Kenji Sumida, David L. Rogow, Jarad A. Mason, Thomas M. McDonald, Eric D. Bloch, Zoey R. Herm, Tae-Hyun Bae, Jeffrey R. Long

Carbon Dioxide Capture in Metal–Organic Frameworks

Carbon capture and storage (CCS) is broadly recognised as having the potential to play a key role in meeting climate change targets, delivering low carbon heat and power, decarbonising industry and, more recently, its ability to facilitate the net removal of CO2 from the atmosphere. However, despite this broad consensus and its technical maturity, CCS has not yet been deployed on a scale commensurate with the ambitions articulated a decade ago. Thus, in this paper we review the current state-of-the-art of CO2 capture, transport, utilisation and storage from a multi-scale perspective, moving from the global to molecular scales. In light of the COP21 commitments to limit warming to less than 2 °C, we extend the remit of this study to include the key negative emissions technologies (NETs) of bioenergy with CCS (BECCS), and direct air capture (DAC). Cognisant of the non-technical barriers to deploying CCS, we reflect on recent experience from the UK's CCS commercialisation programme and consider the commercial and political barriers to the large-scale deployment of CCS. In all areas, we focus on identifying and clearly articulating the key research challenges that could usefully be addressed in the coming decade.

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Carbon capture and storage (CCS): the way forward

In recent years, Carbon Capture and Storage (Sequestration) (CCS) has been proposed as a potential method to allow the continued use of fossil-fuelled power stations whilst preventing emissions of CO2 from reaching the atmosphere. Gas, coal (and biomass)-fired power stations can respond to changes in demand more readily than many other sources of electricity production, hence the importance of retaining them as an option in the energy mix. Here, we review the leading CO2 capture technologies, available in the short and long term, and their technological maturity, before discussing CO2 transport and storage. Current pilot plants and demonstrations are highlighted, as is the importance of optimising the CCS system as a whole. Other topics briefly discussed include the viability of both the capture of CO2 from the air and CO2 reutilisation as climate change mitigation strategies. Finally, we discuss the economic and legal aspects of CCS.

Carbon capture and storage update

Post-combustion CO2 capture from the flue gas is one of the key technology options to reduce greenhouse gases, because this can be potentially retrofitted to the existing fleet of coal-fired power stations. Adsorption processes using solid sorbents capable of capturing CO2 from flue gas streams have shown many potential advantages, compared to other conventional CO2 capture using aqueous amine solvents. In view of this, in the past few years, several research groups have been involved in the development of new solid sorbents for CO2 capture from flue gas with superior performance and desired economics. A variety of promising sorbents such as activated carbonaceous materials, microporous/mesoporous silica or zeolites, carbonates, and polymeric resins loaded with or without nitrogen functionality for the removal of CO2 from the flue gas streams have been reviewed. Different methods of impregnating functional groups, including grafting techniques and modifying the support materials, have been discussed to en...

Post-Combustion CO2 Capture Using Solid Sorbents: A Review

In the last few years there has been a rapid growth in governmental funding and research activities worldwide for CO2 capture, storage and utilization (CSU), due to increasing awareness of the link between CO2 accumulation in the atmosphere and global warming. Among the various technologies and processes that have been developed and are emerging for CSU of CO2, solid CO2-adsorbents are widely applied. In this review, these solid CO2-adsorbents are classified into three types according to their sorption/desorption temperatures: low-, intermediate- and high-temperature adsorbents with temperatures ranging from below 200 °C, between 200–400 °C and above 400 °C, respectively. For each type of solid CO2-adsorbent, the synthesis, interaction mechanism with CO2 and sorption performance, potential applications and problems are reviewed. In the last section, several representative CO2-sorption-enhanced catalytic reactions are discussed. It is expected that this review will not only summarize the main research activities in this area, but also find possible links between fundamental studies and industrial applications.

CO2 capture by solid adsorbents and their applications: current status and new trends

CO2 capture by adsorption: Materials and process development

Capture of CO2 from flue gas streams using adsorption processes must deal with the prospect of high humidity streams containing bulk CO2 as well as other impurities such as SOx, NOx, etc. Most studies to date have ignored this aspect of CO2 capture. In this study, we have experimentally examined the capture of CO2 from a 12% synthetic flue gas stream at a relative humidity of 95% at 30 °C. A 13X adsorbent was used and the migration of the water and its subsequent impact on capture performance was evaluated. Binary breakthrough of CO2/water vapor was performed and indicated a significant effect of water on CO2 adsorption capacity, as expected. Cyclic experiments indicate that the water zone migrates a quarter of the way into the column and stabilizes its position so that CO2 capture is still possible although decreased. The formation of a water zone creates a “cold spot” which has implications for the system performance. The recovery of CO2 dropped from 78.5% to 60% when moving from dry to wet flue gas while the productivity dropped by 22%. Although the concentration of water leaving the bed under vacuum was 27%(vol), the low vacuum pressure prevented condensation of water in this stream. However, the vacuum pump acted as a condenser and separator to remove bulk water. An important consequence of the presence of a water zone was to elevate the vacuum level thereby reducing CO2 working capacity. Thus although there is a detrimental effect of water on CO2 capture, long term recovery of CO2 is still possible in a single VSA process. Pre-drying of the flue gas steam is not required. However, careful consideration of the impact of water and accommodation thereof must be made particularly when the feed stream temperature increases resulting in higher feed water concentration.

Capture of CO2 from high humidity flue gas by vacuum swing adsorption with zeolite 13X

Effect of process parameters on power requirements of vacuum swing adsorption technology for CO2 capture from flue gas

Alkali and alkaline-earth cation exchanged chabazite zeolites for adsorption based CO2 capture

Vacuum swing adsorption (VSA) capture of CO2 from flue gas streams is a promising technology for greenhouse gas mitigation. In this study we use a detailed, validated numerical model of the CO2VSA process to study the effect of a range of operating and design parameters on the system performance. The adsorbent used is 13X and a feed stream of 12% CO2 and dry air is used to mimic flue gas. Feed pressures of 1.2 bar are used to minimize flue gas compression. A 9-step cycle with two equalisations and a 12-step cycle including product purge were both used to understand the impact of several cycle changes on performance. The ultimate vacuum level used is one of the most important parameters in dictating CO2 purity, recovery and power consumption. For vacuum levels of 4 kPa and lower, CO2 purities of >90% are achievable with a recovery of greater than 70%. Both purity and recovery drop quickly as the vacuum level is raised to 10 kPa. Total power consumption decreases as the vacuum pressure is raised, as expected, but the recovery decreases even quicker leading to a net increase in the specific power. The specific power appears to minimize at a vacuum pressure of approximately 4 kPa for the operating conditions used in our study. In addition to the ultimate vacuum level, vacuum time and feed time are found to impact the results for differing reasons. Longer evacuation times (to the same pressure level) imply lower flow rates and less pressure drop providing improved performance. Longer feed times led to partial breakthrough of the CO2 front and reduced recovery but improved purity. The starting pressure of evacuation (which is not necessarily equal to the feed pressure) was also found to be important since the gas phase was enriched in CO2 prior to removal by vacuum leading to improved CO2 purity. A 12-step cycle including product purge was able to produce high purity CO2 (>95%) with minimal impact on recovery. Finally, it was found that for 13X, the optimal feed temperature was around 67°C to maximize system purity. This is a consequence of the temperature dependence of the working selectivity and working capacity of 13X. In summary, our numerical model indicates that there is considerable scope for improvement and use of the VSA process for CO2 capture from flue gas streams.

Jun Zhang

Papers

CO2 capture by adsorption: Materials and process development

Capture of CO2 from high humidity flue gas by vacuum swing adsorption with zeolite 13X

Effect of process parameters on power requirements of vacuum swing adsorption technology for CO2 capture from flue gas

Alkali and alkaline-earth cation exchanged chabazite zeolites for adsorption based CO2 capture

Capture of CO2 from flue gas streams with zeolite 13X by vacuum-pressure swing adsorption