Ru/Ir‐Based Electrocatalysts for Oxygen Evolution Reaction in Acidic Conditions: From Mechanisms, Optimizations to Challenges

Advanced Science, Год журнала: 2024, Номер 11(21)

Опубликована: Март 19, 2024

Abstract The generation of green hydrogen by water splitting is identified as a key strategic energy technology, and proton exchange membrane electrolysis (PEMWE) one the desirable technologies for converting renewable sources into hydrogen. However, harsh anode environment PEMWE oxygen evolution reaction (OER) involving four‐electron transfer result in large overpotential, which limits overall efficiency production, thus efficient electrocatalysts are needed to overcome high overpotential slow kinetic process. In recent years, noble metal‐based (e.g., Ru/Ir‐based metal/oxide electrocatalysts) have received much attention due their unique catalytic properties, already become dominant acidic OER process applied commercial devices. these still face thorny problem conflicting performance cost. this review, first, metal briefly classified according forms existence, mechanisms outlined. Then, focus on summarizing improvement strategies with respect activity stability over years. Finally, challenges development prospects discussed.

Язык: Английский

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Mechanism of Particle-Mediated Inhibition of Demetalation for Single-Atom Catalytic Sites in Acidic Electrochemical Environments

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(28), С. 15528 - 15537

Опубликована: Июль 10, 2023

Demetalation, caused by the electrochemical dissolution of metal atoms, poses a significant challenge to practical application single-atom catalytic sites (SACSs) in proton exchange membrane-based energy technologies. One promising approach inhibit SACS demetalation is use metallic particles interact with SACSs. However, mechanism underlying this stabilization remains unclear. In study, we propose and validate unified which can Fe Metal act as electron donors, decreasing oxidation state increasing density at FeN4 position, thereby strengthening Fe-N bond, inhibiting dissolution. Different types, forms, contents increase bond strength varying extents. A linear correlation between state, strength, amount supports mechanism. Our screening particle-assisted led 78% reduction dissolution, enabling continuous operation for up 430 h fuel cell. These findings contribute development stable SACSs applications.

Язык: Английский

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Single-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Фев. 28, 2024

Abstract The development of facile tailoring approach to adjust the intrinsic activity and stability atomically-precise metal nanoclusters catalysts is great interest but remians challenging. Herein, well-defined Au 8 modified by single-atom sites are rationally synthesized via a co-eletropolymerization strategy, in which uniformly dispersed nanocluster co-entrenched on poly-carbazole matrix. Systematic characterization theoretical modeling reveal that functionalizing single-atoms enable altering electronic structures clusters, amplifies their electrocatalytic reduction CO 2 ~18.07 fold compared isolated clusters. rearrangements structure not only strengthen adsorption key intermediates *COOH, also establish favorable reaction pathway for reaction. Moreover, this strategy fixing cross-linked polymer networks efficiently deduce performance deactivation caused agglomeration during catalytic process. This work contribute explore improvement

Язык: Английский

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Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Фев. 29, 2024

Abstract The exploration of sustainable energy utilization requires the implementation advanced electrochemical devices for efficient conversion and storage, which are enabled by usage cost-effective, high-performance electrocatalysts. Currently, heterogeneous atomically dispersed catalysts considered as potential candidates a wide range applications. Compared to conventional catalysts, metal atoms in carbon-based have more unsaturated coordination sites, quantum size effect, strong metal–support interactions, resulting exceptional catalytic activity. Of these, dual-atomic (DACs) attracted extensive attention due additional synergistic effect between two adjacent atoms. DACs advantages full active site exposure, high selectivity, theoretical 100% atom utilization, ability break scaling relationship adsorption free on sites. In this review, we summarize recent research advancement DACs, includes (1) comprehensive understanding synergy atomic pairs; (2) synthesis DACs; (3) characterization methods, especially aberration-corrected scanning transmission electron microscopy synchrotron spectroscopy; (4) energy-related last part focuses great catalysis small molecules, such oxygen reduction reaction, CO 2 hydrogen evolution N reaction. future challenges opportunities also raised prospective section.

Язык: Английский

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Advances of Synergistic Electrocatalysis Between Single Atoms and Nanoparticles/Clusters

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Июль 9, 2024

Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts. Both synergy effect and high atomic utilization of active sites in the composite catalysts result enhanced electrocatalytic performance, simultaneously provide a radical analysis interrelationship between structure activity. In this review, recent advances single-atomic site coupled are emphasized. Firstly, synthetic strategies, characterization, dynamics types clusters/nanoparticles introduced, then key factors controlling discussed. Next, several clean energy catalytic reactions performed over synergistic illustrated. Eventually, encountering challenges recommendations for future advancement energy-transformation electrocatalysis outlined.

Язык: Английский

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Constructing a Highly Active Pd Atomically Dispersed Catalyst for Cinnamaldehyde Hydrogenation: Synergistic Catalysis between Pd–N₃ Single Atoms and Fully Exposed Pd Clusters

ACS Catalysis, Год журнала: 2024, Номер 14(4), С. 2369 - 2379

Опубликована: Янв. 31, 2024

Fabricating highly active catalysts with fully exposed metal atoms is necessary to greatly enhance the catalytic efficiency of selective hydrogenation. Here, we precisely constructed a carbon-nitride-nanosheet-supported Pd atomically dispersed catalyst (PdSA+C/g-C3N4) by simple low-temperature impregnation strategy. Importantly, obtained PdSA+C/g-C3N4 includes Pd–N3 single and subnanoclusters atomic-layer thickness. Moreover, exhibits 100% cinnamaldehyde (CAL) conversion rate 97.3% phenylpropanal selectivity during CAL hydrogenation, which much better than most reported catalysts. Meanwhile, turnover frequency 9.19 s–1, about 12 times higher that single-atom Further mechanism studies show synergistic effect between in key improve hydrogenation activity CAL. Specifically, hydrogen preferentially adsorbs dissociates on nanoclusters, while atoms. After that, could overflow from clusters thus improving reaction kinetics. This work develops method prepare multimetal sites provides an insight into reaction.

Язык: Английский

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Encaging Co nanoparticle in atomic Co N4-dispersed graphite nanopocket evokes high oxygen reduction activity for flexible Zn-air battery

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 347, С. 123792 - 123792

Опубликована: Апрель 24, 2024

Язык: Английский

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Manipulating the Electronic Properties of an Fe Single Atom Catalyst via Secondary Coordination Sphere Engineering to Provide Enhanced Oxygen Electrocatalytic Activity in Zinc‐Air Batteries

Advanced Materials, Год журнала: 2024, Номер 36(44)

Опубликована: Сен. 16, 2024

Abstract Oxygen reduction and evolution reactions are two key processes in electrochemical energy conversion technologies. Synthesis of nonprecious metal, carbon‐based electrocatalysts with high oxygen bifunctional activity stability is a crucial, yet challenging step to achieving conversion. Here, an approach address this issue: synthesis atomically dispersed Fe electrocatalyst (Fe 1 /NCP) over porous, defect‐containing nitrogen‐doped carbon support, described. Through incorporation phosphorus atom into the second coordination sphere iron, durability boundaries catalyst pushed unprecedented level alkaline environments, such as those found zinc‐air battery. The rationale delicately incorporate P heteroatoms defects close central metal sites (FeN 4 ‐OH) order break local symmetry electronic distribution. This enables suitable binding strength oxygenated intermediates. In situ characterizations theoretical studies demonstrate that these synergetic interactions responsible for stability. These intrinsic advantages /NCP enable potential gap mere 0.65 V power density 263.8 mW cm −2 when incorporated findings underscore importance design principles access high‐performance green

Язык: Английский

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Structural Regulation Strategies of Atomic Cobalt Catalysts for Oxygen Electrocatalysis

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

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Lowering the Kinetic Barrier via the Synergistic Catalysis of N-CNTs Supported RhP Subnanoclusters and Confined Co Nanoparticles for Olefins Hydroformylation

ACS Catalysis, Год журнала: 2025, Номер 15(2), С. 1399 - 1410

Опубликована: Янв. 9, 2025

Developing synergistic sites for a multistep elementary reaction is important, but challenging. Herein, the coexistence of Co nanoparticles confined inside carbon nanotubes and RhP subnanoclusters loaded on outside nanotube (Co@N-CNTs|RhP) synthesized by defect-assisted impregnation strategy. Notably, have engineering distance 0.66 nm. The turnover frequency over Co@N-CNTs|RhP catalyst could reach 82603 h–1 during diisobutylene hydroformylation, 15 times higher than that commercial Rh homogeneous catalysts. More importantly, obtained achieved 25 catalytic cycles. Kinetic experiments show key to promote hydroformylation diisobutylene, which reduces activation energy 64.6 kJ/mol. Further in situ DRIFT spectra theoretical calculations reveal modified are conducive adsorption H2, CO, while responsible formation aldehydes. This work provides profound insight construction efficient multisite heterogeneous long-chain olefin conversion reactions.

Язык: Английский

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