Tuning Surface Reactivity and Electric Field Strength via Intermetallic Alloying

Ezra L. Clark, Rasmus Nielsen, Jakob Ejler Sørensen, Julius Lucas Needham, Brian Seger, Ib Chorkendorff*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

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Abstract

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.

Original languageEnglish
JournalACS Energy Letters
Volume8
Issue number10
Pages (from-to)4414-4420
ISSN2380-8195
DOIs
Publication statusPublished - 2023

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