Towards superior metal phthalocyanine catalysts for electrochemical oxygen reduction: A comprehensive screening under experimental conditions

Yang，Huanhuan1,2,3; Bashir，Beenish2,3; Luo，Guangfu2,3

2023-10-01

10.1016/j.cej.2023.145101

Chemical Engineering Journal   影响因子和分区

1385-8947

1873-3212

Metal phthalocyanines (MPcs) represent a promising class of single-atom catalysts with diverse structures, high thermal stability, and versatile chemical properties. In this work, we have computationally screened nineteen MPcs (metal M = V–Zn, Mo–Ag, and W–Pt ordered based on the atomic number) to assess their suitability as electrochemical oxygen reduction reaction (ORR) catalysts, with consideration of a broad range of experimental conditions, including the oxygen adsorption, temperature effects, partial pressure, solvation effects, pH effects, and demetallation decomposition. Using density functional theory calculations based on the hybrid functional, we find that the ORR behaviors on these MPcs fall into three categories, which are characterized by their distinct oxygen adsorption ability. We correctly predict the experimental ORR performance trend of common MPcs and forecast Rh−, Ir−, Ru−, and MnPc as the four most effective ORR catalysts, outperforming the state-of-the-art FePc in terms of catalytic activity and stability. This study highlights the crucial role of oxygen adsorption, predicts superior MPcs for ORR electrocatalysis, and offers detailed guidance on the optimal working conditions.

First-principles calculations Metal phthalocyanine Oxygen reduction reaction Single-atom catalyst

SCI ; EI

英语

通讯

Guangdong Provincial Key Laboratory of Computational Science and Material Design[2019B030301001] ; Introduced Innovative R&D Team of Guangdong[2017ZT07C062] ; Shenzhen Science and Technology Innovation Committee[JCYJ20200109141412308]

Engineering

Engineering, Environmental ; Engineering, Chemical

WOS:001063122900001

ELSEVIER SCIENCE SA

20233314535672

Atoms ; Catalyst activity ; Chemical stability ; Electrocatalysis ; Electrolytic reduction ; Gas adsorption ; Oxygen ; pH effects

Ore Treatment:533.1 ; Chemistry:801 ; Chemistry, General:801.1 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

ENGINEERING

2-s2.0-85167433123

Scopus

1.Harbin Institute of Technology,Harbin,150080,China
2.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
3.Guangdong Provincial Key Laboratory of Computational Science and Material Design,Southern University of Science and Technology,Shenzhen,518055,China

Yang，Huanhuan,Bashir，Beenish,Luo，Guangfu. Towards superior metal phthalocyanine catalysts for electrochemical oxygen reduction: A comprehensive screening under experimental conditions[J]. Chemical Engineering Journal,2023,473.

Yang，Huanhuan,Bashir，Beenish,&Luo，Guangfu.(2023).Towards superior metal phthalocyanine catalysts for electrochemical oxygen reduction: A comprehensive screening under experimental conditions.Chemical Engineering Journal,473.

Yang，Huanhuan,et al."Towards superior metal phthalocyanine catalysts for electrochemical oxygen reduction: A comprehensive screening under experimental conditions".Chemical Engineering Journal 473(2023).