From Single-Atom to Dual-Atom: A Universal Principle for the Rational Design of Heterogeneous Fenton-like Catalysts

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Апрель 22, 2025

Developing efficient heterogeneous Fenton-like catalysts is the key point to accelerating removal of organic micropollutants in advanced oxidation process. However, a general principle guiding reasonable design highly has not been constructed up now. In this work, total 16 single-atom and 272 dual-atom transition metal/nitrogen/carbon (TM/N/C) for H2O2 dissociation were explored systematically based on high-throughput density functional theory machine learning. It was found that TM/N/C exhibited distinct volcano-type relationship between catalytic activity •OH adsorption energy. The favorable energies range -3.11 ∼ -2.20 eV. Three different descriptors, namely, energetic, electronic, structural found, which can correlate intrinsic properties their activity. Using energy, stability, activation energy as evaluation criteria, two CoCu/N/C CoRu/N/C screened out from candidates, higher than best catalyst due synergistic effect. This work could present conceptually novel understanding inspire structure-oriented viewpoint volcano relationship.

Язык: Английский

Regulation of Active Site Accessibility Enables Efficient Electrocatalytic CO₂ Methanation

Industrial & Engineering Chemistry Research, Год журнала: 2025, Номер unknown

Опубликована: Янв. 4, 2025

Electrocatalytic CO2 Reduction Reaction (ECO2RR) driven by renewable energy, which could convert into fuels or value-added chemicals, has become an effective approach to address environmental issues and the energy crisis. However, due low selectivity, inferior activity, unmanageable reconstruction of catalysts, path ECO2RR remains a significant challenge. In this study, series electrocatalysts composed copper–lanthanum nanoparticles dispersed within nitrogen-doped carbon framework (LaCu@NCF-x, where x represents abbreviation calcination temperatures) were synthesized calcining mixture polymers metal ions, in thermal control is key catalyst preparation process. Phase morphological characterizations reveal that degree carbonization accessibility active sites modulated temperature calcination. The study highlights importance synergistic confinement effects encapsulating layer, not only provides favorable matrix for but also mitigates electrocatalysts, thereby significantly enhancing its performance CH4 production during ECO2RR. particular, LaCu@NCF-3 demonstrates maximum Faraday efficiency (FE) up 64.6% at −1.177 V vs RHE superior stability. Moreover, it maintains high selectivity (FECH4 ≥ 60%) over wide potential range from −0.977 −1.577 RHE. This novel fabrication efficient stable Cu-based electrocatalyst CH4.

Язык: Английский