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

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

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Lattice Strain with Stabilized Oxygen Vacancies Boosts Ceria for Robust Alkaline Hydrogen Evolution Outperforming Benchmark Pt

Advanced Materials, Год журнала: 2024, Номер 36(33)

Опубликована: Июнь 12, 2024

Abstract Earth‐abundant metal oxides are usually considered as stable but catalytically inert toward hydrogen evolution reaction (HER) due to their unfavorable intermediate adsorption performance. Herein, a heavy rare earth (Y) and transition (Co) dual‐doping induced lattice strain oxygen vacancy stabilization strategy is proposed boost CeO 2 robust alkaline HER. The compression increased (O v ) concentration in synergistically improve the water dissociation on O sites sequential at activated ‐neighboring sites, leading significantly enhanced HER kinetics. Meanwhile, Y doping offers effect by its stronger Y─O bonding over Ce─O, which endows catalyst with excellent stability. Y,Co‐CeO electrocatalyst exhibits an ultra‐low overpotential (27 mV 10 mA cm −2 Tafel slope (48 dec −1 ), outperforming benchmark Pt electrocatalyst. Moreover, anion exchange membrane electrolyzer incorporated achieves stability of 500 h under 600 . This synergistic sheds new light rational development efficient oxide‐based electrocatalysts.

Язык: Английский

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Enabling Logistics Automation in Nanofactory: Cobalt Phosphide Embedded Metal–Organic Frameworks for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Advanced Materials, Год журнала: 2024, Номер 36(26)

Опубликована: Апрель 14, 2024

Electrocatalytic nitrate reduction reaction (NitRR) in neutral condition offers a promising strategy for green ammonia synthesis and wastewater treatment, the rational design of electrocatalysts is cornerstone. Inspired by modern factory where both machines logistics matter manufacturing, it reported that cobalt phosphide (CoP) nanoparticles embedded zinc-based zeolite imidazole frameworks (Zn-ZIF) function as nanofactory with high performance. By selective phosphorization ZnCo bimetallic framework (ZnCo-ZIF), generated CoP act "machines" (active sites) molecular manufacturing (NO

Язык: Английский

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Tungsten Nitride/Tungsten Oxide Nanosheets for Enhanced Oxynitride Intermediate Adsorption and Hydrogenation in Nitrate Electroreduction to Ammonia

ACS Nano, Год журнала: 2023, Номер 17(24), С. 25091 - 25100

Опубликована: Дек. 6, 2023

Electrochemical NO3– reduction reaction (NO3RR) is a promising technique for green NH3 synthesis. Tungsten oxide (WO3) has been regarded as an effective electrocatalyst electrochemical However, the weak adsorption and sluggish hydrogenation of oxynitride intermediates (NOx, e.g., *NO3 *NO2) over WO3 materials hinder efficiency converting to NH3. Herein, we design heterostructure tungsten nitride (WN) (WN/WO3) nanosheets optimize *NO2 adsorptions facilitate hydrogenations achieve highly efficient NO3RR produce Theoretical calculations predict that locally introducing WN into will shorten distance between adjacent W atoms, resulting in being strongly adsorbed on active sites form bidentate ligands instead relatively monodentate ligands. Furthermore, facilitates H2O dissociation supply requisite protons, which beneficial hydrogenations. Inspired by theoretical prediction, WN/WO3 are successfully fabricated through high-temperature nitridation process. The transmission electron microscopy, X-ray photoelectron spectroscopy, absorption near-edge spectroscopy investigations confirm amorphous introduced situ composite heterostructure. as-prepared exhibit high Faraday 88.9 ± 7.2% appreciable yield rate 8.4 mg h–1 cm–2 toward production, much higher than individual WN. enhanced behaviors *NOx characterized Fourier-transform infrared consistent with predictions. This work develops facile nanomaterials tune NOx boosting from

Язык: Английский

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Concave single-atom Co nanozymes with densely edge-hosted active sites for highly sensitive immunoassay

Chemical Engineering Journal, Год журнала: 2024, Номер 495, С. 153479 - 153479

Опубликована: Июнь 25, 2024

Язык: Английский

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Self‐Encapsulated Ni Nanoparticles on Delignified Wood Carbon for Efficient Urea‐Assisted Hydrogen Production

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 8, 2024

Abstract Developing efficient, low‐cost electrocatalysts for industrial‐level hydrogen production remains a significant challenge. Here lattice‐distorted Ni nanoparticles (NPs) encapsulated within nitrogen‐doped carbon shell on delignified wood (Ni‐NC@DWC) are constructed through chitosan‐induced assembly and the pyrolysis process. Experimental theoretical results indicate that lattice distortion due to strong metal‐support interactions, boosts electron transfer reaction intermediate adsorption/desorption, enhancing both urea oxidation (UOR) evolution (HER). Interestingly, active center 3+ ‐O is dynamically cyclically generated during UOR. When utilized as self‐standing electrode in an alkaline electrolyte, Ni‐NC@DWC exhibits low potentials of 24 mV 1.244 V at 100 mA cm −2 HER UOR, respectively. Moreover, achieves ultrasmall cell voltage 1.13 urea‐assisted water splitting can operate stably over 1000 h. Furthermore, when it self‐assembled anion exchange membrane (AEM) electrolyzer, requires only 1.62 2000 industrial operates 150 h without degradation, confirming highly attractive economical, sustainable, scalable production.

Язык: Английский

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

Angewandte Chemie, Год журнала: 2024, Номер 136(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

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Main‐Group Metal‐Nonmetal Dynamic Proton Bridges Enhance Ammonia Electrosynthesis

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(45)

Опубликована: Авг. 13, 2024

The electrochemical nitrogen reduction reaction (eNRR) is a crucial process for the sustainable production of ammonia (NH

Язык: Английский

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Identifying Upper d-Band Edge as Activity Descriptor for Ammonia Oxidation on PtCo Alloys in Low-Temperature Direct Ammonia Fuel Cells

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Янв. 3, 2025

Low-temperature direct ammonia fuel cell (DAFC) stands out as a more secure technology than the hydrogen system, while there is still lack of elegant bottom-up synthesis procedures for efficient oxidation reaction (AOR) electrocatalysts. The widely accepted d-band center, even with consideration width, usually fails to describe variations in AOR reactivity many practical conditions, and accurate activity descriptor necessary less empirical path. Herein, upper edge, εu, derived from model, identified an effective accurately establishing descriptor–activity relationship. Using PtCo alloy varying atomic composition example, εu value succeeds reflecting corresponding trends activity, showing striking linear correlation coefficient determination (R2) high 0.90. effectiveness established relationship verified experimentally. optimum electrocatalyst delivers excellent peak current density 74.04 A g–1 at 5 mV s–1, assembled DAFC generates power density, outperforming majority extensively reported systems. This work brings fundamental insights into between chemical electronic structure benefits rational optimization next-generation low-temperature DAFC.

Язык: Английский

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Modulation of Fe0-FexSy heterostructure by sulfurization constitutes an electron transfer channel for efficient triclosan degradation

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 159297 - 159297

Опубликована: Янв. 1, 2025

Язык: Английский

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