solution showed demonstrated ORR par commercial Pt/C electrocatalysts. In anion-exchange membrane fuel cell (AEMFC), material pyrolyzed 1000 °C exhibited peak power density 553 mW cm-2 60 °C. work demonstrates excellent precursor forming hollow structures, making it high-performance Pt-free cells.

Language: Английский

Nano-/Microrobots for Environmental Remediation in the Eyes of Nanoarchitectonics: DOI Creative Commons
Anna Jančík Procházková, Katsuhiko Ariga

Research, Journal Year: 2025, Volume and Issue: 8

Published: Jan. 1, 2025

Nano-/microrobots have been demonstrated as an efficient solution for environmental remediation. Their strength lies in their propulsion abilities that allow active “on-the-fly” operation, such pollutant detection, capture, transport, degradation, and disruption. Another advantage is versatility, which allows the engineering of highly functional solutions a specific application. However, latter can bring complexity to applications; versatility dimensionality, morphology, materials, surface decorations, other modifications has crucial effect on resulting abilities, compatibility with environment, overall functionality. Synergy between decorations its projection functionality object nanoarchitectonics. Here, we scrutinize nano-/microrobots eyes nanoarchitectonics: list general concepts help assess synergy limitations individual procedures fabrication processes operation at macroscale. The nanoarchitectonics approached from microscopic level, focusing dimensionality through nanoscopic evaluating influence decoration nanoparticles quantum dots, moving molecular single-atomic level very fine tuning presented review aims lay provide overview advanced nano-/microrobot remediation beyond.

Language: Английский

Citations

0
Electron delocalization engineering via hierarchical modulation in single-atom catalysts for highly efficient electrochemical CO2 reduction DOI
Xu Han, Hong Liu, Pengfei Cao

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160634 - 160634

Published: Feb. 1, 2025

Language: Английский

Citations

0
Metal-saloph Complexes Pre-coordination for Fe Single Atom Catalyst towards Oxygen Reduction Reaction in Rechargeable Quasi-solid-state Zn-air Battery DOI
Lichen Zhang,

Lingbo Zong,

Fenghong Lu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125189 - 125189

Published: Feb. 1, 2025

Language: Английский

Citations

0
Molecularly Woven Polymer Aerogels DOI
Xinhai Zhang, Xinwei Chen, Ruixue Bai

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 26, 2025

Aerogels with abundant nanopores and large specific surface areas have extensive potential in various applications but are constrained by fragility difficulty degradation. Currently, the exploration of adaptive reprocessing aerogels has become increasingly urgent, as demand for intelligent sustainable materials intensifies. Here, we present a molecular weaving strategy to construct molecularly woven polymer (WPAs) via catalyst-free aldimine condensation between prewoven aldehyde-functionalized Cu(I) bisphenanthroline (Cu(PBD)2) flexible 4,4′-diaminodibenzyl (DB). The key feature this system consists entirely dense nodes that can be readily activated external stimuli, where ions also reversibly removed needed, while preserving porous structures. Consequently, achieve adjustable mechanical properties WPAs, 10-fold enhancement elasticity after removing ions. Moreover, destroyed WPAs demonstrate straightforward capacity rather than tedious monomer recovery due dissociation Cu(I)-coordination bonds, activation sequential thread motions, accelerated imine bond exchange enabled adjacent This work offers new perspective on designing customizable verifies feasibility emergent technique more complex functional material system.

Language: Английский

Citations

0
Digital Descriptors in Predicting Catalysis Reaction Efficiency and Selectivity DOI

Qin Zhu,

Yuming Gu, Jing Ma

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: 16(9), P. 2357 - 2368

Published: Feb. 26, 2025

Accurately controlling the interactions and dynamic changes between multiple active sites (e.g., metals, vacancies, lone pairs of heteroatoms) to achieve efficient catalytic performance is a key issue challenge in design complex reactions involving 2D metal-supported catalysts, metal-zeolites, metal–organic metalloenzymes. With aid machine learning (ML), descriptors play central role optimizing electrochemical elucidating essence activity, predicting more thereby avoiding time-consuming trial-and-error processes. Three kinds descriptors─active center descriptors, interfacial reaction pathway descriptors─are crucial for understanding designing catalysts. Specifically, as sites, synergize with metals significantly promote reduction energy-relevant small molecules. By combining some physical interpretable can be constructed evaluate performance. Future development ML models faces constructing vacancies multicatalysis systems rationally selectivity, stability Utilization generative artificial intelligence multimodal automatically extract would accelerate exploration mechanisms. The transferable from catalysts metalloenzymes provide innovative solutions energy conversion environmental protection.

Language: Английский

Citations

0
Recent advances in proton-conducting solid oxide electrolysis cells DOI
Jianxiong Wang, Wei Chen, Yuhuan Wang

et al.

Materials Science and Engineering B, Journal Year: 2025, Volume and Issue: 317, P. 118188 - 118188

Published: March 4, 2025

Language: Английский

Citations

0
Constructing Three-Dimensional Fe-Based Electrodes for Oxygen Evolution at Large Current Density DOI
Shuai Niu, Yanqiu Wu, Jing Zhang

et al.

Journal of Alloys and Compounds, Journal Year: 2025, Volume and Issue: unknown, P. 179638 - 179638

Published: March 1, 2025

Language: Английский

Citations

0
Electron-Coupling Effect Modulating the d-Band Center of Asymmetric Cobalt Single-Atom Sites for Electrocatalytic Oxygen Reduction DOI
Qi Li, Yingjie Chang, Ying-Yu Liao

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 2752 - 2758

Published: March 7, 2025

We introduce an aggregation-induced deposition approach for rapidly synthesizing asymmetric Co-N3O single-atom sites (SAs) with a precise atomic configuration on hollow carbon matrix (Co-SAs/NHC). This design leverages the electron-coupling effect between Co SAs across adjacent layers, enhancing intrinsic activity and durability of catalyst. In ORR, Co-SAs/NHC catalyst displayed half-wave potential improvement 51 mV, achieving mass 5-fold that commercial Pt/C. Remarkably, after 30 000 cycles, there was negligible loss just 17 mV. Density functional theory calculations revealed optimized electronic structure d-band center atom, thereby reducing adsorption energy OH* intermediates. work offers pathway developing industrial-grade catalysts (SACs) satisfactory catalytic durability.

Language: Английский

Citations

0
Efficient and Long-Lasting Removal of High-Level Formaldehyde at Room Temperature over a Cobalt Single-Atom Catalyst Anchored on Graphene-like Carbon Nanosheets DOI

Bing Du,

Feng Wen,

Yunhan Zhao

et al.

ACS ES&T Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: March 8, 2025

Language: Английский

Citations

0
Synergistic Effects in Earth‐Abundant Bimetallic Aerogels for Enhanced Oxygen Evolution Reaction DOI Open Access
Wei Wei,

Ruomei Yin,

Houxu Mei

et al.

Energy Technology, Journal Year: 2025, Volume and Issue: unknown

Published: March 20, 2025

Inexpensive and efficient earth‐abundant metal catalysts are required for electrocatalytic water splitting to meet future energy conversion storage demand, but its practical production is limited by uncertain factors such as slow oxygen evolution reaction (OER) kinetics, low electrical conductivity, unclear catalytic mechanism. A facile one‐step reduction in situ gelation proposed synthesize a series of nickel‐based bimetallic aerogels (Ni x Fe y , Ni Co Cu ) utilizing the synergistic effect between bimetals surface electronic structure adjustment strategy realize OER performance improvement. Meanwhile, density functional theory calculations show that introduction transition into can cause center d ‐band shift down, induce strong effects on surface, regulate adsorption intermediates (*OH, *O, *OOH), enhancing aerogel thereby achieving higher intrinsic activity 45 55 catalyst. This work sheds light design high‐performance electrocatalysts.

Language: Английский

Citations

0