Electrostatic potential-derived charge: a universal OER performance descriptor for MOFs. Issue 44 (2nd November 2022)

• Record Type: Journal Article
• Authors: Xue, Xiangdong; Gao, Hongyi; Liu, Jiangtao; Yang, Ming; Feng, Shihao; Liu, Zhimeng; Lin, Jing; Kasemchainan, Jitti; Wang, Linmeng; Jia, Qilu; Wang, Ge
• Is Part Of: Chemical science. Volume 13:Issue 44(2022)
• Page Start: 13160
• Page End: 13171
• Publication Date: 2022-11-02
• Subjects: Chemistry -- Periodicals; 540.5
• DOI: 10.1039/d2sc04898a
• Languages: English
• ISSNs: 2041-6520

Abstract

Abstract : The electrostatic potential-derived charge (ESPC) is identified as a robust and universal OER performance descriptor of MOFs. By using ESPC as a bridge, the composition design principle of MOFs can be easily derived. Abstract : Metal–organic frameworks (MOFs) provide opportunities for the design of high-efficiency catalysts attributed to their high compositional and structural tunability. Meanwhile, the huge number of MOFs poses a great challenge to experimental-intensive development of high-performance functional applications. By taking the computationally feasible and structurally representative trigonal prismatic secondary building units (SBUs) of MOFs as the entry point, we introduce a descriptor-based approach for designing high-performance MOFs for the oxygen evolution reaction (OER). The electrostatic potential-derived charge (ESPC) is identified as a robust and universal OER performance descriptor of MOFs, showing a distinct linear relationship with the onset potentials of OER elemental steps. Importantly, we establish an ESPC-based physical pattern of active site–intermediate binding strength, which interprets the rationality of ESPC as an OER performance descriptor. We further reveal that the SBUs with Ni/Cu as active site atoms while Mn/Fe/Co/Ni as spectator atoms have excellent OER activity through the variation pattern of ESPC along with metal composition. The universal correlation between ESPC and OER activity provides a rational rule for designing high-performance MOF-based OER electrocatalysts and can be easily extended to design functional MOFs for a rich variety of catalytic applications.