In Silico Design of Covalent Organic Framework-Based Electrocatalysts

• DOI: 10.1021/jacsau.1c00258
• Publication Date: 2021-07-22T12:40:22Z
• Authors: Wei Zhou; Li Yang; Xiao Wang; Wenling Zhao; Junxia Yang; Dong Zhai; Lei Sun; Weiqiao Deng
• Keywords: Overpotential; XANES; Oxygen evolution; Covalent organic framework

Covalent organic frameworks (COFs) are an emerging type of porous crystalline material for efficient catalysis the oxygen evolution reaction (OER). However, it remains a grand challenge to address best candidates from thousands possible COFs. Here, we report methodology design candidate screened 100 virtual M–NxOy (M = 3d transition metal)-based model catalysts via density functional theory (DFT) and machine learning (ML). The intrinsic descriptors OER activity were addressed by used predicting structure with performances. One predicted structures Ni–N2O2 unit is subsequently employed synthesize corresponding Ni–COF. X-ray absorption spectra characterizations, including XANES EXAFS, validate successful synthesis coordination environment. studies electrocatalytic activities confirm that Ni–COF comparable reported COF-based catalysts. current reaches 10 mA cm–2 at low overpotential 335 mV. Furthermore, stable over 65 h during electrochemical testing. This work provides accelerating strategy new crystalline-material-based electrocatalysts.