Beyond the top of the volcano? – A unified approach to electrocatalytic oxygen reduction and oxygen evolution
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Beyond the top of the volcano? – A unified approach to electrocatalytic oxygen reduction and oxygen evolution. / Busch, Michael; Halck, Niels B.; Kramm, Ulrike I.; Siahrostami, Samira; Krtil, Petr; Rossmeisl, Jan.
I: Nano Energy, Bind 29, 2016, s. 126-135.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
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TY - JOUR
T1 - Beyond the top of the volcano? – A unified approach to electrocatalytic oxygen reduction and oxygen evolution
AU - Busch, Michael
AU - Halck, Niels B.
AU - Kramm, Ulrike I.
AU - Siahrostami, Samira
AU - Krtil, Petr
AU - Rossmeisl, Jan
PY - 2016
Y1 - 2016
N2 - We study the oxygen reduction (ORR) and the oxygen evolution reaction (OER) and based on previous obtained mechanistic insight we provide a unified general analysis of the two reactions simultaneously. The analysis shows that control over at least two independent binding energies is required to obtain a reversible perfect catalyst for both ORR and OER. Often only the reactivity of the surface is changed by changing from one material to another and all binding energies scale with the reactivity. We investigate the limitation in efficiency imposed by these linear scaling relations. This analysis gives rise to a double volcano for ORR and OER, with a region in between, forbidden by the scaling relations. The reversible perfect catalyst for both ORR and OER would fall into this “forbidden region”. Previously, we have found that hydrogen acceptor functionality on oxide surfaces can improve the catalytic performance for OER beyond the limitations originating from the scaling relations. We use this concept to search for promising combinations of binding sites and hydrogen donor/acceptor sites available in transition metal doped graphene, which can act as a catalyst for ORR and OER. We find that MnN4-site embedded in graphene by itself or combined with a COOH is a promising combination for a great combined ORR/OER catalyst.
AB - We study the oxygen reduction (ORR) and the oxygen evolution reaction (OER) and based on previous obtained mechanistic insight we provide a unified general analysis of the two reactions simultaneously. The analysis shows that control over at least two independent binding energies is required to obtain a reversible perfect catalyst for both ORR and OER. Often only the reactivity of the surface is changed by changing from one material to another and all binding energies scale with the reactivity. We investigate the limitation in efficiency imposed by these linear scaling relations. This analysis gives rise to a double volcano for ORR and OER, with a region in between, forbidden by the scaling relations. The reversible perfect catalyst for both ORR and OER would fall into this “forbidden region”. Previously, we have found that hydrogen acceptor functionality on oxide surfaces can improve the catalytic performance for OER beyond the limitations originating from the scaling relations. We use this concept to search for promising combinations of binding sites and hydrogen donor/acceptor sites available in transition metal doped graphene, which can act as a catalyst for ORR and OER. We find that MnN4-site embedded in graphene by itself or combined with a COOH is a promising combination for a great combined ORR/OER catalyst.
KW - Density functional theory
KW - Electrocatalysis
KW - Oxygen evolution
KW - Oxygen reduction
KW - Volcano
U2 - 10.1016/j.nanoen.2016.04.011
DO - 10.1016/j.nanoen.2016.04.011
M3 - Journal article
AN - SCOPUS:84965069069
VL - 29
SP - 126
EP - 135
JO - Nano Energy
JF - Nano Energy
SN - 2211-2855
ER -
ID: 170764900