Applied Surface Science, Journal Year: 2025, Volume and Issue: unknown, P. 162854 - 162854
Published: March 1, 2025
Language: Английский
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(42)
Published: Sept. 2, 2023
Abstract Designing novel single‐atom catalysts (SACs) supports to modulate the electronic structure is crucial optimize catalytic activity, but rather challenging. Herein, a general strategy proposed utilize metalloid properties of trap and stabilize single‐atoms with low‐valence states. A series supported on surface tungsten carbide (M‐WC x , M=Ru, Ir, Pd) are rationally developed through facile pyrolysis method. Benefiting from WC exhibit weak coordination W C atoms, resulting in formation active centers similar metals. The unique metal‐metal interaction effectively stabilizes single atoms improves orbital energy level distribution sites. As expected, representative Ru‐WC exhibits superior mass activities 7.84 62.52 mg Ru −1 for hydrogen oxidation evolution reactions (HOR/HER), respectively. In‐depth mechanistic analysis demonstrates that an ideal dual‐sites cooperative mechanism achieves suitable adsorption balance H ad OH energetically favorable Volmer step. This work offers new guidance precise construction highly SACs.
Language: Английский
Citations
106
Small Structures, Journal Year: 2023, Volume and Issue: 4(8)
Published: March 22, 2023
With the further exploitation of renewable energy sources, electrochemical hydrogen evolution reaction (HER) is considered a key technology to solve environmental problems and achieve global carbon neutrality. Currently, alkaline water electrolyzers (AWEs) have been revitalized as traditional electrolytic production industry, yet they face great challenges in achieving new technological breakthroughs due catalytic properties electrode materials. In media, besides slow kinetics oxygen reaction, sluggish HER needing dissociation mass transfer at high current densities are among major factors limiting development electrolysis for industrial applications. Therefore, it importance design electrocatalysts with activity stability (>500 mA cm −2 ) applications “Research Development level” (R&D level). Herein, brief overview AWEs scale presented, some mainstream recognized catalysis mechanisms electrolytes summarized. Based on requirements application theoretical guidance, activation strategies also This review will propose insights into future electrolysis.
Language: Английский
Citations
71
ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(11), P. 7597 - 7605
Published: May 22, 2023
Ruthenium (Ru)-based catalysts exhibited great potential for the alkaline hydrogen evolution reaction. However, strong adsorption of H on Ru surface and undesirable agglomeration are obstacles to further boosting their reaction (HER) performance. Herein, we develop C60 fullerenol C60(OH)24 stabilize, disperse, activate nanoparticles through Ru–O–C60 connections. Despite ultrahigh content (38.6 wt %), densely uniformly dispersed substrate due anchoring confinement effects fullerenols. Moreover, electron-withdrawing properties induce electrons flow from interface, which enhances electronic metal–support interaction, thereby optimizing behavior different intermediates. The synthesized Ru–OC60-300 has a remarkably small overpotential (4.6 mV at 10 mA cm–2) Tafel slope (24.7 dec–1), showing high activity stability toward HER. Density functional theory simulations reveal that interface engineering weakens Ru–H affinity, promotes water dissociation, accelerates kinetics.
Language: Английский
Citations
48
Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)
Published: Jan. 10, 2024
Abstract The state-of-the-art alkaline hydrogen evolution catalyst of united ruthenium single atoms and small nanoparticles has sparked considerable research interest. However, it remains a serious problem that primarily proceeds on the less active instead more efficient in catalyst, hence largely falling short its full activity potential. Here, we report by combining highly oxophilic cerium fully-exposed nanoclusters nitrogen functionalized carbon support, centers are facilely reversed to driven strong oxophilicity cerium, which significantly improves with mass up −10.1 A mg −1 at −0.05 V. This finding is expected shed new light developing rational regulation for evolution.
Language: Английский
Citations
45
Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(23)
Published: May 1, 2023
Abstract MXenes are promising substrates for supported noble metal electrocatalysts. Yet, it is a significant challenge to modulate the metal–support interaction (MSI) enhancing catalytic performance. Herein, employing facile HF etching method, cation vacancy structures in Ti 3 C 2 T x controllably tuned, producing nearly vacancy‐free (Ti ‐V 0 ), single atom S or cluster ) engineered MXenes. Ruthenium atomic clusters, as model catalyst, successfully anchor on all MXene substrates. Different from terminal O/F coordination groups routine surfaces, clusters create unique lattice carbon ligand environment toward Ru species, which induces ultra‐strong MSI. As result, compared and , modulated (Ru@Ti exhibit optimized balance of H O adsorption/dissociation OH/H desorption, thereby delivering superior electrocatalytic performance alkaline hydrogen evolution reaction (HER). Within wide range laboratory‐level (90 mA cm −2 industrial‐level (1.5 A current density, Ru@Ti outperforms commercial Pt/C terms overpotential mass activity. Moreover, universal substrate catalysts, can also Ir/Pt/Rh enable excellent HER This work expands scope MSI between catalysts.
Language: Английский
Citations
42
Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(17)
Published: Jan. 17, 2024
Abstract Understanding and modulating the unique electronic interaction between single‐metal atoms high entropy compounds are of great significance to enable their high‐efficiency oxygen electrocatalysis for aprotic lithium‐oxygen (Li‐O 2 ) batteries. Herein, a novel bi‐functional electrocatalyst is first time created by immobilizing single‐atom ruthenium (Ru) on lanthanum‐based perovskite oxide La(Mn 0.2 Co Fe Ni Cr )O 3 (Ru@HEPO), which demonstrates activity stability in Li‐O The heteronuclear coordination Ru HEPO facilitates fast electron transfer from establishing Ru‐O‐M (M stands Mn, Co, Fe, Ni) bridges, well redistributes electrons within Ru@HEPO hence significantly improving its interfacial charge kinetics electrocatalytic activity. Additionally, strong coupling Mn enhances hybridization 3d O 2p orbitals, promotes inherent affinity toward LiO intermediate, thereby reducing reaction energy barrier electrode. As result, Ru@HEPO‐based batteries deliver remarkable electrochemical performances, such as efficiency (87.3% at 100 mA g −1 ), excellent rate capability (low overpotential 0.52 V durable cyclability (345 cycles 300 ). This work opens up promising avenue development entropy‐based electrocatalysts precisely tailoring distributions an atomic scale.
Language: Английский
Citations
37
Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(7), P. 3844 - 3878
Published: Jan. 1, 2024
This review provides a systematic summary of the nanostructure engineering Ru-modified electrocatalysts for electrocatalytic water splitting. These regulation strategies, such as single atom sites, doping, alloying and interfacial are summarized in detail.
Language: Английский
Citations
33
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(28)
Published: March 11, 2024
Abstract Electrochemical water splitting to produce green hydrogen offers a promising technology for renewable energy conversion and storage, as well realizing carbon neutrality. The efficiency, stability, cost of electrocatalysts toward evolution reaction (HER) electrocatalytic overall (EOWS) at large current densities are essential practical application. In this review, the key factors that determine catalytic performance summarized from angel thermodynamic kinetic correlation. corresponding design strategies presented. electronic structure density active sites affect adsorption/desorption intermediates considered aspects, while charge transfer mass transport capabilities closely associated with electrode resistance intermediate diffusion assigned effects. Recent development bifunctional integrated EOWS is also discussed in detail. Finally, perspective direction on under proposed. This comprehensive overview will offer profound insights guidance continued advancement field.
Language: Английский
Citations
30
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(22)
Published: Feb. 7, 2024
Abstract In recent years, single‐atom catalysts (SACs) have become the most active part of catalytic field due to their excellent activity. Among them, Ru SACs exhibit performance in many applications high atomic utilization efficiency, activity and selectivity, relatively low cost. order understand structure–performance relationship potential mechanism SACs, this review summarizes research progress fields electrocatalytic water splitting, fuel cells, nitrogen reduction, nitrate reduction years. The process single atom different synthesis methods modification strategies is summarized. Finally, some opportunities challenges for future development are prospected.
Language: Английский
Citations
30
Joule, Journal Year: 2024, Volume and Issue: 8(6), P. 1790 - 1803
Published: June 1, 2024
Language: Английский
Citations
24