Amorphization Engineering of Bimetallic Metal‐Organic Frameworks to Identify Volcano‐Type Trend toward Oxygen Evolution Reaction

Abstract Amorphous metal‐organic frameworks (MOFs) with aperiodic atomic arrangements, featuring high intrinsic activity and rich active sites, have emerged as promising oxygen evolution reaction (OER) catalysts. However, the quantitative structure‐activity relationships (SARs) that determine the OER activity, the key to a rational catalyst design, remain unresolved. Inspired by controllable amorphization engineering, the amorphous MOF structures are rationally constructed as an ideal platform to explore the SAR in catalyzing OER. The mechanistic studies show that the OER activity could be volcano‐shape correlated with either constant adsorption energy difference between OOH* and O* (Δ G OOH* − Δ G O* ) or the position of the d band center. The amorphous MOF (Ni 8 Co 2 ‐BDC), situated close to the volcano summit, possesses an appropriate E d energy level, which exhibits the balanced intermediates adsorption/desorption ability and consequently results in the boosted catalytic activity and long‐term stability. This work supplies new perspectives to investigate the SAR in amorphous MOF structures, thereby guiding the rational design of advanced OER catalysts.