Applied Energy, Год журнала: 2025, Номер 391, С. 125925 - 125925
Опубликована: Апрель 13, 2025
Язык: Английский
Journal of the American Chemical Society, Год журнала: 2024, Номер 146(31), С. 21357 - 21366
Опубликована: Июль 25, 2024
With more flexible active sites and intermetal interaction, dual-atom catalysts (DACs) have emerged as a new frontier in various electrocatalytic reactions. Constructing typical p-d orbital hybridization between p-block d-block metal atoms may bring avenues for manipulating the electronic properties thus boosting activities. Herein, we report distinctive heteronuclear dual-metal atom catalyst with asymmetrical FeSn dual embedded on two-dimensional C2N nanosheet (FeSn–C2N), which displays excellent oxygen reduction reaction (ORR) performance half-wave potential of 0.914 V an alkaline electrolyte. Theoretical calculations further unveil powerful stannum ferrum sites, triggers electron delocalization lowers energy barrier *OH protonation, consequently enhancing ORR activity. In addition, FeSn–C2N-based Zn–air battery provides high maximum power density (265.5 mW cm–2) specific capacity (754.6 mA h g–1). Consequently, this work validates immense along perception into logical design DACs.
Язык: Английский
Процитировано
22
Nature Communications, Год журнала: 2025, Номер 16(1)
Опубликована: Янв. 7, 2025
Owing to their synergistic interactions, dual-atom catalysts (DACs) with well-defined active sites are attracting increasing attention. However, more experimental research and theoretical investigations needed further construct explicit understand the synergy that facilitates multistep catalytic reactions. Herein, we precisely design a series of asymmetric selenium-based comprise heteronuclear SeN2–MN2 (M = Fe, Mn, Co, Ni, Cu, Mo, etc.) for efficient oxygen reduction reaction (ORR). Spectroscopic characterisation calculations revealed selenium atoms can efficiently polarise charge distribution other metal through short-range regulation. In addition, compared Se or Fe single-atom sites, SeFe facilitate in conversion energy barrier from *O *OH via coadsorption intermediates. Among these designed catalysts, selenium-iron achieves superior alkaline ORR performance, half-wave potential 0.926 V vs. reversible hydrogen electrode. SeN2–FeN2-based Zn–air battery has high specific capacity (764.8 mAh g−1) maximum power density (287.2 mW cm−2). This work may provide good perspective designing DACs improve efficiency. Dual-atom precise gaining attention, but studies optimise construction synergy. Here authors report dual- atom reaction.
Язык: Английский
Процитировано
3
Nature Communications, Год журнала: 2024, Номер 15(1)
Опубликована: Ноя. 1, 2024
Double-atom catalysts (DACs) have opened distinctive paradigms in the field of rapidly developing atomic catalysis owing to their great potential for promoting catalytic performance various reaction systems. However, increasing loading and extending service life metal active centres represents a considerable challenge efficient utilization DACs. Here, we rationally design asymmetric nitrogen, sulfur-coordinated diatomic iron on highly defective nitrogen-doped carbon nanosheets (denoted A-Fe
Язык: Английский
Процитировано
14
International Journal of Hydrogen Energy, Год журнала: 2024, Номер 82, С. 1081 - 1100
Опубликована: Авг. 9, 2024
Язык: Английский
Процитировано
13
Advanced Functional Materials, Год журнала: 2025, Номер unknown
Опубликована: Март 3, 2025
Abstract Oxygen electrocatalysis is a core reaction in renewable energy devices, greatly promoting the transformation and upgrading of structure. Nonetheless, performance conversion devices hindered by large overpotential slow kinetics oxygen electrocatalytic reactions. Recently, single‐atom catalysts (SACs) have emerged as promising contenders field because their exceptional metal atom utilization, distinctive coordination environment, adjustable electronic properties. This review presents latest advancements design Co‐based SACs for electrocatalysis. First, OER ORR mechanisms are introduced. Subsequently, strategies regulating structure summarized three aspects, including centers, support carriers. A particular emphasis given to relationship between properties catalysts. Afterward, applications explored. Ultimately, challenges prospects prospected.
Язык: Английский
Процитировано
1
Chinese Journal of Chemistry, Год журнала: 2024, Номер 42(20), С. 2520 - 2535
Опубликована: Июнь 19, 2024
Comprehensive Summary The electrochemical processes of oxygen reduction reaction (ORR) and evolution (OER) play a crucial role in various energy storage conversion systems. However, the inherently slow kinetics reversible reactions present an urgent demand for development efficient electrocatalysts. Recently, metal‐organic framework (MOF) derivatives have attracted extensive attention electrocatalysis research due to their unique porous structure, abundant active sites, tunable structural properties. Especially, optimization electronic structure sites MOF has been proven as effective strategy enhance catalytic activity. In this review, we provide overview strategies advanced catalysts O—O bond activation reactions, including construction synergistic effects between multiple heterogeneous interfaces, utilization metal support interactions, precise modulation organic ligands surrounding at atomic level. Furthermore, review offers theoretical insights into mechanisms derivatives, well identification sites. Finally, potential challenges prospects are discussed. This contributes understanding advancement Key Scientists
Язык: Английский
Процитировано
7
Advanced Functional Materials, Год журнала: 2024, Номер 34(46)
Опубликована: Июнь 19, 2024
Abstract Simultaneously improving activity and stability is a crucial yet challenge in the development of metallic single‐atom‐based catalysts. In current work, novel approach introduced to address this issue by combining post‐adsorption secondary pyrolysis techniques create synergistic catalytic system, which single atoms (SAs) Fe sites played NC matrix (Fe─NC) are coupled with high‐entropy atomic clusters (HEACs). Theoretical calculations reveal that incorporation HEACs lead rehybridization 3d orbital configuration Fe‐N 4 , helps balance adsorption/desorption energy oxygenated intermediates. situ spectroscopy further reveals rate‐limiting step OH * desorption on HEAC/Fe─NC oxygen reduction reaction (ORR) more facile compared Fe─NC, implying higher ORR activity. Moreover, effect diffusion activation barriers entropy contributes structural HEAC/Fe─NC, resulting remarkable durability. Consequently, unique catalyst exhibits half‐wave potentials 0.927 0.828 V an aqueous solution KOH (0.1 m ) HClO ), respectively, along excellent The findings propose strategy for modulating electronic structure SAs catalysts enhancing their through strong interactions between HEACs.
Язык: Английский
Процитировано
6
Chemical Science, Год журнала: 2024, Номер unknown
Опубликована: Янв. 1, 2024
Utilizing double coordination shell modulation, we construct a novel nitrogen-free single-atom manganese configuration catalyst on graphene oxide (Mn–S 1 O 4 G), which exhibits excellent ORR and zinc–air battery performances.
Язык: Английский
Процитировано
6
npj Computational Materials, Год журнала: 2024, Номер 10(1)
Опубликована: Авг. 28, 2024
The development of non-noble metal electrocatalysts for the Oxygen Evolution Reaction (OER) is advancing towards use multi-element materials. To reveal complex correlations OER electrocatalysts, we developed an iterative workflow combining high-throughput experiments and AI-generated content (AIGC) processes. An increased number 909 (compared to 145 in previous literature) universal descriptors inorganic materials science were constructed used as Artificial Neural Network (ANN) input. A large statistical ensembles with each ANN individual ensemble having a reduced integrated new Hierarchical (HNN) algorithm. This algorithm addresses longstanding challenge balancing overwhelming descriptor numbers insufficient datasets traditional approaches problems. As result, combination AIGC experimental validation significantly enhanced prediction accuracy, increase R2 values from 0.7 0.98 Tafel slopes.
Язык: Английский
Процитировано
5
Advanced Energy Materials, Год журнала: 2024, Номер unknown
Опубликована: Авг. 21, 2024
Abstract Selective photoreduction of carbon dioxide (CO 2 ) into high‐value C products remains a formidable challenge due to the elusive C−C coupling step. Herein, novel concept is first introduced that an amorphous‐crystalline hybrid structure can galvanize previously inert metal atoms, thereby establishing highly active dual sites. This ingenious configuration promotes coupling, paving way for CO products. Taking Bi MoO 6 nanosheets anchored by amorphous FeOOH species as example, X‐ray photoelectron spectroscopy (XPS) spectra and absorption near edge density functional theoretical (DFT) calculations confirm electron transfer from nanosheets. Thus, introduction activates nonoperative sites construction Bi−Mo sites, verified in situ XPS DFT calculations. Gibbs free energy revealed formation barrier hugely lowed 3.41 0.45 eV thanks presence species. Therefore, FeOOHBi are game changer, delivering sole liquid product, acetic acid, with impressive selectivity ≈86.9%. In contrast, lag behind, only capable producing monoxide photoreduction.
Язык: Английский
Процитировано
4