4.6 Article

Tuning Surface Reactivity and Electric Field Strength via Intermetallic Alloying

Journal

ACS ENERGY LETTERS
Volume 8, Issue 10, Pages 4414-4420

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.3c01639

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This paper investigates the effect of intermetallic alloying on the catalytic activity in electrochemical reactions. It is found that intermetallic phases allow for independent control over d-band energetics and work function, resulting in enhanced intrinsic activity for CO2 reduction. However, the propensity of these alloys to segregate in air poses a significant obstacle to studying their electrocatalytic activity.
Many electrosynthesis reactions, such as CO2 reduction to multicarbon products, involve the formation of dipolar and polarizable transition states during the rate-determining step. Systematic and independent control over surface reactivity and electric field strength would accelerate the discovery of highly active electrocatalysts for these reactions by providing a means of reducing the transition state energy through field stabilization. Herein, we demonstrate that intermetallic alloying enables independent and systematic control over d-band energetics and work function through the variation of alloy composition and oxophilic constituent identity, respectively. We identify several intermetallic phases exhibiting properties that should collectively yield higher intrinsic activity for CO reduction compared to conventional Cu-based electrocatalysts. However, we also highlight the propensity of these alloys to segregate in air as a significant roadblock to investigating their electrocatalytic activity.

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