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
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
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
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.