Unraveling the Interfacial Polarization Effect between Pd and Polymeric Carbon Nitride toward Efficient CO2 Electroreduction to CO

Tingting Fan; Jiguang Zhang; Yanping Zhang; Xintao Ma; Pingping Huang; Shuhong Zhang; Zhou Chen; Miao Wang; Yunyun Dong; Xiaodong Yi

doi:10.1021/acsami.2c00133

Unraveling the Interfacial Polarization Effect between Pd and Polymeric Carbon Nitride toward Efficient CO₂ Electroreduction to CO

ACS Appl Mater Interfaces. 2022 Mar 16;14(10):12314-12322. doi: 10.1021/acsami.2c00133. Epub 2022 Mar 3.

Authors

Tingting Fan¹, Jiguang Zhang¹, Yanping Zhang¹, Xintao Ma¹, Pingping Huang¹, Shuhong Zhang¹, Zhou Chen², Miao Wang^{2

3}, Yunyun Dong⁴, Xiaodong Yi¹

Affiliations

¹ College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P. R. China.
² College of Materials, Xiamen University, Xiamen 361005, P. R. China.
³ Department of Biomaterials, Key Laboratory of Biomedical Engineering of Fujian Province, College of Materials, Xiamen University, Xiamen 361005, P. R. China.
⁴ College of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252059, P. R. China.

PMID: 35239316
DOI: 10.1021/acsami.2c00133

Abstract

The efficient electrochemical conversion of carbon dioxide (CO₂) to carbon monoxide (CO) using renewable energy is an effective route to pursue carbon neutrality. Optimizing the binding energy of CO on palladium (Pd) metal-based materials used in this process is to make sure the timely desorption of CO from their active sites is critical. Tuning the electronic structure of the Pd center is an effective strategy to optimize its catalytic performance. Herein, we rationally design Pd nanoparticles (NPs)/polymeric carbon nitride (CN) (Pd/CN) composite, which alters the electronic structure of Pd by introducing the interfacial polarization effect to accelerate CO desorption and improve CO selectivity of Pd catalyst. The optimized Pd/CN exhibits a CO Faradaic efficiency of 92.7% at -0.9 V versus reversible hydrogen electrode in CO₂-saturated 0.1 M KHCO₃ solution. Experimental investigations and theoretical calculations jointly confirm that the enhanced CO selectivity and stability originate from the electron transfer at the Pd/CN interface, and the weakened *CO adsorption on the palladium hydride surface.

Keywords: CO desorption; CO2 reduction reaction; electrocatalysis; interfacial polarization effect; palladium electrocatalyst; polymeric carbon nitride.