An experimental study of the effect of ionic liquids on the low temperature oxidation of coal

Fourier transform infrared spectroscopy(FTIR) and constant heating rate experiments were performed to study the low temperature oxidation of coal treated by an ionic liquid,1-allyl-3-methylimidazolium chloride.The inerting effect of the ionic liquid toward the low temperature oxidation process is discussed.The results show that:(1) The hydroxyl content associated with hydrogen bonds,the aliphatic methyl content,the methylene group content,and the ether oxygen bond content are reduced in the treated coal.At the same time the content of aromatic C@C bonds is constant but these chemical bonds weaken and some substituted aromatic hydrocarbon content increases while other types decrease.This demonstrates that(AMIm)Cl dissolves and destroys the coal surface microstructure;(2) The oxygen consumption of the treated coal is less than what is seen in raw coal.The CO,CO 2,C 2 H 4,and C 2 H 6 content from the treated coal is reduced compared to the untreated coal;(3) The apparent activation energy for the oxidizing reaction is different in the treated and raw coals.Micro-structural changes and macroscopic gas production allow us to conclude that(AMIm)Cl can effectively inhibit low temperature oxidation of coal.

Calculation of Apparent Activation Energy of Coal Oxidation at Low Temperatures by Measuring CO Yield

By analyzing previous studies on activation energy of coal oxidation at low temperatures, a theoretical calculation model of apparent activation energy is established. Yield of CO is measured by using the characteristic detector of coal oxidation at 30-90 ℃. The impact of parameters, such as airflow and particle size, on activation energies is analyzed. Finally, agreement was obtained between activation energies and the dynamic oxygen absorbed in order to test the accuracy of the model. The results show that： 1） a positive exponential relation between concentration of CO and temperature in the process of the experiment is obtained： increases are almost identical and the initial CO is low; 2） the apparent activation energies increase gradually with the sizes of particle at the same airflow, but the gradients increase at a decreasing rate; 3） the apparent activation energies increase linearly with airflow. For the five coal particles, the differences among the energies are relatively high when the airflow was low, but the differences were low when the airflow was high; 4） the optimum sizes of particle, 0.125-0.25 ram, and the optimum volume of airflow, 100 mL/min, are determined from the model; 5） the apparent activation energies decrease with an increase in oxygen absorbed. A negative exponential relation between the two is obtained,

Synthesis of Pd nanoparticles supported on CeO_2 nanotubes for CO oxidation at low temperatures

Developing efficient supported Pd catalysts and understanding their catalytic mechanism in CO oxidation are challenging research topics in recent years.This paper describes the synthesis of Pd nanoparticles supported on CeO2 nanotubes via an alcohol reduction method.The effect of the support morphology on the catalytic reaction was explored.Subsequently,the performance of the prepared catalysts was investigated toward CO oxidation reaction and characterized by Nitrogen sorption,X-ray diffraction,X-ray photoelectron spectroscopy,transmission electron microscopy,and CO-temperature-programmed desorption techniques.The results indicated that the catalyst of Pd on CeO2 nanotubes exhibits excellent activity in CO oxidation at low temperatures,due to its large surface area,the high dispersion of Pd species,the mesoporous and tubular structure of the CeO2-nanotube support,the abundant Ce3＋,formation of Pd–O–Ce bonding,and enhanced metal–support interaction on the catalyst surface.

La-doped Pt/TiO_2 as an efficient catalyst for room temperature oxidation of low concentration HCHO

Catalytic oxidation of formaldehyde (HCHO) is the most efficient way to purify indoor air of HCHO pollutant. This work investigated rare earth La‐doped Pt/TiO2 for low concentration HCHO oxidation at room temperature. La‐doped Pt/TiO2 had a dramatically promoted catalytic performance for HCHO oxidation. The reasons for the La promotion effect were investigated by N2 adsorption, X‐raydiffraction, CO chemisorption, X‐ray photoelectron spectroscopy, transmission electron microscopy(TEM) and high‐angle annular dark field scanning TEM. The Pt nanoparticle size was reduced to 1.7nm from 2.2 nm after modification by La, which led to higher Pt dispersion, more exposed activesites and enhanced metal‐support interaction. Thus a superior activity for indoor low concentrationHCHO oxidation was obtained. Moreover, the La‐doped TiO2 can be wash‐coated on a cordieritemonolith so that very low amounts of Pt (0.01 wt%) can be used. The catalyst was evaluated in asimulated indoor HCHO elimination environment and displayed high purifying efficiency and stability.It can be potentially used as a commercial catalyst for indoor HCHO elimination.

Oxidation of CO on Nanometer Metal Oxides at Low Temperatures

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Preparation of Palladium Supported on Ferric Oxide Nano-catalysts for Carbon Monoxide Oxidation in Low Temperature

Catalytic property of Pd/Fe2O3 catalysts on carbon monoxide(CO) oxidation at low temperature were investigated in this paper. Both the as-prepared and H2-pretreated Pd/Fe2O3 catalysts show catalytic performances on CO oxidation. The CO was completely converted at 333 K for the as-prepared sample,whereas at 313 K for H2-pretreated Pd/Fe2O3-573 catalyst. The catalytic performance of the Pd/Fe2O3 catalyst decreases with increased calcination temperature. This may be due to the increased crystallinity of the support and decreased metal-support interaction. Progressive deactivation of the catalysts during long-time reaction was associated with the formation of carbonates on the catalyst surface that inhibits CO activation or intermediate transformation.

A Review on Complete Oxidation of Methane at Low Temperatures

This paper reviews recent developments in complete oxidation of methane atlow temperatures over noble metal catalysts in the past 20 years. The Pd/Al_2O_3 catalyst system isfully discussed. The review mainly focuses on the kinetic aspects of methane oxidation over thiscatalyst, and methane activation behavior over Pd and PdO phases (the form of PdO on the surface,transient behavior, the nature of the active sites, the influence of metal particle size and theirstructure sensitivities, and so on). Some Pd catalysts supported on other oxides besides the Al_2O_3support are briefly discussed. Possible routes of non-noble metal catalysts as substitutes for thePd catalyst are also proposed.

Mechanism of oxidation of low rank coal by nitric acid

The pretreatment of low rank coal with nitric acid oxidation can promote its bio-liquefaction. However, the detailed mechanism of which remains an unresolved problem. In the present work, the characteristics of Fushun coal before and after oxidation by nitric acid were investigated combined with elemental composition, pore volume and pore size, Zeta potential, FT-IR, and 13C solid NMR spectrum analysis. The results show that the inorganic substance inlaid in coal are dissolved by ni- tric acid, which results in the decrease of coal ash content and increase of pore volume and pore size. Furthermore, there exist obvious chemical reactions between nitric acid and the functional groups of coal including aromatic ring carboxylation, side chain alkyl of aromatic ring oxidation and aromatic ring nitration. Among these reactions, some led to the increase in content of carboxyl, aliphatic carbon connected with O and humic acid carbon, while others caused the reduction of aromaticity, methyl carbon, substituted aryl carbon and side chain.

A comparative study of CuO/TiO_2-SnO_2,CuO/TiO_2 and CuO/SnO_2 catalysts for low-temperature CO oxidation

Nanometer SnO2 particles were synthesized by sol-gel dialytic processes and used as a support to prepare CuO supported catalysts via a deposition-precipitation method. The samples were characterized by means of TG-DTA, XRD, H2-TPR and XPS. The catalytic activity of the CuO/TiO2-SnO2 catalysts was markedly depended on the loading of CuO, and the optimum CuO loading was 8 wt.% （Tloo = 80 ℃）. The CuO/TiO2-SnO2 catalysts exhibited much higher catalytic activity than the CuO/TiO2 and CuO/SnO2 catalysts. H2-TPR result indicated that a large amount of CuO formed the active site for CO oxidation in 8 wt.% CuO/TiO2-SnO2 catalyst.

Low-temperature oxidation behavior of MoSi_2 powders

The oxidation behavior of molybdenum disilicide （MoSi2） powders at 400, 500, and 600℃ for 12 h in air were investigated by using X-ray diffraction （XRD） and transmission electron microscopic （TEM） techniques. Significant changes were observed in volume, mass, and color. Especially at 500℃, the volume expansion was found to be as high as 7-8 times, the color changed from black to yellow-white, and the mass gain was about 169.34% after 8 h, with SiO2 and MoO3 as main reaction products. The gains in volume and mass were less at 400 and 600℃ compared with those at 500℃, probably due to the less reaction rate at 400℃ and the formation of silica glass scale at 600℃, which would protect the matrix and restrain the diffusion of oxygen and molybdenum. Thus, the accelerated oxidation behavior of MoSi2 powder appeared at 500℃ and the volume expansion was the sign of accelerated oxidation.

In situ catalytic upgrading of heavy crude oil through low-temperature oxidation

The low-temperature catalytic oxidation of heavy crude oil（Xinjiang Oilfield,China） was studied using three types of catalysts including oil-soluble,watersoluble,and dispersed catalysts.According to primary screening,oil-soluble catalysts,copper naphthenate and manganese naphthenate,are more attractive,and were selected to further investigate their catalytic performance in in situ upgrading of heavy oil.The heavy oil compositions and molecular structures were characterized by column chromatography,elemental analysis,and Fourier transform infrared spectrometry before and after reaction.An Arrhenius kinetics model was introduced to calculate the rheological activation energy of heavy oil from the viscosity-temperature characteristics.Results show that the two oil-soluble catalysts can crack part of heavy components into light components,decrease the heteroatom content,and achieve the transition of reaction mode from oxygen addition to bond scission.The calculated rheological activation energy of heavy oil from the fitted Arrhenius model is consistent with physical properties of heavy oil（oil viscosity and contents of heavy fractions）.It is found that the temperature,oil composition,and internal molecular structures are the main factors affecting its flow ability.Oil-soluble catalyst-assisted air injection or air huff-n-puff injection is a promising in situ catalytic upgrading method for improving heavy oil recovery.

Study on Fractional Separation and GC-MS Analysis of Flash Coal Tar Pyrolysed at Low Temperatures

The composition of low temperature pyrolysis coal tar has an effect on its further processing and reasomble utlization In this paper, the compeition or coal tars produced from both low temperature pyroysis in a fluidized bed aud flash pyrolysis with solid heat carrier have been investigated by the methch of fractional seperation and Gas Chromatography-Mass Spectrometry (GC-MS)- It is observed that the degree of coalification maceral and secondary reaction temperature (freeboard temperature in a fluidized bed) have some iufluence on the composition of coal tars- The main compoundes are phenol cresols,xylenols, naphthalene, alkylnaphthalenes, antbraceue, phenanthrene,acenaphthylene, fluoren, indene and so

Single atom gold catalysts for low-temperature CO oxidation

Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The active sites are traditionally believed to be Au nanoclusters or nanoparticles in the size range of 0.5–5 nm. Only in the last few years have single‐atom Au catalysts been proved to be active for CO oxidation. Recent advances in both experimental and theoretical studies on single‐atom Au catalysts unambiguously demonstrated that when dispersed on suitable oxide supports the Au single atoms can be extremely active for CO oxidation. In this mini‐review, recent advances in the development of Au single‐atom catalysts are discussed, with the aim of illus‐trating their unique catalytic features during CO oxidation.

Oxidation Degradation of Aqueous Carbofuran Induced by Low Temperature Plasma

The oxidative degradation of aqueous carbofuran, a heavily used toxic carbamate insecticide by low temperature plasma, was investigated. The results show that the treatment efficiency increases with the increase in initial concentration. Raising the treatment temperature and changing the pH value can result in enhanced degradation of carbofuran in solution. The results also show that low temperature plasma treatment can effectively remove chemical oxygen demand （COD） of carbofuran in the solution.

Recent progress in CO oxidation over Pt-group-metal catalysts at low temperatures

CO oxidation is probably the most studied reaction in heterogeneous catalysis.This reaction has become a hot topic with the discovery of nanogold catalysts,which are active at low temperatures（at or below room temperature）.Au catalysts are the benchmark for judging the activities of other metals in CO oxidation.Pt-group metals（PGMs） that give comparable performances are of particular interest.In this mini-review,we summarize the advances in various PGM（Pt,Pd,Ir,Rh,Ru）catalysts that have high catalytic activities in low-temperature CO oxidation arising from reducible supports or the presence of OH species.The effects of the size of the metal species and the importance of the interface between the metal and the reducible support are covered and discussed in terms of their promotional role in CO oxidation at low temperatures.

Separation and analysis of six fractions in low temperature coal tar by column chromatography

The low temperature coal tar(CT)is taken as the raw material,and the extraction and column chromatography are used for detailed and accurate characterization in this paper.The n-heptane soluble fraction(CT-HS)and insoluble fraction(CT-HI)were obtained by n-heptane Soxhlet extraction.The extraction rate of CT-HS reached 92.79%(mass),which indicated that there are few heavy compounds in it.Further,different solvents(methylbenzene,benzene,ethyl acetate,methylbenzene-ethanol)were used to elute CT-HS by chromatographic column to obtain five fractions(saturates,aromatics,heteroatoms,phenolics and resins,named CT-SA,CT-AR,CT-HE,CT-PH,CT-RE,respectively).The yields of CTSA,CT-AR,CT-HE,CT-PH,CT-RE are 42.12%,10.43%,2.19%,9.50%and 6.63%(mass),respectively.Gas chromatography-mass spectrometry analysis of eluting components show that alkanes are the main components in CT,followed by polycyclic aromatics,and the corresponding fractions are CT-SA and CT-AR,respectively.The relative content of aliphatics in CT-SA is 76.93%,and the relative content of aromatics in CT-AR is 75.05%.This separation technology effectively separates and enriches different components in CT,and the activation energy required for the pyrolysis process of a single eluting fraction is lower than that of CT,which is expected to provide an important reference for the separation,analysis and conversion of complex oil products such as coal-oil co-processing products,coal tar and other complex heavy carbon oil products.

Conversions of fuel-N, volatile-N, and char-N to NO and N_2O during combustion of a single coal particle in O_2/N_2 and O_2/H_2O at low temperature

Oxy-steam combustion is a promising next-generation combustion technology.Conversions of fuel-N,volatile-N,and char-N to NO and N2O during combustion of a single coal particle in O2/N2and O2/H2O were studied in a tube reactor at low temperature.In O2/N2,NO reaches the maximum value in the devolatilization stage and N2O reaches the maximum value in the char combustion stage.In O2/H2O,both NO and N2O reach the maximum values in the char combustion stage.The total conversion ratios of fuel-N to NO and N2O in O2/N2are obviously higher than those in O2/H2O,due to the reduction of H2O on NO and N2O.Temperature changes the trade-off between NO and N2O.In O2/N2and O2/H2O,the conversion ratios of fuel-N,volatile-N,and char-N to NO increase with increasing temperature,and those to N2O show the opposite trends.The conversion ratios of fuel-N,volatile-N,and char-N to NO reach the maximum values at 〈O2〉=30 vol%in O2/N2.In O2/H2O,the conversion ratios of fuel-N and char-N to NO reach the maximum values at 〈O2〉=30 vol%,and the conversion ratio of volatile-N to NO shows a slightly increasing trend with increasing oxygen concentration.The conversion ratios of fuel-N,volatile-N,and char-N to N2O decrease with increasing oxygen concentration in both atmospheres.A higher coal rank has higher conversion ratios of fuel-N to NO and N2O.Anthracite coal exhibits the highest conversion ratios of fuel-N,volatile-N,and char-N to NO and N2O in both atmospheres.This work is to develop efficient ways to understand and control NO and N2O emissions for a clean and sustainable atmosphere.

Fabrication and Characterization of VO_2 Thin Films by Direct Current Facing Targets Magnetron Sputtering and Low Temperature Oxidation

Low valence vanadium oxide(VO2-x) thin films were prepared on SiO2/Si substrates at room temperature by direct current facing targets reactive magnetron sputtering, and then proc- essed through rapid thermal annealing. The effects of the annealing on the structure and phase transition property of VO2 were discussed. X-ray photoelectron spectroscopy, X-ray diffraction tech- nique and Fourier transform infrared spectroscopy were employed to study the phase composition and structure of the thin films. The resistance-temperature property was measured. The results show that VO2 thin film is obtained after annealed at 320 ℃ for 3 h, its phase transition tempera- ture is 56 ℃, and the resistance changes by more than 2 orders. The vanadium oxide thin films are applicable in thermochromic smart windows, and the deposition and annealing process is compatible with micro electromechanical system process.

Synthesis of a chabazite-supported copper catalyst with full mesopores for selective catalytic reduction of nitrogen oxides at low temperature

A series of meso‐microporous copper‐supporting chabazite molecular sieve（CuSAPO‐34） catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction（NH3‐SCR）have been synthesized via a one‐pot hydrothermal crystallization method. The physicochemical properties of the catalysts were characterized by scanning electron microscopy, transmission electron microscopy, N2 adsorption‐desorption measurements, X‐ray diffraction, 27 Al magic angle spinning nuclear magnetic resonance, diffuse reflectance ultraviolet‐visible spectroscopy, inductively coupled plasma‐atomic emission spectroscopy, X‐ray photoelectron spectroscopy, temperature‐programmed reduction measurements, and electron paramagnetic resonance analysis. The formation of micro‐mesopores in the Cu‐SAPO‐34 catalysts decreases diffusion resistance and greatly improves the accessibility of reactants to catalytic active sites. The main active sites for NH3‐SCR reaction are the isolated Cu^2＋ species displaced into the ellipsoidal cavity of the Cu‐SAPO‐34 catalysts.