Dataset Information

Fluorinated MIL-101 for carbon capture utilisation and storage: uptake and diffusion studies under relevant industrial conditions.

ABSTRACT: Carbon capture utilisation and storage (CCUS) using solid sorbents such as zeolites, activated carbon and Metal-Organic Frameworks (MOFs) could facilitate the reduction of anthropogenic CO₂ concentration. Developing efficient and stable adsorbents for CO₂ capture as well as understanding their transport diffusion limitations for CO₂ utilisation plays a crucial role in CCUS technology development. However, experimental data available on CO₂ capture and diffusion under relevant industrial conditions is very limited, particularly for MOFs. In this study we explore the use of a gravimetric Dynamic Vapour Sorption (DVS) instrument to measure low concentration CO₂ uptake and adsorption kinetics on a novel partially fluorinated MIL-101(Cr) saturated with different water vapour concentrations, at ambient pressure and temperature. Results show that up to water P/P ₀ = 0.15 the total CO₂ uptake of the modified material improves and that the introduction of small amounts of water enhances the diffusion of CO₂. MIL-101(Cr)-4F(1%) proved to be a stable material under moist conditions compared to other industrial MOFs, allowing facile regeneration under relevant industrial conditions.

SUBMITTER: Saenz Cavazos PA

PROVIDER: S-EPMC8697625 | biostudies-literature | 2021 Apr

REPOSITORIES: biostudies-literature

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Fluorinated MIL-101 for carbon capture utilisation and storage: uptake and diffusion studies under relevant industrial conditions.

Sáenz Cavazos Paola A PA Díaz-Ramírez Mariana L ML Hunter-Sellars Elwin E McIntyre Sean R SR Lima Enrique E Ibarra Ilich A IA Williams Daryl R DR

RSC advances 20210412 22

Carbon capture utilisation and storage (CCUS) using solid sorbents such as zeolites, activated carbon and Metal-Organic Frameworks (MOFs) could facilitate the reduction of anthropogenic CO2 concentration. Developing efficient and stable adsorbents for CO2 capture as well as understanding their transport diffusion limitations for CO2 utilisation plays a crucial role in CCUS technology development. However, experimental data available on CO2 capture and ...[more]

PMID: 35423892

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Project description:In this study, hybrids of nanoporous MIL-101(Cr) and MIL-53(Al) were synthesized using a hydrothermal method for various time periods, ranging from 8 to 40 h. The prepared materials were characterized by powder X-ray diffraction (PXRD) and elemental analysis, and their specific surface areas were measured by N2 sorption at 77 K using the Brunauer-Emmett-Teller (BET) method. To investigate the practical application of these materials, the pure carbon dioxide and methane adsorption capacities of the samples were determined using the volumetric method. The Langmuir model was used to fit the CO2 and CH4 isotherms. Extended Langmuir (EL) equations and the ideal adsorbed solution theory (IAST) models were used to obtain the CO2/CH4 selectivity. The sample with the highest BET specific surface area was selected as a candidate for further investigations. The thermal stability of the selected sample was investigated by thermogravimetric analysis (TGA). Scanning electron microscopy (SEM) was used to characterize the sample morphology. XRD results showed that the sample synthesized over the shortest time corresponded to MIL-101(Cr), while the sample synthesized over the longest time was in agreement with MIL-53(Al). Samples synthesized for time periods between these two limits were assumed to be composites of both MIL-53(Al) and MIL-101(Cr). TGA results indicated that the hybrid materials were thermally stable at temperatures about 100 °C higher than for pure MIL-101(Cr). The BET specific surface area (1746 m2 g-1) and CO2 adsorption capacity (16 mmol g-1) of the selected hybrid sample were about 50% and 35% higher, respectively, compared with those of pure MIL-53(Al), but 30% and 20% lower, respectively, compared with those of pure MIL-101(Cr). Binary adsorption modeling showed the high selectivity of the MIL-101(Cr) and MIL-53(Al) hybrid material for CO2 with a minimum separation factor of about 60 at 298 K. This value was much higher than those reported previously and those observed in this work for the original MIL-101(Cr) or MIL-53(Al). These results demonstrated that the hybrid of MIL-101(Cr) and MIL-53(Al) was a promising material for selective CO2 capture from natural and biogas.

Project description:Due to the dramatically increased atmospheric CO2 concentration and consequential climate change, significant effort has been made to develop sorbents to directly capture CO2 from ambient air (direct air capture, DAC) to achieve negative CO2 emissions in the immediate future. However, most developed sorbents have been studied under a limited array of temperature (>20 °C) and humidity conditions. In particular, the dearth of experimental data on DAC at sub-ambient conditions (e.g., -30 to 20 °C) and under humid conditions will severely hinder the large-scale implementation of DAC because the world has annual average temperatures ranging from -30 to 30 °C depending on the location and essentially no place has a zero absolute humidity. To this end, we suggest that understanding CO2 adsorption from ambient air at sub-ambient temperatures, below 20 °C, is crucial because colder temperatures represent important practical operating conditions and because such temperatures may provide conditions where new sorbent materials or enhanced process performance might be achieved. Here we demonstrate that MIL-101(Cr) materials impregnated with amines (TEPA, tetraethylenepentamine, or PEI, poly(ethylenimine)) offer promising adsorption and desorption behavior under DAC conditions in both the presence and absence of humidity under a wide range of temperatures (-20 to 25 °C). Depending on the amine loading and adsorption temperature, the sorbents show different CO2 capture behavior. With 30 and 50 wt % amine loadings, the sorbents show weak and strong chemisorption-dominant CO2 capture behavior, respectively. Interestingly, at -20 °C, the CO2 adsorption capacity of 30 wt % TEPA-impregnated MIL-101(Cr) significantly increased up to 1.12 mmol/g from 0.39 mmol/g at ambient conditions (25 °C) due to the enhanced weak chemisorption. More importantly, the sorbents also show promising working capacities (0.72 mmol/g) over 15 small temperature swing cycles with an ultralow regeneration temperature (-20 °C sorption to 25 °C desorption). The sub-ambient DAC performance of the sorbents is further enhanced under humid conditions, showing promising and stable CO2 working capacities over multiple humid small temperature swing cycles. These results demonstrate that appropriately designed DAC sorbents can operate in a weak chemisorption modality at low temperatures even in the presence of humidity. Significant energy savings may be realized via the utilization of small temperature swings enabled by this weak chemisorption behavior. This work suggests that significant work on DAC materials that operate at low, sub-ambient temperatures is warranted for possible deployment in temperate and polar climates.

Dataset Information

Fluorinated MIL-101 for carbon capture utilisation and storage: uptake and diffusion studies under relevant industrial conditions.

Publications

Fluorinated MIL-101 for carbon capture utilisation and storage: uptake and diffusion studies under relevant industrial conditions.

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