Carbon capture test unit design and development using amine-based solid sorbent

https://doi.org/10.1016/j.cherd.2016.06.020Get rights and content

Highlights

  • The baseline design and development of a CO2 capture reactor system is presented.

  • Subsequent modifications to promote better performance are presented.

  • The paper discusses the changes associated with a sorbent change.

  • The system consisted of four fluid beds, with a circulating amine based sorbent.

Abstract

This paper presents the design and development of a reactor system and the subsequent modifications to evaluate an integrated process to scrub carbon dioxide (CO2) from synthetic flue gas using amine based solid sorbents. The paper presents the initial system design and then discusses the various changes implemented to address the change in sorbent from a 180 μm Geldart group B material to a 115 μm Geldart group A material as well as issues discovered during experimental trials where the major obstacle in system operation was the ability to maintain a constant circulation of a solid sorbent stemming from this change in sorbent material.

The system primarily consisted of four fluid beds, through which an amine impregnated solid sorbent was circulated and adsorption, pre-heat, regeneration, and cooling processes occurred. Instrumentation was assembled to characterize thermal, hydrodynamic, and gas adsorption performance in this integrated unit. A series of shakedown tests were performed and the configuration altered to meet the needs of the sorbent performance and achieve desired target capture efficiencies. Methods were identified, tested, and applied to continuously monitor critical operating parameters including solids circulation rate, adsorbed and desorbed CO2, solids inventories, and pressures.

Introduction

The United States emits more CO2 than any other country, except China, with nearly 40% from fossil fuel-fired power plants (U.S. DOE, 2012). Successful carbon management relies on the development of cost effective methods to capture CO2 from the flue gas of existing power plants (Ciferno, 2008, Pires et al., 2011, Susarla et al., 2015). Baseline studies for adding CO2 capture and sequestration to existing power plants indicate that, using conventional technology, the cost of electricity would nearly double from coal fired pulverized coal power plants (Black, 2010). CO2 capture can be realized in a two-step sequestration process where CO2 is first separated from product gases and then stored in geological locations within the earth. Chemical solvent based absorption systems have been utilized and studied for nearly a century and have not shown the ability to limit significant cost or loss in efficiency below target values (Burchell et al., 1997, Yong et al., 2002).

Chemical adsorption using solid sorbents has been widely investigated and considered to be a promising alternative to liquid solvents for CO2 capture. The use of light weight and selective solid sorbents coated with polyamines offer potential cost savings over conventional liquid based systems (Fisher and Keller, 2011, Yang and Hoffman, 2009). Solid sorbents have the potential to be used over a wide range of temperatures up to 700 °C and have been shown to be less environmentally impactful, when compared to liquid adsorbents. The use of solid sorbents has the potential to reduce process costs as compared to conventional liquid based systems by reducing evaporative heat losses (Frimpong et al., 2013, Zhenissova et al., 2014). Solid sorbents with high CO2 capacity and readily adsorb and release CO2 can improve the cost competitiveness of these processes.

Amine sorbents have a high capacity for CO2, can be hydrophobic, and can readily adsorb and release CO2 (Gray et al., 2003, Gray et al., 2004, Gray et al., 2005, Gray et al., 2008, Heydari-Gorji et al., 2011, Monazam et al., 2012, Samanta et al., 2012, Siriwardane, 2005). These sorbents adsorb CO2 at low temperatures and release it at elevated temperatures. Scale up to utility applications requires that the solids are transported or conveyed between the adsorber and the regenerator. Fluidized bed technology appeared to be well suited for this type of thermal swing process because gas-solids suspensions can be readily transported between different reactors. Unfortunately, recent attempts to demonstrate integrated adsorption and regeneration were unable to achieve significant CO2 capture during continuous flow process with an amine based sorbents. Sjostroma et al. (2011) identified multiple potential causes such as deficiencies in sorbent and operating conditions. Long term stable operation and continuous solids circulation between two fluidized beds has been reported to demonstrate a system design that allows for high CO2 capture efficiency but is still limited to an efficiency lower than 90%. Factors affecting the working capacity of the sorbents, which limits the capture efficiency, are mainly due to high adsorption temperatures and short absorber residence times (Zhao et al., 2013). Recently, a system study done by Proll et al. (2016) with a double loop fluidized bed, showed reduction in sorbent circulation rates resulting in lower energy demand for the capture process. The study showed the potential of high carbon capture rates as well as low overall heat requirements through a temperature or thermal swing process. Temperature swing adsorption technology has previously shown reduction in thermal energy requirement while maintaining continuous CO2 capture in circulating fluidized bed systems and bubbling fluidized beds (Veneman et al., 2012, Zhang et al., 2014).

A small scale system was designed and constructed to evaluate various solid sorbents operated in a circulating fluid bed system using a thermal swing process. The original design incorporated the hydrodynamic characteristics of a certain class of particles; however, the sorbent that was ultimately available deviated from these. Other factors were also discovered that required modification of the system. The evolution of the experimental system is traced from concept through shakedown to final configuration. The design basis is described and causes for major modifications identified. Critical process measurement and control systems were developed to improve process stability and provide real-time measurement of process performance.

Sjostroma et al. (2011) demonstrated that CO2 adsorption occurs within a short section (less than 0.7 m) in the entrance of the riser. Ryan et al. (2013) and Breault and Huckaby (2013) present CFD simulations showing the CO2 removal all taking place within the 0.7 m riser entrance region. As a result, the focus of this research was to further elucidate regeneration of the sorbent in a closed loop system since adsorption had been experimentally demonstrated.

Section snippets

Unit design and development

A small scale circulating fluidized bed system (Carbon Capture Unit or C2U) was designed to test the effectiveness of solid amine based sorbents for use in the capture of CO2 from flue gas. The original C2U design can been seen in Fig. 1 where each component is identified along with fluidization gas inlet locations marked numerically. The C2U consisted of four fluidized bed vessels: the adsorber, the regenerator, plus the upper and lower loop seals. Nitrogen was supplied at all fluidization

Operation of original design

Operation was initiated by first introducing minimal flows (2Umf) of humidified nitrogen to the regenerator, adsorber and each loop seal. Humidification was controlled at 2 vol% which is near saturation under ambient conditions. The experiments were run with a synthetic flue-gas that contained a CO2 concentration of 6–21% and a 2% by volume of moisture. The remaining was nitrogen. These experiments did not consider the effects of trace components such as SO2, O2 or ash.

Sorbent within the

The modifications

The C2U configuration was altered a number of times to obtain a controllable circulating system capable of operating on the Geldart group A material rather than the original Geldart group B material. The sorbent properties for the group A material where previously shown in Table 2. The original configuration, designated Mod 0, is depicted in Fig. 1 where the underflow tube below the regenerator transitioned into the L-valve. The adsorber consisted of a 45 cm tall fluidized bed section situated

Summary

Significant CO2 capture was demonstrated in a relatively simple, continuous fluidized bed processes. The adsorption of carbon dioxide (CO2) by immobilized amine (PEI) on mesoporous silica was investigated using a series of coupled fluidized beds referred to as the C2U. This test unit employed fluidized bed technology to adsorb CO2 from a simulated mixture of gases representing the flue gas from a pulverized coal power plant. The sorbent was then transferred using non-mechanical valve technology

Nomenclature

    App

    projected particle area (m2)

    CD

    drag coefficient

    CO2%

    CO2 volume concentration in adsorber flow (%)

    dp

    particle diameter (m)

    Dt

    heat transfer tube diameter (m)

    Fa

    total flow to adsorber plenum (slpm)

    Fls

    total flow to loopseal plenums (slpm)

    Fmv

    total move air flow (slpm)

    Fr

    total flow to regenerator plenum (slpm)

    g

    gravitational acceleration (9.8 m/s2)

    hc

    heat transfer coefficient between immersed tube and bed (W/m2 K)

    kg

    gas conductive heat transfer coefficient (W/m K)

    LMTD

    log mean temperature difference (K)

    Minv

Disclaimer

This project was funded by the Department of Energy, National Energy Technology Laboratory, an agency of the United States Government, through a support contract with URS Energy & Construction, Inc. Neither the United States Government nor any agency thereof, nor any of their employees, nor URS Energy & Construction, Inc., nor any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any

Acknowledgements

This work was funded by the U.S. Department of Energy, Office of Fossil Energy's Carbon Capture Simulation Initiative through the National Energy Technology Laboratory.

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