Enhancing the Understanding of the Oxygen Evolution Reaction on Bimetallic Two-Dimensional MOFs through Theoretical Investigation

Abstract

Bimetallic two-dimensional (2D) conjugated phthalocyanine-based metal−organic frameworks (MOFs) show excellent electrocatalytic activity due to the advantages of a well-regulated electronic structure and excellent conductivity. However, the application of the bimetallic 2D MOFs in the oxygen evolution reaction (OER) is still in its infancy, and the intrinsic structure−activity relationships are ambiguous. Here, a theoretical study was carried out to investigate the potential of two cutting-edge carbon dioxide reduction electrocatalysts, CuPc-ZnO 4 and CoPc-CuO 4 , for OER and clarify their intrinsic features. It is concluded that compared with the reported OER catalyst NiPc-NiO 4 , CoPc-CuO 4 is more favorable while CuPc-ZnO 4 is not. The favorable CoPc site is attributed to a stronger O* interaction effect relative to OH* rather than the interaction with individual intermediates. Originally, it is revealed that besides the electronic structure of the d-band center, the structural flexibility of catalytic sites is also an important factor regulating the catalytic activity. The results enhance the understanding of OER activity on bimetallic 2D MOFs.

Regulating Excess Electrons in Reducible Metal Oxides for Enhanced Oxygen Evolution Reaction Activity: A Mini‐Review

“…[8] Therefore, substantial research efforts have been dedicated to unraveling the OER mechanism and developing strategies for designing highly efficient OER catalysts. [3,[9][10][11][12][13][14][15] Since the early 20th century, the Sabatier principle has been empirically discovered to elucidate catalytic activity, [20] providing a guiding framework for the rational design of catalysts. [19,21] This principle establishes a link between the micro-level adsorption properties of reaction intermediates and the macrolevel catalytic activities.…”