Electrocatalytic Hydrogen Evolution of Immobilized Copper Complex on Carbonaceous Materials: From Neutral Water to Seawater

Chempluschem. 2024 Feb 17:e202300679. doi: 10.1002/cplu.202300679. Online ahead of print.

Abstract

Electrochemical hydrogen evolution reaction (HER) is an appealing strategy to utilize renewable electricity to produce green H2 . Moreover, use of neutral-pH electrolyte such as water and seawater for the HER has long been desired for eco-friendly energy production that aligns with net zero emission goal. Herein, new heterogeneous catalysts were developed by dispersing an HER-active copper complex containing N4 -Schiff base macrocycle (CuL) on carbonaceous materials, i. e. multi-walled carbon nanotube (CNT) and graphene oxide (GO), via non-covalent interaction and investigated their HER performance. It was found that CuL/GO exhibited higher HER activity than CuL/CNT, possibly due to its significantly larger amount of CuL immobilized onto GO. In addition, CuL/GO showed satisfactory HER performance in a neutral (pH 7) NaCl electrolyte solution. Notably, the performances of CuL/GO were boosted up when performed in natural seawater sample with the faradaic efficiency of 70 % and 3 times higher amount of H2 at -0.6 V vs reversible hydrogen electrode (RHE), in comparison to the HER in a NaCl electrolyte. Furthermore, it possessed a low overpotential of 139 mV at -10 mA/cm2 . This demonstrated the potential use of CuL/GO as an effective HER catalyst in seawater for further sustainable development.

Keywords: HER; carbonaceous support; copper complex; electrocatalyst; heterogeneous catalyst.