石炭灰フライアッシュから合成したゼオライトの水質 Title 浄化作用. 高見, 優子, 村山, 憲弘, 小川, 和男, 山本, 秀樹, Author(s) 芝田, 隼次. Citation 資源と素材 : 資源素材学会誌, 116(9):

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石炭灰フライアッシュから合成したゼオライトの水質 Title 浄化作用高見, 優子, 村山, 憲弘, 小川, 和男, 山本, 秀樹, Author(s) 芝田, 隼次 Citation 資源と素材 : 資源素材学会誌, 116(9): 789-794 Issue Date 2000 URL http://hdl.handle.

1 石炭灰フライアッシュから合成したゼオライトの水質 Title 浄化作用高見, 優子, 村山, 憲弘, 小川, 和男, 山本, 秀樹, Author(s) 芝田, 隼次 Citation 資源と素材 : 資源素材学会誌, 116(9): Issue Date 2000 URL 資源素材学会 ( Rights se/shigentosozai/_vols/-char/ja) Type Journal Article Textversion publisher Kansai University

2 (Shigen to Sozai) Vol.116 p (2000) f* Water Purification Property of Zeolite Synthesized from Coal Fly Ash by Yuko TAKAMI 1, Norihiro MURAYAMA 2, Kazuo OGAWA 2 Hideki YAMAMOTO 1 and Junji SHIBATA 1 1. Department of Chemical Engineering, Faculty of Engineering, Kansai University, Suita-shi R&D Department, Kimura Chemical Plants Co., Ltd., Amagasaki-shi Cation exchange properties of K and Ca type zeolites were investigated using Na type zeolite synthesized from coal fly ash under hydrothermal conditions. The caion exchange capacity (CEC) of the Na type zeolite was about 300 meq / 100 g. The cation exchange amount of Ca type zeolite substituted from Na type zeolite was measured for NH 4 and PO 4 3 in order to evaluate the efficiency of zeolite as a water purification agent. Na type zeolite was exchanged with K and Ca 2 in the ph region of around 7. The exchanged amount of K did not depend on the kinds of anion in the aqueous solution, while the amount of exchanged Ca 2 depended on them. It was found that the substitution percentage from Na to Ca 2 reached to about 90 % of CEC, if the cation exchange operation was repeated. In the cation exchange reaction for NH 4, Na type zeolite exchanged much more NH 4 than Ca type zeolite. InthecaseofPO 4 3, Ca type zeolite removed PO 4 3 from the aqueous solution by the precipitation reaction between Ca 2 released from the zeolite and PO 4 3 in the solution. On the other hand, Na type zeolite could not remove PO 4 3 from the aqueous solution. In the adsorption behaviors of NH 4 and PO 4 3 from the mixed aqueous solution with Ca type zeolite, approximately 90 % and 46 % removal was accomplished for NH 4 and PO 4 3, respectively. The ion of PO 4 3 was precipitated quantitatively with Ca 2 released from Ca type zeolite in the solution. KEY WORDS Coal Fly Ash, Zeolite, Alkali Hydrothermal Reaction, Water Purification, Eutrophication, Ion Exchange 1 É iû û š 1) í» îå Ž 2) 5) í 6) 9) É Àç š 10) Âšù j Si Al SiO 4 AlO Ò 1. p p 2. ( ) å 3. ( ) å 4. p ¼± 5. p ¼± [ ] FAX ( pø î ) í ç { å å ph { 11) (Cation Exchange Capacity, CEC) (Si / Al) Â Â ï î 10) î û šå í çêš Ân 2 í 7)8) 10) Fig.1 ñ g ( ù ) ³ Š

{ Fig. 1 Flow diagram of zeolite manufacturing process and ion removal process. g ( ù ) gg Àç 10)12) ( ç ù ) ù 3 3 1 í ( )å 7) í åå JIS j 2.

0 g (2 200eq/m 3 )K Ca 2 40 cm 3 ºª É Na K Ca 2 KNO 3 KCl K 2 SO 4 CH 3 COOK Ca(NO 3 ) 2 CaCl 2 (CH 3 COO) 2 Ca ½ Na K Ca 2 ~ ç» 100 g ½ (meq/100g) å (ICPS 1000 III ( ) ) ~ 3 3 ç 3 1 g 3 2 g 1.

3 { Fig. 1 Flow diagram of zeolite manufacturing process and ion removal process. g ( ù ) gg Àç 10)12) ( ç ù ) ù í ( )å 7) í åå JIS j 2.0 mol / dm g 400 cm 3 ½ 800 cm 3 ºª 393 K 3 À ºª 500 rpm î 7) P g 3 2 Fig.1 ñî å gg n À Na Ca 2 ³ Ca 2 K Êš 3 1 g 1.0 g (2 200eq/m 3 )K Ca 2 40 cm 3 ºª É Na K Ca 2 KNO 3 KCl K 2 SO 4 CH 3 COOK Ca(NO 3 ) 2 CaCl 2 (CH 3 COO) 2 Ca ½ Na K Ca 2 ~ ç» 100 g ½ (meq/100g) å (ICPS 1000 III ( ) ) ~ 3 3 ç 3 1 g 3 2 g 1.0 g NH 4 3 PO 4 40 cm 3 ³ NH 4 PO 3 4 ç NH 4 Cl H 3 PO ç» 100 g ½ (meq/100g) NH 4 (DX 500, 3 ) PO 4 å (ICPS 1000 III ( ) ) ~ 3 4 íéš ~ Â ní SEM æµ Â ~ g { (S 2400, û ) ½g X (JDX 3530S, { ) X (JDX 3530S, { ) í Éšl 7) Table 1 Fig.2( å 7) ) g P g Éš SEM æ ñ CEC meq / 100 g p ( ) ) CEC ~ 14) m 2 /g Table 1 Physical properties of synthesized zeolite (zeolite P) Fig. 2 SEM photograph of Na zeolite synthesized from coal fly ash. Š ƒ

$3 Effect of equilibrium ph on the amount of Al eluted from zeolite and X-ray diffraction$ intensity of zeolite P. 50 1 100 mm Ž 25 mm SEM æ (Fig.

3 ñph Â ï Â í ph P g X ph4 ph4 š Â ˆ ñâˆì SEM æ Fig.

4 Surface structure of zeolite broken by H. Fig.

4 í Fig. 3 Effect of equilibrium ph on the amount of Al eluted from zeolite and X-ray diffraction intensity of zeolite P mm Ž 25 mm SEM æ (Fig.2) ÂÉg 4 2 ph g Éš Table 1 ñ CEC 300 meq / 100 g p Si / Al å {Â ïš Êš ph ph X n Fig.3 ñph Â ï Â í ph P g X ph4 ph4 š Â ˆ ñâˆì SEM æ Fig.4 ñâ{dï Ì å g 1 (Na ) 1 (K ) ph HCl n K Na ph Fig.5 ñph7 Fig. 4 Surface structure of zeolite broken by H. Fig. 5 Effect of ph on the amount of K adsorbed on zeolite and Na released from zeolite. Fig. 6 Effect of ph on the amount of Ca 2 adsorbed on zeolite and Na released from zeolite. K Na 200 meq / 100 g ~ ñé» ûk Na ~ å ph5 ph Na K ph iâ ï Na» K { 1 (Na ) 2 (Ca 2 ) Ca 2 Na ph Fig.6 ñph8.5 Ca 2 Na i Ca 2 É Ca 2 çé Ca 2 ph4 6 ph Na Ca 2 ph4 Ca 2 Š

{ Ca 2 ñî 7) í m{ Â o Â ï Ca 2 Ca 2 å Ca 2 ph6 i Fig.5, 6 K ph5 Ca 2 ph6 Â ï K Ca 2 š å š ph7 4 3 Êš {Âï Na K nm Fig.7 ñ K 180 200 meq / 100 g K SO 2 4 Na K Na K Fig.

5 { Ca 2 ñî 7) í m{ Â o Â ï Ca 2 Ca 2 å Ca 2 ph6 i Fig.5, 6 K ph5 Ca 2 ph6 Â ï K Ca 2 š å š ph7 4 3 Êš {Âï Na K nm Fig.7 ñ K meq / 100 g K SO 2 4 Na K Na K Fig.8 ñ K Na K Na K É» û Na K Âï Na Ca 2 nm Fig.9 ñ CaCl 2 Ca meq / 100 g ñ Ca(NO 3 ) 2 (CHCOO) 2 Ca Ca 2 80 meq /100g Ca 2 Ca 2 Ca 2 Âï š Na Ca 2 Na Ca 2 Fig. 7 Adsorption isotherm of K for zeolite at 298 K and amount of Al dissolved from zeolite in various solutions. Fig. 9 Adsorption isotherm of Ca 2 for zeolite at 298 K and amount of Al dissoled from zeolite in various solutions. Fig. 8 Exchange isotherm for Na K system in zeolite. Fig. 10 Exchange isotherm for Na Ca 2 system in zeolite. Š

6 í Fig.10 ñ Ca 2 i Na Ca 2 Ca 2 i Na Ca 2 Fig.6 ñ (a) Ca 2 É 4 4 ½ Ca 2 Ca 2 CEC Ca 2 m Ca 2 Fig.11 ñm 5 Ca 2 CEC Ca 2 (75 meq / dm 3 ) Ca 2 mà š Ca 2 Ca meq / 100 g 73 % Ca 2 (1,000 meq / dm 3 ) mš Ca 2 Ca meq / 100 g 94 % ñ Ca 2 { î 9) ç 90 % Ca çêš ggnh 4 Fig.12 ñg g NH 4 NH 4 ñ 1 g NH meq / 100 g 70 % g 290 meq / 100 g NH 4 96 % g g NH 4 š Ca 2 2 ½m NH % šåå Fig. 11 Cation exchange behavior of zeolite between Na and Ca 2 in batch operation. Fig. 12 Cation exchange behavior of NH 4 with synthesized zeolites. Fig. 13 Adsorption of PO 4 3 with synthesized zeolite and amount of Al eluted from zeolite. gg PO 4 3 ç Fig.13 ñ PO ppm g PO 3 4 ç 72.2 ppm ñ g PO 3 4 ç g PO ,000 ppm 15,000 ppm (ph3.7 ) g Âï gm PO 3 4 5,000 ppm ph5.6 PO 3 4 ç å g PO 3 4 ç ph ÂˆÂ Ca 2 PO 3 4 g NH 3 4 PO 4 5ppm çnh 4 90 % NH 4» Ca 2 PO 3 4 ~ å PO % PO 3 4 Š

7 { g À» Ca 2» Ca 2 ph7 ~ å 5 í gû šå Êš NH 4 PO 3 4 çêš g K Ca 2 p NH 4 g g o PO 3 4 g» Ca 2 3 PO 4 g PO 3 4 ç NH 4 PO3 4 NH 4 90 % NH 4» Ca 2 3 ~ å PO 4 Ð 1) Øí ( ÿ 2 È ), p.ii 1 II 12, (1995) 2)É å p , (1994) 3) Querol, X., Plana, F., Alastuey, A. and Lopez-Soler, A. Fuel,Vol.76,No.8,p , (1997) 4) lin, C. F. and Hsi, H. C. Environmental Science and Technology, Vol. 29, No. 4 p , (1995) 5) Amrhein, C., Haghnia, G.H., Kim, T.S., Mosher, P.A., Gagajena, RC., Amanios, T. and De La Torre, L. Environmental Science and Technology, Vol. 30, No. 3, p , (1996) 6) í Vol.116,No.1,p.31 36, (2000) 7) Vol. 115, No. 13 p , (1999) 8) Vol. 116, No.6,p , (2000) 9) Vol. 116, No. 4, p , (2000) 10){ 12 p p. 23, (2000) 11)p ò (1987) 12) ¾ { Vol. 4, p , (1997) 13) É ÿ 111 w pî 14)p Vol. 33, No. 2, p , (1989) Š

Effective Synthesis of Artificial Zeolite from Coal Fly Ash

Effective Synthesis of Artificial Zeolite from Coal Fly Ash Introduction Large quantities of coal are used in power plants around the world every year. The disposal of the huge amount of coal fly ash (CFA)

石炭灰フライアッシュから合成したゼオライトの水質 Title 浄化作用. 高見, 優子, 村山, 憲弘, 小川, 和男, 山本, 秀樹, Author(s) 芝田, 隼次. Citation 資源と素材 : 資源 素材学会誌, 116(9):

石炭灰フライアッシュから合成したゼオライトの水質 Title 浄化作用. 高見, 優子, 村山, 憲弘, 小川, 和男, 山本, 秀樹, Author(s) 芝田, 隼次. Citation 資源と素材 : 資源素材学会誌, 116(9):