Intrinsic Electrocatalytic Activity for Oxygen Evolution of Crystalline 3d‐Transition Metal Layered Double Hydroxides

Dionigi, Fabio; Zhu, Jing; Zeng, Zhenhua; Merzdorf, Thomas; Sarodnik, Hannes; Gliech, Manuel; Pan, Lujin; Li, Wei‐Xue; Greeley, Jeffrey; Strasser, Peter

doi:10.1002/ange.202100631

Cited by 48 publications

(37 citation statements)

References 58 publications

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Section: A Brief Summary Of Metal Oxide‐based Oer Catalystsmentioning

confidence: 99%

“…[ 95 ] By the combination of experiments with theoretical calculation, Strasser's group studied the intrinsic OER activities of late 3d transition metal‐based LDH in alkaline medium. [ 77 ] As shown in Figure 6g, a volcano plot determined by the OH* → O* → OOH* step was constructed. They pointed out that the intrinsic activity trend originated from the dual‐metal‐site nature of the reaction centers.…”

Section: A Brief Summary Of Metal Oxide‐based Oer Catalystsmentioning

confidence: 99%

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Structural Variations of Metal Oxide‐Based Electrocatalysts for Oxygen Evolution Reaction

et al. 2021

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including solar, wind, hydro, and biofuel, are highly desired to reduce our reliance on fossil fuels. However, according to the data provided by International Energy Agency, the global energy demand is 120 Mtoe in 2019, most (80%) of which was derived from fossil fuels (coal, natural gas, oil), leading to a huge CO 2 emission (33Gt in 2019). [1][2][3] One of the difficulties hindering the widespread use of these renewable energy sources is their intermittent and unpredictable nature. [4,5] Electrochemical reaction, a promising strategy for converting intermittent electricity into chemical energy, can produce a wide variety of important fuels and chemical feedstock, including hydrogen, hydrocarbons and ammonia. [6][7][8] The feedstocks for these productions obtained from electrochemical reactions can be offered by abundant and universal source, such as water, carbon dioxide and nitrogen. In last decades, due to the net-zero carbon emission features, electrochemical reactions have initiated extensive investigations based on water splitting reaction, nitrogen reduction reaction (NRR) and carbon dioxide reduction reaction. [9][10][11][12] In these green technologies, electrocatalytic oxygen evolution reaction (OER), a core reaction of these process, has a direct impact on device efficiency and cost effectiveness (Figure 1). [13,14] However, OER involves multistep four-electron transferring steps associated with OH breaking and OO formations, thus suffering from sluggish kinetics and requiring a high energy loss (high potential). Therefore, efficient and stable OER electrocatalysts are required to make these renewable energy storage/conversion processes to be viable and scalable technologies. [15,16,221,222] The OER catalysts can be classified into two categories: [17,18] molecular catalysts for homogeneous system and solid catalysts for heterogeneous system. In the homogeneous catalytic system, the molecular catalysts and the electrolyte are in solution, and the OER takes place in the liquid phase. The performance of molecular OER catalysts can be explained and understood at a molecular level by many relatively simple spectroscopic physicochemical techniques. Based on the mechanistic understanding at a molecular level, their geometric and electronic properties are much easier to be fine-tuned to achieve optimum performance by careful selection of the metal ion and ligand environment. Despite all these advantages, molecular catalysts are still not appropriate to be used in practical Electrocatalytic oxygen evolution reaction (OER), an important electrode reaction in electrocatalytic and photoelectrochemical cells for a carbonfree energy cycle, has attracted considerable attention in the last few years. Metal oxides have been considered as good candidates for electrocatalytic OER because they can be easily synthesized and are relatively stable during the OER process. However, inevitable structural variations still occur to them due to the complex reaction steps and harsh working conditions of OER, thus impending the ...

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Section: A Brief Summary Of Metal Oxide‐based Oer Catalystsmentioning

confidence: 99%

Section: A Brief Summary Of Metal Oxide‐based Oer Catalystsmentioning

confidence: 99%

Structural Variations of Metal Oxide‐Based Electrocatalysts for Oxygen Evolution Reaction

et al. 2021

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“…Electrochemical water oxidation is critical to clean energy production and utilization. , Hindered by the sluggish four-electron transfer process, the overall energy storage and transformation efficiency is controlled by the oxygen evolution reaction (OER). , Developing high-performance OER electrocatalysts could alleviate this problem. Ni-based hydroxides are regarded as a family of the most active OER catalysts in alkaline electrolytes and have attracted intensive attention both experimentally and computationally in recent years. − The mechanistic studies toward identifying active sites and structures have led to massive progress in these materials. − Upon Fe incorporation, even with a trace amount, the OER performance could be enhanced dramatically in alkaline electrolytes. , However, the role of Fe is still under enormous debate and needs to be clarified. − Fe incorporation in the lattice could modify the metal local environment in 3d transition metal hydroxides. Due to the local environment change, the electronic properties of 3d transition metals should be altered accordingly, which ultimately modifies catalytic performance.…”

Section: Introductionmentioning

confidence: 99%

Revealing the Dynamics and Roles of Iron Incorporation in Nickel Hydroxide Water Oxidation Catalysts

Kuai

et al. 2021

J. Am. Chem. Soc.

146

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The surface of an electrocatalyst undergoes dynamic chemical and structural transformations under electrochemical operating conditions. There is a dynamic exchange of metal cations between the electrocatalyst and electrolyte. Understanding how iron in the electrolyte gets incorporated in the nickel hydroxide electrocatalyst is critical for pinpointing the roles of Fe during water oxidation. Here, we report that iron incorporation and oxygen evolution reaction (OER) are highly coupled, especially at high working potentials. The iron incorporation rate is much higher at OER potentials than that at the OER dormant state (low potentials). At OER potentials, iron incorporation favors electrochemically more reactive edge sites, as visualized by synchrotron X-ray fluorescence microscopy. Using X-ray absorption spectroscopy and density functional theory calculations, we show that Fe incorporation can suppress the oxidation of Ni and enhance the Ni reducibility, leading to improved OER catalytic activity. Our findings provide a holistic approach to understanding and tailoring Fe incorporation dynamics across the electrocatalyst–electrolyte interface, thus controlling catalytic processes.

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“…The interface between E-Ni and NiFe LDH is built by Ni (111) and NiFe LDH (001) (Figures S26, S27) because of a small interfacial lattice mismatch, which is a common approach in constructing a heterostructure for theoretical calculations. 48 The charge density difference of Ni/NiFe LDH was analyzed (Figure 5a,b 58,59 Overall, the theoretical simulation reveals that the abundant heterostructure interfaces considerably improve the electronic conductivity and reduce reaction barriers, thus resulting in superior OWS activity. 2.5.…”

Section: Resultsmentioning

confidence: 92%

Engineering Different Reaction Centers on Hierarchical Ni/NiFe Layered Double Hydroxide Accelerating Overall Water Splitting

Chen

Liu

Yao

et al. 2021

ACS Appl. Energy Mater.

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The insufficient and inert active sites limited the layered double hydroxides' (LDHs) hydrogen evolution reaction (HER) performance. Rationally integrating different active centers can promote bifunctional performance and synergistically enhance HER and OER performance. But it is still rarely reported to reasonably integrate different halfreaction centers and boost each other. Besides, the mechanism of different reaction centers that optimized each other is unclear. In this work, a 3D hierarchical heterostructure Ni/ NiFe LDH, constructed by electrodeposition, provides abundant reaction centers that activate HER performance. Simultaneously, NiFe LDHs served as OER active centers, and metallic Ni improves its electric conductivity. Theoretical calculations also were used to confirm these further. Additionally, the unique hierarchical geometric structure increases the electrolyte contact area. The merits, as mentioned above, synergistically accelerate overall water splitting (OWS) and exhibit outstanding electrocatalysis performance. HER current density of the Ni/NiFe LDH heterostructure (312 mA cm −2 ) is 104 times as large as that of NiFe LDH (3.0 mA cm −2 ) with 150 mV overpotential. At 1.46 V, the OWS cell, constructed of both anode and cathode by as-synthesized Ni/NiFe LDH, can drive water splitting (10 mA cm −2 ), below noble metal Pt/C||RuO 2 (1.53 V). This finding provides guidance for rationally integrating different reaction centers in bi-or multi-functional electrocatalytic processes.

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Intrinsic Electrocatalytic Activity for Oxygen Evolution of Crystalline 3d‐Transition Metal Layered Double Hydroxides

Cited by 48 publications

References 58 publications

Structural Variations of Metal Oxide‐Based Electrocatalysts for Oxygen Evolution Reaction

Structural Variations of Metal Oxide‐Based Electrocatalysts for Oxygen Evolution Reaction

Revealing the Dynamics and Roles of Iron Incorporation in Nickel Hydroxide Water Oxidation Catalysts

Engineering Different Reaction Centers on Hierarchical Ni/NiFe Layered Double Hydroxide Accelerating Overall Water Splitting

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