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Pyridinic nitrogen-substituted graphene membranes for exceptional CO2 capture
Sushu Zhang, Yang Yang, Jingyu Wang⁎
https://doi.org/10.1016/j.cjsc.2024.100440
ABSTRACT
This work underscores the effectiveness of introducing functional heteroatoms at the edges of pores of 2D oxidized graphene for improving CO2/N2 separation. The strong affinity between pyridinic N and CO2, coupled with the 2D nature of pores, enables high selectivity even in dilute CO2 mixtures with a little sacrifice of permeance as compared to graphene membranes without NH3 treatment. These results emphasized the challenges in simultaneously optimizing the gas permeance and selectivity for CO2/N2 separation in future study. The scalability and feasibility of this approach, utilizing gaseous reactants (O3 for oxidation and NH3 for pyridinic-N incorporation), make it an attractive candidate for large-scale carbon capture applications. The impressive CO2/N2 separation performance of pyridinic-N-substituted graphene membrane can be adaptive to multiple carbon sources, including concentrated emissions (from steel and cement plants, coal-fired power stations) and low CO2 concentration (from aluminum production and natural gas processing). The techno-economic analysis of carbon capture indicated the cost of US$ 20 per tonCO2 for concentrated CO2 feed and US$ 76 per tonCO2 for dilute CO2 feed capture. The selective carbon capture technology in this work realized the separation of diluted CO2 to improve the recycling of CO2 so that the emission to atmosphere could be alleviated. This research on screening competitive sorption regimes can be applied to develop high-performance and cost-effective CO2 separation membranes, addressing critical global environmental challenges.
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