Regulating electronic states of nitride/hydroxide to accelerate kinetics for oxygen evolution at large current density

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: April 4, 2023

Rational design efficient transition metal-based electrocatalysts for oxygen evolution reaction (OER) is critical water splitting. However, industrial water-alkali electrolysis requires large current densities at low overpotentials, always limited by intrinsic activity. Herein, we report hierarchical bimetal nitride/hydroxide (NiMoN/NiFe LDH) array as model catalyst, regulating the electronic states and tracking relationship of structure-activity. As-activated NiMoN/NiFe LDH exhibits industrially required density 1000 mA cm-2 overpotential 266 mV with 250 h stability OER. Especially, in-situ electrochemical spectroscopic reveals that heterointerface facilitates dynamic structure to optimize structure. Operando impedance spectroscopy implies accelerated OER kinetics intermediate due fast charge transport. The mechanism revealed combination theoretical experimental studies, indicating as-activated follows lattice oxidation kinetics. This work paves an avenue develop catalysts via tuning states.

Language: Английский

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Surface Reconstruction of Water Splitting Electrocatalysts

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(33)

Published: July 8, 2022

Abstract Water electrolysis is regarded as an efficient and green method to produce hydrogen gas, a clean energy carrier that holds the key solving global problems. So far, efficiency large‐scale application of water are restricted by electrocatalytic activity applied catalysts. Recently, reconstruction phenomenon electrocatalysts during catalytic reaction has been discovered, which could form reactive sites for both oxygen evolution reactions. Regulation process generate large number species with high since demonstrated effective strategy enhance performance electrocatalysts. This review summarizes recent progress in regulation strategies First, mechanism briefly introduced, critical factors regarding systematically discussed, followed brief introduction advanced characterization reconstruction. Moreover, modulation summarized reported examples highlighting promoted effects on process. Finally, challenges facing surface‐reconstructed catalysts future discussed.

Language: Английский

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Synergistic effect of multiple vacancies to induce lattice oxygen redox in NiFe-layered double hydroxide OER catalysts

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 323, P. 122091 - 122091

Published: Nov. 3, 2022

Language: Английский

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Dynamic rhenium dopant boosts ruthenium oxide for durable oxygen evolution

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Jan. 21, 2023

Heteroatom-doping is a practical means to boost RuO2 for acidic oxygen evolution reaction (OER). However, major drawback conventional dopants have static electron redistribution. Here, we report that Re in Re0.06Ru0.94O2 undergo dynamic accepting-donating adaptively boosts activity and stability, which different from with dopant We show during OER, (1) accept electrons at the on-site potential activate Ru site, (2) donate back large overpotential prevent dissolution. confirm via situ characterizations first-principle computation electron-interaction between facilitates adsorbate mechanism lowers adsorption energies intermediates stability of Re0.06Ru0.94O2. demonstrate high mass 500 A gcata.-1 (7811 gRe-Ru-1) number S-number = 4.0 × 106 noxygen nRu-1 outperform most electrocatalysts. conclude can be used active sites therefore guide design adaptive electrocatalysts clean energy conversions.

Language: Английский

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Advances in Oxygen Evolution Electrocatalysts for Proton Exchange Membrane Water Electrolyzers

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(14)

Published: Feb. 17, 2022

Abstract Proton exchange membrane water electrolyzer (PEMWE) technology is of interest in the context electrocatalytic hydrogen generation from renewable energies. It has benefits immediate response, higher proton conductivity, lower ohmic losses, and gas crossover rate. One key step toward to large‐scale application, development highly efficient, durable, compatible anodic oxygen evolution electrocatalysts acidic media decrease usage expensive scarce precious metals. Within this scenario, an in‐depth understanding reaction mechanisms including adsorption mechanism lattice first provided aid innovative materials elucidate origin catalyst degradation. Second, recent progress acid reviewed with emphasis on underlying structure–performance relationships. Third, current application status research PEMWEs along representative examples are discussed. Last, remaining challenges promising insights proposed inspire future studies production energy.

Language: Английский

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Triggering Lattice Oxygen Activation of Single‐Atomic Mo Sites Anchored on Ni–Fe Oxyhydroxides Nanoarrays for Electrochemical Water Oxidation

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(29)

Published: May 17, 2022

Tuning the reactivity of lattice oxygen is significance for lowering energy barriers and accelerating evolution reaction (OER). Herein, single-atomic Mo sites are anchored on Ni-Fe oxyhydroxide nanoarrays by a facile metal-organic-framework-derived strategy, exhibiting superior performance toward OER in alkaline media. In situ electrochemical spectroscopy isotope-labeling experiments reveal involvement during cycles. Combining theoretical experimental investigations electronic configuration, it comprehensively confirmed that incorporation enables higher oxidation state metal strengthened metal-oxygen hybridization, as well formation oxidized ligand holes above Fermi level. word, considerable acceleration water achieved via enhancing triggering activation. This work may provide new insights designing ideal electrocatalysts tuning chemical activating anions ligands.

Language: Английский

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Identification of the Origin for Reconstructed Active Sites on Oxyhydroxide for Oxygen Evolution Reaction

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(6)

Published: Nov. 21, 2022

The regulation of atomic and electronic structures active sites plays an important role in the rational design oxygen evolution reaction (OER) catalysts toward electrocatalytic hydrogen generation. However, precise identification for surface reconstruction behavior during OER remains elusive water-alkali electrolysis. Herein, irreversible accompanied by copper dynamic cobalt iron layered double hydroxide (CoFe LDH) precatalyst to form CoFeCuOOH species with high-valent Co is reported, identifying origin reconstructed through operando UV-Visible (UV-vis), situ Raman, X-ray absorption fine-structure (XAFS) spectroscopies. Density functional theory analysis rationalizes this typical structure causing transfer intramolecular electrons ligand holes, promoting sites. Specifically, unambiguous explored 18 O isotope-labeling differential electrochemical mass spectrometry (DEMS) supported theoretical calculation, confirming mechanism switch oxygen-vacancy-site (OVSM) pathway on lattice oxygen. This work enables elucidate vital active-site generation representative contribution OVSM efficient performance.

Language: Английский

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Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Sept. 27, 2023

The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxidation mechanism (LOM) can break theoretical limit of conventional adsorbate and enhance kinetics, yet unsatisfied stability remains grand challenge. Here, we report high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms O vacancies (AuSA-MnFeCoNiCu LDH), which not only displays low overpotential 213 mV at 10 mA cm-2 high mass activity 732.925 A g-1 250 in 1.0 M KOH, but also delivers good 700 h continuous operation ~100 cm-2. Combining advanced spectroscopic techniques density functional theory calculations, it demonstrated that synergistic interaction between incorporated leads an upshift 2p band weakens metal-O bond, thus triggering LOM, reducing energy barrier, boosting intrinsic activity.

Language: Английский

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Electrocatalytic water splitting: Mechanism and electrocatalyst design

Nano Research, Journal Year: 2023, Volume and Issue: 16(7), P. 9142 - 9157

Published: April 2, 2023

Language: Английский

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Pd–PdO Nanodomains on Amorphous Ru Metallene Oxide for High‐Performance Multifunctional Electrocatalysis

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(12)

Published: Jan. 4, 2023

Developing highly efficient multifunctional electrocatalysts is crucial for future sustainable energy pursuits, but remains a great challenge. Herein, facile synthetic strategy used to confine atomically thin Pd-PdO nanodomains amorphous Ru metallene oxide (RuO2 ). The as-synthesized electrocatalyst (Pd2 RuOx-0.5 h) exhibits excellent catalytic activity toward the pH-universal hydrogen evolution reaction (η10 = 14 mV in 1 m KOH, η10 12 0.5 H2 SO4 , and 22 PBS), alkaline oxygen 225 mV), overall water splitting (E10 1.49 V) with high mass operational stability. Further reduction endows material RuOx-2 promising activity, evidenced by halfway potential, four-electron selectivity, poison tolerance. enhanced attributed rational integration of favorable nanostructures, including 1) nanosheet morphology, 2) coexisting defective crystalline phases, 3) multi-component heterostructural features. These structural factors effectively regulate material's electronic configuration adsorption intermediates at active sites energetics.

Language: Английский

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