Ru-FeNi Alloy Heterojunctions on Lignin-derived Carbon as Bifunctional Electrocatalysts for Efficient Overall Water Splitting

Angew Chem Int Ed Engl. 2023 Aug 14;62(33):e202306333. doi: 10.1002/anie.202306333. Epub 2023 Jul 7.

Abstract

Rational design of efficient, stable, and inexpensive bifunctional electrocatalysts for oxygen evolution reactions (OER) and hydrogen evolution reactions (HER) is a key challenge to realize green hydrogen production via electrolytic water splitting. Herein, Ru nanoparticles and FeNi alloy heterojunction catalyst (Ru-FeNi@NLC) encapsulated via lignin-derived carbon was prepared by self-assembly precipitation and in situ pyrolysis. The designed catalyst displays excellent performance at 10 mA cm-2 with low overpotentials of 36 mV for HER and 198 mV for OER, and only needs 1.48 V for overall water splitting. Results and DFT calculations show the unique N-doped lignin-derived carbon layer and Ru-FeNi heterojunction contribute to optimized electronic structure for enhancing electron transfer, balanced free energy of reactants and intermediates in the sorption/desorption process, and significantly reduced reaction energy barrier for the HER and OER rate-determining steps, thus improved reaction kinetics. This work provides a new in situ pyrolysis doping strategy based on renewable biomass for the construction of highly active, stable and cost-effective catalysts.

Keywords: Bifunctional Electrocatalysts; Heterojunction; Lignin-Derived Carbon; Water Splitting.