From Bad Electrochemical Practices to an Environmental and Waste Reducing Approach for the Generation of Active Hydrogen Evolving Electrodes

Ring, Lisa; Pollet, Bruno G.; Chatenet, Marian; Abbou, Sofyane; Küpper, Karsten; Schmidt, Mercedes; Huck, Marten; Gries, Aurelia; Steinhart, Martin; Schäfer, Helmut

doi:10.1002/anie.201908649

Cited by 29 publications

(26 citation statements)

References 66 publications

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“…This is to be expected as Pt is a far more efficient electrocatalyst for the HER than Au. This is consistent with previous work where it was shown that Pt decoration of Ni42 steel also resulted in excellent HER activity [34] …”

Section: Resultssupporting

confidence: 93%

Activating Iron Based Materials for Overall Electrochemical Water Splitting via the Incorporation of Noble Metals

Sayeed

Heron

Love

et al. 2020

Chemistry An Asian Journal

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Although the presence of iron in mixed metal oxide based catalysts has shown significant performance improvement in the oxygen evolution reaction (OER), iron oxides themselves demonstrate much poorer activity. In this study, we investigate improving the performance of iron catalysts via surface decoration with gold or platinum for not only the OER but also the hydrogen evolution reaction (HER) for overall water splitting in an alkaline electrolyte. Two types of iron catalysts were synthesised, iron nanocubes and iron oxide via electrochemical deposition methods which were decorated with either Au or Pt via galvanic replacement. It was found that the presence of Au significantly enhanced the OER performance of iron oxide and the HER performance of iron nanocubes. The presence of Pt resulted in moderate improvement in the OER but significant improvement for the HER but did not surpass the performance of gold decorated iron nanocubes. This indicates that the speciation of the iron catalyst and the decorating metal was important for tuning the activity to the OER and the HER. For the OER, the formation of iron oxide/Au interfaces was determined to be an important component for high activity whereas the metallic nature of metal decorated iron nanocubes was important for the HER. Therefore, iron based catalysts can be modified to demonstrate bifunctional behaviour for overall water splitting via the inclusion of gold nanoparticles.

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Section: Resultssupporting

confidence: 93%

Activating Iron Based Materials for Overall Electrochemical Water Splitting via the Incorporation of Noble Metals

Sayeed

Heron

Love

et al. 2020

Chemistry An Asian Journal

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“…Encouraged by the initial HER cycling tests, the electrochemical performance of PdNP@GNF was tested over a larger number of cycles, up to 30000 cycles, and compared with that of the Pt/C electrocatalyst benchmark after 5000 and 30000 cycles under the same conditions (Figure 3 c,d and Figure 4 ). It is worth noting that accelerated durability tests were carried out using a carbon counter electrode, which rule out Pt dissolution‐redeposition effects[ 54 , 55 , 56 ] on the observed electrochemical performance. It is remarkable that as the number of HER cycles increases, the performance of the PdNP@GNF catalyst continues to improve, overtaking Pt/C after about 15000 cycles (Table 1 and Figure 4 c).…”

Section: Electrocatalysis Of the Her In Pdnp@gnf Nanoreactorsmentioning

confidence: 99%

Palladium Nanoparticles Hardwired in Carbon Nanoreactors Enable Continually Increasing Electrocatalytic Activity During the Hydrogen Evolution Reaction

et al. 2021

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Catalysts typically lose effectiveness during operation, with much effort invested in stabilising active metal centres to prolong their functional lifetime for as long as possible. In this study palladium nanoparticles (PdNP) supported inside hollow graphitised carbon nanofibers (GNF), designated as PdNP@GNF, opposed this trend. PdNP@GNF exhibited continuously increasing activity over 30000 reaction cycles when used as an electrocatalyst in the hydrogen evolution reaction (HER). The activity of PdNP@GNF, expressed as the exchange current density, was always higher than activated carbon (Pd/C), and after 10000 cycles PdNP@GNF surpassed the activity of platinum on carbon (Pt/C). The extraordinary durability and self‐improving behaviour of PdNP@GNF was solely related the unique nature of the location of the palladium nanoparticles, that is, at the graphitic step‐edges within the GNF. Transmission electron microscopy imaging combined with spectroscopic analysis revealed an orchestrated series of reactions occurring at the graphitic step‐edges during electrocatalytic cycling, in which some of the curved graphitic surfaces opened up to form a stack of graphene layers bonding directly with Pd atoms through Pd−C bonds. This resulted in the active metal centres becoming effectively hardwired into the electrically conducting nanoreactors (GNF), enabling facile charge transport to/from the catalytic centres resulting in the dramatic self‐improving characteristics of the electrocatalyst.

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“…Hydrogen is an ideal renewable energy resource because it has the highest energy density per mass and is easy to burn without release of pollutants. [1][2][3][4][5] Water splitting is a green approach for hydrogen production that be used for energy storage of intermittent sources such as solar or wind in the form of fuels. [6][7][8][9][10][11] Hydrogen evolution reaction (HER) is one of two half reactions in water splitting that requires a catalyst to reduce the overpotential.…”

Section: Introductionmentioning

confidence: 99%

Ultrahigh Pt‐Mass‐Activity Hydrogen Evolution Catalyst Electrodeposited from Bulk Pt

Liu

Wang

Zhao

et al. 2022

Adv Funct Materials

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Maximizing the Pt utilization is important for the widescale implementation of Pt-based hydrogen evolution reaction (HER) electrocatalysts, owing to the scarcity of Pt. Here, three-component heterostructured HER catalysts with ultrahigh Pt mass activity in which hollow PtCu alloy nanospheres are supported on an array of WO 3 on Cu foam, are reported. It has been pointed out that the use of Pt counter electrode in a three-electrode configuration in evaluating catalysts' HER performances in acidic media carries the risk of contaminating the working electrode in previous reports. Here, the authors rationally utilize this "contaminating" to "activate" low-HER-activity materials, maximizing the Pt utilization. As a result, ultrahigh Pt mass activity is achieved, that is 1.35 and 10.86 A mg −1 Pt at overpotentials of 20 and 100 mV, respectively, 27 and 13 times higher than those of commercial Pt/C catalysts, outperforming some state-of-the-art Pt-single-atom catalysts. The hollow sphere structure and PtCu alloying increase the number and reactivity of active sites. Density function calculations and electrochemical experiments reveal that the synergy between WO 3 and Pt is also responsible for the high HER activity where the hydrogen spillover effect triggers the Volmer-Heyrovsky mechanism and promotes the rapid removal of H * from Pt to re-expose the active sites.

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From Bad Electrochemical Practices to an Environmental and Waste Reducing Approach for the Generation of Active Hydrogen Evolving Electrodes

Cited by 29 publications

References 66 publications

Activating Iron Based Materials for Overall Electrochemical Water Splitting via the Incorporation of Noble Metals

Activating Iron Based Materials for Overall Electrochemical Water Splitting via the Incorporation of Noble Metals

Palladium Nanoparticles Hardwired in Carbon Nanoreactors Enable Continually Increasing Electrocatalytic Activity During the Hydrogen Evolution Reaction

Ultrahigh Pt‐Mass‐Activity Hydrogen Evolution Catalyst Electrodeposited from Bulk Pt

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