Designing Atomically Dispersed Au on Tensile-Strained Pd for Efficient CO2 Electroreduction 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

doi:10.1021/jacs.0c12696

Designing Atomically Dispersed Au on Tensile-Strained Pd for Efficient CO₂ Electroreduction to Formate

J Am Chem Soc. 2021 Apr 14;143(14):5386-5395. doi: 10.1021/jacs.0c12696. Epub 2021 Mar 16.

Authors

Jinsol Bok^{1

2}, Si Young Lee^{3

4}, Byoung-Hoon Lee^{1

2}, Cheonghee Kim⁵, Dang Le Tri Nguyen³, Ji Won Kim^{3

6}, Euiyeon Jung^{1

2}, Chan Woo Lee^{1

2}, Yoon Jung^{1

2}, Hyeon Seok Lee^{1

2}, Jiheon Kim^{1

2}, Kangjae Lee^{1

2}, Wonjae Ko^{1

2}, Young Seong Kim¹, Sung-Pyo Cho⁷, Jong Suk Yoo⁵, Taeghwan Hyeon^{1

2}, Yun Jeong Hwang^{1

8}

Affiliations

¹ Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea.
² School of Chemical and Biological Engineering, and Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea.
³ Clean Energy Research Center, Korea Institute of Science and Technology, Seoul 02792, Republic of Korea.
⁴ Division of Energy and Environmental Technology, KIST School, Korea University of Science and Technology, Seoul 02792, Republic of Korea.
⁵ Department of Chemical Engineering, University of Seoul, Seoul 02504, Republic of Korea.
⁶ Department of Chemical and Biomolecular Engineering, Yonsei-KIST Convergence Research Institute, Yonsei University, Seoul 03722, Republic of Korea.
⁷ National Center for Inter-University Research Facilities, Seoul National University, Seoul 08826, Republic of Korea.
⁸ Department of Chemistry, Seoul National University, Seoul 08826, Republic of Korea.

PMID: 33725440
DOI: 10.1021/jacs.0c12696

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.