Characterization of Metal Oxide-modified Walnut-shell Activated Carbon and Its Application for Phosphine Adsorption: Equilibrium, Regeneration, and Mechanism Studies
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摘要
We prepared a kind of metal oxide-modified walnut-shell activated carbon(MWAC) by KOH chemical activation method and used for PH_3 adsorption removal. Meanwhile, the PH_3 adsorption equilibrium was investigated experimentally and fitted by the Toth equation, and the isosteric heat of PH_3 adsorption was calculated by the Clausius-Clapeyron Equation. The exhausted MWAC was regenerated by water washing and air drying. Moreover, the properties of five different samples were characterized by N_2 adsorption isotherm, SEM/EDS, XPS, and FTIR. The results showed that the maximum PH_3 equilibrium adsorption capacity was 595.56 mg/g. The MWAC had an energetically heterogeneous surface due to values of isosteric heat of adsorption ranging from 43 to 90 kJ/mol. The regeneration method provided an effective way for both adsorption species recycling and exhausted carbon regeneration. The high removal efficiency and big equilibrium adsorption capacity for PH_3 adsorption on the MWAC were related to its large surface area and high oxidation activity in PH_3 adsorption-oxidation to H_3 PO_4 and P_2 O_5. Furthermore, a possible PH_3 adsorption mechanism was proposed.
We prepared a kind of metal oxide-modified walnut-shell activated carbon(MWAC) by KOH chemical activation method and used for PH_3 adsorption removal. Meanwhile, the PH_3 adsorption equilibrium was investigated experimentally and fitted by the Toth equation, and the isosteric heat of PH_3 adsorption was calculated by the Clausius-Clapeyron Equation. The exhausted MWAC was regenerated by water washing and air drying. Moreover, the properties of five different samples were characterized by N_2 adsorption isotherm, SEM/EDS, XPS, and FTIR. The results showed that the maximum PH_3 equilibrium adsorption capacity was 595.56 mg/g. The MWAC had an energetically heterogeneous surface due to values of isosteric heat of adsorption ranging from 43 to 90 kJ/mol. The regeneration method provided an effective way for both adsorption species recycling and exhausted carbon regeneration. The high removal efficiency and big equilibrium adsorption capacity for PH_3 adsorption on the MWAC were related to its large surface area and high oxidation activity in PH_3 adsorption-oxidation to H_3 PO_4 and P_2 O_5. Furthermore, a possible PH_3 adsorption mechanism was proposed.
We prepared a kind of metal oxide-modified walnut-shell activated carbon(MWAC) by KOH chemical activation method and used for PH_3 adsorption removal. Meanwhile, the PH_3 adsorption equilibrium was investigated experimentally and fitted by the Toth equation, and the isosteric heat of PH_3 adsorption was calculated by the Clausius-Clapeyron Equation. The exhausted MWAC was regenerated by water washing and air drying. Moreover, the properties of five different samples were characterized by N_2 adsorption isotherm, SEM/EDS, XPS, and FTIR. The results showed that the maximum PH_3 equilibrium adsorption capacity was 595.56 mg/g. The MWAC had an energetically heterogeneous surface due to values of isosteric heat of adsorption ranging from 43 to 90 kJ/mol. The regeneration method provided an effective way for both adsorption species recycling and exhausted carbon regeneration. The high removal efficiency and big equilibrium adsorption capacity for PH_3 adsorption on the MWAC were related to its large surface area and high oxidation activity in PH_3 adsorption-oxidation to H_3 PO_4 and P_2 O_5. Furthermore, a possible PH_3 adsorption mechanism was proposed.
引文
[1]Ning P,Wang XY.Advanced Purification and Comprehensive Utilization of Yellow Phosphorous off Gas[J].Frontiers of Environmental Science&Engineering,2015,9(2):181-189
[2]Ma LP,Ning P,Zhang YY,et al.Experimental and Modeling of Fixedbed Reactor for Yellow Phosphorous Tail Gas Purification over Impregnated Activated Carbon[J].Chemical Engineering Journal,2008,137(3):471-479
[3]Ning P,Yi HH,Yu QF,et al.Effect of Zinc and Cerium Addition on Property of Copper-based Adsorbents for Phosphine Adsorption[J].Journal of Rare Earths,2010,28(4):581-586
[4]Yu QF,Tang XL,Yi HH,et al.Equilibrium and Heat of Adsorption of Phosphine on CaCl2-Modified Molecular Sieve[J].Asia-Pacific Journal of Chemical Engineering,2009,4(5):612-617
[5]Wang XQ,Ning P,Shi Y,et al.Adsorption of Low Concentration Phosphine in Yellow Phosphorus off-gas by Impregnated Activated Carbon[J].Journal of Hazardous Materials,2009,171(1-3):588-593
[6]Yu QF,Li M,Ning P,et al.Preparation and Phosphine Adsorption of Activated Carbon Prepared from Walnut Shells by KOH Chemical Activation[J].Separation Science and Technology,2014,49(15):2 366-2375
[7]Ren ZD,Quan SS,Zhu YC,et al.Purification of Yellow Phosphorus Tail Gas for the Removal of PH3 on the Spot with Flower-shaped CuO/AC[J].Rsc Advances,2015,5(38):29 734-29 740
[8]Yang LP,Yi HH,Tang XL,et al.Effect of Rare Earth Addition on CuFe/AC Adsorbents for Phosphine Adsorption from Yellow Phosphorous Tail Gas[J].Journal of Rare Earths,2010,28(0):322-325
[9]Elliot B,Balma F,Johnson F.Exhaust Gas Incineration and the Combustion of Arsine and Phosphine[J].Solid State Technology,1990,33(1):89-92
[10]Herman T,Soden S.Efficieny Handling Effluent Gases through Chemical Scrubbing[C].AIP Conference Proceedings,1988,166(1):99-108
[11]Li JY,Ning P,Qu GF.Research on the Cu(II)-Co(II)Catalyzed Oxidation of Phosphine in Aqueous Solution[J].Journal of Wuhan University Technology,2007,29(10):63-65,69
[12]Colabella JM,Stall RA,Sorenson CT.The Adsorption and Subsequent Oxidation of AsH3 and PH3 on Activated Carbon[J].Journal of Crystal Growth,1988,92:189-195
[13]Hsu JN,Tsai CJ,Chiang C,et al.Silane Removal at Ambient Temperature by Using Alumina-supported Metal Oxide Adsorbents[J].Journal of the Air&Waste Management Association,2007,57(2):204-210
[14]Ning P,Bart H-J,Wang XQ,et al.Removal of P4,PH3 and H2S from Yellow Phosphorus Tail Gas by a Catalytic Oxidation Process[J].Engineering Science,2005,7(6):27-35
[15]Yi HH,Yu QF,Tang XL,et al.Phosphine Adsorption Removal from Yellow Phosphorus Tail Gas over CuO-ZnO-La2O3/Activated Carbon[J].Industrial&Engineering Chemistry Research,2011,50(7):3 960-3 965
[16]Bhatnagar A,Sillanpaa M.Utilization of Agro-industrial and Municipal Waste Materials as Potential Adsorbents for Water Treatment-AReview[J].Chemical Engineering Journal,2010,157(2-3):277-296
[17]Yorgun S,Y?ld?z D.Preparation and Characterization of Activated Carbons from Paulownia Wood by Chemical Activation with H3PO4[J].Journal of the Taiwan Institute of Chemical Engineers,2015,53:122-131
[18]Yu QF,Li M,Ji X,et al.Characterization and Methanol Adsorption of Walnut-shell Activated Carbon Prepared by KOH Activation[J].Journal of Wuhan University of Technology-Material Science Edition,2016;31(2):260-268
[19]Nowicki P,Pietrzak R,Wachowska H.Sorption Properties of Active Carbons Obtained from Walnut Shells by Chemical and Physical Activation[J].Catalysis Today,2010,150(1-2):107-114
[20]Yang J,Qiu KQ.Preparation of Activated Carbons from Walnut Shells via Vacuum Chemical Activation and Their Application for Methylene Blue Removal[J].Chemical Engineering Journal,2010,165(1):209-217
[21]Gu X,Su Z,Xi H.New Activated Carbon with High Thermal Conductivity and Its Microwave Regeneration Performance[J].Journal of Wuhan University of Technology-Material Science Edition,2016,31(2):328-333
[22]Yu QF.Adsorbent Preparation and Adsorption Mechanism Research for Low Concentration PH3 Adsorption Removal[D].Kunming:Kunming University of Science&Technology,2011
[23]Yu QF,Yi HH,Tang XL,et al.Adsorption and Prediction of Adsorption Isotherm onto Activated Carbon[J].Journal of Wuhan University Technology,2010;32(1):34-37
[24]Yu QF,Ning P,Yi HH,et al.Effect of Preparation Conditions on the Property Cu/AC Adsorbents for Phosphine Adsorption[J].Separation Science and Technology,2012,47:527-533
[25]Li S,Hao JM,Ning P,et al.Preparation of Cu-Fe Nanocomposites Loaded Diatomite and Their Excellent Performance in Simultaneous Adsorption/oxidation of Hydrogen Sulfide and Phosphine at Low Temperature[J].Separation and Purification Technology,2017,180(1):23-35
[26]Xu XW,Huang GQ,Qi S.Properties of AC and 13X Zeolite Modified with CuCl2 and Cu(NO3)2 in Phosphine Removal and the Adsorptive Mechanisms[J].Chemical Engineering Journal,2017,316:563-72
[27]Rothstein DP,Wu B-G,Lee TV,et al.Adsorption Isotherms and Isosteric Heats of Adsorption for Ethane,Propane,and N-butane on Polystyrene[J].Journal of Colloid and Interface Science,1985,106(2):399-409
[28]Hill T.Statistical Mechanics of Adsorption.V.Thermodynamics and Heat of Adsorption[J].The Journal of Chemical Physics,1949,17:520-535
[29]Martinez M,Torres M,Guzman C,et al.Preparation and Characteristics of Activated Carbon from Olive Stones and Walnut Shells[J].Industrial Crops and Products,2006,23(1):23-28
[30]ZahmakIran M,zkar S,Kodaira T,et al.A Novel,Simple,Organic Free Preparation and Characterization of Water Dispersible Photoluminescent Cu2O Nanocubes[J].Materials Letters,2009,63(3-4):400-402
[31]Moulder J,Chastain J.Handbook of X-ray Photoelectron Spectroscopy[M].Perkin-Elmer Eden Prairie,MN,1992
[32]Chapman A,Thirlwell L.Spectra of Phosphorus Compounds--I the Infra-red Spectra of Orthophosphates[J].Spectrochimica Acta,1964,20(6):937-947
[33]Stefov V.Infrared and Raman Spectra of Magnesium Ammonium Phosphate Hexahydrate(Struvite)and Its Isomorphous Analogues.I.Spectra of Protiated and Partially Deuterated Magnesium Potassium Phosphate Hexahydrate[J].Journal of Molecular Structure,2004,689(1-2):1-10
[2]Ma LP,Ning P,Zhang YY,et al.Experimental and Modeling of Fixedbed Reactor for Yellow Phosphorous Tail Gas Purification over Impregnated Activated Carbon[J].Chemical Engineering Journal,2008,137(3):471-479
[3]Ning P,Yi HH,Yu QF,et al.Effect of Zinc and Cerium Addition on Property of Copper-based Adsorbents for Phosphine Adsorption[J].Journal of Rare Earths,2010,28(4):581-586
[4]Yu QF,Tang XL,Yi HH,et al.Equilibrium and Heat of Adsorption of Phosphine on CaCl2-Modified Molecular Sieve[J].Asia-Pacific Journal of Chemical Engineering,2009,4(5):612-617
[5]Wang XQ,Ning P,Shi Y,et al.Adsorption of Low Concentration Phosphine in Yellow Phosphorus off-gas by Impregnated Activated Carbon[J].Journal of Hazardous Materials,2009,171(1-3):588-593
[6]Yu QF,Li M,Ning P,et al.Preparation and Phosphine Adsorption of Activated Carbon Prepared from Walnut Shells by KOH Chemical Activation[J].Separation Science and Technology,2014,49(15):2 366-2375
[7]Ren ZD,Quan SS,Zhu YC,et al.Purification of Yellow Phosphorus Tail Gas for the Removal of PH3 on the Spot with Flower-shaped CuO/AC[J].Rsc Advances,2015,5(38):29 734-29 740
[8]Yang LP,Yi HH,Tang XL,et al.Effect of Rare Earth Addition on CuFe/AC Adsorbents for Phosphine Adsorption from Yellow Phosphorous Tail Gas[J].Journal of Rare Earths,2010,28(0):322-325
[9]Elliot B,Balma F,Johnson F.Exhaust Gas Incineration and the Combustion of Arsine and Phosphine[J].Solid State Technology,1990,33(1):89-92
[10]Herman T,Soden S.Efficieny Handling Effluent Gases through Chemical Scrubbing[C].AIP Conference Proceedings,1988,166(1):99-108
[11]Li JY,Ning P,Qu GF.Research on the Cu(II)-Co(II)Catalyzed Oxidation of Phosphine in Aqueous Solution[J].Journal of Wuhan University Technology,2007,29(10):63-65,69
[12]Colabella JM,Stall RA,Sorenson CT.The Adsorption and Subsequent Oxidation of AsH3 and PH3 on Activated Carbon[J].Journal of Crystal Growth,1988,92:189-195
[13]Hsu JN,Tsai CJ,Chiang C,et al.Silane Removal at Ambient Temperature by Using Alumina-supported Metal Oxide Adsorbents[J].Journal of the Air&Waste Management Association,2007,57(2):204-210
[14]Ning P,Bart H-J,Wang XQ,et al.Removal of P4,PH3 and H2S from Yellow Phosphorus Tail Gas by a Catalytic Oxidation Process[J].Engineering Science,2005,7(6):27-35
[15]Yi HH,Yu QF,Tang XL,et al.Phosphine Adsorption Removal from Yellow Phosphorus Tail Gas over CuO-ZnO-La2O3/Activated Carbon[J].Industrial&Engineering Chemistry Research,2011,50(7):3 960-3 965
[16]Bhatnagar A,Sillanpaa M.Utilization of Agro-industrial and Municipal Waste Materials as Potential Adsorbents for Water Treatment-AReview[J].Chemical Engineering Journal,2010,157(2-3):277-296
[17]Yorgun S,Y?ld?z D.Preparation and Characterization of Activated Carbons from Paulownia Wood by Chemical Activation with H3PO4[J].Journal of the Taiwan Institute of Chemical Engineers,2015,53:122-131
[18]Yu QF,Li M,Ji X,et al.Characterization and Methanol Adsorption of Walnut-shell Activated Carbon Prepared by KOH Activation[J].Journal of Wuhan University of Technology-Material Science Edition,2016;31(2):260-268
[19]Nowicki P,Pietrzak R,Wachowska H.Sorption Properties of Active Carbons Obtained from Walnut Shells by Chemical and Physical Activation[J].Catalysis Today,2010,150(1-2):107-114
[20]Yang J,Qiu KQ.Preparation of Activated Carbons from Walnut Shells via Vacuum Chemical Activation and Their Application for Methylene Blue Removal[J].Chemical Engineering Journal,2010,165(1):209-217
[21]Gu X,Su Z,Xi H.New Activated Carbon with High Thermal Conductivity and Its Microwave Regeneration Performance[J].Journal of Wuhan University of Technology-Material Science Edition,2016,31(2):328-333
[22]Yu QF.Adsorbent Preparation and Adsorption Mechanism Research for Low Concentration PH3 Adsorption Removal[D].Kunming:Kunming University of Science&Technology,2011
[23]Yu QF,Yi HH,Tang XL,et al.Adsorption and Prediction of Adsorption Isotherm onto Activated Carbon[J].Journal of Wuhan University Technology,2010;32(1):34-37
[24]Yu QF,Ning P,Yi HH,et al.Effect of Preparation Conditions on the Property Cu/AC Adsorbents for Phosphine Adsorption[J].Separation Science and Technology,2012,47:527-533
[25]Li S,Hao JM,Ning P,et al.Preparation of Cu-Fe Nanocomposites Loaded Diatomite and Their Excellent Performance in Simultaneous Adsorption/oxidation of Hydrogen Sulfide and Phosphine at Low Temperature[J].Separation and Purification Technology,2017,180(1):23-35
[26]Xu XW,Huang GQ,Qi S.Properties of AC and 13X Zeolite Modified with CuCl2 and Cu(NO3)2 in Phosphine Removal and the Adsorptive Mechanisms[J].Chemical Engineering Journal,2017,316:563-72
[27]Rothstein DP,Wu B-G,Lee TV,et al.Adsorption Isotherms and Isosteric Heats of Adsorption for Ethane,Propane,and N-butane on Polystyrene[J].Journal of Colloid and Interface Science,1985,106(2):399-409
[28]Hill T.Statistical Mechanics of Adsorption.V.Thermodynamics and Heat of Adsorption[J].The Journal of Chemical Physics,1949,17:520-535
[29]Martinez M,Torres M,Guzman C,et al.Preparation and Characteristics of Activated Carbon from Olive Stones and Walnut Shells[J].Industrial Crops and Products,2006,23(1):23-28
[30]ZahmakIran M,zkar S,Kodaira T,et al.A Novel,Simple,Organic Free Preparation and Characterization of Water Dispersible Photoluminescent Cu2O Nanocubes[J].Materials Letters,2009,63(3-4):400-402
[31]Moulder J,Chastain J.Handbook of X-ray Photoelectron Spectroscopy[M].Perkin-Elmer Eden Prairie,MN,1992
[32]Chapman A,Thirlwell L.Spectra of Phosphorus Compounds--I the Infra-red Spectra of Orthophosphates[J].Spectrochimica Acta,1964,20(6):937-947
[33]Stefov V.Infrared and Raman Spectra of Magnesium Ammonium Phosphate Hexahydrate(Struvite)and Its Isomorphous Analogues.I.Spectra of Protiated and Partially Deuterated Magnesium Potassium Phosphate Hexahydrate[J].Journal of Molecular Structure,2004,689(1-2):1-10