From Theory to Experiment: Cascading of Thermocatalysis and Electrolysis in Oxygen Evolution Reactions
Xing Fan, Siyu Tan, Junjun Yang, Yunxia Liu, Wenyi Bian, Fan Liao, Haiping Lin, Youyong Li
Abstract
The role of elevated temperatures in electrolysis has generally been regarded as accelerations of electron transport, mass transport, and adsorption/desorption processes. In the present work, with first-principles calculations, we demonstrate that thermally activated on-surface reactions can significantly increase the efficiency of energy conversions in electrolysis via a thermally and electrically cascaded mechanism. In the oxygen evolution reaction (OER), to be specific, the formation of high-energy *OOH on Fe can be assisted by thermally activated combination of *O and *OH on the surface of iron-benzenehexathiol coordination polymer (Fe-BHT). Such theoretical predictions are then confirmed by our experimental measurements. The OER efficiency on Fe-BHT increases with increasing temperature and outperforms the state-of-the-art IrO2 catalyst at around 80 °C. This research may shed light on an avenue for designing and preparing electrocatalysts with enhanced catalytic performance.