Highly-efficient natural gas desulfurization and simultaneous H2O2 synthesis based on the electrochemical coupling reaction strategy

Abstract

Hydrogen sulfide (H2S) generated by natural gas exploitation is a dangerous and harmful gas that needs to be purified. Electrochemical Natural Gas Desulfurization offers a promising way for H2S purification and resource utilization in ambient conditions. However, poor energy efficiency and low resource value limit the prospective application in the industry. Herein, we propose a gas-liquid flow electrocatalysis system that couples H2S oxidation and O2 reduction processes to effectively recover sulfur and H2O2 with low energy consumption. Gas diffusion and mass transfer are accelerated by gas-liquid flow cells, which also significantly decrease the resistance. Besides, I-/I3- redox pairs promote selective H2S oxidation while inhibiting water decomposition, resulting in a 56% reduction in oxidation potential. Moreover, the surface proton concentration is elevated by employing a modified carbon gas diffusion electrode (GDE), which assists to maintains a high H2O2 faradic efficiency. The system is able to operate at a high current density of 102 mA/cm2 at an Ecell voltage of 3.5 V, yielding S and H2O2 at rates of 60 mg cm−2 h−1 and 50 mg cm−2 h−1 respectively. A techno-economic model forecasts the effects of system efficiency and energy prices on operational costs and illustrates potential routes to a plant-gate levelized application in the petrochemical industry.