Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 56, Issue 23, Pages 16811-16821Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.2c04658
Keywords
water treatment; micropollutant; Arrhenius equation; nanopore; activation energy
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Funding
- Helmholtz Association Recruitment Initiative
- Helmholtz ERC Recognition
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Nanofiltration membranes can retain micropollutants to a large extent, but breakthrough and incomplete removal may occur. This study investigates the permeation of micropollutants in tight and loose membranes, focusing on the energy barriers for transport. The results show that the energy barriers for steroid hormone transport in tight membranes are entropically dominated, while the loose membranes enable partitioning at the pore entrance.
Nanofiltration (NF) membranes can retain micropollutants (MPs) to a large extent, even though adsorption into the membrane and gradual permeation result in breakthrough and incomplete removal. The permeation of MPs is investigated by examining the energy barriers (determined using the Arrhenius concept) for adsorption, intrapore diffusion, and permeation encountered by four different steroid hormones in tight and loose NF membranes. Results show that the energy barriers for steroid hormone transport in tight membrane are entropically dominated and underestimated because of the high steric exclusion at the pore entrance. In contrast, the loose NF membrane enables steroid hormones partitioning at the pore entrance, with a permeation energy barrier (from feed toward the permeate side) ranging between 96 and 116 kJ/mol. The contribution of adsorption and intrapore diffusion to the energy barrier for steroid hormone permeation reveals a significant role of intrapore diffusive transport on the obtained permeation energy barrier. Overall, the breakthrough phenomenon observed during the NF of MPs is facilitated by the low energy barrier for adsorption. Experimental evidence of such principles is relevant for understanding mechanisms and ultimately improving the selectivity of NF.
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