A comparison between the effects of ordinary walnut shell and phosphoric acid modified walnut shell on adsorption of Cr(Ⅵ) was carried out. The experimental results showed that owing to larger surface void of modif...A comparison between the effects of ordinary walnut shell and phosphoric acid modified walnut shell on adsorption of Cr(Ⅵ) was carried out. The experimental results showed that owing to larger surface void of modified walnut shell its adsorption of Cr(Ⅵ) was better. When the temperature was 35 ℃, adsorbent particle size was 1.0-1.6 mm, shaker shock rate was 200 r/min, and dosage of walnut shell was 0.80 g, the Cr(Ⅵ) removal rate reached 99.4%. The fitting of adsorption isotherm and kinetics model showed that, Langmuir isotherm model could reflect the adsorption process of modified walnut shell; and both the adsorption processes of ordinary and modified walnut shells accorded with the pseudo-second-order kinetic equations.展开更多
The modification of HZSM-5 zeolite with phosphorus and steam has been studied. Results show that 1% phosphorus and steam modified HZSM-5 has the highest catalytic activity for n-heptane. Physicochemical and catalytic ...The modification of HZSM-5 zeolite with phosphorus and steam has been studied. Results show that 1% phosphorus and steam modified HZSM-5 has the highest catalytic activity for n-heptane. Physicochemical and catalytic properties of 1% phosphorus and steam modified HZSM-5 zeolites have been investigated. The X-ray diffraction (XRD) results exhibit that there is considerable variation in the relative intensity of the individual diffraction peaks. The acidity of the samples decreases with an increase in the steaming temperature, which is determined by the IR of adsorbed pyridine and temperature programmed desorption (TPD) of ammonia. The oxidation state of phosphorus shown by XPS is +5, and a model for surface structure modification is proposed. The nitrogen adsorption isotherm for all samples is a combination of type I and type IV, all hysteresis loops resemble the H4-type. The density functional and cluster model methods have been invoked to select the phosphorus grafting model, and it was found that the phosphorus grafting model were more probable in the form of the terminal oxygen coordinating with aluminum.展开更多
In the process of catalytic destruction of chlorinated volatile organic compounds(CVOCs),the catalyst is prone to chlorine poisoning and produce polychlorinated byproducts with high toxicity and persistence,bringing g...In the process of catalytic destruction of chlorinated volatile organic compounds(CVOCs),the catalyst is prone to chlorine poisoning and produce polychlorinated byproducts with high toxicity and persistence,bringing great risk to atmospheric environment and human health.To solve these problems,this work applied phosphate to modify K-OMS-2 catalysts.The physicochemical properties of catalysts were determined by using X-ray powder diffraction(XRD),scanning electron microscope(SEM),X-ray photoelectron spectroscopy(XPS),hydrogen temperature programmed reduction(H_(2)-TPR),pyridine adsorption Fouriertransform infrared(Py-IR)and water temperature programmed desorption(H_(2)O-TPD),and chlorobenzene was selected as a model pollutant to explore the catalytic performance and byproduct inhibition function of phosphating.Experimental results revealed that 1 wt.%phosphate modification yielded the best catalytic activity for chlorobenzene destruction,with the 90%conversion(T90)at approximately 247℃.The phosphating significantly decreased the types and yields of polychlorinated byproducts in effluent.After phosphating,we observed significant hydroxyl groups on catalyst surface,and the active centerwas transformed into Mn(IV)-O…H,which promoted the formation of HCl,and enhanced the dechlorination process.Furthermore,the enriched Lewis acid sites by phosphating profoundly enhanced the deep oxidation ability of the catalyst,which promoted a rapid oxidation of reaction intermediates,so as to reduce byproducts generation.This study provided an effective strategy for inhibiting the toxic byproducts for the catalytic destruction of chlorinated organics.展开更多
A series of HZSM-5 zeolites modified with different amounts of phosphoric acid(P/HZSM-5) was prepared. The physicochemical features of the P/HZSM-5 catalysts were characterized via X-ray diffraction(XRD), N2 adsor...A series of HZSM-5 zeolites modified with different amounts of phosphoric acid(P/HZSM-5) was prepared. The physicochemical features of the P/HZSM-5 catalysts were characterized via X-ray diffraction(XRD), N2 adsorption-desorption, NH3-temperatttre programmed desorption(NH3-TPD) and Fourier tranform infrared(FTIR) spectra of the adsorbed pyridine, and the performances of the catalysts for Prins condensation to isoprene from isobutylene and formaldehyde were investigated. The maximum isobutene conversion and isoprene selectivity were 10.3% and 94.6% on the HZSM-5 catalyst with a Si/A1 molar ratio of 600 using 5%(mass fraction) phosphoric acid. The phosphoric acid modification not only modulated the amount of acidic sites but also regulated the acid type. An appropriate amount of weak Lewis and Bronsted acid sites served as the active sites for the condensation of isobutene with formaldehyde, and the strong acid sites could cause side reactions and coke deposition.展开更多
The surface of a commercial Y3Al5O12:Ce^3+ phosphor was modified by 99% NH_4F+CH_3COOH solution in a supersonic bath with water temperature of 80 oC for 4 h. The scanning electron microscopy(SEM) results showed t...The surface of a commercial Y3Al5O12:Ce^3+ phosphor was modified by 99% NH_4F+CH_3COOH solution in a supersonic bath with water temperature of 80 oC for 4 h. The scanning electron microscopy(SEM) results showed that the edge angles were not as sharp as the unmodified particles and the flat surfaces turned rough with many micro-structures covered. Positron lifetime measurements quantitatively showed that surface defects were removed away by more than 50%. As a result, the photoluminescence determinations showed that the backscatter loss was reduced by 4.2% and the emission power was enhanced by 5.6% after the surface modification. The conversion efficiency was greatly improved from 47.3% to 51.1%, as presented by the fluorescence images. Therefore, it would be greatly helpful for the improvement of efficiency, transparency and stability of pc-LED. Moreover, this method was significantly suitable for mass production due to its easy operation and low cost.展开更多
基金Supported by National Natural Science Foundation of China(51168013)National Key Technology Support Program(2014BAC04B03)~~
文摘A comparison between the effects of ordinary walnut shell and phosphoric acid modified walnut shell on adsorption of Cr(Ⅵ) was carried out. The experimental results showed that owing to larger surface void of modified walnut shell its adsorption of Cr(Ⅵ) was better. When the temperature was 35 ℃, adsorbent particle size was 1.0-1.6 mm, shaker shock rate was 200 r/min, and dosage of walnut shell was 0.80 g, the Cr(Ⅵ) removal rate reached 99.4%. The fitting of adsorption isotherm and kinetics model showed that, Langmuir isotherm model could reflect the adsorption process of modified walnut shell; and both the adsorption processes of ordinary and modified walnut shells accorded with the pseudo-second-order kinetic equations.
文摘The modification of HZSM-5 zeolite with phosphorus and steam has been studied. Results show that 1% phosphorus and steam modified HZSM-5 has the highest catalytic activity for n-heptane. Physicochemical and catalytic properties of 1% phosphorus and steam modified HZSM-5 zeolites have been investigated. The X-ray diffraction (XRD) results exhibit that there is considerable variation in the relative intensity of the individual diffraction peaks. The acidity of the samples decreases with an increase in the steaming temperature, which is determined by the IR of adsorbed pyridine and temperature programmed desorption (TPD) of ammonia. The oxidation state of phosphorus shown by XPS is +5, and a model for surface structure modification is proposed. The nitrogen adsorption isotherm for all samples is a combination of type I and type IV, all hysteresis loops resemble the H4-type. The density functional and cluster model methods have been invoked to select the phosphorus grafting model, and it was found that the phosphorus grafting model were more probable in the form of the terminal oxygen coordinating with aluminum.
基金supported by the National Natural Science Foundation of China(Nos.21922607 and 22106133)the Outstanding Youth Project of Zhejiang Natural Science Foundation(No.LR19E080004).
文摘In the process of catalytic destruction of chlorinated volatile organic compounds(CVOCs),the catalyst is prone to chlorine poisoning and produce polychlorinated byproducts with high toxicity and persistence,bringing great risk to atmospheric environment and human health.To solve these problems,this work applied phosphate to modify K-OMS-2 catalysts.The physicochemical properties of catalysts were determined by using X-ray powder diffraction(XRD),scanning electron microscope(SEM),X-ray photoelectron spectroscopy(XPS),hydrogen temperature programmed reduction(H_(2)-TPR),pyridine adsorption Fouriertransform infrared(Py-IR)and water temperature programmed desorption(H_(2)O-TPD),and chlorobenzene was selected as a model pollutant to explore the catalytic performance and byproduct inhibition function of phosphating.Experimental results revealed that 1 wt.%phosphate modification yielded the best catalytic activity for chlorobenzene destruction,with the 90%conversion(T90)at approximately 247℃.The phosphating significantly decreased the types and yields of polychlorinated byproducts in effluent.After phosphating,we observed significant hydroxyl groups on catalyst surface,and the active centerwas transformed into Mn(IV)-O…H,which promoted the formation of HCl,and enhanced the dechlorination process.Furthermore,the enriched Lewis acid sites by phosphating profoundly enhanced the deep oxidation ability of the catalyst,which promoted a rapid oxidation of reaction intermediates,so as to reduce byproducts generation.This study provided an effective strategy for inhibiting the toxic byproducts for the catalytic destruction of chlorinated organics.
文摘A series of HZSM-5 zeolites modified with different amounts of phosphoric acid(P/HZSM-5) was prepared. The physicochemical features of the P/HZSM-5 catalysts were characterized via X-ray diffraction(XRD), N2 adsorption-desorption, NH3-temperatttre programmed desorption(NH3-TPD) and Fourier tranform infrared(FTIR) spectra of the adsorbed pyridine, and the performances of the catalysts for Prins condensation to isoprene from isobutylene and formaldehyde were investigated. The maximum isobutene conversion and isoprene selectivity were 10.3% and 94.6% on the HZSM-5 catalyst with a Si/A1 molar ratio of 600 using 5%(mass fraction) phosphoric acid. The phosphoric acid modification not only modulated the amount of acidic sites but also regulated the acid type. An appropriate amount of weak Lewis and Bronsted acid sites served as the active sites for the condensation of isobutene with formaldehyde, and the strong acid sites could cause side reactions and coke deposition.
基金Project supported by National Natural Science Foundation of China(11175049,51177017)
文摘The surface of a commercial Y3Al5O12:Ce^3+ phosphor was modified by 99% NH_4F+CH_3COOH solution in a supersonic bath with water temperature of 80 oC for 4 h. The scanning electron microscopy(SEM) results showed that the edge angles were not as sharp as the unmodified particles and the flat surfaces turned rough with many micro-structures covered. Positron lifetime measurements quantitatively showed that surface defects were removed away by more than 50%. As a result, the photoluminescence determinations showed that the backscatter loss was reduced by 4.2% and the emission power was enhanced by 5.6% after the surface modification. The conversion efficiency was greatly improved from 47.3% to 51.1%, as presented by the fluorescence images. Therefore, it would be greatly helpful for the improvement of efficiency, transparency and stability of pc-LED. Moreover, this method was significantly suitable for mass production due to its easy operation and low cost.