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Lu, Hong

Publications and source records attributed to Lu, Hong.

Parametric Testing and Evaluation of a Novel Biphasic Absorption Process for Post-Combustion Carbon Capture

A novel biphasic CO2 absorption process (BiCAP) is being developed at the University of Illinois. BiCAP is enabled by using a new class of biphasic solvents developed based on multi-property criteria for postcombustion carbon capture. The process was previously demonstrated at the lab-scale, including in 10 kWe absorption and desorption column systems. In the current study, the process has been scaled up by building and testing a 40 kWe integrated capture skid at a power plant. Parametric tests for two biphasic solvents were conducted with the synthetic flue gas made of bottle CO2 gas and air to validate the performance and operational flexibility of the unit with respect to varying process or operating conditions. Operation of the phase separator, which is unique equipment to BiCAP, was verified to be stable and efficient. Two liquid phases could be separated via static settlement based on a density difference and >90% of the CO2 absorbed was concentrated in the separated CO2-rich phase. Results of parametric tests showed that the minimum heat duty appeared at the optimal stripping pressure. A higher stripping temperature was more favourable to improve overall energy performance. Introducing a secondary cold solvent feed stream to the top of the stripper via bypassing the cross heat exchanger helped reduce the heat loss carried with water vapour. Test results also revealed that the heat duty requirement was comparable when the CO2 concentration in flue gas decreased from ~11 to 4 vol.% as the phase separation decoupled the absorption and desorption steps in BiCAP. Under typical steady-state conditions, both biphasic solvents lowered the process heat duty by >40% compared with the reference 30 wt.% monoethanolamine solvent.

Absorption↗

Catalytic Removal of Oxygen Impurities from Pressurized Oxy-Combustion Flue Gas for the Production of High-Purity Carbon Dioxide

Flue gas purification is important for pressurized oxy-combustion systems to produce pure carbon dioxide (CO 2 ) streams ready for storage or utilization. A catalytic approach to removing oxygen (O 2 ) impurities from pressurized oxy-combustion flue gas via reduction with methane (CH 4 ) was investigated in this work. Two types of catalysts were studied: palladium (Pd)-based catalysts supported on titania (TiO 2 ) prepared by incipient wetness impregnation and cobalt–manganese (CoMn) composite catalysts prepared by coprecipitation. The performance of the catalysts was evaluated in a high-pressure–high-temperature, fixed-bed reactor at a pressure of 15 bar and a gas hourly space velocity of 30 000 h –1 (standard conditions), with a simulated feeding gas composed of 3 vol % O 2 , 1.5 vol % CH 4 , and CO 2 as the balance gas. Among the Pd catalysts, 5% Pd/TiO 2 achieved the maximum 86% O 2 removal at ≥350 °C. The CoMn oxide catalysts displayed comparable or better activities for O 2 reduction compared with the Pd catalysts. Among them, the Co 40 Mn 1 catalyst exhibited the best performance, able to reduce 99.9% of O 2 impurities at ~370 °C with negligible carbon monoxide (CO) formation (<10 ppmv). Both trivalent and divalent Co and Mn were detected on the catalyst surface, and the superior activity of Co 40 Mn 1 might be associated with the resultant disordered structure. Furthermore, the activity of the catalyst was not affected by the presence of a trace amount of nitric oxide (NO) gas contaminant. Results of this study provide the basis for scale-up studies in both the synthesis and performance of non-noble metal catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Signature of Many-Body Localization of Phonons in Strongly Disordered Superlattices

Many-body localization (MBL) has attracted significant research attention due to its immunity to thermalization, role in logarithmic entanglement entropy growth, and opportunities to reach exotic quantum orders. However, experimental realization of MBL in solid-state systems has remained challenging. Here we report evidence of a possible phonon MBL phase in disordered GaAs/AlAs superlattices. Through grazing-incidence inelastic X-ray scattering, we observe a strong deviation of the phonon population from equilibrium in disordered samples doped with ErAs nanodots at low temperature, signaling a departure from thermalization. This behavior occurs within finite phonon energy and wavevector windows, suggesting a localization-thermalization crossover. We support our observation by proposing a theoretical model for the effective phonon Hamiltonian in disordered superlattices, and showing that it can be mapped exactly to a disordered 1D Bose-Hubbard model with a known MBL phase. The large on-site repulsion qualitatively explains the experimental findings. Furthermore, our work provides mode-resolved experimental evidence of phonon localization, potentially extending the scope of MBL to disordered solid-state systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

High-efficiency catalytic reduction of residual oxygen for purification of carbon dioxide streams from high-pressure oxy-combustion systems

Pressurized oxy-combustion is a promising technology for carbon capture, utilization, and storage. For the captured CO 2 to be used for enhanced oil recovery or stored in geological formations, flue gas impurities, including residual O 2 in the CO 2 stream, must be purified to meet the purity specifications. A catalytic approach to reducing residual O 2 with CH 4 was investigated in this study. Five CoMn- and Cu-based catalysts were synthesized or acquired, and a reverse-flow fixed-bed reactor was used to assess their performance for O 2 removal from a simulated oxy-combustion flue gas at 15 bar. The impacts of the operating parameters on O 2 removal, such as temperature, gas hourly space velocity, O 2 /CH 4 ratio, and gas pressure, were investigated. Among the tested catalysts, the two CoMn catalysts were superior in both activity and selectivity, with the reaction lighting off at about 350 °C and achieving 99% O 2 removal at about 500 °C. Finally, the kinetics of the catalytic reaction is discussed, and the Mars–van Krevelen redox mechanism is deemed valid for describing the reaction pathway for the top-performing CoMn catalysts. The catalytic reaction was determined to be first order in CH 4 and zero order in O 2 under the test conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Modeling, Design, and Testing of a Novel Biphasic Solvent-Enabled Absorption System for Post-Combustion Carbon Capture

A novel absorption process enabled by a new class of biphasic solvents for post-combustion carbon capture (BiCAP) is presently being developed at the University of Illinois at Urbana-Champaign. The new biphasic solvents are water-lean solvent blends that develop dual liquid phases with the absorbed CO2 highly enriched in one of the phases. These solvents are superior in CO2 capacity and have high thermal and oxidative stability compared to MEA. The BiCAP technology features a unique process configuration of multi-stage CO2 absorption and liquid–liquid phase separation during CO2 absorption, allowing continual separation and removal of the CO2-enriched liquid phase for maintaining low solvent viscosity and a fast absorption rate. A 40 kWe-scale skid has recently been constructed at the Abbott Power Plant in Champaign, IL, to test the BiCAP solvent in continuous operation with a slipstream of real post-combustion flue gas. Along with improvements in the stripping configuration including cold feed bypass, the process is expected to achieve a minimum reboiler duty of 2,210 kJ/kg CO2 captured at a stripper operating pressure of 6 bar.

20 FOSSIL-FUELED POWER PLANTS↗

Catalytic Reduction of Residual Oxygen for the Purification of Carbon Dioxide Streams from Pressurized Oxy-Combustors

Pressurized oxy-combustion (OC) is regarded as an energy-efficient alternative to atmospheric OC. To utilize the captured carbon dioxide (CO2) from pressurized OC for enhanced oil recovery or carbon storage in geological formations, the CO2 product stream must meet the required purity specifications. One major impurity in OC flue gases is residual O2 (e.g., 3 vol%). In this study, a catalytic approach has been investigated to remove the residual O2 through a reduction reaction with injected methane (CH4) in a reverse-flow fixed-bed (RFFB) reactor. The performance was tested for a supported copper (Cu)-based catalyst synthesized by incipient wetness impregnation and a cobalt-manganese (CoMn) oxide catalyst synthesized by a coprecipitation method. A commercial Cu-based catalyst was also studied as the reference. Experimental results revealed that under the reverse-flow operation, the temperature profiles in the reactor were symmetrical on both sides of the catalyst zone and were more homogenous than those under the conventional one-direction-flow operation. Among the tested catalysts, the CoMn catalyst was the most reactive for promoting the reduction of O2 with CH4, able to attain >95% O2 removal at 475 °C and a gas hourly space velocity (GHSV) of 18,000 h-1 with a feed gas containing 3 vol% O2. Under all experiments, the concentrations of carbon monoxide (CO) were lower than 30 ppmv in the effluent gas streams. The reaction between O2 and CH4 could be depicted by using the Mars–van Krevelen redox mechanism based on a two-step reduction–oxidation reaction pathway.

36 MATERIALS SCIENCE↗

Catalytic Removal of Oxygen and Pollutants in Exhaust Gases from Pressurized Oxy-Combustors

The primary goal of this project was to develop and validate advanced catalytic materials and systems for purifying the flue gas generated from pressurized oxy-combustors in an effort to achieve the purity specifications of carbon dioxide (CO 2 ) streams required by the U.S. Department of Energy (USDOE) for application in enhanced oil recovery. The technology has shown great potential for improving energy efficiency, simplifying process complexity, and lowering costs compared with current state-of-the-art oxy-combustion flue gas purification technologies. Laboratory studies were conducted for the development, characterization, and screening of metal catalysts for residual oxygen (O 2 ) reduction with methane (CH 4 ) and multifunctional carbon catalysts for combined nitrogen oxides (NO x ), sulfur oxides (SO x ), and mercury (Hg) removal. A bench-scale reverse-flow fixed-bed (RFFB) reactor and a trickle-bed direct-contact cooler (DCC) reactor capable of treating 15 standard liters per min of pressurized oxy-combustion flue gas were fabricated and tested with both a simulated flue gas in the laboratory and a slipstream of actual flue gas at a 100 kW th Staged, Pressurized Oxy-Combustion (SPOC) pilot facility. Process simulation and techno-economic studies were performed to evaluate the energy efficiency and cost of the developed catalytic flue gas purification process integrated into a conceptual 550-MWe SPOC power plant. The goal and objectives of the project have been successfully accomplished. A cobalt-manganese (CoMn) oxide catalyst was developed and demonstrated in the bench-scale RFFB reactor in either a reverse-flow or one-direction flow mode of operation that met the success criterion of performance for residual O 2 reduction. A carbon catalyst was developed and demonstrated in the bench-scale DCC reactor that met the success criterion of performance for combined NO x /SO x /Hg removal. Slipstream testing of the integrated DCC-RFFB system at the SPOC pilot facility demonstrated stable operation and verified the superior performance obtained in the laboratory. The techno-economic analysis showed that a 550-MWe SPOC plant integrated with the catalytic flue gas purification process would result in costs of electricity of $\$$96.94/MWh and $\$$80.27/MWh in two assessed cases compared with $\$$91.07/MWh reported for the USDOE’s Current Technology Case, which generated only a partially pure CO 2 stream. On the basis of the results and findings from this project, scale-up studies of materials production and system demonstration and optimization studies of reactors and processes are recommended at the next stage of technology development.

20 FOSSIL-FUELED POWER PLANTS↗

Observation of Weyl fermions in a magnetic non-centrosymmetric crystal

The absence of inversion symmetry in non-centrosymmetric materials has a fundamental role in the emergence of a vast number of fascinating phenomena, like ferroelectricity, second harmonic generation, and Weyl fermions. The removal of time-reversal symmetry in such systems further extends the variety of observable magneto-electric and topological effects. Here we report the striking topological properties in the non-centrosymmetric spin-orbit magnet PrAlGe by combining spectroscopy and transport measurements. By photoemission spectroscopy below the Curie temperature, we observe topological Fermi arcs that correspond to projected topological charges of ±1 in the surface Brillouin zone. In the bulk, we observe the linear energy-dispersion of the Weyl fermions. We further observe a large anomalous Hall response in our magneto-transport measurements, which is understood to arise from diverging bulk Berry curvature fields associated with the Weyl band structure. These results establish a novel Weyl semimetal phase in magnetic non-centrosymmetric PrAlGe.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗