Symmetry‐Broken Ru Nanoparticles with Parasitic Ru‐Co Dual‐Single Atoms Overcome the Volmer Step of Alkaline Hydrogen Oxidation DOI

Xueqin Mu,

Suli Liu, Mengyang Zhang

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(12)

Published: Jan. 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.

Language: Английский

Stabilizing Low‐Valence Single Atoms by Constructing Metalloid Tungsten Carbide Supports for Efficient Hydrogen Oxidation and Evolution DOI Open Access
Luqi Wang,

Zipeng Xu,

Chun‐Han Kuo

et al.

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

110

Flower‐Like Amorphous MoO3−x Stabilized Ru Single Atoms for Efficient Overall Water/Seawater Splitting DOI Creative Commons
Feng Dong, Pengyan Wang, Rui Qin

et al.

Advanced Science, Journal Year: 2023, Volume and Issue: 10(18)

Published: April 24, 2023

Benefitting from the maximum atom utilization efficiency, special size quantum effects and tailored active sites, single-atom catalysts (SACs) have been promising candidates for bifunctional toward water splitting. Besides, due to unique structure properties, some amorphous materials found possess better performance than their crystalline counterparts in electrocatalytic Herein, by combining advantages of ruthenium (Ru) single atoms substrates, molybdenum-based oxide stabilized single-atomic-site Ru (Ru SAs-MoO

Language: Английский

Citations

75

Symmetry‐Broken Ru Nanoparticles with Parasitic Ru‐Co Dual‐Single Atoms Overcome the Volmer Step of Alkaline Hydrogen Oxidation DOI

Xueqin Mu,

Suli Liu, Mengyang Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(12)

Published: Jan. 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.

Language: Английский

Citations

73

Recent advances of bifunctional electrocatalysts and electrolyzers for overall seawater splitting DOI
Xiaoyan Wang,

Meiqi Geng,

Shengjun Sun

et al.

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 12(2), P. 634 - 656

Published: Dec. 2, 2023

This review summarizes advances in bifunctional electrocatalysts and electrolyzers for seawater splitting, including various catalysts ( e.g. , phosphides, chalcogenides, borides, nitrides, (oxy)hydroxides) membrane-based/membrane-less systems.

Language: Английский

Citations

53

Asymmetric Bond Delta‐Polarization at the Interfacial Se─Ru─O Bridge for Efficient pH‐Robust Water Electrolysis DOI
Ya Chen, Yaoda Liu, Lei Li

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: June 10, 2024

Abstract The rationalization of pH‐robust catalysis is highly desired but challengeable for overall water electrolysis (WE). It requests a metal active site that can make an efficient adaption with both cathodic hydrogen and anodic oxygen evolution reactions (HER/OER). Herein, RuO 2‐x /RuSe 2 heterostructure electrocatalyst profiled interfacial Se─Ru─O bridge the splitting studies. An asymmetric bond delta‐polarization (Δp) found at bridge, including Δp > 0 Ru─O part < Ru─Se side by experiment calculation results. enlarged polarizability (Δp 0) in principle trigger lattice mediated (LOM) pathway OER; meanwhile, reduced benefit HER due to strengthened d‐p band hybridization. Resultantly, deliver ultralow overpotentials 25/10 mV Pt‐beyond 210/255 OER 10 mA cm −2 acidic/alkaline media, respectively. In especial, acidic WE be stably operated 200 h low cell voltage 1.478 V . This research clarifies polarization as criterion rational design catalysts.

Language: Английский

Citations

43

Nanostructure engineering of ruthenium-modified electrocatalysts for efficient electrocatalytic water splitting DOI
Yun Tong, Pengzuo Chen

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

Metal natural product complex Ru-procyanidins with quadruple enzymatic activity combat infections from drug-resistant bacteria DOI Creative Commons

Jie Shan,

Xu Jin,

Cong Zhang

et al.

Acta Pharmaceutica Sinica B, Journal Year: 2024, Volume and Issue: 14(5), P. 2298 - 2316

Published: Jan. 26, 2024

Bacterial infection hampers wound repair by impeding the healing process. Concurrently, inflammation at site triggers production of reactive oxygen species (ROS), causing oxidative stress and damage to proteins cells. This can lead chronic wounds, posing severe risks. Therefore, eliminating bacterial reducing ROS levels are crucial for effective healing. Nanozymes, possessing enzyme-like catalytic activity, convert endogenous substances into highly toxic substances, such as ROS, combat bacteria biofilms without inducing drug resistance. However, current nanozyme model with single enzyme activity falls short meeting complex requirements antimicrobial therapy. Thus, developing nanozymes multiple enzymatic activities is essential. Herein, we engineered a novel metalloenzyme called Ru-procyanidin nanoparticles (Ru-PC NPs) diverse aid infections. Under acidic conditions, due their glutathione (GSH) depletion peroxidase (POD)-like Ru-PC NPs combined H2O2 exhibit excellent antibacterial effects. in neutral environment, NPs, catalase (CAT) decompose O2, alleviating hypoxia ensuring sufficient supply. Furthermore, possess exceptional antioxidant capacity through superior superoxide dismutase (SOD) effectively scavenging excess nitrogen (RNS) environment. maintains balance system prevents inflammation. also promote polarization macrophages from M1 M2, facilitating More importantly, show good biosafety negligible toxicity. In vivo models have confirmed efficacy inhibiting promoting The focus this work highlights quadruple its potential reduce bacteria-infected

Language: Английский

Citations

30

Unique CoP Microflower Decorated with Phosphorous‐Enriched PtP2 onto Nickel Foam with Interfacial Electronic Interactions to Boost Alkaline Water‐Splitting DOI

Wen‐Li Yu,

Qichang Li, Weiping Xiao

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(27)

Published: March 1, 2024

Abstract The development of stable and efficient electrocatalysts for overall freshwater/seawater water‐splitting has received significant attention. In this study, the fabrication electrocatalytic properties phosphorus‐enriched PtP 2 dispersed on CoP (PtP /CoP) HER OER in both alkaline fresh/seawater media are described. Physical characterization density functional theory calculations reveal that strong electronic interfacial interactions between optimized reaction kinetics by regulating adsorption/desorption intermediates cleavage reactants. Additionally, operando electrochemical impedance spectroscopy reveals /CoP significantly decreased phase angle with increasing applied potential compared CoP, demonstrating construction heterostructure provides a faster charge transfer surface inner layer. Notably, catalyst only requires overpotentials 101 298 mV to achieve benchmark 100 mA cm −2 freshwater OER. Moreover, prepared featured 108 330 an seawater electrolyte. Furthermore, high‐efficiency water electrolysis operation can be achieved using as anode cathode (1.63 V@100 ) coupled satisfactory durability. This finding deeper comprehension interaction Pt‐less compounds matrix electrocatalysis bifunctional electrocatalysts.

Language: Английский

Citations

25

Innovations in Electrocatalysts, Hybrid Anodic Oxidation, Eelectrolyzers for Enhanced Direct Seawater Electrolysis DOI
Dong Liu,

Yaohai Cai,

Xin Wang

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(19), P. 6897 - 6942

Published: Jan. 1, 2024

This review focuses on the latest developments in direct seawater electrolysis, specifically electrocatalysts, hybrid anodic oxidation, and electrolyzers, providing a glimpse into future of environmentally friendly hydrogen generation.

Language: Английский

Citations

25

Recent advances in hydrogen production coupled with alternative oxidation reactions DOI

Guoliang Gao,

Zixu Sun, Xueli Chen

et al.

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 509, P. 215777 - 215777

Published: March 26, 2024

Language: Английский

Citations

22