An indium-induced-synthesis In0.17Ru0.83O2 nanoribbon as highly active electrocatalyst for oxygen evolution in acidic media at high current densities above 400 mA cm−2

Shi, Chen; Wang, Changlai; Gao, Fei‐Yue; Yang, Yang; Huang, Minxue; Tong, Huigang; Cheng, Zhiyu; Wang, Pengcheng; Wang, Peichen; Tu, Jinwei; Zeng, Xuehao; Chen, Qianwang

doi:10.1039/d1ta10022j

Cited by 16 publications

(11 citation statements)

References 56 publications

(68 reference statements)

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“…[33] The O 1s signals of FeÀ N/PÀ C (Figure S6c) indicates that O species mostly exist in the forms of adsorbed states and carbon-oxygen covalent bonds, while the fitting results show a weak peak assigned to FeÀ O, which may be caused by binding axial oxygen atoms at the FeÀ N 4 metal atomic site. [48,49] To exclude the possibility of Fe 2 O 3 , we investigated it in detail by EXAFS analyses.…”

Section: Methodsmentioning

confidence: 99%

Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Zhang

Liu

et al. 2023

Angew Chem Int Ed

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The electrochemical conversion of nitrate pollutants into value‐added ammonia is a feasible way to achieve artificial nitrogen cycle. However, the development of electrocatalytic nitrate‐to‐ammonia reduction reaction (NO3‐RR) has been hampered by high overpotential and low Faradaic efficiency. Here we develop an iron single‐atom catalyst coordinated with nitrogen and phosphorus on hollow carbon polyhedron (denoted as Fe‐N/P‐C) as a NO3‐RR catalyst electrode. Owing to the tuning effect of phosphorus atoms on breaking local charge symmetry of the single‐Fe‐atom catalyst, it facilitates the adsorption of nitrate ions and enrichment of some key reaction intermediates during the NO3‐RR process. The Fe‐N/P‐C catalyst exhibits 90.3% ammonia Faradaic efficiency with a yield rate of 17980 μg h‐1 mgcat‐1, greatly outperforming the reported Fe‐based catalysts. Furthermore, operando SR‐FTIR spectroscopy measurements reveal the reaction pathway based on key intermediates observed under different applied potentials and reaction durations. Density functional theory calculations demonstrate that the optimized free energy of NO3‐RR intermediates is ascribed to the asymmetric atomic interface configuration, which achieves the optimal electron density distribution. This work demonstrates the enhanced function of heteroatom doping on single atoms for NO3‐RR, and provides an effective strategy for improving the catalytic performance of single atom catalysts in different electrochemical reactions.

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Section: Methodsmentioning

confidence: 99%

Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Zhang

Liu

et al. 2023

Angew Chem Int Ed

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“…Additionally, the dband center of several oxides was computed, revealing a correlation between the d-band center and work function. [65][66][67] The positional variation of the d-band center inuences the interaction among surface electrons, the surrounding environment, and the electron distribution on the surface. With increasing atomic number, the d-band centers of CoO, NiO, and ZnO progressively decrease, distancing further from the Fermi level and diminishing electron transmittance.…”

Section: Dft Calculationmentioning

confidence: 99%

High-efficiency oxygen reduction by late transition metal oxides to produce H₂O₂

Zhang,

Jiang,

Zhang

et al. 2024

J. Mater. Chem. A

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“…Typical examples that have been reported are Nd-doped RuO 2 (Nd 0.1 RuO x ) [111] and In-doped RuO 2 (In 0.17 Ru 0.83 O 2 ). [112] After doping, they all show a significant drop in the d-band center, which balances the adsorption and resolution of the key intermediates of OOH* and reduces the reaction energy barrier. In addition to the above mentioned, effective dopants of RuO 2 have been reported as Mn, [113] Cu, [114] Pt/Ni, [115] Pt/Co, [47] K, [116] Mo/Ce, [117] La, [118] Si, [119] Se, [120] B, [121] etc.…”

Section: Heteroatom Doped Ru Dioxidesmentioning

confidence: 99%

The Promising Seesaw Relationship Between Activity and Stability of Ru‐Based Electrocatalysts for Acid Oxygen Evolution and Proton Exchange Membrane Water Electrolysis

Fan,

Zhang,

et al. 2023

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The development of electrocatalysts that are not reliant on iridium for efficient acid‐oxygen evolution is a critical step towards the proton exchange membrane water electrolysis (PEMWE) and green hydrogen industry. Ruthenium‐based electrocatalysts have garnered widespread attention due to their remarkable catalytic activity and lower commercial price. However, the challenge lies in balancing the seesaw relationship between activity and stability of these electrocatalysts during the acid‐oxygen evolution reaction (OER). This review delves into the progress made in Ru‐based electrocatalysts with regards to acid OER and PEMWE applications. It highlights the significance of customizing the acidic OER mechanism of Ru‐based electrocatalysts through the coordination of adsorption evolution mechanism (AEM) and lattice oxygen oxidation mechanism (LOM) to attain the ideal activity and stability relationship. The promising tradeoffs between the activity and stability of different Ru‐based electrocatalysts, including Ru metals and alloys, Ru single‐atomic materials, Ru oxides, and derived complexes, and Ru‐based heterojunctions, as well as their applicability to PEMWE systems, are discussed in detail. Furthermore, this paper offers insights on in situ control of Ru active sites, dynamic catalytic mechanism, and commercial application of PEMWE. Based on three‐way relationship between cost, activity, and stability, the perspectives and development are provided.

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An indium-induced-synthesis In_0.17Ru_0.83O₂ nanoribbon as highly active electrocatalyst for oxygen evolution in acidic media at high current densities above 400 mA cm⁻²

Abstract: Ruthenium dioxide-based electrocatalyst possesses the most potential in acidic oxygen evolution reaction (OER), however, most of them show low current density, low mass activity and unsatisfied stability under strong acidic...

Cited by 16 publications

References 56 publications

Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia

High-efficiency oxygen reduction by late transition metal oxides to produce H₂O₂

The Promising Seesaw Relationship Between Activity and Stability of Ru‐Based Electrocatalysts for Acid Oxygen Evolution and Proton Exchange Membrane Water Electrolysis

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An indium-induced-synthesis In0.17Ru0.83O2 nanoribbon as highly active electrocatalyst for oxygen evolution in acidic media at high current densities above 400 mA cm−2

Abstract: Ruthenium dioxide-based electrocatalyst possesses the most potential in acidic oxygen evolution reaction (OER), however, most of them show low current density, low mass activity and unsatisfied stability under strong acidic...

Cited by 16 publications

References 56 publications

Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia

High-efficiency oxygen reduction by late transition metal oxides to produce H2O2

The Promising Seesaw Relationship Between Activity and Stability of Ru‐Based Electrocatalysts for Acid Oxygen Evolution and Proton Exchange Membrane Water Electrolysis

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An indium-induced-synthesis In_0.17Ru_0.83O₂ nanoribbon as highly active electrocatalyst for oxygen evolution in acidic media at high current densities above 400 mA cm⁻²

High-efficiency oxygen reduction by late transition metal oxides to produce H₂O₂