ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3378 - 3390
Опубликована: Фев. 10, 2025
Язык: Английский
Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(42)
Опубликована: Сен. 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.
Язык: Английский
Процитировано
114
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(12)
Опубликована: Янв. 30, 2024
Abstract Efficient dual‐single‐atom catalysts are crucial for enhancing atomic efficiency and promoting the commercialization of fuel cells, but addressing sluggish kinetics hydrogen oxidation reaction (HOR) in alkaline media facile site generation remains formidable challenges. Here, we break local symmetry ultra‐small ruthenium (Ru) nanoparticles by embedding cobalt (Co) single atoms, which results release Ru atoms from on reduced graphene oxide (Co 1 1,n /rGO). In situ operando spectroscopy theoretical calculations reveal that oxygen‐affine Co atom disrupts nanoparticles, resulting parasitic within nanoparticles. The interaction between forms effective active centers. parasitism modulates adsorption OH intermediates sites, accelerating HOR through faster formation *H 2 O. As anticipated, /rGO exhibits ultrahigh mass activity (7.68 A mg −1 ) at 50 mV exchange current density (0.68 mA cm −2 ), 6 7 times higher than those Ru/rGO, respectively. Notably, it also displays exceptional durability surpassing commercial Pt catalysts. This investigation provides valuable insights into hybrid multi‐single‐atom metal nanoparticle catalysis.
Язык: Английский
Процитировано
76
Journal of the American Chemical Society, Год журнала: 2023, Номер 145(49), С. 27010 - 27021
Опубликована: Ноя. 10, 2023
Two-dimensional (2D) Pt-group ultrathin nanosheets (NSs) are promising advanced electrocatalysts for energy-related catalytic reactions. However, improving the electrocatalytic activity of 2D NSs through addition abundant grain boundaries (GBs) and understanding underlying formation mechanism remain significant challenges. Herein, we report controllable synthesis a series Rh-based nanocrystals (e.g., Rh nanoparticles, NSs, with GBs) CO-mediated kinetic control route. In light NSs' structural advantages GB modification, rich GBs exhibit an enhanced compared to pure commercial Pt/C toward hydrogen oxidation reaction (HOR) in alkaline media. Both experimental results theoretical computations corroborate that have capacity ameliorate adsorption free energy intermediates during HOR, thus resulting outstanding HOR performance. Our work offers novel perspectives realm developing sophisticated metal conversion field.
Язык: Английский
Процитировано
59
Journal of the American Chemical Society, Год журнала: 2024, Номер 146(11), С. 7858 - 7867
Опубликована: Март 8, 2024
Developing efficient bifunctional materials is highly desirable for overall proton membrane water splitting. However, the design of iridium with high acidic splitting activity and durability, as well an in-depth understanding catalytic mechanism, challenging. Herein, we successfully developed subnanoporous Ir3Ni ultrathin nanocages crystallinity The shell enables NCs optimized exposure active sites. Importantly, nickel incorporation contributes to favorable thermodynamics electrocatalysis OER after surface reconstruction hydrogen adsorption free energy in HER electrocatalysis, which induce enhanced intrinsic oxygen evolution reaction (OER) (HER). Together, achieve 3.72 A/mgIr(η=350 mV) 4.47 A/mgIr(η=40 mass activity, are 18.8 times 3.3 higher than that commercial IrO2 Pt, respectively. In addition, their crystalline identity ensures a robust nanostructure, enabling good durability during oxidation. This work provides new revenue toward structural insightful metal alloy mechanisms electrocatalysis.
Язык: Английский
Процитировано
48
Small, Год журнала: 2023, Номер 20(1)
Опубликована: Авг. 30, 2023
Abstract Upgrading overall water splitting (OWS) system and developing high‐performance electrocatalysts is an attractive way to the improve efficiency reduce consumption of hydrogen (H 2 ) production from electrolyzed water. Here, a Pt cluster/Ir metallene heterojunction structure (Pt/Ir hetero‐metallene) with unique Pt/Ir interface reported for conversion ethylene glycol (EG) glycolic acid (GA) coupled H production. With assistance oxidation (EGOR), Pt/Ir||Pt/Ir hetero‐metallene two‐electrode electrolysis exhibits lower cell voltage 0.36 V at 10 mA cm −2 . Furthermore, Faradaic EG GA as high 87%. The excellent performance this new heterostructure arise charge redistribution strain effects induced by Pt–Ir interactions between heterogeneous interfaces, well larger specific surface area more active sites due structure.
Язык: Английский
Процитировано
45
Science Advances, Год журнала: 2024, Номер 10(20)
Опубликована: Май 17, 2024
The ocean, a vast hydrogen reservoir, holds potential for sustainable energy and water development. Developing high-performance electrocatalysts production under harsh seawater conditions is challenging. Here, we propose incorporating protective V 2 O 3 layer to modulate the microcatalytic environment create in situ dual-active sites consisting of low-loaded Pt Ni N. This catalyst demonstrates an ultralow overpotential 80 mV at 500 mA cm −2 , mass activity 30.86 times higher than Pt-C maintains least hours seawater. Moreover, assembled anion exchange membrane electrolyzers (AEMWE) demonstrate superior durability even demanding industrial conditions. In localized pH analysis elucidates environmental regulation mechanism layer. Its role as Lewis acid enables sequestration excess OH − ions, mitigate Cl corrosion, alkaline earth salt precipitation. Our protection strategy by using presents promising cost-effective approach large-scale green production.
Язык: Английский
Процитировано
37
Energy & Environmental Science, Год журнала: 2024, Номер 17(12), С. 3960 - 4009
Опубликована: Янв. 1, 2024
The general principles in terms of reactivity and stability to design efficient electrocatalysts for the alkaline hydrogen oxidation reaction are reviewed. performance catalysts anion-exchange membrane fuel cells is further discussed.
Язык: Английский
Процитировано
30
Advanced Materials, Год журнала: 2024, Номер 36(32)
Опубликована: Май 25, 2024
Abstract High‐entropy alloys (HEAs) confine multifarious elements into the same lattice, leading to intense lattice distortion effect. The tends induce local microstrain at atomic level and thus affect surface adsorptions toward different adsorbates in various electrocatalytic reactions, yet remains unexplored. Herein, this work reports a class of sub‐2 nm IrRuRhMoW HEA nanoparticles (NPs) with distinct induced by for boosting alkaline hydrogen oxidation (HOR) evolution reactions (HER). This demonstrates that distortion‐rich catalysts optimized electronic structure can downshift d‐band center generate uncoordinated oxygen sites enhance oxophilicity. As result, NPs show remarkable HOR kinetic current density 8.09 mA µg −1 PGM 50 mV versus RHE, 8.89, 22.47 times higher than those IrRuRh without internal strain commercial Pt/C, respectively, which is best value among all reported non‐Pt based catalysts. also display great HER performances turnover frequency (TOF) 5.93 H 2 s 70 4.6‐fold Pt/C catalyst, exceeding most noble metal‐based Experimental characterizations theoretical studies collectively confirm weakened (H ad ) enhanced hydroxyl (OH adsorption are achieved simultaneously modulating binding energy oxophilicity originated from intensified ligand effect over NPs, guarantees HOR/HER.
Язык: Английский
Процитировано
28
Nature Communications, Год журнала: 2024, Номер 15(1)
Опубликована: Май 18, 2024
Abstract Hydroxide exchange membrane fuel cells (HEMFCs) have the advantages of using cost-effective materials, but hindered by sluggish anodic hydrogen oxidation reaction (HOR) kinetics. Here, we report an atomically dispersed Ir on Mo 2 C nanoparticles supported carbon (Ir SA -Mo C/C) as highly active and stable HOR catalysts. The specific current density C/C is 4.1 mA cm −2 ECSA , which 10 times that Ir/C. Negligible decay observed after 30,000-cycle accelerated stability test. Theoretical calculations suggest high activity attributed to unique substrate, makes sites with optimized H binding also provides enhanced OH sites. By a low loading (0.05 mg ) anode, fabricated HEMFC can deliver peak power 1.64 W . This work illustrates precious metal carbides may be promising strategy for performance HEMFCs.
Язык: Английский
Процитировано
27
Advanced Materials, Год журнала: 2024, Номер 36(38)
Опубликована: Июль 24, 2024
Constructing well-defined active multisites is an effective strategy to break linear scaling relationships develop high-efficiency catalysts toward multiple-intermediate reactions. Here, dual-intermetallic heterostructure composed of tungsten-bridged Co
Язык: Английский
Процитировано
20