Designing Atomically Dispersed Au on Tensile-Strained Pd for Efficient CO2Electroreduction to Formate

Jinsol Bok, Si Young Lee, Byoung Hoon Lee, Cheonghee Kim, Dang Le Tri Nguyen, Ji Won Kim, Euiyeon Jung, Chan Woo Lee, Yoon Jung, Hyeon Seok Lee, Jiheon Kim, Kangjae Lee, Wonjae Ko, Young Seong Kim, Sung Pyo Cho, Jong Suk Yoo, Taeghwan Hyeon, Yun Jeong Hwang

Research output: Contribution to journalArticlepeer-review

79 Scopus citations

Abstract

Pd is one of the most effective catalysts for the electrochemical reduction of CO2 to formate, a valuable liquid product, at low overpotential. However, the intrinsically high CO affinity of Pd makes the surface vulnerable to CO poisoning, resulting in rapid catalyst deactivation during CO2 electroreduction. Herein, we utilize the interaction between metals and metal-organic frameworks to synthesize atomically dispersed Au on tensile-strained Pd nanoparticles showing significantly improved formate production activity, selectivity, and stability with high CO tolerance. We found that the tensile strain stabilizes all reaction intermediates on the Pd surface, whereas the atomically dispersed Au selectively destabilizes CO∗ without affecting other adsorbates. As a result, the conventional COOH∗ versus CO∗ scaling relation is broken, and our catalyst exhibits 26- and 31-fold enhancement in partial current density and mass activity toward electrocatalytic formate production with over 99% faradaic efficiency, compared to Pd/C at -0.25 V versus RHE.

Original languageEnglish
Pages (from-to)5386-5395
Number of pages10
JournalJournal of the American Chemical Society
Volume143
Issue number14
DOIs
StatePublished - 14 Apr 2021

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