scholarly journals Atmospheric-Pressure Cold Plasma Activating Au/P25 for CO Oxidation: Effect of Working Gas

Nanomaterials ◽  
2018 ◽  
Vol 8 (9) ◽  
pp. 742 ◽  
Author(s):  
Jingsen Zhang ◽  
Lanbo Di ◽  
Feng Yu ◽  
Dongzhi Duan ◽  
Xiuling Zhang

Commercial TiO2 (P25) supported gold (Au/P25) attracts increasing attention. In this work, atmospheric-pressure (AP) cold plasma was employed to activate the Au/P25-As catalyst prepared by a modified impregnation method. The influence of cold plasma working gas (oxygen, argon, hydrogen, and air) on the structure and performance of the obtained Au/P25 catalysts was investigated. X-ray diffraction (XRD), UV-Vis diffuse reflectance spectroscopy (DRS), transmission electron microscopy (TEM), and X-ray spectroscopy (XPS) were adopted to characterize the Au/P25 catalysts. CO oxidation was used as model reaction probe to test the Au/P25 catalyst. XRD results reveal that supporting gold and AP cold plasma activation have little effect on the P25 support. CO oxidation activity over the Au/P25 catalysts follows the order: Au/P25-O2P > Au/P25-As > Au/P25-ArP ≈ Au/P25-H2P > Au/P25-AirP. Au/P25-AirP presents the poorest CO oxidation catalytic activity among the Au/P25 catalysts, which may be ascribed to the larger size of gold nanoparticles, low concentration of active [O]s, as well as the poisoning [NOx]s. The poor catalytic performance of Au/P25-ArP and Au/P25-H2P is ascribed to the lower concentration of [O]s species. 100% CO conversion temperatures for Au/P25-O2P is 40 °C, which is 30 °C lower than that over the as-prepared Au/P25-As catalyst. The excellent CO oxidation activity over Au/P25-O2P is mainly attributed to the efficient decomposition of gold precursor species, small size of gold nanoparticles, and the high concentration of [O]s species.

Catalysts ◽  
2020 ◽  
Vol 10 (8) ◽  
pp. 907
Author(s):  
Hongyang Wang ◽  
Tengda Zhang ◽  
Yufa Zhou ◽  
Xiuling Zhang ◽  
Lanbo Di

Atmospheric pressure cold plasma is an environmentally friendly and novel method to synthesize supported metal catalysts, which usually uses active hydrogen species to reduce metal ions. Ethanol is a hydrogen-rich renewable liquid hydrogen source, and it is more convenient to store and transport than H2. In this study, a “storage-discharge” ethanol cold plasma was used to prepare Pd/Al2O3-EP catalysts, and the obtained catalysts are used for CO oxidation. The complete oxidation of CO temperature (T100) over Pd/Al2O3-EP was 145 °C, which was comparable to the performance of Pd/Al2O3-HP that was synthesized by atmospheric pressure hydrogen cold plasma. Pd/Al2O3-EP-C obtained by calcining Pd/Al2O3-EP at 450 °C for 2 h in air atmosphere in order to remove residual carbon species showed much higher CO oxidation activity, and T100 was 130 °C. The Pd/Al2O3 catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron diffraction (XPS), Brunauer–Emmett–Teller (BET), and transmission electron microscopy (TEM), and the structure-performance relationship was analyzed. The results indicate that the “storage-discharge” ethanol cold plasma can reduce the Pd precursor ions into metallic Pd state, and the dissociation of ethanol forms lots of highly active chemisorbed oxygen species, which can enhance the performance of Pd/Al2O3-EP for CO oxidation. In contrast, Pd/Al2O3-EP-C shows much higher CO oxidation activity, which is mainly attributed to the removal of the residual carbon species, and the exposure of more Pd active sites and chemisorbed oxygen species. The “storage-discharge” ethanol cold plasma is a safe and efficient novel method for synthesizing supported Pd catalysts, and it has important potential for the preparation and application of supported metal catalysts.


Nanomaterials ◽  
2019 ◽  
Vol 9 (10) ◽  
pp. 1437 ◽  
Author(s):  
Zhuang Li ◽  
Jingsen Zhang ◽  
Hongyang Wang ◽  
Zhihui Li ◽  
Xiuling Zhang ◽  
...  

Treatment with atmospheric-pressure (AP) hydrogen cold plasma is an effective method for preparing highly active supported metal catalytic materials. However, this technique typically uses H2 as working gas, which is explosive and difficult to transport. This study proposes the use of PdCl2 as a Pd precursor and activated carbon as the support to fabricate Pd/C catalytic materials (Pd/C-EP-Ar) by using ethanol—which is renewable, easily stored, and safe—combined with AP cold plasma (AP ethanol cold plasma) followed by calcination in Ar gas at 550 °C for 2 h. Both Pd/C-EP and Pd/C-HP fabricated using AP ethanol and hydrogen cold plasma (without calcination in Ar gas) respectively, exhibit low CO oxidation reactivity. The activity of Pd/C-EP is lower than Pd/C-HP, which is mainly ascribed to the carbon layer formed by ethanol decomposition during plasma treatment. However, the 100% CO conversion temperature (T100) of Pd/C-EP-Ar is 140 °C, which is similar to that of Pd/C-HP-Ar fabricated using AP hydrogen cold plasma (calcined in Ar gas at 550 °C for 2 h). The characterization results of X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy indicated that the carbon layer formed by ethanol decomposition enhanced the interaction of metal nanoparticles to the support, and a high Pd/C atomic ratio was obtained. This was beneficial to the high CO oxidation performance. This work provides a safe method for synthesizing high-performance Pd/C catalytic materials avoiding the use of H2, which is explosive and difficult to transport.


Nanomaterials ◽  
2019 ◽  
Vol 9 (8) ◽  
pp. 1118 ◽  
Author(s):  
Qiuwan Han ◽  
Dongyang Zhang ◽  
Jiuli Guo ◽  
Baolin Zhu ◽  
Weiping Huang ◽  
...  

The gold catalysts supported on various morphologies of α-Fe2O3 in carbon monoxide (CO) oxidation reaction have been studied for many researchers. However, how to improve the catalytic activity and thermal stability for CO oxidation is still important. In this work, an unusual morphology of α-Fe2O3 was prepared by hydrothermal method and gold nanoparticles were supported using a deposition-precipitation method. Au/α-Fe2O3 catalyst exhibited great activity for CO oxidation. The crystal structure and microstructure images of α-Fe2O3 were carried out by X-ray diffraction (XRD) and scanning electron microscopy (SEM) and the size of gold nanoparticles was determined by transmission electron microscopy (TEM). X-ray photoelectron spectra (XPS) and Fourier transform infrared spectra (FTIR) results confirmed that the state of gold was metallic. The 1.86% Au/α-Fe2O3 catalyst calcined at 300 °C had the best catalytic performance for CO oxidation reaction and the mechanism for CO oxidation reaction was also discussed. It is highly likely that the small size of gold nanoparticle, oxygen vacancies and active sites played the decisive roles in CO oxidation reaction.


2014 ◽  
Vol 955-959 ◽  
pp. 51-55
Author(s):  
Ting Ting Hu ◽  
Lin Hua Zhu

Gold catalysts supported on Na-MMT and Al-PILM noted as Au/Na-MMT and Au/Al-PILM respectively were prepared using Au(en)2Cl3 as precursor, and the catalytic oxidation activity for CO oxidation was investigated. The influence of different carriers on the conversion of CO was discussed. The phase of catalysts, the actual gold loading and the morphology of gold nanoparticles were characterized by X-ray diffraction(XRD), X-ray fluorescence analysis(XRF) and Transmission electron microscopy(TEM). The results showed that Au/Al-PILM exhibited higher catalytic activity for the oxidation reaction of CO, and 100% conversion of CO was achieved at reaction temperature of 250°C when gold precursor was loaded on the Al-PILM carrier at 60°Cand calcined it at 450°C for 1h.


Author(s):  
Parisa Sadeghpour ◽  
Mohammad Haghighi ◽  
Mehrdad Esmaeili

Aim and Objective: Effect of two different modification methods for introducing Ni into ZSM-5 framework was investigated under high temperature synthesis conditions. The nickel successfully introduced into the MFI structures at different crystallization conditions to enhance the physicochemical properties and catalytic performance. Materials and Methods: A series of impregnated Ni/ZSM-5 and isomorphous substituted NiZSM-5 nanostructure catalysts were prepared hydrothermally at different high temperatures and within short times. X-ray diffraction (XRD), Field emission scanning electron microscopy (FESEM), Energy dispersive X-ray (EDX), Brunner, Emmett and Teller-Barrett, Joyner and Halenda (BET-BJH), Fourier transform infrared (FTIR) and Temperature-programmed desorption of ammonia (TPDNH3) were applied to investigate the physicochemical properties. Results: Although all the catalysts showed pure silica MFI–type nanosheets and coffin-like morphology, using the isomorphous substitution for Ni incorporation into the ZSM-5 framework led to the formation of materials with lower crystallinity, higher pore volume and stronger acidity compared to using impregnation method. Moreover, it was found that raising the hydrothermal temperature increased the crystallinity and enhanced more uniform incorporation of Ni atoms in the crystalline structure of catalysts. TPD-NH3 analysis demonstrated that high crystallization temperature and short crystallization time of NiZSM-5(350-0.5) resulted in fewer weak acid sites and medium acid strength. The MTO catalytic performance was tested in a fixed bed reactor at 460ºC and GHSV=10500 cm3 /gcat.h. A slightly different reaction pathway was proposed for the production of light olefins over impregnated Ni/ZSM-5 catalysts based on the role of NiO species. The enhanced methanol conversion for isomorphous substituted NiZSM-5 catalysts could be related to the most accessible active sites located inside the pores. Conclusion: The impregnated Ni/ZSM-5 catalyst prepared at low hydrothermal temperature showed the best catalytic performance, while the isomorphous substituted NiZSM-5 prepared at high temperature was found to be the active molecular sieve regarding the stability performance.


2013 ◽  
Vol 832 ◽  
pp. 15-20 ◽  
Author(s):  
Sara Faiz Hanna Tasfy ◽  
Noor Asmawati Mohd Zabidi ◽  
Duvvuri Subbarao

Iron-based nanocatalyst was prepared via impregnation method on SiO2 support. The effects of promoters, namely, K and Cu, on the physical properties and catalytic performance in FTS have been investigated. The FTS performance of the synthesized nanocatalysts was examined in a fixed-bed microreactor at temperature of 523K, atmospheric pressure, 1.5 reactant ratio (H2/CO) and space velocity of 3L/g-cat.h. In FTS reaction, Cu promoter resulted in a lower CO conversion and C5+ hydrocarbons selectivity but higher selectivity to the lighter hydrocarbons (C1-C4) comparedto those obtained using the K promoter. Higher CO conversion (28.9%) and C5+ hydrocarbons selectivity (54.4%) were obtained using K as a promoter compared to that of Cu promoter. However, the K-promoted nanocatalyst resulted in a lower CO conversion but higher selectivity of the heavy hydrocarbons (C5+) compared to those obtained using the un-promoted nanocatalyst.


Catalysts ◽  
2018 ◽  
Vol 8 (11) ◽  
pp. 541 ◽  
Author(s):  
Haiping Xiao ◽  
Chaozong Dou ◽  
Hao Shi ◽  
Jinlin Ge ◽  
Li Cai

A series of poisoned catalysts with various forms and contents of sodium salts (Na2SO4 and Na2S2O7) were prepared using the wet impregnation method. The influence of sodium salts poisoned catalysts on SO2 oxidation and NO reduction was investigated. The chemical and physical features of the catalysts were characterized via NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), and Fourier Transform Infrared Spectroscopy (FT-IR). The results showed that sodium salts poisoned catalysts led to a decrease in the denitration efficiency. The 3.6% Na2SO4 poisoned catalyst was the most severely deactivated with denitration efficiency of only 50.97% at 350 °C. The introduction of SO42− and S2O72− created new Brønsted acid sites, which facilitated the adsorption of NH3 and NO reduction. The sodium salts poisoned catalysts significantly increased the conversion of SO2–SO3. 3.6%Na2S2O7 poisoned catalyst had the strongest effect on SO2 oxidation and the catalyst achieved a maximum SO2–SO3-conversion of 1.44% at 410 °C. Characterization results showed sodium salts poisoned catalysts consumed the active ingredient and lowered the V4+/V5+ ratio, which suppressed catalytic performance. However, they increased the content of chemically adsorbed oxygen and the strength of V5+=O bonds, which promoted SO2 oxidation.


Catalysts ◽  
2019 ◽  
Vol 9 (9) ◽  
pp. 724 ◽  
Author(s):  
Yan Cui ◽  
Leilei Xu ◽  
Mindong Chen ◽  
Chufei Lv ◽  
Xinbo Lian ◽  
...  

CuO-based catalysts are usually used for CO oxidation owing to their low cost and excellent catalytic activities. In this study, a series of metal oxide (La2O3, Fe2O3, PrO2, Sm2O3, and MnO2)-doped CuO-based catalysts with mesoporous Ce0.8Zr0.2O2 support were simply prepared by the incipient impregnation method and used directly as catalysts for CO catalytic oxidation. These mesoporous catalysts were systematically characterized by X-ray powder diffraction (XRD), N2 physisorption, transmission electron microscopy (TEM), energy-dispersed spectroscopy (EDS) mapping, X-ray photoelectron spectroscopy (XPS), and H2 temperature programmed reduction (H2-TPR). It was found that the CuO and the dopants were highly dispersed among the mesoporous framework via the incipient impregnation method, and the strong metal framework interaction had been formed. The effects of the types of the dopants and the loading amounts of the dopants on the low-temperature catalytic performances were carefully studied. It was concluded that doped transition metal oxides could regulate the oxygen mobility and reduction ability of catalysts, further improving the catalytic activity. It was also found that the high dispersion of rare earth metal oxides (PrO2, Sm2O3) was able to prevent the thermal sintering and aggregation of CuO-based catalysts during the process of calcination. In addition, their presence also evidently improved the reducibility and significantly reduced the particle size of the CuO active sites for CO oxidation. The results demonstrated that the 15CuO-3Fe2O3/M-Ce80Zr20 catalyst with 3 wt. % of Fe2O3 showed the best low-temperature catalytic activity toward CO oxidation. Overall, the present Fe2O3-doped CuO-based catalysts with mesoporous nanocrystalline Ce0.8Zr0.2O2 solid solution as support were considered a promising series of catalysts for low-temperature CO oxidation.


2019 ◽  
Vol 79 (9) ◽  
pp. 1675-1684 ◽  
Author(s):  
Guang Xian ◽  
Nan Zhang ◽  
Guangming Zhang ◽  
Yi Zhang ◽  
Zhiguo Zou

Abstract FeNiCeOx was firstly prepared by ultrasonic impregnation method and used to remove diclofenac in a Fenton-like system. The catalytic activity was improved successfully by doping Ni into FeCeOx. The diclofenac removal efficiency reached 97.9% after 30 min reaction. The surface morphology and properties of FeNiCeOx were characterized by Brunauer-Emmett-Teller (BET), scanning electron microscopy (SEM), X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), Raman and X-ray photoelectron spectroscopy (XPS) analyses. FeNiCeOx in this paper had larger specific surface area than those prepared by other methods, which was attributed to the cavitation effect and hot-spot effect during the ultrasonic synthesis process. Low crystallinity of Fe2O3 and NiO showed by characterization could lead to high interaction of Fe and Ni ions with support of CeO2. They substituted Ce in CeO2, caused lattice contraction and formed more oxygen vacancies, which favoured the catalytic reaction. Meanwhile, Fe and Ce ions both had redox cycles of Fe3+/Fe2+ and Ce4+/Ce3+, which facilitated the electron transfer in the reaction. The synergistic effect among Fe, Ni and Ce might lead to better catalytic performance of FeNiCeOx than any binary metal oxides constituted from the above three elements. Finally, the potential mechanism of diclofenac removal in FeNiCeOx-H2O2 system is proposed.


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