Kraft Lignin-Derived Microporous Nitrogen-Doped Carbon Adsorbent for Air and Water Purification
Oleg Tkachenko, Alina Nikolaichuk, Nataliia Fihurka, Andreas Backhaus, Julie B. Zimmerman, Maria Strømme, Tetyana M. Budnyak
Abstract
High Resolution Image Download MS PowerPoint Slide The study presents a streamlined one-step process for producing highly porous, metal-free, N-doped activated carbon (N-AC) for CO 2 capture and herbicide removal from simulated industrially polluted and real environmental systems. N-AC was prepared from kraft lignin─a carbon-rich and abundant byproduct of the pulp industry, using nitric acid as the activator and urea as the N-dopant. The reported carbonization process under a nitrogen atmosphere renders a product with a high yield of 30% even at high temperatures up to 800 °C. N-AC exhibited a substantial high N content (4–5%), the presence of aliphatic and phenolic OH groups, and a notable absence of carboxylic groups, as confirmed by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Boehm’s titration. Porosity analysis indicated that micropores constituted the majority of the pore structure, with 86% of pores having diameters less than 0.6 nm. According to BET adsorption analysis, the developed porous structure of N-AC boasted a substantial specific surface area of 1000 m 2 g –1 . N-AC proved to be a promising adsorbent for air and water purification. Specifically, N-AC exhibited a strong affinity for CO 2, with an adsorption capacity of 1.4 mmol g –1 at 0.15 bar and 20 °C, and it demonstrated the highest selectivity over N 2 from the simulated flue gas system (27.3 mmol g –1 for 15:85 v/v CO 2 /N 2 at 20 °C) among all previously reported nitrogen-doped AC materials from kraft lignin. Moreover, N-AC displayed excellent reusability and efficient CO 2 release, maintaining an adsorption capacity of 3.1 mmol g –1 (at 1 bar and 25 °C) over 10 consecutive adsorption–desorption cycles, confirming N-AC as a useful material for CO 2 storage and utilization. The unique cationic nature of N-AC enhanced the adsorption of herbicides in neutral and weakly basic environments, which is relevant for real waters. It exhibited an impressive adsorption capacity for the herbicide 2,4-dichlorophenoxyacetic acid (2,4- D ) at 96 ± 6 mg g –1 under pH 6 and 25 °C according to the Langmuir–Freundlich model. Notably, N-AC preserves its high adsorption capacity toward 2,4- D from simulated groundwater and runoff from tomato greenhouse, while performance in real samples from Fyris river in Uppsala, Sweden, causes a decrease of only 4–5%. Owing to the one-step process, high yield, annual abundance of kraft lignin, and use of environmentally friendly activating agents, N-AC has substantial potential for large-scale industrial applications.