Self-healing oxygen evolution catalysts

Thorarinsdottir, Agnes E.; Veroneau, Samuel S.; Nocera, Daniel G.

doi:10.1038/s41467-022-28723-9

Cited by 70 publications

(72 citation statements)

References 100 publications

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“…To leverage high OER performance with long-term stability, electrochemical systems can benchmark self-healing properties, which are commonly observed in biological systems, including photosynthesis systems. , By definition, a self-healing system should recover from structural damage through a thermodynamically favorable, spontaneous regeneration reaction. , In other words, the operating conditions of functional surfaces should also promote the structural regeneration process simultaneously. Because atomic dissolution is a major degradation mechanism in the OER, the self-healing strategy can effectively address OER stability problems by supplementing the active site loss. , …”

Section: Dynamic Electrochemical Interfacesmentioning

confidence: 99%

“…Previously, the active sites were considered to be fixed if the loading mass or surface area of the catalyst was determined; this was known as the so-called “frozen” surface. However, as clearly validated, the number of active sites changes during the reaction via vigorous dissolution and redeposition, which indicates that the “frozen” surface concept can no longer be applied to dynamic interfaces . As discussed in the previous chapter, self-healing provides a unique opportunity to regenerate active sites during electrochemical reactions.…”

Section: Dynamic Electrochemical Interfacesmentioning

confidence: 99%

“…Because atomic dissolution is a major degradation mechanism in the OER, the self-healing strategy can effectively address OER stability problems by supplementing the active site loss. 18 , 19 …”

Section: Dynamic Electrochemical Interfacesmentioning

confidence: 99%

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Dynamic Electrochemical Interfaces for Energy Conversion and Storage

Shin

Yoo

Sung

et al. 2022

JACS Au

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Electrochemical energy conversion and storage are central to developing future renewable energy systems. For efficient energy utilization, both the performance and stability of electrochemical systems should be optimized in terms of the electrochemical interface. To achieve this goal, it is imperative to understand how a tailored electrode structure and electrolyte speciation can modify the electrochemical interface structure to improve its properties. However, most approaches describe the electrochemical interface in a static or frozen state. Although a simple static model has long been adopted to describe the electrochemical interface, atomic and molecular level pictures of the interface structure should be represented more dynamically to understand the key interactions. From this perspective, we highlight the importance of understanding the dynamics within an electrochemical interface in the process of designing highly functional and robust energy conversion and storage systems. For this purpose, we explore three unique classes of dynamic electrochemical interfaces: self-healing, active-site-hosted, and redox-mediated interfaces. These three cases of dynamic electrochemical interfaces focusing on active site regeneration collectively suggest that our understanding of electrochemical systems should not be limited to static models but instead expanded toward dynamic ones with close interactions between the electrode surface, dissolved active sites, soluble species, and reactants in the electrolyte. Only when we begin to comprehend the fundamentals of these dynamics through operando analyses can electrochemical conversion and storage systems be advanced to their full potential.

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Section: Dynamic Electrochemical Interfacesmentioning

confidence: 99%

Section: Dynamic Electrochemical Interfacesmentioning

confidence: 99%

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Dynamic Electrochemical Interfaces for Energy Conversion and Storage

Shin

Yoo

Sung

et al. 2022

JACS Au

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show abstract

“…However, for this monolithic device operation, it is not possible to easily distinguish the cathodic CoWS catalyst dissolution from the anodic CoWO catalyst dissolution, if the latter also occurs, or quantify the degree of redeposition of these catalysts. Indeed, efficient redeposition of cobalt, manganese, and nickel oxides from low-concentration metal salts in the electrolyte causing the healing capability of these catalysts has been previously reported . However, the situation experienced here is significantly more complex as we deal both with two distinct OER and HER catalysts and with bimetal catalysts with the possibility for monometallic phases to redeposit in addition to the initial bimetallic phases.…”

Section: Resultsmentioning

confidence: 92%

Water-Splitting Artificial Leaf Based on a Triple-Junction Silicon Solar Cell: One-Step Fabrication through Photoinduced Deposition of Catalysts and Electrochemical Operando Monitoring

et al. 2022

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Solar hydrogen generation via water splitting using a monolithic photoelectrochemical cell, also called artificial leaf, could be a powerful technology to accelerate the transition from fossil to sustainable energy sources. Identification of scalable methods for the fabrication of monolithic devices and gaining insights into their operating mode to identify solutions to improve performance and stability represent great challenges. Herein, we report on the one-step fabrication of a CoWO|ITO|3jn-a-Si|Steel|CoWS monolithic device via the simple photoinduced deposition of CoWO and CoWS as oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) catalyst layers, respectively, onto an illuminated ITO|3jn-a-Si|Steel solar cell using a single-deposition bath containing the [Co(WS4)2]2– complex. In a pH 7 phosphate buffer solution, the best device achieved a solar-to-hydrogen conversion yield of 1.9%. Evolution of the catalyst layers and that of the 3jn-a-Si light-harvesting core during the operation of the monolithic device are examined by conventional tools such as scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), and inductively coupled plasma optical emission spectroscopy (ICP-OES) together with a bipotentiostat measurement. We demonstrate that the device performance degrades due to the partial dissolution of the catalyst. Still, this degradation is healable by simply adding [Co(WS4)2]2– to the operating solution. However, modifications on the protecting indium-doped tin oxide (ITO) layer are shown to initiate irreversible degradation of the 3jn-a-Si light-harvesting core, resulting in a 10-fold decrease of the performances of the monolithic device.

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“…2), and the oxygen evolution reaction (OER) at the anode, where water is oxidized to produce O2 (Eq. 3) [50,51].…”

Section: Catalysts For Oermentioning

confidence: 99%

Revealing nanoscale lithiation and dissolution pathways by in situ cryogenic electron microscopy

Tiukalova¹

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Materials for energy storage and conversion devices are of high importance to meet future industrial energy demands. Detailed understanding of chemical processes occurring at the solid/liquid interfaces and alterations of the structure at the atomic scale is critical for the design and development of future devices. This Ph.D. work focuses on two central systems of particular relevance for energy applications, i.e., LiNi0.5Mn1.5O4 Li-ion battery cathode material and two catalysts (La2LiIrO6, ZnCo1.2Ni0.8O4) for the oxygen evolution reaction (OER) applications. Through a deep understanding of the evolution of the structure at the local atomic scale, the overall aim is to get insights into the atomic structure-property relationship to improve our understanding and provide information that will help develop materials capable of higher capacity, longer lifetime, and overall better performance.During operation, electrochemical reactions introduce structural and chemical changes to the active materials that are not necessarily reversible. These alterations cause degradation of the device performance and limit their lifetime. A detailed understanding of the correlation between electrochemical processes and atomic-scale transformations is essential to improve the performance of the devices. Owing to its high-resolution transmission electron microscopy (TEM) -based imaging and spectroscopic analysis is able to provide unique information that is not available with other methods. In addition, with the recent development of dedicated in situ and operando TEM-capabilities, it is possible to observe structural changes under the application of external stimuli such as at cryogenic temperature or presence of a liquid electrolyte, allowing to study dynamical processes in their native operation environment. The development of in situ cryogenic temperature stages for materials science applications has opened up many new possibilities, including learning new information about beam-sensitive materials that are challenging to characterize with conventional room temperature imaging at the atomic level. This Ph.D. work focuses on three material systems studied in detail under various HR(S)TEM and spectroscopy methods: LiNi0.5Mn1.5O4 as a promising cathode material, ZnCo1.2Ni0.8O4 and La2LiIrO6 as catalysts for OER. It was found that LiNi0.5Mn1.5O4

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Self-healing oxygen evolution catalysts

Cited by 70 publications

References 100 publications

Dynamic Electrochemical Interfaces for Energy Conversion and Storage

Dynamic Electrochemical Interfaces for Energy Conversion and Storage

Water-Splitting Artificial Leaf Based on a Triple-Junction Silicon Solar Cell: One-Step Fabrication through Photoinduced Deposition of Catalysts and Electrochemical Operando Monitoring

Revealing nanoscale lithiation and dissolution pathways by in situ cryogenic electron microscopy

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