scholarly journals Improvement of Methane Combustion Activity for Pd/ZrO2 Catalyst by Simple Reduction/Re-oxidation Treatment

Author(s):  
Chansong Kim ◽  
Eunpyo Hong ◽  
Chae-Ho Shin

The improvement of the methane combustion activity was observed in cyclic temperature-programmed and isothermal reactions over Pd/ZrO2 catalysts by simple reduction/re-oxidation treatment. The catalytic activity increased during the initial stages of isothermal reaction, and the light-off temperature was lowered as the number of cycles increased in the cyclic temperature-programmed reaction. To reveal the origin of activation, variations in the reduction properties after the activation period were carefully investigated through CH4 temperature-programmed reduction (TPR) measurements. From the CH4-TPR results, it was confirmed that the reduction temperature decreased significantly after activation. The observation of the CH4-TPR peak at relatively low temperatures is directly proportional to the catalytic activity of CH4 combustion. It was therefore concluded that repeated reduction/re-oxidation occurred in the reactant stream, and this phenomenon allowed the combustion reaction to proceed more easily at lower temperatures.

Catalysts ◽  
2019 ◽  
Vol 9 (10) ◽  
pp. 838 ◽  
Author(s):  
Chansong Kim ◽  
Eunpyo Hong ◽  
Chae-Ho Shin

The improvement of methane combustion activity was observed in cyclic temperature-programed and isothermal reactions over Pd/ZrO2 catalysts by simple reduction/reoxidation treatment. The catalytic activity increased during the initial stages of isothermal reaction, and the light-off temperature was lowered as the number of cycles increased in the cyclic temperature-programed reaction. To reveal the origin of activation, variations in the reduction properties after the activation period were carefully investigated through CH4 temperature-programed reduction (TPR) measurements. From the CH4-TPR results, it was confirmed that the reduction temperature decreased significantly after activation. The observation of the CH4-TPR peak at relatively low temperatures is directly proportional to the catalytic activity of CH4 combustion. It was therefore concluded that repeated reduction/reoxidation occurred in the reactant stream, and this phenomenon allowed the combustion reaction to proceed more easily at lower temperatures.


Catalysts ◽  
2021 ◽  
Vol 11 (7) ◽  
pp. 772
Author(s):  
Yanxiong Liu ◽  
Changhua Hu ◽  
Longchun Bian

The correlation between the occurrence state of surface Pd species of Pd/CeO2 for lean CH4 combustion is investigated. Herein, by using a reduction-deposition method, we have synthesized a highly active 0.5% PdO/CeO2-RE catalyst, in which the Pd nanoparticles are evenly dispersed on the CeO2 nanorods CeO2-R. Based on comprehensive characterization, we have revealed that the uniformly dispersed Pd nanoparticles with a particle size distribution of 2.3 ± 0.6 nm are responsible for the generation of PdO and PdxCe1−xO2−δ phase with –Pd2+–O2−–Ce4+– linkage, which can easily provide oxygen vacancies and facilitate the transfer of reactive oxygen species between the CeO2-R and Pd species. As a consequence, the remarkable catalytic activity of 0.5% Pd/CeO2-RE is related to the high concentration of PdO species on the surface of the catalyst and the synergistic interaction between the Pd species and the CeO2 nanorod.


2019 ◽  
Vol 10 ◽  
pp. 1391-1400 ◽  
Author(s):  
Machiko Takigami ◽  
Rieko Kobayashi ◽  
Takafumi Ishii ◽  
Yasuo Imashiro ◽  
Jun-ichi Ozaki

Carbon-based oxygen reduction reaction (ORR) catalysts are regarded as a promising candidate to replace the currently used Pt catalyst in polymer electrolyte fuel cells (PEFCs); however, the active sites remain under discussion. We predicted that warped graphitic layers (WGLs) are responsible for the ORR catalytic activity in some carbon catalysts (i.e., carbon alloy catalysts (CACs)). To prove our assumption, we needed to use WGLs consisting of carbon materials, but without any extrinsic catalytic elements, such as nitrogen, iron, or cobalt, which effectively enhance ORR activity. The present study employed a fullerene extraction residue as a starting material to construct WGLs. The oxidation of the material at 600 °C exposed the WGLs by removing the surrounding amorphous moieties. Transmission electron microscopy (TEM) observations revealed the formation of WGLs by oxidation treatment at 600 °C in an O2/N2 stream. Extending the oxidation time increased the purity of the WGL phase, but also simultaneously increased the concentration of oxygen-containing surface functional groups as monitored by temperature programmed desorption (TPD). The specific ORR activity increased with oxidation up to 1 h and then decreased with the intensive oxidation treatment. Correlations between the specific ORR activity and other parameters confirmed that the development of the WGL and the increase in the O/C ratio are the competing factors determining specific ORR activity. These results explain the maximum specific ORR activity after 1 h of oxidation time. WGLs were found to lower the heat of adsorption for O2 and to increase the occurrence of heterogeneous electron transfer.


1998 ◽  
Vol 45 (1-4) ◽  
pp. 173-178 ◽  
Author(s):  
Kohji Narui ◽  
Keiichi Furuta ◽  
Hirohide Yata ◽  
Akio Nishida ◽  
Yasuhiko Kohtoku ◽  
...  

2010 ◽  
Vol 96 ◽  
pp. 135-139
Author(s):  
Cai Rong Gong ◽  
Hai Feng Chen ◽  
Guo Liang Fan ◽  
Chong Lin Song ◽  
Gang Lv

A series of complex oxide Cu1-xKxFe2O4 fibers have been prepared via a sol-gel process related electron-spinning procedure, in which x is among 0, 0.05, 0.1 and 0.2 corresponding to the quantity of Cu2+ partial substitution by K+. The average diameter of the fiber was 500 nm. The catalytic activity of the catalysts in removal of NOx and carbon black from diesel exhaust gases were examined in detail using temperature-programmed reaction technique. The results show that after partial substitution of Cu2+ with K+, the catalytic activities have been improved. Cu0.95K0.05Fe2O4 as an optimal catalyst can significantly decrease the ignition temperature (Tig) of the PM, and has high catalytic activity on the removal of NOx.


2013 ◽  
Vol 634-638 ◽  
pp. 563-566
Author(s):  
Fu Chen Ding ◽  
Cui Tao Ren ◽  
Bin Li ◽  
Hong Wang ◽  
Cui Qing Li

The LaBO3/HZSM-5 samples were prepared by the impregnation method. The structure of catalysts was examined by XRD. The catalytic activity for the combustion of soot particulate was evaluated by a technique of the temperature-programmed reaction. In the LaBO3/HZSM-5 catalyst, the Mn as B-site ion, the catalyst was the good candidate catalyst for the soot catalytic combustion. In the LaMnO3/HZSM-5 catalyst, the catalytic activity was tunable by changing the metal components of the perovskite-type oxide at B-site, the Fe partial substitution for Mn of LaMnO3/HZSM-5 enhanced the catalytic activity, and the combustion temperature of soot particle was lower than LaMnO3/HZSM-5 sample without substitution, corresponding Tm of 401oC and the selectivity of CO2 77.0%.


Catalysts ◽  
2020 ◽  
Vol 10 (11) ◽  
pp. 1355
Author(s):  
Marek Lewandowski ◽  
Rafał Janus ◽  
Mariusz Wądrzyk ◽  
Agnieszka Szymańska-Kolasa ◽  
Céline Sayag ◽  
...  

The catalytic activity of bulk molybdenum carbide (Mo2C) in the hydrodenitrogenation (HDN) of indole was studied. The catalyst was synthesized using a temperature-programmed reaction of the respective oxide precursor (MoO3) with the carburizing gas mixture of 10 vol.\% CH4/H2. The resultant material was characterized using X-ray diffraction, CO chemisorption, and nitrogen adsorption. The catalytic activity was studied in the HDN of indole over a wide range of conversion thereof and in the presence of a low amount of sulfur (50 ppm), which was used to simulate the processing of real petroleum intermediates. The molybdenum carbide has shown high activity under the tested operating conditions. Apparently, the bulk molybdenum carbide turned out to be selective towards the formation of aromatic products such as ethylbenzene, toluene, and benzene. The main products of HDN were ethylbenzene and ethylcyclohexane. After 99% conversion of indole HDN was reached (i.e., lack of N-containing compounds in the products was observed), the hydrogenation of ethylbenzene to ethylcyclohexane took place. Thus, the catalytic behavior of bulk molybdenum carbide for the HDN of indole is completely different compared to previously studied sulfide-based systems.


2011 ◽  
Vol 364 ◽  
pp. 519-523 ◽  
Author(s):  
S. Sivasangar ◽  
Yun Hin Taufiq-Yap

Methane reforming is the most feasible techniques to produce hydrogen for commercial usage. Hence, dry reforming is the environment friendly method that uses green house gases such as CO2and methane to produce fuel gas. Catalysts play a vital role in methane conversion by enhancing the reforming process. In this study Ni/γ-Al2O3was selected as based catalyst and CeO2and Fe2O3dopants were added to investigate their effect on catalytic activity in dry reforming. The catalysts synthesized through wet impregnation method and characterized by using XRD, TEM and SEM-EDX. The catalytic tests were carried out using temperature programmed reaction (TPRn) and the products were detected by using an online mass spectrometer. The results revealed that these dopants significantly affect the catalytic activity and selectivity of the catalyst during reaction. Hence, Fe2O3doped catalyst shows higher hydrogen production with stable catalytic activity.


2011 ◽  
Vol 8 (s1) ◽  
pp. S349-S357 ◽  
Author(s):  
Mingxin Guo ◽  
Rongshu Zhu ◽  
Minhua Dong ◽  
Feng Ouyang

The behaviour of a series of Ir-based catalysts supported on SiO2, ZSM-5 and γ-Al2O3 with various Ir loadings prepared by impregnation method was conducted by temperature programmed reaction (TPR) technique. The result implies that NO is oxidized to NO2while simultaneously being reduced to N2or N2O in the NO reactions over iridium catalysts. The surface active phase over iridium catalysts that promote the NO reactions is IrO2. The catalytic activity increases with the increase of the Ir loading and support materials have a little effect on the catalytic activity. When the loading is less than 0.1%, the catalytic activity was found to be dependent on the nature of support materials and in order: Ir/ZSM-5>Ir/γ-Al2O3>Ir/SiO2. When the loading is higher than 0.1%, the catalytic activity for NO oxidation is in order: Ir/ZSM-5>Ir/SiO2>Ir/γ -Al2O3, which is correlated with Ir dispersion on the surface of support materials and the catalytic activity for NO reduction is in sequence: Ir/γ -Al2O3>Ir/SiO2>Ir/ZSM-5, which is attributed to the adsorbed-dissociation of NO2. Compared to Pt/γ-Al2O3, Ir/γ-Al2O3catalyst is more benefit for the NO reduction.


2021 ◽  
Author(s):  
Petar Djinović ◽  
Janez Zavašnik ◽  
Janvit Teržan ◽  
Ivan Jerman

AbstractCeO2, V2O5 and CeVO4 were synthesised as bulk oxides, or deposited over activated carbon, characterized by XRD, HRTEM, CO2-TPO, C3H8-TPR, DRIFTS and Raman techniques and tested in propane oxidative dehydrogenation using CO2. Complete oxidation of propane to CO and CO2 is favoured by lattice oxygen of CeO2. The temperature programmed experiments show the ~ 4 nm AC supported CeO2 crystallites become more susceptible to reduction by propane, but less prone to re-oxidation with CO2 compared to bulk CeO2. Catalytic activity of CeVO4/AC catalysts requires a 1–2 nm amorphous CeVO4 layer. During reaction, the amorphous CeVO4 layer crystallises and several atomic layers of carbon cover the CeVO4 surface, resulting in deactivation. During reaction, V2O5 is irreversibly reduced to V2O3. The lattice oxygen in bulk V2O5 favours catalytic activity and propene selectivity. Bulk V2O3 promotes only propane cracking with no propene selectivity. In VOx/AC materials, vanadium carbide is the catalytically active phase. Propane dehydrogenation over VC proceeds via chemisorbed oxygen species originating from the dissociated CO2. Graphic Abstract


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