Design of High-Performance Wood-Derived N-Doped Ecr Electrocatalysts Based on Marcus Theory

Abstract

The conversion of CO2 into high-value compounds by electrochemical CO2 reduction reaction (ECR) is a promising technology. However, it is a challenge to efficiently design and screen high-performance electrocatalysts. In this paper, we combined the Marcus equation with the theory of thermal-kinetic correlation to successfully predict the optimal N-C doping ratio. Poplar wood -derived 3D N-doped graphitized carbon with optimal N doping content (pyridine-N 1.87 At%, pyrrole-N, 1.52 At%), high specific surface area (471.2 m2 g-1), and abundant nanopores were successfully obtained with the assistance of melamine (N source), which exhibited a high ECR activity of 86.78% at a low applied potential of -0.71 V (vs. RHE) and long-term stability of at least 10 cycles. This extends the application of the Marcus equation and improves new ideas for the future design of high-performance electrocatalysts.

Keywords: thermal-kinetic correlation, Marcus equation, wood-derived, electrocatalysts, carbon dioxide reduction