Nghiên cứu quá trình oxy hoá penicillin trên điện cực anốt pbo2 thép không gỉ 304 bằng phương pháp điện hoá

Tieu ban: Moi tru&ng vd Ndng lugng ISBN: 978-604-913-013-7 NGHIEN CUXJ QUA TRINH OXY HOA PENICILLIN TREN DIEN CU^C ANOT Pb02/THEP KHONG GI 304 B A N G P H U O N G PHAP DIEN HOA Dinh Thi Mai Thanh, Nguyen Thu Phu-ong, Nguyen Thi Thu Trang Vien Ky thuat nhiet doi; 18 - Hoang QuIc Viet, Cau Gidy, Ha Noi Email: thanhvktnd@vahoo.com Tom tat: Lap mg Pb02 duac tdng hap diin hda trin nin thep khdng gi 304 qua hai giai dogn: giai dogn thic nhdt dung dichpH kiem gdm NaOH 3,5M + PbO bdo hda vd giai dogn thic hai dung dich axit: Pb(N03)2 0,5M + HNO3 0,1M vdi su cd mat cua TiOi 5g/l Nhieng phdn tich cdu true hinh hpc vd thdnh phdn bdng SEM, tdn xg ndng lupng tia X da chi su cd mat cita Ti02 lap mg Pb02 Hieu sudt phdn hity penicillin Ig/l tren diin cue andt Pb02-Ti02 dgt khodng 83,8% cao hon so vdi diin cue Pb02 Kit qud ndy da cho thdy sir cd mat ciia Ti02 lap mg Pb02 da Idm tdng khd ndng xiic tdc cho qud trinh phdn hiiy pecicillin Abstract: Pb02 is eledrosynthesized on 304 stainless steel via two phases: the first phase is in alkaline pH solution including 3.5M NaOH and saturated PbO and the second stage is in solutions acidics of 0.5M Pb(N03)2 and O.IM HNO3 with the presence of Ti02 5g/l The analysis of morphology, composition, by SEM and energy dispersive X-ray showed that the presence of Ti02 on PbO2 coating Degradation efficiency of Ig/l penicillin on PbO2-TiO2 anodic electrode reached nearly 83.8% higher than PbO2 electrode The result showed that the presence of Ti02 on Pb02 coating increase catalytic capacity for the process of organic substance decomposition l.MdDAU Pb02 la oxit CO dp ben an mon cao, c6 hoat tinh xiic tac tot va qua the oxy hoa cao hon mot so dien cue tra thuong dung nhu: platin, cacbon Vi vay no co kha nang ung dung nhieu ITnh vuc (bao ve catot, san xuat oxy va ozon, xir ly moi truong ) Pb02 tong hgp tren mgt so vat lieu nen da dugc nghien cuu sir dung lam dien cue anot cho nhieu qua trinh dien phan cong nghiep Trong nhiing nghien ciiu gan day dugc thuc hien tai Phong An mon va bao ve kim loai Vien Ky thuat nhiet dod da dua them mot so ion nhu: Fe^"^, F" vao dung dich ting hgp dien boa Pb02 nham nang cao bam dinh, dp ben an mon va tinh chat xiic tac cua lop ma Pb02 [13] Vai nhiing cong bo mod nhat ciia nhom tac gia A.B.Velichenko va cong su da dua them nhiing oxit cua kim loai chuyen tiep vao de che tao vat lieu composit vai Pb02 dac biet la nhiing oxit co cau tnic nano nhu Ti02 nham cai thien kha nang xiic tac quang ciia vat lieu dl img dyng xir ly cac chat him co doc hai c6 mat nuac thai cong nghiep va nuac thai y te bang phuang phap dien hoa [4-6] Trong bai bao chiing toi nghien cim cbl tao vat lieu PbO2/TKG304 vai sir co mat va vang m^t cua Ti02 5g/l va khao sat kha nang lam dien cue anot qua trinh xir ly penicillin g/1 bang phuong phap dong ap dat 132 Hgi nghi Khoa hgc ky' niem 35 ndm Vien Khoa hgc vd Cong nghe Viet Nam - Hd Not 10/2010 DIEU KIEN T H l / C NGHIEM Thep khong gi 304 (TKG304) duoc sir dung lam vat lieu nen de tong hgp Pb02, kich thuoc 2,5x10cm, dugc danh bong ca hpc bang giay nham tho loai 240, 320 (ciia Trung Quoc) va giay nham tinh loai 600, 800, 1200 (ciia Nhat Ban) sau rira sach mau bang nuoc cat, trang lai bang con, de kho va sir dung epoxy de gioi ban dien tich lam viec 10 cm" Truoc tien hanh tong hgp Pb02, tat ca cac mau TKG304 deu dugc danli bong dien hoa dung dich NaOH + etanol ty le 1:1, vai mat dp dong ap dat 0,05A/cm^ thai gian 600 giay Lop ma Pb02 dugc tong hgp bang phuong phap dong ap dat theo bai giai doan: giai doan thii nhat tong hgp Pb02 tren TKG 304 dung dich kiem gom PbO bao boa + NaOH 3,5M a nhiet dp 40''C, thu dugc vat lieu PbO2/TKG304, nia sach bdng nuoc cat, lau kho va dugc nhiing vao dung dich axit gIm Pb(N03)2 0,5M + FINO3 0,1M voi su co mat va vang mat Ti02 5g/l de thuc hien giai doan thii bai la tong hgp Pb02 moi truang axit, a nhiet dp 25 °C, voi mat dp dong ap mA/cm^ Ca hai giai doan tong hgp Pb02 deu dugc thirc hien binh dien boa dien cue: Dien cue dli cacbon 250NG co dien tich lan hon nhieu so voi dien cue lam viec Dien cue so sanh calomen Hg/HgCl/KCl bao boa (SCE).Dien cue lam viec la TKG304 dung moi truang kilm va PbO2/TKG304 dung moi truang axit Qua trinh phan tich cdu tnic hinh hpc va phan cua lop ma Pb02 tong hgp dung dich axit dugc thuc hien tren may SEM Jeol 6490 ket hgp voi thiet bi phan tich EDX Jeol 2300 ciia Trung tam danh gia hu hong vat lieu, Vien Khoa hpc Vat lieu Qua trinh oxy boa penicillin nong dp ap dat 10 mA/cm^ tren dien cue anot penicillin qua trinh xir ly dugc spectrometer, Citra 40-My, tai Vien Ky cong thiic sau [7]: lg/1 + Na2S04 0,05M dugc thuc hien mat dp dong PbO2/TKG304 PbO2-TiO2/TKG304 Sir phan buy nghien cim bang UV-vis tren thiet bi UVthuat nhiet doi Hieu suat phan hiiy dugc tinh theo ri( %) = A z A 0 % Trong do: r| - Hieu sudt phan buy (%); Ao - cuong dp hap thu tai thoi diem ban dau; Ar cuofng dp bap thu tai thoi diem t KET QUA VA THAO LUAN 3.1 Phan tich cau triic hinh hoc va phan cua lop ma Pb02 Hinh giai thieu cdu tnic binh hpc cua be mat mau Pb02 tong hgp a mat dp dong ap mA/cm^ dung dich axit vai sir vang mat va co mat ciia Ti02 Be mat mau PbO2/TKG304 cho thdy sir tin tai ro net cua tinh the Pb02 dang hinh thoi kich thuoc thay dli tir din ^m (hinh la) Khi co mat cua Ti02, cau tnic hinh hpc ciia lop ma Pb02 duong nhu khong thay dli, nhien tren be mat quan sat thay nhiing tinh the nho mau trdng d6 co thi la Ti02 tham gia vao lop ma Pb02 Ket qua se dugc khang dinh bang phan tich tan xa tia x theo nang lupng 133 Tieu ban: Moi tru&ng vd Ndng lugng ISBN: 978-604-913-013-7 (b) (a) Hinh 1: Hinh dnh SEM cua Idp mg Pb02 tdng hop dung dich Pb(N03)2 0,5M + HNO3 0, IM vdi su vdng mat (a) vd cd mat Ti02 g/l (b) Pho tan xa tia X theo nang lugng cua hai mau Pb02 ting hgp dung dich Pb(N03)2 0,5M + HNO3 0,1M voi sir vdng mat va c6 mat Ti02 g/1 dugc chi tren hinh Tren gian dl phi chi nhiing pic dac trung cua nguyen tl O va Pb vai phdn (%>) vl khIi lugng: 7,19 % va 92,31% (hinh 2a) Khi c6 mat cua Ti02 dung dich ting hgp, tren gian dl phi ngoai hai pic cua O (7,79%) va Pb (91,49%) co pic cua Ti vai ham lugng 0,54% (hinh 2b) Kit qua khang dinh sir co mat cua Ti02 lop ma Pb02 ting hgp dung dich CO mat Ti02 5g/l 005 2400 210018001500- b Nguyin td % B O Pb ii 1200900 600 300 - % ° 11 c — AM 000 \.* ' Xi 0- 0- ^ 3.00 6.00 9.00 PbLb J khdi lupng % nguyin tir 0,49 4,85 7,19 47,8 92,31 47,35 1-^-.,, 12.00 15,00 18,00 21.00 kcV (a) ""2 i 1800- LlTiL P 1500- H £ ! 1200- 900- 1 fiOO - 300- t^ •a J Qi 0- i ^ P a PbLb 2400 2100- TiKb PbMsu 2700 J •!l 1 A „_A_ —T- \ Nguyen td B O Ti Pb % KLidi lucmg % Nguyin tir 0,18 1,76 7,79 50,9 0.54 1,18 91,49 46,16 (b) Hinh 2: Phd tdn xg ndng luang tia Xciia lop mg Pb02 tdng hop dung dich Pb(N03)2 0,5M + HNO3 0, IM vdi su vdng mat (a) vd cd mat TiOi g/l (b) 134 Hgi nghi Khoa hgc ky' niem 35 ndm Vien Khoa hoc vd Cong nghe Viet Nam - Hd Noi 10/2010 3.2 Xac dinh dien the oxy hoa penicillin Hinh giai thieu duong cong phan cue anot cua dien cue PbO2/TKG304 va Pb02TiO2/TKG304, dung dich Na2S04 0,05 M (duong net diit) va dung dich NajSOa 0,05M + penicillin lg/1 (duong net liln) Tiln hanh.phan cue khoang tbi tir dien the can bang den 2,5V/SCE voi tic quet thi la mV/S Trong khoang dien thi din 1,5 V/SCE, mat dp dong gan nhu bang khong xay phan ung oxy h6a dli vod ca hai dung dich dien thi lan hon 1,51 V/SCE, mat dp dong dien tang manh theo sir tang dien thi co qua trinh oxy boa nuac (doi vod dung dich Na2S04 0,05 M) va sir oxy hoa dong thai nuac va penicilin tren be mat dien cue (dli vai dung dich Na2S04 0,05M + penicillin lg/1) 3.3 Xac dinh duong chuan cua penicillin bdng phuong phap trdc quang Hinh the hien su thay doi dp hap thu cue dai tai buac song 335 nm theo nIng dp ciia peniccilin 0,1 den g/1 Khi nIng dp tang, dp hdp thu cue dai tang len, nhien sir tang khong tuyen tinh tuyet dli thi hien a cac nIng dp 0,2; 0,4; 0,7 va lg/1 Tir 10 dilm gia tri thuc nghiem da xac dinh dugc duong thang tuyIn tinh gdn diing gpi la duang chudn ciia penicilin voi phuong trinh duong thdng y = l,2863x + 0,16093 va he s l tuyIn tinh R^ = 0,99598 Dua vao phuong trinh co the xac dugc nIng dp penicilin sau tiln hanh xir ly bdng phuang phap dien boa 30- 25- 25- / 20- 159 / / / / / 20- / ^ / ^' 000 — // 5- 0.5 1.0 // 10- £ 10- — 15J E // /' 5- ^' 0- 1.5 2.0 / / / ' / / // 2.5 0.5 1.0 E (V/SCE) 1.5 2.0 2.5 E (V/SCE) Anot PbO2/TKG304 Anot PbO2-TiO2/TKG304 Hinh 3: Dudng cong phdn cue andt cua logi dien cue Pb02 dung dich Na2S04 0,05 M (dudng net diet) vd Na2S04 0,05 M+penicillin Ig/l (dudng net liin) 1.41.2- m y ^ 1.00.8^ / 0.60.4- n ?0.0 y = 1,286 3x + 0.16093 R^ =0,99598 ^/W 0.2 ' — 0.4 0.6 0.8 1.0 Nong penicillin (g/l) Hinh 4: Dudng chudn ciia penicillin 135 ISBN: 978-604-913-013-7 Tieu ban: Moi tru&ng vd Ndng lugng 3.4 Xu- ly penicilin bdng phu-ong phap ap dong Hai loai vat lieu PbO2/TKG304 va PbO2-TiO2/TKG304 dugc sir dung lam anot qua trinh oxy boa 200 ml dung dich penicilin lg/1 + Na2S04 0,05M a mat dong mA/cm^ Bang thi hien hdp thu cue dai a buac song 355 nm cua hai mau dung dich dugc xir ly thai gian gio bdng phuang phap dien boa tren dien cue anot PbO2/TKG304 va PbO2-TiO2/TKG304 Dli voi dung dich sir dung anot PbO2-TiO2/TKG304 co hdp thu nho hon so voi dung dich sir dung anot PbO2/TKG304 Bdng 1: Su thay ddi dd hdp thu ciia penicilin d buac sdng 335nm sau gio oxy hda a mat dd ddng dp ddt 5mA/cm^ trin andt PbO2/TKG304 vd PbO2-TiO2/TKG304 Dd hdp thu cue dgi (d buac sdng 335 nm) Thdi gian diin phdn (gicf) PbO2-TiO2/TKG304 PbO2/TKG304 1,418 0,349 0,229 Dua vao phuang trinh duong chuan xac dinh dugc nong cua penicillin sau gia tien hanh oxy boa tren dien cue anot PbO2/TKG304 va PbO2-TiO2/TKG304 tuong ung la 0,146 g/1 va 0,053 g/1 Hieu sudt phan buy penicillin tren dien cue anot PbO2-TiO2/TKG304 (83,8%) cao hon tren dien cue anot PbO2/TKG304 (75,4%)) Dieu khang dinh kha nang xuc tac dien hoa cua dien cue anot Pb02 voi su c6 mat cua Ti02 Bdng 2: Ndng dd vd hiiu xudt phdn huy penicilin sau gio oxy hda d mat dp ddng dp ddt mA/cm Thdi gian diin phdn (gior) Ndng dp penicilin (g/l) PbO2/TKG30 PbO2/TKG304 PbO2-TiO2/TKG304 Hiiu xudt phdn hiiy (%>) 0,146 PbO2-TiO2/TKG304 0,053 75,4 83,8 KET LUAN Da tong hgp cong Pb02 tren nen thep khong gi qua hai giai doan: giai doan thii nhat dung dich kiem va giai doan thii hai dung dich axit vai su co mat va vdng mat Ti02 5g/l Ket qua phan tich SEM ket hgp voi tan xa tia X theo nang lugng cho thdy sir CO mat cua Ti02 lop ma Pb02 Qua trinh oxy boa penicillin lg/1 a mat dong ap dat mA/cm^ tren hai loai dien cue anot PbO2/TKG304 va PbO2-TiO2/TKG304 cho thdy sau gia tiln hanh oxy boa, hieu sudt phan huy peicillin tren dien cue PbO2-TiO2/TKG304 la 83,8%) cao han so vai truang hgp sir dung anot PbO2/TKG304 Ket qua khdng dinh kha nang xiic tac dien hoa cua Ti02 lap ma Pb02 qua trinh xir ly cac hgp chdt hiiu ca 136 Hgi nghi Khoa hgc ky niem 35 ndm Vien Khoa hgc vd Cong nghe Viet Nam - Hd Noi 10/2010 TAI LIEU THAM KHAO Nguyen Thi Nggc Diep, "Luan vdn thge si hda hpc ", Truong DH Su pham Ha Noi, nam 2009 Dinh Thi Mai Thanh, Mai Xuan Huong, Dang Vii Minh, "Study the process of electrosynthesis and physieochemical properties of Co-Pb02 catalytic electrode", Vietnamese Journal of Science and Technology, (2006), Vol 44 (5), p 77-82 Dinh Thi Mai Thanh, "Su dnh hudmg ciia ion Fe^^ vd F den qud trinh tdng hpp dien hod Pb02 ", Tap chi Hoa hgc Tap 48, sl (2010), tr 99-104 A.B Velicbenko, R.Amadelli, V.A Knysb, T.V Luk'yanenko, F.I.Danilov, "Kinetics of lead dioxide electrodeposition from nitrate solutions containing colloidal Ti02 ", Journal of electroanalytical 632 (2009) 192-196 R Amadelli, L Samiolo, A.B.Vehchenko, V.A.Knysh, T.V.Luk'yanenko, F.I.Danilov, "Composite Pb02-Ti02 materials deposited from colloidal electrolyte: Electrosynthesis and physieochemical properties", Electrochimica Acta 54 (2009) 5239-5245 Yuehai Song, Gang Wei, Rongchun Xiong, "Structure and properties of Pb02-Ce02 anodes on stainless steel", Electrochimica Acta 52 (2007)7022-7027 Minghua Zhou, Qinghong Yu, Lecheng Lei, Geoff Barton, "Electro-Fenton method for the removal of methyl red in an eficient electrochemical systeme, Separation and Purification", Technology 57 (2007) 380-387 137 ... 335nm sau gio oxy hda a mat dd ddng dp ddt 5mA/cm^ trin andt PbO2/ TKG304 vd PbO2- TiO2/TKG304 Dd hdp thu cue dgi (d buac sdng 335 nm) Thdi gian diin phdn (gicf) PbO2- TiO2/TKG304 PbO2/ TKG304 1,418... cua penicillin sau gia tien hanh oxy boa tren dien cue anot PbO2/ TKG304 va PbO2- TiO2/TKG304 tuong ung la 0,146 g/1 va 0,053 g/1 Hieu sudt phan buy penicillin tren dien cue anot PbO2- TiO2/TKG304... dien boa tren dien cue anot PbO2/ TKG304 va PbO2- TiO2/TKG304 Dli voi dung dich sir dung anot PbO2- TiO2/TKG304 co hdp thu nho hon so voi dung dich sir dung anot PbO2/ TKG304 Bdng 1: Su thay ddi dd