Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption

Zheng, Xueli; Zhang, Bo; Luna, Phil De; Liang, Yufeng; Comin, Riccardo; Voznyy, Oleksandr; Han, Lili; Arquer, F. Pelayo Garcı́a de; Liu, Min; Dinh, Cao-Thang; Regier, Tom; Dynes, James J.; He, Sisi; Xin, Huolin L.; Peng, Huisheng; Prendergast, David; Du, Xi‐Wen; Sargent, Edward H.

doi:10.1038/nchem.2886

Cited by 519 publications

(424 citation statements)

References 44 publications

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“…The obtained strip shows a smooth surface and is in shiny silver color, an indication of the metallic characteristic. We further activate the surface of the NiFePB by dipping the strip in an acidic solution for 10 min, which creates catalytically active sites accounting for metal oxides/hydroxides MO x /M(OH) x that have been identified as active sites in OER . The X‐ray diffraction (XRD) pattern of the activated NiFePB (inset of Figure a; Figure S2, Supporting Information) shows only one broad peak centered at 45°, which confirms its amorphous structure .…”

Section: Resultsmentioning

confidence: 88%

Designing Highly Efficient and Long‐Term Durable Electrocatalyst for Oxygen Evolution by Coupling B and P into Amorphous Porous NiFe‐Based Material

Wang

Zhang

et al. 2019

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Oxygen evolution reaction (OER) is of great significance for hydrogen production via water electrolysis, which, however, demands development of highly active, durable, and cost‐effective electrocatalysts in order to stride into a renewable energy era. Herein, highly efficient and long‐term durable OER by coupling B and P into an amorphous porous NiFe‐based electrocatalyst is reported, which possesses an amorphous porous metallic bulk structure and high corrosion resistance, and overcomes the issues associated with currently used catalyst nanomaterials. The PB codoping in the activated NiFePB (a‐NiFePB) delocalizes both Fe and Ni at Fermi energy level and enhances p–d hybridization as simulated by density functional theory calculations. The harmonized electronic structure and unique porous framework of the a‐NiFePB consequently improve the OER activity. The activated NiFePB thus exhibits an extraordinarily low overpotential of 197 mV for harvesting 10 mA cm−2 OER current density and 233 mV for reaching 100 mA cm−2 under chronopotentiometry condition, with the Tafel slope harmoniously conforming to 34 mV dec−1. Impressive long‐term stability of this new catalyst is evidenced by only limited activity decay after 1400 h operation at 100 mA cm−2. This work strategically directs a way for heading up a promising energy conversion alternative.

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Section: Resultsmentioning

confidence: 88%

Designing Highly Efficient and Long‐Term Durable Electrocatalyst for Oxygen Evolution by Coupling B and P into Amorphous Porous NiFe‐Based Material

Wang

Zhang

et al. 2019

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“…Furthermore, the better electrocatalytic activity of h-TMCN is also reflected by its smaller charge transfer resistance (R ct ; Figure 5d). [38] To examine the stability of the electrodes, we had varied the overpotential sequentially for each 10 h on the h-TMCN electrode and contrast Ni foam substrate for OER (Figure 5e). Energy Mater.…”

Section: D H-tmcn Heterostructure Nanosheets As Catalysts For Oer Anmentioning

confidence: 99%

Rational Design of Holey 2D Nonlayered Transition Metal Carbide/Nitride Heterostructure Nanosheets for Highly Efficient Water Oxidation

Kou

Wang

et al. 2019

Advanced Energy Materials

212

120

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Due to integrated advantages in electrochemical functionalities for energy conversion, 2D nonlayered heterostructure nanosheets offer new and fascinating opportunities for electrocatalysis but their fabrication is challenging when compared with the widely studied 2D layered heterostructure. Herein, a bottom‐up approach is established for facile synthesis of holey 2D transition metal carbide/nitride heterostructure nanosheets (h‐TMCN) with regulated hole sizes by controlled thermal annealing of the Mo/Zn bimetallic imidazolate frameworks (Mo/Zn BIFs). Ex situ phase and structural identifications disclose that the Mo/Zn BIFs precursor experiences interconnected three steps of transformation to produce h‐TMCN. Especially, the slow successive solid‐state diffusion of nitrogen and carbon into immediate noncrystalline molybdenum oxides allows the intergrowth of Mo2C and Mo2N into the 2D nonlayered heterostructure. X‐ray fine structure analysis coupled with high resolution X‐ray photoelectron spectroscopy demonstrate that Mo2C and Mo2N in the microdomains can chemically bond with each other, producing the abundant active N–Mo–C interfaces toward water splitting. Consequently, h‐TMCN affords low overpotentials, high turnover frequencies, rapid charge transfer, and superior long‐term stability toward electrocatalytic water oxidation. The present work demonstrates the feasibility of developing a broad range of 2D nonlayered heterostructures for high efficiency chemical energy conversion.

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“…It is generally acknowledged that higher valence state of nickel results in higher OER catalytic activity . Thus, various approaches to prepare nickel oxides with higher valence state and improved catalytic performance have been pursued . As a typical example, Zou et al.…”

Section: Nickel‐oxide‐based Electrocatalystsmentioning

confidence: 99%

Recent Progress on Nickel‐Based Oxide/(Oxy)Hydroxide Electrocatalysts for the Oxygen Evolution Reaction

Chen

Rui

Zhu

et al. 2018

Chemistry A European J

190

127

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Developing clean and sustainable energies as alternatives to fossil fuels is in strong demand within modern society. The oxygen evolution reaction (OER) is the efficiency-limiting process in plenty of key renewable energy systems, such as electrochemical water splitting and rechargeable metal-air batteries. In this regard, ongoing efforts have been devoted to seeking high-performance electrocatalysts for enhanced energy conversion efficiency. Apart from traditional precious-metal-based catalysts, nickel-based compounds are the most promising earth-abundant OER catalysts, attracting ever-increasing interest due to high activity and stability. In this review, the recent progress on nickel-based oxide and (oxy)hydroxide composites for water oxidation catalysis in terms of materials design/synthesis and electrochemical performance is summarized. Some underlying mechanisms to profoundly understand the catalytic active sites are also highlighted. In addition, the future research trends and perspectives on the development of Ni-based OER electrocatalysts are discussed.

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Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption

Cited by 519 publications

References 44 publications

Designing Highly Efficient and Long‐Term Durable Electrocatalyst for Oxygen Evolution by Coupling B and P into Amorphous Porous NiFe‐Based Material

Designing Highly Efficient and Long‐Term Durable Electrocatalyst for Oxygen Evolution by Coupling B and P into Amorphous Porous NiFe‐Based Material

Rational Design of Holey 2D Nonlayered Transition Metal Carbide/Nitride Heterostructure Nanosheets for Highly Efficient Water Oxidation

Recent Progress on Nickel‐Based Oxide/(Oxy)Hydroxide Electrocatalysts for the Oxygen Evolution Reaction

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