TY - JOUR

T1 - Tuning the Activity of Pt(111) for Oxygen Electroreduction by Subsurface Alloying

A1 - Stephens,Ifan

A1 - Bondarenko,A.S.

A1 - Perez-Alonso,F.J.

A1 - Vallejo,Federico Calle

A1 - Bech,Lone

A1 - Johansson,Tobias Peter

A1 - Jepsen,A.K.

A1 - Frydendal,R.

A1 - Knudsen,B.P.

A1 - Rossmeisl,Jan

A1 - Chorkendorff,Ib

AU - Stephens,Ifan

AU - Bondarenko,A.S.

AU - Perez-Alonso,F.J.

AU - Vallejo,Federico Calle

AU - Bech,Lone

AU - Johansson,Tobias Peter

AU - Jepsen,A.K.

AU - Frydendal,R.

AU - Knudsen,B.P.

AU - Rossmeisl,Jan

AU - Chorkendorff,Ib

PB - American Chemical Society

PY - 2011

Y1 - 2011

N2 - To enable the development of low temperature fuel cells, significant improvements are required to the efficiency of the Pt electrocatalysts at the cathode, where oxygen reduction takes place. Herein, we study the effect of subsurface solute metals on the reactivity of Pt, using a Cu/Pt(111) near-surface alloy. Our investigations incorporate electrochemical measurements, ultrahigh vacuum experiments, and density functional theory. Changes to the OH binding energy, ΔEOH, were monitored in situ and adjusted continuously through the subsurface Cu coverage. The incorporation of submonolayer quantities of Cu into Pt(111) resulted in an 8-fold improvement in oxygen reduction activity. The most optimal catalyst for oxygen reduction has an ΔEOH ≈ 0.1 eV weaker than that of pure Pt, validating earlier theoretical predictions.

AB - To enable the development of low temperature fuel cells, significant improvements are required to the efficiency of the Pt electrocatalysts at the cathode, where oxygen reduction takes place. Herein, we study the effect of subsurface solute metals on the reactivity of Pt, using a Cu/Pt(111) near-surface alloy. Our investigations incorporate electrochemical measurements, ultrahigh vacuum experiments, and density functional theory. Changes to the OH binding energy, ΔEOH, were monitored in situ and adjusted continuously through the subsurface Cu coverage. The incorporation of submonolayer quantities of Cu into Pt(111) resulted in an 8-fold improvement in oxygen reduction activity. The most optimal catalyst for oxygen reduction has an ΔEOH ≈ 0.1 eV weaker than that of pure Pt, validating earlier theoretical predictions.

U2 - 10.1021/ja111690g

DO - 10.1021/ja111690g

JO - American Chemical Society. Journal

JF - American Chemical Society. Journal

SN - 0002-7863

IS - 14

VL - 133

SP - 5485

ER -