Hoạt động thương mại và truyền giáo của Bồ Đào Nha ở Ấn Độ, Trung Quốc (thế kỷ XVI-XIX).

Header Page of 89 VIN HN LM KHOA HC V CễNG NGH VIT NAM HC VIN KHOA HC V CễNG NGH Lấ TH MAI HOA NGHIấN CU TNG HP V C TRNG VT LIU MI, CU TRC NANO NG DNG TRONG QUANG HểA XC TC PHN HY THUC NHUM LUN N TIN S HểA HC Chuyờn ngnh: Húa lý thuyt v Húa lý Mó s: 62.44.01.19 Ngi hng dn khoa hc: PGS.TS V Anh Tun H ni, nm 2016 Footer Page of 89 Header Page of 89 LI CM N Trc ht, em xin trõn trng cm n n PGS.TS V Anh Tun v cỏc thy, cụ giỏo ó tn tỡnh hng dn v truyn t kin thc, kinh nghim, h tr v giỳp em sut quỏ trỡnh em thc hin lun ỏn Tụi xin chõn thnh cm n th cỏn b phũng Húa lý B mtVin Húa hc- Vin Hn lõm Khoa hc v Cụng ngh Vit Nam ó nhit tỡnh giỳp tụi thi gian thc hin cỏc ni dung ca lun ỏn Tụi xin chõn thnh cm n sõu sc ti gia ỡnh, bn bố, ng nghip ti V Giỏo dc v o to, Dy ngh, Ban Tuyờn giỏo Trung ng ó quan tõm, ng viờn v to iu kin thun li giỳp tụi sut thi hc v nghiờn cu Tỏc gi lun ỏn Lờ Th Mai Hoa Footer Page of 89 i Header Page of 89 LI CAM OAN Tụi xin cam oan, õy l cụng trỡnh nghiờn cu tụi thc hin di s hng dn ca ngi hng dn khoa hc Mt s nhim v nghiờn cu l thnh qu th ó c cỏc ng s cho phộp s dng Cỏc s liu v kt qu trỡnh by lun ỏn l trung thc v cha tng cụng b bt k cụng trỡnh lun ỏn no khỏc Tỏc gi lun ỏn Lờ Th Mai Hoa Footer Page of 89 ii Header Page of 89 DANH MC CC T VIT TT GO Graphen oxit GOVS Graphen oxit búc lp bng vi súng GOSA Graphen oxit búc lp bng siờu õm rGO Graphen oxit kh v graphen AOPs H2O2 Phng phỏp oxy húa nõng cao (Advanced Oxidation Processes) Hydrogen peroxide *OH Hydroxyl TS Tng lng cht rn (Total Solids) SS Cht rn huyn phự (Suspended Solid) DO Hm lng oxy hũa tan (Disolved oxigen) BOD Nhu cu oxi húa sinh hc (Biochemical oxigen Demand) COD Nhu cu oxi húa hc (Chemical oxigen Demand) TOC Tng cacbon hu c (Total Organic Carbon) TOD Nhu cu oxy tng cng (Total Oxygen Demand) Fe3O4-GO Fe3O4 bc Graphen oxit (GO) CoFe2O4-GO Coban (Co), Fe2O4 bc Graphen oxit (GO) ZnFe2O4-GO Km (Zn), Fe2O4 bc Graphen oxit (GO) Fe0-Fe3O4-GO Fe, Fe3O4 bc Graphen oxit (GO) Fe(III)-GO Fe(III) oxo cluster Graphen oxit (GO) CVD Phng phỏp lng ng pha hi húa hc CNTs ng nano cacbon XRD Ph nhiu x Rnghen (X-ray Diffraction) FTIR BT Quang ph hng ngoi (Fourier Transform Infrared Spectroscopy) Ph in t quang tia X (X-ray Photoelectron Spectroscopy) Kớnh hin vi in t truyn qua (Transmission electron microscopy) Kớnh hin vi in t truyn qua phõn gii cao (High resolution Transmission electron microscopy) ng nhit hp ph kh nitrogen (Braunauer Emmett Teller) UV-Vis Ph hp th t ngoi kh kin VMS Phng phỏp xỏc nh t tớnh ca vt liu bng t k mu rung (Vibrating Sample Magnetometer) XPS TEM HR-TEM Footer Page of 89 iii Header Page of 89 DANH MC CC HèNH V Hỡnh 1.1 Hỡnh 1.2 Hỡnh 1.3 Hỡnh 1.4 Hỡnh 1.5 Hỡnh 1.6 Hỡnh 1.7 Hỡnh 1.8 Hỡnh 1.9 Hỡnh 1.10 Hỡnh 1.11 Hỡnh 1.12 Hỡnh 1.13 Hỡnh 2.1 Hỡnh 2.2 Hỡnh 2.3 Hỡnh 2.4 Hỡnh 2.5 Hỡnh 2.6 Hỡnh 2.7 Hỡnh 2.8 Hỡnh 2.9 Hỡnh 2.10 Hỡnh 2.11 Hỡnh 2.12 Hỡnh 2.13 Hỡnh 2.14 Footer Page of 89 Graphen - vt liu cú cu trỳc c bn (2D) cho cỏc vt liu cacbon khỏc (0D, 1D, v 3D) Cỏc liờn kt ca mi nguyờn t cacbon mng graphen Phng phỏp tỏch lp graphit bng bng dớnh C ch to mng graphen bng phng phỏp nung nhit SiC Quỏ trỡnh oxi húa t graphit thnh GO (a) v quỏ trỡnh kh GO bng hydrazine (b) c xut C ch ngh ca quỏ trỡnh tng hp GO v graphen Nc thi dt nhum Cụng thc cu to ca RR195 Cỏc phng phỏp loi b mu thuc nhum Phn ng Fenton ng th v Fenton d th C ch phn ng ca TiO2/graphen vi Methylene blue C ch phn ng ca ZnO vi cỏc cht hu c C ch phn ng ca Fe3O4/graphen vi cỏc cht hu c S tng hp graphen oxit vi súng (GOVS) v graphen oxit siờu õm (GOSA) t graphen oxit S tng hp Fe3O4-GO S tng hp CoFe2O4-GO S tng hp ZnFe2O4-GO S tng hp Fe0-Fe3O4-GO ng chun v ph UV-Vis ca thuc nhum RR195 th lgC theo t i vi phn ng bc S chựm tia ti v chựm tia nhiu x trờn tinh th tự ca pic phn x gõy kớch thc ht Quỏ trỡnh phỏt quang in t Nguyờn tc phỏt x tia X dựng ph S nguyờn lý s to nh phõn gii cao HRTEM Cỏc dng ng ng nhit hp ph-kh hp ph theo phõn loi IUPAC Bc chuyn ca cỏc electron phõn t iv 10 12 13 14 15 19 31 41 42 44 46 47 48 50 51 52 55 57 57 59 61 63 64 65 Header Page of 89 Hỡnh 3.1 Hỡnh 3.2 Hỡnh 3.3 Hỡnh 3.4a Hỡnh 3.4b Hỡnh 3.5 Hỡnh 3.6 Hỡnh 3.7 Hỡnh 3.8 Hỡnh 3.9 Hỡnh 3.10 Hỡnh 3.11 Hỡnh 3.12 Hỡnh 3.13 Hỡnh 3.14 Hỡnh 3.15 Hỡnh 3.16 Hỡnh 3.17 Hỡnh 3.18 Hỡnh 3.19 Hỡnh 3.20 Hỡnh 3.21 Hỡnh 3.22 Hỡnh 3.23 Hỡnh 3.24 Hỡnh 3.25 Footer Page of 89 Gin XRD ca graphen oxit v graphen nh HR-TEM ca GOSA (graphen siờu õm) (a), GOVS (graphen vi súng) (b) v rGO (c) Ph FT-IR ca GOSA, GOVS v rGO sau tng hp Ph XPS ca GOSA (a,b), GOVS (c,d) v rGO (e,f) Ph XPS ca rGOSA kh nhit t GOSA Gin XRD ca graphen oxit (GO) Gin XRD ca Fe3O4-GO Gin XRD ca CoFe2O4-GO Gin XRD ca ZnFe2O4 GO Gin XRD ca Fe0-Fe3O4-GO Gin XRD ca GO v Fe(III)-GO nh HR- TEM ca Fe3O4-GO vi phúng i khỏc nh HR- TEM ca CoFe2O4-GO nh HR- TEM ca ZnFe2O4 -GO nh HR- TEM ca Fe0-Fe3O4-GO nh HR- TEM ca Fe(III)-GO vi cỏc phúng i khỏc Ph FTIR ca Fe3O4-GO Ph FTIR ca CoFe2O4-GO Ph FTIR ca ZnFe2O4-GO Ph FTIR ca Fe0-Fe3O4-GO Ph FTIR ca Fe(III)-GO v GO Ph XPS ca Fe3O4-GO: (a)- Ph XPS tng ca Fe3O4-GO; (b)- Ph XPS Fe2p tỏch ca Fe3O4-GO; (c)- Ph XPS O1s tỏch ca Fe3O4-GO; (d) Ph XPS C1s tỏch ca Fe3O4-GO Ph XPS ca Fe0-Fe3O4-GO: (a)- Ph XPS tng ca Fe0Fe3O4-GO; (b)- Ph XPS Fe2p tỏch ca Fe0- Fe3O4-GO; (c)Ph XPS O1s tỏch ca Fe0-Fe3O4-GO; (d) Ph XPS C1s tỏch ca Fe0-Fe3O4-GO Ph XPS ca vt liu Fe(III)- GO: (a)- Ph XPS tng ca Fe(III)-GO; (b)- Ph XPS O1s tỏch ca Fe(III)-GO; (c)- Ph XPS Fe2p tỏch ca Fe(III)-GO; (d) Ph XPS C1s tỏch ca Fe(III)-GO Phõn b mao qun ca Fe0-Fe3O4-GO v Fe3O4-GO ng ng nhit hp ph - kh hp ph N2 ca Fe0-Fe3O4- v 67 68 69 71 72 73 74 75 76 76 77 78 78 79 79 80 81 81 82 83 83 84 85 87 88 88 Header Page of 89 Hỡnh 3.26 Hỡnh 3.27 Hỡnh 3.28 Hỡnh 3.29 Hỡnh 3.30 Hỡnh 3.31 Hỡnh 3.32 Hỡnh 3.33 Hỡnh 3.34 Hỡnh 3.35 Hỡnh 3.36 Hỡnh 3.37 Hỡnh 3.38 Hỡnh 3.39 Hỡnh 3.40 Hỡnh 3.41 Hỡnh 3.42 Hỡnh 3.43 Hỡnh 3.44 Hỡnh 3.45 Footer Page of 89 GO v Fe3O4-GO ng ng nhit hp ph - kh hp ph N2 ca ZnFe2O4-GO Phõn b mao qun ca ZnFe2O4-GO ng cong t tr ca Fe0-Fe3O4-GO v Fe3O4-GO ng cong t tr ca ZnFe3O4-GO Hot tớnh quang xỳc tỏc Fe3O4-GO S ph thuc chuyn húa theo thi gian phn ng cỏc iu kin khỏc ca CoFe2O4 GO bn xỳc tỏc qua cỏc ln chy phn ng quỏ trỡnh phõn hy RR195 trờn CoFe2O4-GO Ph UV_Vis quỏ trỡnh phõn hy RR195 di iu kin chiu x (A) v khụng chiu x (B) trờn CoFe2O4-GO S ph thuc chuyn húa theo thi gian phn ng cỏc iu kin khỏc ca ZnFe2O4-GO bn xỳc tỏc qua cỏc ln chy phn ng khỏc quỏ trỡnh phõn hy RR195 trờn ZnFe2O4-GO Ph UV_Vis quỏ trỡnh phõn hy RR195 di iu kin chiu x trờn ZnFe2O4-GO Ph UV_Vis quỏ trỡnh phõn hy RR195 di iu kin khụng chiu x trờn ZnFe2O4-GO S ph thuc chuyn húa theo thi gian phn ng cỏc iu kin khỏc trờn Fe0 -Fe3O4-GO Hot tớnh xỳc tỏc ca Fe0-Fe3O4-GO v Fe304-GO Ph UV_Vis quỏ trỡnh phõn hy RR195 di iu kin chiu x trờn Fe0-Fe3O4-GO Ph UV_Vis quỏ trỡnh phõn hy RR195 di iu kin khụng chiu x trờn Fe0-Fe3O4-GO bn xỳc tỏc qua cỏc ln chy phn ng quỏ trỡnh phõn hy RR195 trờn Fe0-Fe3O4-GO S ph thuc chuyn húa theo thi gian phn ng cỏc iu kin khỏc trờn Fe(III)-GO S ph thuc t l nng C/C0 ca thuc nhum hot tớnh RR195 theo thi gian phn ng cỏc iu kin khỏc trờn CoFe2O4-GO S ph thuc t l nng C/C0 ca thuc nhum hot tớnh vi 89 90 91 92 94 95 97 97 98 99 100 100 101 103 103 104 104 106 108 109 Header Page of 89 RR195 theo thi gian tip xỳc trờn CoFe2O4-GO ln v ln Hỡnh 3.46 Hỡnh 3.47 Hỡnh 3.48 Hỡnh 3.49 Hỡnh 3.50 Hỡnh 3.51 Hỡnh 3.52 Hỡnh 3.53 Hỡnh 3.54 Hỡnh 3.55 Hỡnh 3.56 Footer Page of 89 Quỏ trỡnh phõn hy RR195 trờn cỏc loi xỳc tỏc khỏc Fe(III)-GO; Fe0-Fe3O4-GO; CoFe3O4-GO; ZnFe2O4-GO; Fe3O4-GO Kh nng t phõn hy ca RR195 mụi trng pH khỏc vi s cú mt H2O2 nh hng pH n kh nng phõn hy RR195 trờn Fe0-Fe3O4GO nh hng ca nng H2O2 n quỏ trỡnh phõn hy RR195 trờn Fe0-Fe3O4-GO nh hng ca nng RR195 ban u n quỏ trỡnh phõn hy RR195 trờn Fe0-Fe3O4-GO ng hc quỏ trỡnh xỳc tỏc quang húa phn ng phõn hy RR195 trờn Fe(III)-GO bc ng hc quỏ trỡnh xỳc tỏc quang húa phn ng phõn hy RR195 trờn Fe(III)-GO bc ng hc quỏ trỡnh xỳc tỏc quang húa phn ng phõn hy RR195 trờn Fe(III)-GO bc ng hc quỏ trỡnh xỳc tỏc quang húa phn ng phõn hy RR195 trờn Fe0-Fe3O4-GO bc ng hc quỏ trỡnh xỳc tỏc quang húa phn ng phõn hy RR195 trờn Fe0-Fe3O4-GO bc ng hc quỏ trỡnh xỳc tỏc quang húa phn ng phõn hy RR195 trờn Fe0-Fe3O4-GO bc vii 111 112 113 114 115 117 118 118 120 120 121 Header Page of 89 DANH MC CC BNG Bng 1.1 Bng 1.2 Bng 1.3 Bng 1.4 Bng 1.5 Bng 1.6 Bng 1.7 Bng Bng 3.1 Bng 3.2 Bng 3.3 Bng 3.4 Bng 3.5 Bng 3.6 Footer Page of 89 Tớnh cht ca Graphen n lp u v nhc im ca mt s phng phỏp x lý cỏc hp cht hu c cú mu Th oxi hoỏ ca mt s tỏc nhõn oxi hoỏ thng gp Mt s phng phỏp AOPs ph bin hin ang s dng x lý nc thi Bng thng kờ mt vi nghiờn cu v TiO2/graphen Bng thng kờ mt vi nghiờn cu v oxit kim loi/graphen Bng thng kờ mt vi nghiờn cu v hn hp oxit/graphen Túm tt phn ng bc 0, 1, v n Thnh phn % cỏc nguyờn t ph XPS ca GO v rGO Cỏc thụng s c trng ca Fe3O4-GO Cỏc thụng s c trng ca Fe0-Fe3O4-GO Cỏc thụng s c trng ca ZnFe2O4-GO Nng RR195 trc v sau quỏ trỡnh quang phõn s dng xỳc tỏc Fe(III)-GO ti cỏc nng khỏc Nng RR195 trc v sau quỏ trỡnh quang phõn s dng xỳc tỏc Fe0-Fe3O4-GO ti cỏc nng khỏc viii 19 27 29 39 42 45 54 73 89 89 90 116-117 119 Header Page 10 of 89 MC LC LI CM N i LI CAM OAN ii DANH MC CC T VIT TT iii DANH MC CC HèNH V iv DANH MC CC BNG viii T VN CHNG TNG QUAN TI LIU 1.1 Vt liu graphen v ng dng x lý cht mu 1.1.1 Vt liu trờn c s graphen 1.1.2 Tõm hot ng ca graphen v graphen oxit 1.1.3 Cỏc phng phỏp tng hp graphen 1.1.3.1 Phng phỏp tỏch c hc 1.1.3.2 Phng phỏp epitaxy C ch phõn hy nhit C ch to mng graphen 1.1.3.3 Phng phỏp húa hc 11 1.2 Cht mu hu c v phng phỏp x lý 13 1.2.1 Gii thiu v ụ nhim cht mu hu c 13 1.2.1.1 Thuc nhum 14 1.2.1.2 Cỏc thụng s ỏnh giỏ nc thi dt nhum 15 1.2.2 Cỏc phng phỏp x lý thuc nhum hot tớnh nc thi dt nhum 1.2.2.1 Cỏc phng phỏp húa lý 17 21 Phng phỏp keo t Phng phỏp hp ph 1.2.2.3 Phng phỏp in húa 24 1.2.2.4 Phng phỏp húa hc 25 1.3 Phng phỏp oxi húa nõng cao (AOPs) 26 1.3.1 Gii thiu cỏc quỏ trỡnh oxi húa nõng cao 26 1.3.2 C s lý thuyt ca quỏ trỡnh Fenton 30 1.3.2.1 Quỏ trỡnh Fenton ng th 30 1.3.2.2 Quỏ trỡnh Fenton d th 32 1.3.2.3 Quỏ trỡnh Photo Fenton 33 Footer Page 10 of 89 Header Page 141 of 89 TI LIấU THAM KHO Geim AK, Novoselov KS, The rise of graphene, Nat Mater, 2007,6, 183-191 Sumit Goenka, Vinayak Sant, Shilpa Sant,Graphene-based nanomaterials for drug delivery and tissue engineering Journal of Controlled Release, 2014,173, 7588 Al-Degs Y S, Khraisheh M A M, Allen S J and Ahmad M N, Effect of Cacbon Surface Chemistry on the Removal of Reactive Dyes from Textile Effluent , Water Research, 2000, 34(3), 927-935 Peiying Zhu, Ming Shen, Shuhua Xiao, Dong Zhang ,Experimental study on the reducibility of graphene oxide by hydrazine hydrate, Physica B: Condensed Matter, 2011, 406, 3, 498-502 Gao.Y, Li Y, Zhang L, Huang H, Hu J, Shah S.M, Su X, Adsorption and removal of tetracycline antibiotics from aqueous solution by graphene oxide, J Colloid Interf Sci 2012, 368, 540546 Yang S.T, S Chen, Y Chang, A Cao, Y Liu, H Wang, Removal of methylene blue 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học tập nghiên... hưởng đến trình Fenton Photo Fenton 35 1.3.3.1 Ảnh hưởng độ pH ……………………………………… 35 1.3.3.2 Ảnh hưởng nồng độ H2O2 tỉ lệ Fe +/H2O2 …………… 35 1.3.3.3 Ảnh hưởng anion vô …………………………… 36 1.3.4 Ảnh hưởng... Đánh giá hoạt tính hệ xúc tác tổng hợp - Nghiên cứu điều kiện ảnh hưởng pH, nồng độ H2O2, nồng độ thuốc nhuộm hoạt tính RR195 ban đầu đến hoạt tính xúc tác vật liệu tổng hợp - Nghiên cứu động học