Improved Ammonia Synthesis and Energy Output from Zinc-Nitrate Batteries by Spin-State Regulation in Perovskite Oxides

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 16, 2025

Electrocatalytic nitrate reduction to ammonia (eNRA) is a promising route toward environmental sustainability and clean energy. However, its efficiency often limited by the slow conversion of intermediates due spin-forbidden processes. Here, we introduce novel A-site high-entropy strategy develop new perovskite oxide (La0.2Pr0.2Nd0.2Ba0.2Sr0.2)CoO3-δ (LPNBSC) for eNRA. The LPNBSC possesses higher concentration high-spin (HS) cobalt-active centers, resulting from an increased [CoO5] structural motifs compared conventional LaCoO3. Consequently, this material exhibits significantly improved electrocatalytic performance (NH3) production, in 3-fold increase yield rate (129 μmol h–1 mgcat.–1) 2-fold Faradaic (FE, 76%) LaCoO3 at optimal potential. Furthermore, LPNBSC-based Zn-nitrate battery reaches maximum FE 82% NH3 57 cm–2. Density functional theory calculations reveal that management perovskites facilitates activation potentially optimizes thermodynamic rate-determining step eNRA process, namely, *HNO3 + H+ e– → *NO2 H2O. This work presents efficient concept modulating spin state B-site metal offers valuable insights design high-performance catalysts.

Язык: Английский

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In-situ characterization technologies and theoretical calculations in carbon dioxide reduction: In-depth understanding of reaction mechanisms and rational design of electrocatalysts

Coordination Chemistry Reviews, Год журнала: 2025, Номер 533, С. 216541 - 216541

Опубликована: Фев. 28, 2025

Язык: Английский

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Interface engineering of Fe doped NiO/NiSe2 tailoring d-band center for enhanced oxygen evolution activity

Applied Surface Science, Год журнала: 2025, Номер unknown, С. 163087 - 163087

Опубликована: Март 1, 2025

Язык: Английский

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Stabilized High‐Valent Indium for Promoted Formate Production from Electrochemical CO₂ Reduction

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 5, 2024

Abstract Electrocatalysts based on high‐valent indium are promising for formate production via CO 2 electroreduction. However, reconstruction often occurs during the reaction progress, resulting in a decline catalytic performance. Here, composite of In O 3 /In S is developed, and its performance exceeds that either individual phase, particularly stability. Analysis morphology, valence state, situ Raman spectroscopy reveals well preserved reaction. Theoretical calculations suggest desorption energy lattice oxygen can be strengthened due to ‐In bonding within composite. This reinforcement facilitates formation more active sites promotes adsorption, further decreasing barrier only 0.12 eV. As result, exhibits selectivity over 95.05% at –1.13 V vs reversible hydrogen electrode accompanied by partial current density 434.4 mA cm –2 . Notably, maintains 95% even after 50 h an industrial‐level 200 , 17 times longer than phase. Furthermore, 18.33% solar‐to‐formate 19.49% solar‐to‐fuel obtained when coupled with III‐V solar cells, demonstrating feasibility.

Язык: Английский

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Multifunctional Strategies of Advanced Electrocatalysts for Efficient Urea Synthesis

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 20, 2024

The electrochemical reduction of nitrogenous species (such as N

Язык: Английский

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An active learning workflow for predicting hydrogen atom adsorption energies on binary oxides based on local electronic transfer features

Green Energy & Environment, Год журнала: 2024, Номер 9(10), С. 1489 - 1496

Опубликована: Июнь 28, 2024

Machine learning combined with density functional theory (DFT) enables rapid exploration of catalyst descriptors space such as adsorption energy, facilitating and effective screening. However, there is still a lack models for predicting energies on oxides, due to the complexity elemental species ambiguous coordination environment. This work proposes an active workflow (LeNN) founded local electronic transfer features (e) principle coordinate rotation invariance. By accurately characterizing electron site atoms their surrounding geometric structures, LeNN mitigates abrupt feature changes different element types clarifies environments. As result, it prediction ∗H energy binary oxide surfaces mean absolute error (MAE) below 0.18 eV. Moreover, we incorporate coverage (θl) leverage neutral network ensemble establish workflow, attaining MAE 0.2 eV 5419 multi-∗H structures. These findings validate universality capability proposed in surfaces.

Язык: Английский

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Insights into plasmon-assisted chemical reactions: from fabrication to characterization

eScience, Год журнала: 2024, Номер unknown, С. 100312 - 100312

Опубликована: Сен. 1, 2024

Язык: Английский

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Bi Doped In2O3 Nanofiber for Efficient Electrocatalytic CO2 Reduction

ChemCatChem, Год журнала: 2024, Номер unknown

Опубликована: Окт. 9, 2024

Abstract Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) to formic acid (HCOOH) is attracted for superfluous CO removal and HCOOH production under ambient conditions. Indium‐based catalysts has considered as a good candidate material RR due their environmentally friendly features. However, the catalytic efficiency limited by poor Faradaic (FE) high overpotential of electrocatalyst, activity stability indium‐based are unsatisfactory, especially in industrial current density that critical commercialization. Herein, fiber Bi‐doped In O 3 was synthesized through electrospinning method, it demonstrate FE 88.2% at −1.5 V versus RHE (reversible hydrogen electrode) with partial −21.8 mA cm −2 H type cell. Specially, Bi‐In electrocatalyst also reach standard, which can work −400 92.7% (yield 6.9 mmol h −1 ) home‐made Flow Importantly, shows 24 long‐term test −300 . The improvement catalyst ascribed optimized electronic structure site, reduced function value beneficial reducing formation energy key *OCHO intermediates.

Язык: Английский

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Reduced Graphene Oxide Regulates Indium Oxide In-Situ Reconstruction for Enhanced CO₂ Electroreduction

ACS Materials Letters, Год журнала: 2025, Номер unknown, С. 796 - 803

Опубликована: Янв. 31, 2025

The practical application of electrocatalytic CO2 reduction requires adaptation to the fluctuating voltage output photovoltaic systems. However, potential-induced in-situ reconstruction catalyst complicates control and leads Faradaic efficiency (FE) instability across potential window. Here, we present a redox graphene-supported indium oxide (G-InOx), where rGO effectively regulates surface evolution InOx from In3+ In0 during reactions. multivalent In generated via lowers energy barriers for *OCHO formation dissociation, enhancing formate production. also environment, optimizing proton delivery active sites. Over wide range (−0.86 −1.37 V vs RHE), G-InOx achieves FEformate nearly 100%. This work offers straightforward efficient strategy scalable, high-performance electroreduction.

Язык: Английский

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In Situ Raman Spectroscopic Studies of CO₂ Reduction Reactions: From Catalyst Surface Structures to Reaction Mechanisms

Chemical Science, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

In situ Raman spectroscopy study of the CO 2 electroreduction reaction.

Язык: Английский

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