Pretreatment of Cylindrical Coconut Activated Carbon and Performance as Catalyst Support

Cylindrical coconut activated carbon（CCAC） support was graphitized at a high temperature（1900 ℃） in argon, then oxidized with an O2-N2-H2O mixture, and treated with nitric acid. Pretreatment of carbon support on its mechanical strength, physical structure, chemical composition and surface properties of cylindrical CCAC support was investigated by X-ray diffraction（XRD）, surface area analysis, scanning electron microscopy（SEM）, energy dis- persive spectroscopy（EDS）, thermogravimetric-differential thermogravimetric（TG-DTG） analysis and temperature programmed desorption-mass spectrometry（TPD-MS）, and the effect of CCAC support on the catalytic activities was also studied. The results show that the degree of graphitization, the purity（phosphorus, sulphur）, pore struc- ture（micropore, mesopore） and oxygen-containing functional groups（--COOH, --OH, --COOR） of carbon supports are obviously different, which have a great influence on the performance of Ru-based catalysts. After a series of pre- treatments, the surface physical and chemical properties of the commercial CCAC are modified and improved, and the activity of as-prepared Ru/AC catalyst is increased significantly.

Mechanism of coconut husk activated carbon modified by Mn(NO3)2

To study the mechanism by which activated carbon is modified by HNO3 and Mn(NO3)2,the pore texture and surface chemical characteristics of carbon materials in coconut husk activated carbon(AC)were examined via scanning electron microscopy(SEM),Brunauer-Emmett-Teller(BET),X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FTIR),and X-ray photoelectron spectroscopy(XPS).After being modified by HNO3,the millipore character of AC became deformed,and the character of the adjacent pores remained consolidated.The surface manganites of Mn/AC-1 presented as block and reticular fiber structures,Mn/AC-2's surface manganites presented as petty mammock crystals,and Mn/AC-3's surface manganites were observed as gauze nanosheets that interlace to fill in the pore canal.Nitric acid modification was shown to enlarge surface pores but decrease the specific surface area of AC.Mn loading can be used to construct a new pore structure that,in turn,increased the total specific surface area as well as the specific surface area and the volume of the millipores.Mn/AC-2's pore structure was optimized at a calcination temperature of 500℃and a loading quantity of 5%.The ash content of AC was considerably reduced after modified by HNO3.The active materials for Mn/AC-1 mainly consisted of Mn3O4,with a few Mn2O3 crystals,whereas Mn/AC-2's materials were mainly Mn3O4 and some MnO crystals.Mn/AC-3 was exclusively composed of Mn3O4.HNO3 activation and Mn loading modification did not considerably affect the functional group species present on the catalyst.Modification conditions using the same loading quantities and higher calcination temperatures decreased the number of O—H and N—H bonds while conversely increasing the number of CC and C—O bonds.On the contrary,the use of a higher loading quantity while maintaining the same calcination temperature increased the number of O—H and N—H bonds.A higher loading quantity is beneficial for increasing Mn^4+species.A higher calcination temperature is beneficial for increasing Mn^3+species.The results can optimize the conditions under which Mn/AC catalyst modification occurs,thus improving the physical and chemical properties of carbon-based sorbents.

Modification Mechanism of Coconut Husk Activated Carbon Using FeSO4 and Fe(NO3)3

Modification conditions determine the surface topography and the active material phase composition of a catalyst.To study the influence of modification on a carbon-based sorbent,coconut husk activated carbon(AC)which was activated using HNO3 and modified by FeSO4 and Fe(NO3)3 was examined.The pore textures and surface chemical characteristics of the carbon materials were examined by scanning electron microscopy(SEM),Brunner-Emmet-Teller(BET),X-ray diffraction(XRD)and Fourier transform infrared(FTIR)spectroscopy.The surface topography,the pore structure,active materials,and functional groups of AC,AC modificated by HNO3(HNO3/AC for short),and AC modificated by FeSO4 and Fe(NO3)3(Fe/AC for short)were systematically studied.Subsequently,the mechanism of modifying the conditions for the carbon materials was determined.Results showed that the surface micro topography of HNO3/AC became unsystematic and disordered.After modification with FeSO4,the ferriferous oxide was mainly present as a near-spherical crystal.Ferriferous oxides from Fe(NO3)3 modification mainly exhibited a plate shape.HNO3 modification could enlarge the pores but decrease the specific surface area of AC.FeSO4 modification resulted in a new net post structure in the pore canal of AC.Fe(NO3)3 modification caused the pore space structure to develop in the interior,and a higher calcination temperature was useful for ablation.The ash content of the AC was substantially reduced upon HNO3 modification.Upon FeSO4 modification,α-FeOOH,α-Fe2O3 andγ-Fe2O3 coexisted under the condition of a lower concentration of FeSO4 and a lower calcination temperature,and a higher FeSO4 concentration and calcination temperature generated moreα-Fe2O3.The same Fe(NO3)3 modification and a higher calcination temperature were beneficial to the minor chipping formation ofγ-Fe2O3.A higher Fe(NO3)3 loading produced a lower graphitization degree.HNO3 modification formed various new oxygen-containing functional groups and few nitrogen-containing groups.Based on the cover,FeSO4 and Fe(NO3)3 modification could decrease the oxygen-containing and nitrogen-containing functional groups.These results could optimize the modification condition and improve physical and chemical properties of carbon-based sorbents.

Low-Temperature Denitrification Performance of Cu2O/Activated Carbon Catalysts for Selective Catalytic Reduction of NOx by CO

To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstructure,the specific surface area,the pore volume,the crystal structure,and functional groups presented in the prepared Cu2O/AC catalysts were thoroughly characterized.By using scanning electron microscopy(SEM),nitrogen adsorption/desorption isotherms,Fourier-transform infrared(FTIR)spectroscopy and X-ray diffractometry(XRD),the effects of Cu2O loading and calcination temperature on Cu2O/AC catalysts were investigated at low temperature(150℃).The research shows that Cu on the Cu2O/AC catalyst is in the form of Cu2O with good crystalline performance and is spherical and uniformly dispersed on the AC surface.The loading of Cu2O increases the active sites and the specific surface area of the reaction gas contact,which is conducive to the rapid progress of the carbon monoxide selective catalytic reduction(CO-SCR)reaction.When the loading of Cu2O was 8%and the calcination temperature was 500℃,the removal rate of NOx facilitated by the Cu2O/AC catalyst reached 97.9%.These findings provide a theoretical basis for understanding the denitrification of sintering flue gas.

Low-temperature Denitration Mechanism of NH_(3)-SCR over Fe/AC Catalyst

To study the modification mechanism of activated carbon(AC)by Fe and the low-temperature NH_(3)-selective catalytic reduction(SCR)denitration mechanism of Fe/AC catalysts,Fe/AC catalysts were prepared using coconut shell AC activated by nitric acid as the support and iron oxide as the active component.The crystal structure,surface morphology,pore structure,functional groups and valence states of the active components of Fe/AC catalysts were characterised by X-ray diffraction,scanning electron microscopy,nitrogen adsorption and desorption,Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy,respectively.The effect of Fe loading and calcination temperature on the low-temperature denitration of NH_(3)-SCR over Fe/AC catalysts was studied using NH_(3)as the reducing gas at low temperature(150℃).The results show that the iron oxide on the Fe/AC catalyst is spherical and uniformly dispersed on the surface of AC,thereby improving the crystallisation performance and increasing the number of active sites and specific surface area on AC in contact with the reaction gas.Hence,a rapid NH_(3)-SCR reaction was realised.When the roasting temperature remains constant,the iron oxide crystals formed by increasing the amount of loading can enter the AC pore structure and accumulate to form more micropores.When the roasting temperature is raised from 400 to 500℃,the iron oxide is mainly transformed fromα-Fe_(2)O_(3)toγ-Fe_(2)O_(3),which improves the iron oxide dispersion and increases its denitration active site,allowing gas adsorption.When the Fe loading amount is 10%,and the roasting temperature is 500℃,the NO removal rate of the Fe/AC catalyst can reach 95%.According to the study,the low-temperature NH_(3)-SCR mechanism of Fe/AC catalyst is proposed,in which the redox reaction between Fe~(2+)and Fe~(3+)will facilitate the formation of reactive oxygen vacancies,which increases the amount of oxygen adsorption on the surface,especially the increase in surface acid sites,and promotes and adsorbs more reaction gases(NH_(3),O_(2),NO).The transformation from the standard SCR reaction to the fast SCR reaction is accelerated.

Physicochemical properties of coconut husk activated carbon modified by Fe(N0_(3))_(3)and Mn(N0_(3))_(2)

Fe-loaded activated carbon(AC)has high surface acidity and more active sites,while manganese-loaded AC has high oxygen content.Coconut husk AC modified by Fe-Mn was studied with the aim of revealing the modification mechanism.First,HNO_(3)AC was prepared using the nitric acid immersion method.Second,Fe-Mn/AC was prepared using the Fe(N0_(3))_(3)and Mn(N0_(3))_(2)sequential immersion.The effects of HNO_(3),Fe(N0_(3))_(3),and Mn(N0_(3))_(2)on the pore texture and surface chemical characteristics of carbon materials were examined by scanning electron microscopy,Brunauer-Emmett-Teller(BET)analysis,X-ray diffraction and Fourier-transform infrared spectroscopy.The surface topography,pore structure,active material,and functional groups of AC,HNO_(3)/AC,and Fe-Mn/AC were systematically studied.The following results were obtained.The surface of HNO_(3)AC has more ditches and air voids;the micropores of HNO_(3)AC are deformed and flattened compared to those of AC.The surface of Fe-Mn/AC exhibits an accumulation phenomenon.MnFe_(2)O_(4)and FeMn_(2)O_(4)formed more pore structures.AC and HNO_(3)AC have numerous micropores.The higher loading quantity of Fe-Mn results in bigger specific surface.The active components of Fe-Mn/AC-1,Fe-Mn/AC-2,Fe-Mn/AC-3,and Fe-Mn/AC-4 are MnFe_(2)O_(4),MnO_(0.43)Fe_(2.57)O_(4),Mn_(3)O_(4),and ot-Fe_(2)O_(3)>respectively.The surface functional groups of AC and HNO_(3)AC are oxygen-containing functional groups.The effect of Fe-Mn modifying conditions on functional group species is rare;however,Fe/AC has more oxygen-containing functional groups.These research findings can aid in the desulfurization and denitrification of the Fe-Mn/AC catalyst.