Metal Phthalocyanine-Derived Single-Atom Catalysts for Selective CO2 Electroreduction under High Current Densities

Yang Wang; Zhan Jiang; Xiao Zhang; Zeyu Niu; Qinqi Zhou; Xiaojun Wang; Huan Li; Zhichao Lin; Hongzhi Zheng; Yongye Liang

doi:10.1021/acsami.0c08940

Metal Phthalocyanine-Derived Single-Atom Catalysts for Selective CO₂ Electroreduction under High Current Densities

ACS Appl Mater Interfaces. 2020 Jul 29;12(30):33795-33802. doi: 10.1021/acsami.0c08940. Epub 2020 Jul 17.

Authors

Yang Wang^{1

2}, Zhan Jiang^{1

2}, Xiao Zhang², Zeyu Niu², Qinqi Zhou², Xiaojun Wang², Huan Li², Zhichao Lin², Hongzhi Zheng², Yongye Liang^{2

3}

Affiliations

¹ School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China.
² Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China.
³ Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Southern University of Science and Technology, Shenzhen 518055, China.

PMID: 32628446
DOI: 10.1021/acsami.0c08940

Abstract

Single-atom catalysts (SACs) with atomically dispersed metal sites in nitrogen-doped carbon matrices (M-N/C) have been identified as promising candidates for the electrocatalytic CO₂ reduction reaction (CO₂RR). However, recent studies aiming at economic viability have been inhibited by the low faradaic efficiency (FE) and instability under high current density. Herein, we report a series of SACs derived from cyano-substituted metal phthalocyanines (MePc-CN) in ZIFs (denoted as Me-SACs (Pc)). These phthalocyanine molecules enable the efficient construction of SACs, affording higher metal loading and less variation when compared with their counterparts from metal nitrates (denoted as Me-SACs (S)). Thus, Me-SACs (Pc) exhibit higher activities and selectivities than Me-SACs (S) in H-cell measurements. In gas-diffusion electrode (GDE) setups, the unstable Fe-SAC (Pc) shows only a 50% FE of CO (FEco) at -100 mA cm^-2. In contrast, Ni-SAC (Pc) exhibits a higher FEco of >96% at current densities from -10 to -200 mA cm^-2 and can stably operate for over 16 h at -200 mA cm^-2. The performances of Ni-SAC (Pc) are comparable to those of precious metal catalysts and the best SACs reported so far, representing a promising candidate for practical electrolyzer devices for CO₂RR.

Keywords: carbon dioxide reduction reaction; gas-diffusion electrode; metal phthalocyanine; single-atom catalysts; zeolitic imidazolate frameworks.