Waste selective catalytic reduction(SCR)catalysts are potential environmental hazards.In this study,the recovery of vanadium and tungsten from waste SCR catalysts by K_(2)CO_(3)roasting and water leaching was investig...Waste selective catalytic reduction(SCR)catalysts are potential environmental hazards.In this study,the recovery of vanadium and tungsten from waste SCR catalysts by K_(2)CO_(3)roasting and water leaching was investigated.The roasting and leaching conditions were optimized:the leaching efficiencies of vanadium and tungsten were 91.19%and 85.36%,respectively,when 18 equivalents of K_(2)CO_(3)were added to perform the roasting at 900℃ for 2 h,followed by leaching at 90°C for 1 h.Notably,in the described conditions,the leaching rate of silicon was only 28.55%.Titanates,including K_(2)Ti_(6)O_(13)and KTi8017,were also produced.Si removal was achieved in 85%efficiency adjusting the pH to 9.5,and the Si impurity thus isolated was composed of amorphous Si.Tungsten and vanadium were precipitated using CaCl_(2).At pH 10 and following the addition of 0.10 mol of H_(2)O_(2)and 16 equivalents of CaCl_(2),the precipitating efficiencies of tungsten and vanadium were 96.89%and 99.65%,respectively.The overall yield of tungsten and vanadium was 82.71%and 90.87%,respectively.展开更多
In this study,the deactivation mechanism caused by high accessibility of strong acid sites for the waste FCC catalyst was proposed and verified for the first time.Based on the proposed deactivation mechanism,magnesium...In this study,the deactivation mechanism caused by high accessibility of strong acid sites for the waste FCC catalyst was proposed and verified for the first time.Based on the proposed deactivation mechanism,magnesium modification through magnesium chloride impregnation was employed for the regeneration of waste FCC catalyst.The regenerated waste FCC catalyst was characterized,with its heavy oil catalytic cracking performance tested.The characterization results indicated that,in comparison with the unmodified waste FCC catalyst,the acid sites strength of the regenerated waste FCC catalyst was weakened,with no prominent alterations of the total acid sites quantity and textural properties.The heavy oil catalytic cracking results suggested that the catalytic cracking performance of the regenerated waste FCC catalyst was greatly improved due to the suitable surface acidity of the sample.In contrast with the unmodified waste FCC catalyst,the gasoline yield over the regenerated waste FCC catalyst significantly increased by 3.04 percentage points,meanwhile the yield of dry gas,LPG,coke and bottoms obviously decreased by 0.36,0.81,1.28 and 0.87 percentage points,respectively,making the regenerated waste FCC catalyst serve as a partial substitute for the fresh FCC catalyst.Finally,the acid property change mechanism was discussed.展开更多
Preparation of biodiesel from waste oils containing 72% of free fatty acids catalyzed by a novel Br?nsted acidic ionic liquid 1-sulfobutyl-3-methylimidazolium hydrosulfate([BHSO_3MIM][HSO_4]) was systematically invest...Preparation of biodiesel from waste oils containing 72% of free fatty acids catalyzed by a novel Br?nsted acidic ionic liquid 1-sulfobutyl-3-methylimidazolium hydrosulfate([BHSO_3MIM][HSO_4]) was systematically investigated.The optimum molar ratio of methanol to waste oils,catalyst amount,reaction temperature and reaction time were 8/1,10%(based on the mass of waste oils),140°C and 6 h,respectively,under which the obtained yield of biodiesel reached 94.9%.Also,[BHSO_3MIM][HSO_4] as a catalyst still retained around 97% of its original catalytic activity after successive re-use of 5 batches(6 h per batch),showing the excellent operational stability.Moreover,the acidic IL [BHSO_3MIM][HSO_4] was able to ef ficiently catalyze conversions of waste oils with different amounts of FFAs(free fatty acids) into biodiesel,and showed tremendous application potential.Therefore,an ef ficient and environmentally friendly catalyst is provided for the synthesis of biodiesel from waste oils with high acid value.展开更多
The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasificati...The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasification reactivity of YCW was measured by thermogravimetric analyzer.Scanning electron microscope–energy dispersive system,nitrogen adsorption analyzer and laser Raman spectroscopy were employed to analyze the char physico-chemical properties.The results show that the optimal IWC loading ratio was 5 wt%at 1000°C.The distribution of IWC on char was uneven and Fe catalyst concentrated on the surface of some chars.The specific surface area of YCW gasified semi-char decreased significantly with the increase of gasification time.i.e.,the specific surface area reduced from 382 m2/g(0 min)to 192 m2/g(3 min),meanwhile,the number of micropores and mesopores decreased sharply at the late gasification stage.The carbon microcrystalline structure of YCW gasified semi-char was gradually destroyed with the increase of gasification time,and the microcrystalline structure with small size was gradually generated,resulting in the decreasing order degree of carbon microcrystalline structure.IWC can catalyze YCW gasification which could provide theoretical guidance for industrial solid waste recycling.展开更多
The strontium modified waste FCC catalyst was prepared by magnetic stirring method and characterized by Xray diffractometry(XRD),UV-Vis diffuse reflectance spectrometry(DRS),X-ray photoelectron spectroscopy(XPS)and sc...The strontium modified waste FCC catalyst was prepared by magnetic stirring method and characterized by Xray diffractometry(XRD),UV-Vis diffuse reflectance spectrometry(DRS),X-ray photoelectron spectroscopy(XPS)and scanning electron microscopy(SEM).Meanwhile,its photocatalytic denitrogenation performance was evaluated in terms of its ability to degrade the N-containing simulation oil under visible light.A mixture of strontium nitrate solution(with a concentration of 0.5 mol/L)and waste FCC catalyst was calcined at 400℃for 5 h prior to taking part in the photocatalytic denitrogenation reaction.The test results showed that the photocatalytic degradation rate of pyridine contained in simulation oil in the presence of the strontium modified FCC catalyst could reach 92.0% under visible light irradiation for 2.5 h.展开更多
In this work, we report a simple and inexpensive approach to synthesize effective multicomponent Cu-Cu2O-CuO catalysts for the Rochow process from industrial waste contact masses (WCMs). WCMs from the organosilane i...In this work, we report a simple and inexpensive approach to synthesize effective multicomponent Cu-Cu2O-CuO catalysts for the Rochow process from industrial waste contact masses (WCMs). WCMs from the organosilane industry were treated with acid followed by reduction with metallic iron powder. The obtained copper powder was then subjected to controlled oxidation in air at different temperatures, followed by ball milling. The orthogonal array approach was applied to optimize this process, and the stirring speed and pH were found to significantly affect the leaching ratio and copper yield, respectively. When used for the Rochow process, the optimized ternary Cu-Cu2O-CuO catalyst greatly enhanced the dimethyldichlorosilane selectivity and Si conversion compared with Cu-Cu2O-CuO catalysts prepared without ball milling, bare Cu catalysts, and Cu-Cu2O-CuO catalysts with different compositions. This could be attributed to their small particle size and the strong synergistic effect among the multiple components in the catalyst with the optimized composition.展开更多
Porous g-C3N4samples were obtained by simply calcining bulk g-C3N4in static air in a muffle oven.The photocatalytic performance of these samples was evaluated through the removal of aqueous organic dyes(methylene blu...Porous g-C3N4samples were obtained by simply calcining bulk g-C3N4in static air in a muffle oven.The photocatalytic performance of these samples was evaluated through the removal of aqueous organic dyes(methylene blue and methyl orange)and tetracycline hydrochloride under visible-light irradiation(λ〉420 nm).Compared to bulk g-C3N4,porous g-C3N4exhibited much better capability for removing these contaminants,especially under visible-light irradiation,due to the enlarged specific surface area and more efficient separation of photogenerated charge carries.In particular,porous g-C3N4obtained by calcining bulk g-C3N4in air at 525℃ showed the highest visible-light-driven catalytic activity among these samples.Superoxide radical anions(·O2^-)were found to be the primary active species responsible for photodegradation.展开更多
Selective catalytic reduction(SCR) catalyst waste is a hazardous solid waste that seriously threatens the environment and public health.In this study,a thermal melting technology is proposed for the treatment of waste...Selective catalytic reduction(SCR) catalyst waste is a hazardous solid waste that seriously threatens the environment and public health.In this study,a thermal melting technology is proposed for the treatment of waste SCR catalysts.The melting characteristics and mineral phase transformation of waste SCR catalysts blended with three different groups of additives were explored by heating stage microscopy,thermogravimetric analysis/differential scanning calorimetry(TG/DSC) analysis,thermodynamic simulation,and X-ray diffraction(XRD) analysis;heavy metal leaching toxicity was tested by inductively coupled plasma-atomic emission spectrometry(I CP-AES) analysis.The results indicated that the melting point of waste SCR catalysts can be effectively reduced with proper additives.The additive formula of 39.00% Fe2 O3(in weight),6.50% CaO,3.30% SiO2,and 1.20% Al2 O3 achieves the optimal fluxing behavior,significantly decreasing the initial melting temperature from 1223℃ to1169℃.Furthermore,the whole heating process of waste SCR catalysts can be divided into three stages:the solid reaction stage,the sintering stage,and the primary melting stage.The leaching concentrations of V,As,Pb,and Se are significantly reduced,from 10.64,1.054,0.195,and 0.347 mg/L to 0.178,0.025,0.048,and 0.003 mg/L,respectively,much lower than the standard limits after melting treatment,showing the strong immobilization capacity of optimal additives for heavy metals in waste SCR catalysts.The results demonstrate the feasibility of harmless melting treatments for waste SCR catalysts with relatively low energy consumption,providing theoretical support for a novel method of disposing of hazardous waste SCR catalysts.展开更多
A waste paper sludge-derived heterogeneous catalyst(WPS-Fe-350) was synthesized via a facile method and successfully applied for the degradation of Orange Ⅱ in the presence of oxalic acid under the illumination of ...A waste paper sludge-derived heterogeneous catalyst(WPS-Fe-350) was synthesized via a facile method and successfully applied for the degradation of Orange Ⅱ in the presence of oxalic acid under the illumination of ultraviolet light emitting diode(UV-LED) Powder X-ray diffraction,Fourier-transform infrared spectroscopy,scanning electronic microscopy and N2 sorption isotherm analysis indicated the formation of α-Fe2O3 in the mesoporous nanocomposite.The degradation test showed that WPS-Fe-350 exhibited rapid Orange Ⅱ(OⅡ) degradation and mineralization in the presence of oxalic acid under the illumination of UV-LED.The effects of p H,oxalic acid concentration and dosage of the catalyst on the degradation of OⅡ were evaluated,respectively.Under the optimal conditions(1 g/L catalyst dosage,2 mmol/L oxalic acid and p H 3.0),the degradation percentage for a solution containing 30 mg/L OⅡ reached 83.4% under illumination by UV-LED for 80 min.Moreover,five cyclic tests for OⅡ degradation suggested that WPS-Fe-350 exhibited excellent stability of catalytic activity.Hence,this study provides an alternative environmentally friendly way to reuse waste paper sludge and an effective and economically viable method for degradation of azo dyes and other refractory organic pollutants in water.展开更多
Catalytic pyrolysis of thermoplastics extracted from waste electrical and electronic equipment (WEEE) was investigated using various fly ash-derived catalysts. The catalysts were prepared from fly ash by a simple me...Catalytic pyrolysis of thermoplastics extracted from waste electrical and electronic equipment (WEEE) was investigated using various fly ash-derived catalysts. The catalysts were prepared from fly ash by a simple method that basically includes a mechanical treatment followed by an acid or a basic activation. The synthesized catalysts were characterized using various analytical techniques. The results showed that not treated fly ash (FA) is characterized by good crystallinity, which in turn is lowered by mechanical and chemical treatment (fly ash after mechanical and acid activation, FAMA) and suppressed almost entirely down to let fly ash become completely amorphous (fly ash al^er mechanical and basic activation FAMB). Simultaneously, the surface area resulted increased. Subsequently, FA, FAMB and FAMA were used in the pyrolysis of a WEEE plastic sample at 400~C and their performance were compared with thermal pyrolysis at the same temperature. The catalysts principally improve the light oil yield: from 59 wt.% with thermal pyrolysis to 83 wt.% using FAMB. The formation of styrene in the oil is also increased: from 243 mg/g with thermal pyrolysis to 453 mg/g using FAMB. As a result, FAMB proved to be the best catalyst, thus producing also the lowest and the highest amount of char and gas, respectively.展开更多
基金from the Fundamental Research Funds for the Central Universities(2010YH14).
文摘Waste selective catalytic reduction(SCR)catalysts are potential environmental hazards.In this study,the recovery of vanadium and tungsten from waste SCR catalysts by K_(2)CO_(3)roasting and water leaching was investigated.The roasting and leaching conditions were optimized:the leaching efficiencies of vanadium and tungsten were 91.19%and 85.36%,respectively,when 18 equivalents of K_(2)CO_(3)were added to perform the roasting at 900℃ for 2 h,followed by leaching at 90°C for 1 h.Notably,in the described conditions,the leaching rate of silicon was only 28.55%.Titanates,including K_(2)Ti_(6)O_(13)and KTi8017,were also produced.Si removal was achieved in 85%efficiency adjusting the pH to 9.5,and the Si impurity thus isolated was composed of amorphous Si.Tungsten and vanadium were precipitated using CaCl_(2).At pH 10 and following the addition of 0.10 mol of H_(2)O_(2)and 16 equivalents of CaCl_(2),the precipitating efficiencies of tungsten and vanadium were 96.89%and 99.65%,respectively.The overall yield of tungsten and vanadium was 82.71%and 90.87%,respectively.
基金supported by the Exploratory Research Program of Petrochemical Research Institute (16-yk-01-03),PetroChina
文摘In this study,the deactivation mechanism caused by high accessibility of strong acid sites for the waste FCC catalyst was proposed and verified for the first time.Based on the proposed deactivation mechanism,magnesium modification through magnesium chloride impregnation was employed for the regeneration of waste FCC catalyst.The regenerated waste FCC catalyst was characterized,with its heavy oil catalytic cracking performance tested.The characterization results indicated that,in comparison with the unmodified waste FCC catalyst,the acid sites strength of the regenerated waste FCC catalyst was weakened,with no prominent alterations of the total acid sites quantity and textural properties.The heavy oil catalytic cracking results suggested that the catalytic cracking performance of the regenerated waste FCC catalyst was greatly improved due to the suitable surface acidity of the sample.In contrast with the unmodified waste FCC catalyst,the gasoline yield over the regenerated waste FCC catalyst significantly increased by 3.04 percentage points,meanwhile the yield of dry gas,LPG,coke and bottoms obviously decreased by 0.36,0.81,1.28 and 0.87 percentage points,respectively,making the regenerated waste FCC catalyst serve as a partial substitute for the fresh FCC catalyst.Finally,the acid property change mechanism was discussed.
基金Supported by the National Natural Science Foundation of China(21676104,21336002,21376096)the Open Funding Project of the State Key Laboratory of Bioreactor Engineeringthe Program of State Key Laboratory of Pulp and Paper Engineering(2017ZD05)
文摘Preparation of biodiesel from waste oils containing 72% of free fatty acids catalyzed by a novel Br?nsted acidic ionic liquid 1-sulfobutyl-3-methylimidazolium hydrosulfate([BHSO_3MIM][HSO_4]) was systematically investigated.The optimum molar ratio of methanol to waste oils,catalyst amount,reaction temperature and reaction time were 8/1,10%(based on the mass of waste oils),140°C and 6 h,respectively,under which the obtained yield of biodiesel reached 94.9%.Also,[BHSO_3MIM][HSO_4] as a catalyst still retained around 97% of its original catalytic activity after successive re-use of 5 batches(6 h per batch),showing the excellent operational stability.Moreover,the acidic IL [BHSO_3MIM][HSO_4] was able to ef ficiently catalyze conversions of waste oils with different amounts of FFAs(free fatty acids) into biodiesel,and showed tremendous application potential.Therefore,an ef ficient and environmentally friendly catalyst is provided for the synthesis of biodiesel from waste oils with high acid value.
基金The present work was supported by the National Natural Science Foundation of China (21968024)the Project of Key Research Plan of Ningxia (2019BCH01001)The authors also gratefully thank Professor Junzhuo Fang for his help in taking SEM–EDS photos.
文摘The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasification reactivity of YCW was measured by thermogravimetric analyzer.Scanning electron microscope–energy dispersive system,nitrogen adsorption analyzer and laser Raman spectroscopy were employed to analyze the char physico-chemical properties.The results show that the optimal IWC loading ratio was 5 wt%at 1000°C.The distribution of IWC on char was uneven and Fe catalyst concentrated on the surface of some chars.The specific surface area of YCW gasified semi-char decreased significantly with the increase of gasification time.i.e.,the specific surface area reduced from 382 m2/g(0 min)to 192 m2/g(3 min),meanwhile,the number of micropores and mesopores decreased sharply at the late gasification stage.The carbon microcrystalline structure of YCW gasified semi-char was gradually destroyed with the increase of gasification time,and the microcrystalline structure with small size was gradually generated,resulting in the decreasing order degree of carbon microcrystalline structure.IWC can catalyze YCW gasification which could provide theoretical guidance for industrial solid waste recycling.
基金financially supported by the Science and Technology Project of Fujian Province(No.CE0015)the Ningde Normal University Project on Serving the Western Coast to the TW Strait(No.2010H103)the National-level College Students’ Innovative Entrepreneurial Training Plan Project of Fujian Normal University(Nos.201210394005 and 201310394015)
文摘The strontium modified waste FCC catalyst was prepared by magnetic stirring method and characterized by Xray diffractometry(XRD),UV-Vis diffuse reflectance spectrometry(DRS),X-ray photoelectron spectroscopy(XPS)and scanning electron microscopy(SEM).Meanwhile,its photocatalytic denitrogenation performance was evaluated in terms of its ability to degrade the N-containing simulation oil under visible light.A mixture of strontium nitrate solution(with a concentration of 0.5 mol/L)and waste FCC catalyst was calcined at 400℃for 5 h prior to taking part in the photocatalytic denitrogenation reaction.The test results showed that the photocatalytic degradation rate of pyridine contained in simulation oil in the presence of the strontium modified FCC catalyst could reach 92.0% under visible light irradiation for 2.5 h.
基金The work was supported by the National Natural Science Foundation of China (grant number 21506224). Z.Z. is grateful for support from the Institute of Chemical and Engineering Sciences.
文摘In this work, we report a simple and inexpensive approach to synthesize effective multicomponent Cu-Cu2O-CuO catalysts for the Rochow process from industrial waste contact masses (WCMs). WCMs from the organosilane industry were treated with acid followed by reduction with metallic iron powder. The obtained copper powder was then subjected to controlled oxidation in air at different temperatures, followed by ball milling. The orthogonal array approach was applied to optimize this process, and the stirring speed and pH were found to significantly affect the leaching ratio and copper yield, respectively. When used for the Rochow process, the optimized ternary Cu-Cu2O-CuO catalyst greatly enhanced the dimethyldichlorosilane selectivity and Si conversion compared with Cu-Cu2O-CuO catalysts prepared without ball milling, bare Cu catalysts, and Cu-Cu2O-CuO catalysts with different compositions. This could be attributed to their small particle size and the strong synergistic effect among the multiple components in the catalyst with the optimized composition.
基金Supported by the National Natural Science Foundation of China(Grant No.21477022)
文摘Porous g-C3N4samples were obtained by simply calcining bulk g-C3N4in static air in a muffle oven.The photocatalytic performance of these samples was evaluated through the removal of aqueous organic dyes(methylene blue and methyl orange)and tetracycline hydrochloride under visible-light irradiation(λ〉420 nm).Compared to bulk g-C3N4,porous g-C3N4exhibited much better capability for removing these contaminants,especially under visible-light irradiation,due to the enlarged specific surface area and more efficient separation of photogenerated charge carries.In particular,porous g-C3N4obtained by calcining bulk g-C3N4in air at 525℃ showed the highest visible-light-driven catalytic activity among these samples.Superoxide radical anions(·O2^-)were found to be the primary active species responsible for photodegradation.
基金Project supported by the National Key Research and Development Program of China (No. 2018YFB0604104)。
文摘Selective catalytic reduction(SCR) catalyst waste is a hazardous solid waste that seriously threatens the environment and public health.In this study,a thermal melting technology is proposed for the treatment of waste SCR catalysts.The melting characteristics and mineral phase transformation of waste SCR catalysts blended with three different groups of additives were explored by heating stage microscopy,thermogravimetric analysis/differential scanning calorimetry(TG/DSC) analysis,thermodynamic simulation,and X-ray diffraction(XRD) analysis;heavy metal leaching toxicity was tested by inductively coupled plasma-atomic emission spectrometry(I CP-AES) analysis.The results indicated that the melting point of waste SCR catalysts can be effectively reduced with proper additives.The additive formula of 39.00% Fe2 O3(in weight),6.50% CaO,3.30% SiO2,and 1.20% Al2 O3 achieves the optimal fluxing behavior,significantly decreasing the initial melting temperature from 1223℃ to1169℃.Furthermore,the whole heating process of waste SCR catalysts can be divided into three stages:the solid reaction stage,the sintering stage,and the primary melting stage.The leaching concentrations of V,As,Pb,and Se are significantly reduced,from 10.64,1.054,0.195,and 0.347 mg/L to 0.178,0.025,0.048,and 0.003 mg/L,respectively,much lower than the standard limits after melting treatment,showing the strong immobilization capacity of optimal additives for heavy metals in waste SCR catalysts.The results demonstrate the feasibility of harmless melting treatments for waste SCR catalysts with relatively low energy consumption,providing theoretical support for a novel method of disposing of hazardous waste SCR catalysts.
基金supported by the Major Science and Technology Projects Focus on Social Development Projects of Zhejiang Province(Nos.2014C03002 and 2012C03004-1)
文摘A waste paper sludge-derived heterogeneous catalyst(WPS-Fe-350) was synthesized via a facile method and successfully applied for the degradation of Orange Ⅱ in the presence of oxalic acid under the illumination of ultraviolet light emitting diode(UV-LED) Powder X-ray diffraction,Fourier-transform infrared spectroscopy,scanning electronic microscopy and N2 sorption isotherm analysis indicated the formation of α-Fe2O3 in the mesoporous nanocomposite.The degradation test showed that WPS-Fe-350 exhibited rapid Orange Ⅱ(OⅡ) degradation and mineralization in the presence of oxalic acid under the illumination of UV-LED.The effects of p H,oxalic acid concentration and dosage of the catalyst on the degradation of OⅡ were evaluated,respectively.Under the optimal conditions(1 g/L catalyst dosage,2 mmol/L oxalic acid and p H 3.0),the degradation percentage for a solution containing 30 mg/L OⅡ reached 83.4% under illumination by UV-LED for 80 min.Moreover,five cyclic tests for OⅡ degradation suggested that WPS-Fe-350 exhibited excellent stability of catalytic activity.Hence,this study provides an alternative environmentally friendly way to reuse waste paper sludge and an effective and economically viable method for degradation of azo dyes and other refractory organic pollutants in water.
文摘Catalytic pyrolysis of thermoplastics extracted from waste electrical and electronic equipment (WEEE) was investigated using various fly ash-derived catalysts. The catalysts were prepared from fly ash by a simple method that basically includes a mechanical treatment followed by an acid or a basic activation. The synthesized catalysts were characterized using various analytical techniques. The results showed that not treated fly ash (FA) is characterized by good crystallinity, which in turn is lowered by mechanical and chemical treatment (fly ash after mechanical and acid activation, FAMA) and suppressed almost entirely down to let fly ash become completely amorphous (fly ash al^er mechanical and basic activation FAMB). Simultaneously, the surface area resulted increased. Subsequently, FA, FAMB and FAMA were used in the pyrolysis of a WEEE plastic sample at 400~C and their performance were compared with thermal pyrolysis at the same temperature. The catalysts principally improve the light oil yield: from 59 wt.% with thermal pyrolysis to 83 wt.% using FAMB. The formation of styrene in the oil is also increased: from 243 mg/g with thermal pyrolysis to 453 mg/g using FAMB. As a result, FAMB proved to be the best catalyst, thus producing also the lowest and the highest amount of char and gas, respectively.