Understanding the effects of electrode meso-macropore structure and solvent polarity on electric double layer capacitors based on a continuum model

The structures of electrode meso-macropore and the solvent polarity are the crucial factors dominating the performance of the electric double layer capacitors(EDLCs),but their impacts are usually tangled and difficult to decouple and quantitate.Here the effects of electrode meso-macropore structure and solvent polarity on the specific capacitance of an EDLC are quantitatively investigated using a steady-state continuum model.The simulation results indicate the specific capacitances are significantly affected by the meso-macropore surface structure.The specific capacitances significantly decrease for both convex surface structures but obviously increase for both concave surface structures,with the increase of curvature radius from 1 to 20 nm.As for solvents,the polar solvent with high saturated dielectric permittivity improves the capacitance performance.Moreover,the electrode meso-macropore structure is of more concern compared with solvent polarity when aiming at enhancing the specific capacitance.These results provide fundamentals for the rational design of porous electrodes and polar electrolytes for EDLCs.

Effect of internal structure of a batch-processing wet-etch reactor on fluid flow and heat transfer

Batch-processing wet-etch reactors are the key equipment widely used in chip fabrication,and their performance is largely affected by the internal structure.This work develops a three-dimensional computational fluid dynamics(CFD)model considering heat generation of wet-etching reactions to investigate the fluid flow and heat transfer in the wet-etch reactor.The backflow is observed below and above the wafer region,as the flow resistance in this region is high.The temperature on the upper part of a wafer is higher due to the accumulation of reaction heat,and the average temperature of the side wafer is highest as its convective heat transfer is weakest.Narrowing the gap between wafer and reactor wall can force the etchant to flow in the wafer region and then facilitate the convective heat transfer,leading to better within-wafer and wafer-to-wafer etch uniformities.An inlet angle of 60°balances fluid by-pass and mechanical energy loss,and it yields the best temperature and etch uniformities.The batch with 25wafers has much wider flow channels and much lower flow resistance compared with that with 50wafers,and thus it shows better temperature and etch uniformities.These results and the CFD model should serve to guide the optimal design of batch-processing wet-etch reactors.

Probing deactivation by coking in catalyst pellets for dry reforming of methane using a pore network model

Dry reforming of methane(DRM) is an attractive technology for utilizing the greenhouse gases(CO_(2) and CH_(4)) to produce syngas. However, the catalyst pellets for DRM are heavily plagued by deactivation by coking, which prevents this technology from commercialization. In this work, a pore network model is developed to probe the catalyst deactivation by coking in a Ni/Al_(2)O_(3) catalyst pellet for DRM. The reaction conditions can significantly change the coking rate and then affect the catalyst deactivation. The catalyst lifetime is higher under lower temperature, pressure, and CH_(4)/CO_(2) molar ratio, but the maximum coke content in a catalyst pellet is independent of these reaction conditions. The catalyst pellet with larger pore diameter, narrower pore size distribution and higher pore connectivity is more robust against catalyst deactivation by coking, as the pores in this pellet are more difficult to be plugged or inaccessible.The maximum coke content is also higher for narrower pore size distribution and higher pore connectivity, as the number of inaccessible pores is lower. Besides, the catalyst pellet radius only slightly affects the coke content, although the diffusion limitation increases with the pellet radius. These results should serve to guide the rational design of robust DRM catalyst pellets against deactivation by coking.

Explosion limits estimation and process optimization of direct propylene epoxidation with H2 and O2

Direct propylene epoxidation with H2 and O2,an attractive process to produce propylene oxide(PO),has a potential explosion danger due to the coexistence of flammable gases(i.e.,C3 H6 and H2)and oxidizer(i.e.,O2).The unknown explosion limits of the multi-component feed gas mixture make it difficult to optimize the reaction process under safe operation conditions.In this work,a distribution method is proposed and verified to be effective by comparing estimated and experimental explosion limits of more than 200 kinds of flammable gas mixture.Then,it is employed to estimate the explosion limits of the feed gas mixture,some results of which are also validated by the classic Le Chatelier’s Rule and flammable resistance method.Based on the estimated explosion limits,process optimization is carried out using commercially high and inherently safe reactant concentrations to enhance reaction performance.The promising results are directly obtained through the interface called gOPT in gPROMS only by using a simple,easy-constructed and mature packed-bed reactor,such as the PO yield of 13.3%,PO selectivity of 85.1%and outlet PO fraction of 1.8%.These results can be rationalized by indepth analyses and discussion about the effects of the decision variables on the operation safety and reaction performance.The insights revealed here could shed new light on the process development of the PO production based on the estimation of the explosion limits of the multi-component feed gas mixture containing flammable gase s,inert gas and O2,followed by process optimization.

Optimization of catalyst pellet structures and operation conditions for CO methanation

A fundamental understanding of the effects of catalyst pellet structures and operation conditions on catalytic performance is crucial for the reactions limited by diffusion mass transfer. In this work, a numerical investigation has been carried out to understand the effect of catalyst pellet shapes(sphere, cylinder, trilobe and tetralobe) on the reaction-diffusion behaviors of CO methanation. The results reveal that the poly-lobe pellets with larger external specific surface area have shorter diffusion path, and thus result in higher effectiveness factors and CO conversion rates in comparison with the spherical and cylindrical pellets. The effects of operating conditions and pore structures on the trilobular catalyst pellet with high performance are further probed. Though lower temperature can contribute to larger effectiveness factors of pellets, it also brings about lower reaction rates, and pressure has little impact on the effectiveness factors of the pellets. The increase in porosity can reduce the pellet internal diffusion limitations effectively and there exists an optimal porosity for the methanation reaction. Finally, the height of the trilobular pellet is optimized under the given geometric volume, and the results demonstrate that the higher the trilobular catalyst, the better the reaction performance within the allowable mechanical strength range.

Modeling of propane dehydrogenation combined with chemical looping combustion of hydrogen in a fixed bed reactor

A redox process combining propane dehydrogenation(PDH)with selective hydrogen combustion(SHC)is proposed,modeled,simulated,and optimized.In this process,PDH and SHC catalysts are physically mixed in a fixed-bed reactor,so that the two reactions proceed simultaneously.The redox process can be up to 177.0%higher in propylene yield than the conventional process where only PDH catalysts are packed in the reactor.The reason is twofold:firstly,SHC reaction consumes hydrogen and then shifts PDH reaction equilibrium towards propylene;secondly,SHC reaction provides much heat to drive the highly endothermic PDH reaction.Considering propylene yield,operating time,and other factors,the preferable operating conditions for the redox process are a feed temperature of 973 K,a feed pressure of 0.1 MPa,and a mole ratio of H_(2) to C_(3)H_(8) of 0.15,and the optimal mass fraction of PDH catalyst is 0.5.This work should provide some useful guidance for the development of redox processes for propane dehydrogenation.

Optimization of LiB electrode with bi-diameter active particles using a microstructure-resolved model

The microstructure of electrodes significantly affects the performance of lithium-ion batteries(LiBs),and using bi-diameter active particles is a simple but effective way to regulate the microstructure of commercial LiB electrodes.Herein,to optimize the LiB cathode of bi-diameter active particles,a microstructure-resolved model is developed and validated.The results indicate that randomly packing of bi-diameter active particles is optimal when the electrolyte diffusion limitation is mild,as it provides the highest volume fraction of active materials.Under strong electrolyte diffusion limitations,layered packing with small particles near the separator is preferred.This is because particles near the current collector have a low lithiation state.Besides,optimizing the random packing can further improve the energy density.For energy-oriented LiBs,a low volume fraction of small particles(0.2)is preferred due to the higher volume fraction of active materials.For power-oriented LiBs,a high volume fraction of small particles(0.8)is better because it reduces diffusion limitations.This work should serve to guide the optimal design of electrode microstructure for achieving high-performance LiBs.

Effects of particle shape and packing style on ethylene oxidation reaction using particle-resolved CFD simulation

Gaining in-depth insights into the effects of particle shapes and packing style on ethylene oxidation reaction is of paramount industrial importance.In this work,reactor models of five packing structures with different particle shapes and three packing structures with different packing styles are established by employing software Blender and COMSOL Multiphysics to explore how the reaction-diffusion behaviors affect ethylene oxidation process.The reliabilities of rigid body dynamics model and particle-resolved reactor model are verified by comparing simulated and experimental pressure drops and ethylene conversions.In all the five packing structures with laminar flow conditions,the high bed porosity and low total particle surface area for the trilobe packing structure give rise to the lowest pressure drop of 27.8 Pa/m,while the internal voids cutting mode provides the excellent heat transfer capacity for the Raschig ring packing structure and the highest ethylene conversion and thereby the highest bed temperature rise of 25.1 K for the four-hole cylinder packing structure.Based on these analyses,changing the packing style to the bottom-up Raschig ring-four hole cylinder packing structure would be a good strategy for the effectively lowered reactor temperature rise by 4.8 K together with the slightly reduced ethylene conversion.