Non-neutral catalyst and reaction energy recovery to minimize the energy consumption for hydrogen production by recyclably indirect H2O electrolysis and CO2 capture

Highlights: • Recyclable electro-driven process of CO₂ capture and indirect H₂O electrolysis. • Non-neutral Ni based catalyst was developed to achieve single-atom catalysis. • Catalyst regeneration is achieved with high activity site. • DFT model and energy recovery model are developed. • Energy consumption for H₂ production and CO₂ capture reduced to 0.4 V and 1 GJ/t. -- Abstract: Hydrogen utilization and CO₂ capture significantly improve the environment. In order to reduce the energy penalty of hydrogen production and CO₂ capture, the idea of this work is to integrate the hydrogen production and CO₂ capture. Here, the recyclable electro-driven process of CO₂ capture and indirect H₂O electrolysis was developed. In the process, the energy recovery system was developed to utilize the reaction heat. The non-neutral Ni based catalyst with single-atom catalysis was designed. DFT model and energy recovery model were developed. The turnover frequency, transmission value, electron density, band structure, reaction kinetics of hydrogen production and CO₂ desorption were determined. A mechanism of second dehydrogenation and second hydrogen release was identified for the non-neutral catalysis. Non-neutral NiAlTiR+ catalyst enhanced the electron transport and made electron dense region extend to the single atom zone. The 90% yield of hydrogen was produced due to the fast electron transport. The well regenerated catalyst during the 25 cycles produced the 80–90% turnover frequency and transmission compared with the fresh catalyst. The non-neutral catalyst, catalyst regeneration and reaction energy recovery reduced the energy consumption for H₂ production and CO₂ capture to 0.4 V and 1 GJ/t.