Design of template-stabilized active and earth-abundant oxygen evolution catalysts in acid

Huynh, Michael; Özel, Tuncay; Liu, Chong; Lau, Eric C.; Nocera, Daniel G.

doi:10.1039/c7sc01239j

Cited by 197 publications

(163 citation statements)

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“…Increasing the thickness of the catalyst layer by using electrolyte solutions with fivefold higher precursor concentrations (225 μ m Fe 2+ +10 μ m Pb 2+ ) produced a sample with an XPS‐detectable amount of Fe and a surface lead:iron ratio of about 3.4:1. These results are not unexpected, as lead(IV) oxide is thermodynamically stable at very positive potentials even in acidic solutions, while iron is predicted to be mainly present as soluble FeO 4 2− species under the conditions employed herein . The potentials required to initiate the formation of catalytically active electrodes with the Fe+Pb solutions (Figure ) can be connected to the Pourbaix diagrams provided in the literature (Ref.…”

Section: Resultssupporting

confidence: 76%

“…This rate of the OER, provided by oxidation of the acidified Luina water sample, is significantly better than the performance reported for pure electrodeposited MnO x during oxidation of the DI water at pH 2.5 (phosphate electrolyte), where an overpotential of up to 1.0 V was required to sustain a current density of only 0.1 mA cm −2 . However, the same study also reports on a significantly more active ternary CoFePbO x system, which enables a 1 mA cm −2 water‐oxidation current density at η =0.57 V at pH 2.0 (Na 2 SO 4 electrolyte).…”

Section: Resultsmentioning

confidence: 70%

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Electrolysis of Natural Waters Contaminated with Transition‐Metal Ions: Identification of A Metastable FePb‐Based Oxygen‐Evolution Catalyst Operating in Weakly Acidic Solutions

et al. 2018

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The possibility of efficient water electrooxidation sustained by continuous (re)generation of catalysts derived from the oxidative electrodeposition of transition‐metal contaminants is examined herein for three natural water samples from Australia and China. The metal composition of the solutions has been determined by inductively coupled plasma optical emission spectrometry, and a range of strategies to produce water‐splitting catalysts by means of in situ electrodeposition have been applied. The performance of the resulting electrocatalysts is below the state‐of‐the‐art level owing to large amounts of impurities in the solutions and non‐optimal concentrations of naturally available catalyst precursors. Nevertheless, these studies have identified the FePb‐based system as a rare example of an electrocatalyst for water oxidation that forms in situ and maintains reasonable activity (≥4.5 mA cm−2 at an overpotential of 0.8 V) in weakly acidic solutions (pH 2.9).

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Section: Resultssupporting

confidence: 76%

Section: Resultsmentioning

confidence: 70%

Electrolysis of Natural Waters Contaminated with Transition‐Metal Ions: Identification of A Metastable FePb‐Based Oxygen‐Evolution Catalyst Operating in Weakly Acidic Solutions

et al. 2018

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“…Because a proton exchange membrane (PEM) electrolyzer, for which a Nafion proton-exchange membrane effectively separates the electrodes and extra gas, can work only in acidic conditions, this low stability in acidic conditions presents a serious challenge. [200][201][202] Therefore, matters of paramount importance include understanding the conditions required for high stability in acidic media and finding new compositions of multimetal oxides based on earth-abundant metals that exhibit high catalytic efficiency and stability in acidic conditions. …”

Section: Definition Of Descriptor For Rational Design Of Catalystsmentioning

confidence: 99%

Recent Progress on Multimetal Oxide Catalysts for the Oxygen Evolution Reaction

Kim

et al. 2018

Advanced Energy Materials

719

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fossil fuels are being widely researched for the development of a sustainable energy system. Among the various candidates for green energy resources, hydrogen energy has been at the center of attention. [1,2] Hydrogen is both inexhaustible and environmentally friendly, because it can be produced from earth-abundant reactants such as water and methane and because no CO 2 or other toxic products are emitted during its conversion into other energy form such as electricity, respectively. Moreover, hydrogen can exhibit significantly larger energy density compared with other energy sources such as gasoline and coal. The most widely used method of hydrogen production today is steam reforming because of its low cost in the process. [3] Nevertheless, the release of carbon monoxide or carbon dioxide as byproducts in the steam reforming process diminishes the environmental merits of hydrogen energy. Thus, as a possible cleaner alternative, an electrolysis method that involves producing hydrogen by electrochemically splitting water has been extensively investigated. Using one of the most abundant resources, water, the production of hydrogen from it yields only oxygen as a byproduct.In the water electrolysis, the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) occur simultaneously, as described by the following equationsIn order for the reaction to proceed, a voltage of 1.23 V is theoretically required between an anode and a cathode. However, an overpotential (represented by the symbol η) should be additionally applied to account for the potential loss resulting from kinetic limitations occurring during the electrochemical reaction. The use of electrocatalysts can lower the overpotential by kinetically facilitating the water-splitting reaction either in HER or OER. Due to the nature of four-electron involving OER, it is generally believed that the OER is much more sluggish than the HER; thus, the development of efficient OER Hydrogen is a promising alternative fuel for efficient energy production and storage, with water splitting considered one of the most clean, environmentally friendly, and sustainable approaches to generate hydrogen. However, to meet industrial demands with electrolysis-generated hydrogen, the development of a low-cost and efficient catalyst for the oxygen evolution reaction (OER) is critical, while conventional catalysts are mostly based on precious metals. Many studies have thus focused on exploring new efficient nonprecious-metal catalytic systems and improving the understandings on the OER mechanism, resulting in the design of catalysts with superior activity compared with that of conventional catalysts. In particular, the use of multimetal rather than single-metal catalysts is demonstrated to yield remarkable performance improvement, as the metal composition in these catalysts can be tailored to modify the intrinsic properties affecting the OER. Herein, recent progress and accomplishments of multimetal catalytic systems, including several important groups of catalysts: layered h...

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“…40 Electrodeposited CoFePbO x films were recently inves-tigated as an OER electrocatalyst at pH 2.5 and were found to be stable towards 12 h of chronopotentiometry carried out at 1 mA cm −2 (ref. 41). An F-doped CuMn-oxide based OER-and oxygen reduction electrode intended to be suitable for electro-catalysis in sulfuric acid was recently shown.…”

Section: Oer Properties Of Surface Modified Steelsmentioning

confidence: 99%

Electro-oxidation of a cobalt based steel in LiOH: a non-noble metal based electro-catalyst suitable for durable water-splitting in an acidic milieu

et al. 2017

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The use of proton exchange membrane (PEM) electrolyzers is the method of choice for the conversion of solar energy when frequently occurring changes of the current load are an issue. However, this technique requires electrolytes with low pH. All oxygen evolving electrodes working durably and actively in acids contain IrOx. Due to their scarcity and high acquisition costs, noble elements like Pt, Ru and Ir need to be replaced by earth abundant elements. We have evaluated a cobalt containing steel for use as an oxygen-forming electrode in H2SO4. We found that the dissolving of ingredients out of the steel electrode at oxi-dative potential in sulfuric acid, which is a well-known, serious issue, can be substantially reduced when the steel is electro-oxidized in LiOH prior to electrocatalysis. Under optimized synthesis conditions a cobalt-containing tool steel was rendered into a durable oxygen evolution reaction (OER) electrocatalyst (weight loss: 39 µg mm −2 after 50 000 s of chronopotentiometry at pH 1) that exhibits overpotentials down to 574 mV at 10 mA cm −2 current density at pH 1. Focused ion beam SEM (FIB-SEM) was success-fully used to create a structure-stability relationship.

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Design of template-stabilized active and earth-abundant oxygen evolution catalysts in acid

Abstract: We demonstrate a rational approach for designing earth-abundant catalysts that are stable and active in acid by treating activity and stability as decoupled elements of mixed metal oxides.

Cited by 197 publications

References 109 publications

Electrolysis of Natural Waters Contaminated with Transition‐Metal Ions: Identification of A Metastable FePb‐Based Oxygen‐Evolution Catalyst Operating in Weakly Acidic Solutions

Electrolysis of Natural Waters Contaminated with Transition‐Metal Ions: Identification of A Metastable FePb‐Based Oxygen‐Evolution Catalyst Operating in Weakly Acidic Solutions

Recent Progress on Multimetal Oxide Catalysts for the Oxygen Evolution Reaction

Electro-oxidation of a cobalt based steel in LiOH: a non-noble metal based electro-catalyst suitable for durable water-splitting in an acidic milieu

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