Modeling of Low-Temperature Reduction of Metal Oxide in Hydrogen Treatment System for Severe Accidents in Nuclear Power Plants

Author(s):  
Kotaro Nakamura ◽  
Masashi Tanabe ◽  
Satoru Abe ◽  
Takashi Mawatari ◽  
Takao Nakagaki

Abstract At the Fukushima Daiichi nuclear power plant, zirconium in the fuel rod cladding reacted with water vapor at elevated temperatures due to a loss of cooling water, resulting in the production of a large amount of hydrogen. This hydrogen leaked from the reactor vessel and accumulated in the top of reactor building, eventually leading to an explosion. A hydrogen treatment system that re-oxidizes hydrogen to water vapor is one of the effective methods to prevent such an explosion. A prominent re-oxidation method is via a fixed bed reactor packed with metal oxide pellets. The advantages of this method are its relatively fast oxidation rate without external oxygen/air injection. In this study, experiments and complementary numerical calculations were performed on the hydrogen re-oxidation reaction by metal oxides. The oxidation of hydrogen by copper oxide is modeled by 5 interacting, elementary reactions consisting of 6 chemical species. Experiments were performed using two packed bed set-ups, with measurement of inlet/outlet gas composition and pre/post-analysis of solid composition used to determine constants of the individual reaction rates for numerical calculations. From these reaction constants, the temporal behavior of the outlet gas was predicted.

2013 ◽  
Vol 726-731 ◽  
pp. 535-538
Author(s):  
Tian Cheng Liu ◽  
Yu Jiao Guo ◽  
Ping Ning ◽  
Guang Yang Tang ◽  
Ming Long Yuan

Catalytic hydrolysis decomposition of dichlorodifluoromethane (CCl2F2) in the presence of water vapor and oxygen was studied over solid acid MoO3/ZrO2 using a fixed-bed reactor. The CCl2F2 adsorption was multilayer chemical adsorption and its process was corresponding with Freundlich model. Its heat was from 56.3 to 73.2 KJ.mol-1, and it was exothermic reaction and chemical adsorption.


2013 ◽  
Vol 475-476 ◽  
pp. 1329-1333 ◽  
Author(s):  
Fen Li ◽  
Jin Wei ◽  
Ying Yang ◽  
Guang Hui Yang ◽  
Tao Lei

In this paper, an efficient metal oxide sorbents for the deep removal of H2S were synthesized using equal volume impregnation (EVIM) method. Modified coconut shell charcoal was selected as support to deposite the particles of copper oxide onto the surface. And copper nitrate were selected as the active component precursors in the preparation process of sorbents. Sorption experiments were carried out at room temperature in fixed-bed reactor. The grain size and crystal form of loading metals were characterized by X-ray diffraction (XRD). We investigated the effects of modifier onto coconut shell charcoal, load rate of metal oxide and calcination temperature on the desulfurization activity of the sorbent. Results show that the best modifier for coconut shell charcoal is KOH, which is significantly better than the other modifiers. And the optimum load rate is 20%(wt), the optimum calcination temperature is 300°C. Copper oxide onto the surface of modified coconut shell charcoal proved to be monoclinic nanoparticles with grain size of 18.7nm. Sulfidation test was carried out on the condition of i) the concentration of hydrogen sulfide gas (mixed with nitrogen ) is 1024.2ppm and ii) gas velocity is 20ml/min, iii) 0.1g sample in the middle of the fixed-bed reactor (length: 450 mm, interior diameter: 5 mm) to test. The sample show excellent sulfur removal efficiency and its breakthrough time is up to 287 min on this condition.


Holzforschung ◽  
2011 ◽  
Vol 65 (4) ◽  
Author(s):  
Christian Kirsch ◽  
Carsten Zetzl ◽  
Irina Smirnova

Abstract The limitations of the current biorefinery process utilizing stirred-tank reactors for the enzymatic step include poor mixing in the case of high biomass loadings, additional steps for the product separation, and a long reaction time. In this study the hydrothermal pretreatment and the enzymatic hydrolysis of the lignocellulosic biomass were combined in one fixed-bed reactor. The influence of the shear forces during recirculation and enzyme stability at elevated temperatures were investigated. It has been shown that the shear forces resulting from pumping have a negligible effect on enzyme activity. However, large pressure drops reduce the enzyme activity significantly. Furthermore, the enzyme stability was significantly increased at elevated temperatures (60°C) by applying static pressures up to 200 bar (56% residual activity at 60°C after 24 h). This is beneficial for the process as a higher temperature accelerates the reaction. Further improvement of the overall process efficiency was achieved by increasing the solid-to-water ratio and circulation of the enzyme solution. At a biomass content of 7%, a glucose concentration of 61 g l-1 and a yield of 85% was achieved. The integrated process was first done on a laboratory scale (50 ml). At 100 bar, 60°C and 10% biomass loading an increased initial reaction rate was observed. However, this effect was followed by the stagnation of the glucose yield as one of the enzymes, Novozyme 188, showed no remarkable stabilization with pressure. Nevertheless, an overall glucose yield of 40% was achieved after 5.5 h, compared to 14 h under normal pressure and 50°C.


Catalysts ◽  
2019 ◽  
Vol 9 (6) ◽  
pp. 518 ◽  
Author(s):  
Asunción Quintanilla ◽  
Jose L. Diaz de Tuesta ◽  
Cristina Figueruelo ◽  
Macarena Munoz ◽  
Jose A. Casas

The deposition of condensation by-products onto the catalyst surface upon wet peroxide and wet air oxidation processes has usually been associated with catalyst deactivation. However, in Part I of this paper, it was demonstrated that these carbonaceous deposits actually act as catalytic promoters in the oxygen-assisted wet peroxide oxidation (WPO-O2) of phenol. Herein, the intrinsic activity, nature and stability of these species have been investigated. To achieve this goal, an up-flow fixed bed reactor packed with porous Al2O3 spheres was used to facilitate the deposition of the condensation by-products formed in the liquid phase. It was demonstrated that the condensation by-products catalyzed the decomposition of H2O2 and a higher amount of these species leads to a higher degree of oxidation degree The reaction rates, conversion values and intermediates’ distribution were analyzed. The characterization of the carbonaceous deposits on the Al2O3 spheres showed a significant amount of condensation by-products (~6 wt.%) after 650 h of time on stream. They are of aromatic nature and present oxygen functional groups consisting of quinones, phenols, aldehydes, carboxylics and ketones. The initial phenol concentration and H2O2 dose were found to be crucial variables for the generation and consumption of such species, respectively.


Processes ◽  
2021 ◽  
Vol 9 (12) ◽  
pp. 2156
Author(s):  
Young Ku ◽  
Chia-Wei Chang ◽  
Shr-Han Shiu ◽  
Hsuan-Chih Wu ◽  
Niels Michiel Moed

Chemical looping with oxygen uncoupling (CLOU) is an innovative alternative to conventional combustion. CuO/ZrO2 oxygen carriers were tested in this system for their effectiveness and resilience. Cupric oxide (CuO) was demonstrated to be a reliable oxygen carrier for oxygen-uncoupling with consistent recyclability even after 50 redox cycles in a thermogravimetric analyzer (TGA). The reduction of CuO to generate Cu2O and oxygen was observed to be improved markedly for experiments operated at higher temperatures; however, the oxidation of Cu2O by air to generate CuO was hindered for experiments carried out at elevated temperatures. The reduction rate of fabricated CuO/ZrO2 particles containing 40% CuO was enhanced with increasing temperature and decreased with increasing particle size for experiments operated in a fixed bed reactor. The geometrical contraction and Avrami-Erofe’ev models were demonstrated to be appropriate for describing the reduction and oxidation of CuO/ZrO2, respectively. The activation energies for the reduction and oxidation were determined to be 250.6 kJ/mol and 57.6 kJ/mol, respectively, based on experimental results in the temperature range between 850 and 1000 °C.


1997 ◽  
Vol 35 (4) ◽  
pp. 149-156 ◽  
Author(s):  
H. Freudenhammer ◽  
D. Bahnemann ◽  
L. Bousselmi ◽  
S.-U. Geissen ◽  
A. Ghrabi ◽  
...  

An introduction to a joint research project is given which deals with the technical application of solar photocatalysis for wastewater detoxification. A non-concentrating thin-film fixed-bed reactor (TFFBR) is used to study applications and areas where a solar-catalytic treatment or recycling of wastewater is possible. This reactor excels by its low cost and an easy-to-build construction using molecular oxygen in air as the oxidising agent. The design parameters of the reactor as well as the process itself have been determined from the reaction kinetics of a model substance, the hydrodynamics and the mass transfer. The treatment of different real wastewaters was successfully carried out, and biologically pre-treated textile wastewater maximum solar degradation rate was about 3 g COD h−1 m−2. A comparison of reaction rates with artifical and solar illumination shows the necessity of outdoor experiments. Due to the reaction rates observed, photocatalysis is suitable as the final stage of purification of biologically or physically pretreated wastewater and will offer a great opportunity for sunrich areas.


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