Header Page of 148 B GIO DC V O TO B QUC PHềNG VIN KHOA HC V CễNG NGH QUN S - TRN QUANG SNG NGHIấN CU S HP PH CA THAN HOT TNH DNG SIấU MN LUN N TIN S HểA HC H NI - 2014 Footer Page of 148 Header Page of 148 B GIO DC V O TO B QUC PHềNG VIN KHOA HC V CễNG NGH QUN S TRN QUANG SNG NGHIấN CU S HP PH CA THAN HOT TNH DNG SIấU MN Chuyờn ngnh: Mó s: Húa lý thuyt v húa lý 62 44 01 19 LUN N TIN S HểA HC NGI HNG DN KHOA HC: GS TSKH Ngc Khuờ PGS TS Lờ Huy Du H NI - 2014 Footer Page of 148 Header Page of 148 i LI CAM OAN Tụi xin cam oan õy l cụng trỡnh nghiờn cu ca riờng tụi Cỏc kt qu nghiờn cu a lun ỏn l trung thc Nhng kt lun khoa hc cha tng c cụng b bt k cụng trỡnh no khỏc Ngy thỏng nm 2014 Tỏc gi Trn Quang Sỏng Footer Page of 148 Header Page of 148 ii LI CM N Tụi xin by t lũng bit n sõu sc ti GS.TSKH Ngc Khuờ v PGS TS Lờ Huy Du ó ch o, hng dn tn tỡnh sõu sỏt, giỳp tụi sut quỏ trỡnh thc hin cng nh hon thnh bn lun ỏn ny Tụi xin chõn thnh cm n Th trng, cỏn b nhõn viờn Vin Cụng ngh mi/ Vin KH&CN quõn s ó h tr v to mi iu kin thun li cho tụi quỏ trỡnh thc hin lun ỏn Tụi xin trõn trng cm n Th trng Vin KH&CN quõn s, Phũng o to/ Vin KH&CN quõn s ó giỳp tụi sut thi gian hc tp, nghiờn cu v hon thnh lun ỏn Tụi xin trõn trng cm n Vin Hoỏ hc - Mụi trng Quõn s/ B T lnh Hoỏ hc; Vin Hoỏ hc - Vt liu/ Vin KH&CN quõn s; Vin Húa hc/ Vin Hn lõm KH&CN Vit Nam; Khoa Húa hc/ Trng HSP H Ni ó giỳp , quỏ trỡnh thc hin lun ỏn Xin chõn thnh cm n gia ỡnh, ngi thõn, ng nghip v bn bố ó quan tõm, ng h, c v ng viờn tụi hon thnh cụng trỡnh ny Trn Quang Sỏng Footer Page of 148 Header Page of 148 iii MC LC Danh mc cỏc ký hiu, cỏc ch vit tt Danh mc cỏc bng Danh mc cỏc hỡnh v, th M U Chng I - TNG QUAN 1.1 Nhng khỏi nim chung v than hot tớnh 1.1.1 S lc v than hot tớnh 1.1.2 Cu trỳc than hot tớnh 1.1.3 Sn xut than hot tớnh v than hot tớnh siờu mn 1.2 Tớnh cht hp ph ca than hot tớnh 1.2.1 Nhit ng hc hp ph 1.2.2 ng hc hp ph trờn than hot tớnh v than hot tớnh siờu mn 1.3 Hin trng nghiờn cu ng dng than hot tớnh v than hot tớnh siờu mn thc t 1.3.1 ng dng quõn s 1.3.2 ng dng y hc 1.3.3 ng dng cụng nghip húa m phm 1.3.4 ng dng lnh vc x lý mụi trng v cỏc lnh vc khỏc v vii ix 4 6 13 19 20 30 33 33 35 36 37 Chng - I TNG V PHNG PHP NGHIấN CU 39 2.1 i tng nghiờn cu 2.2 Nguyờn liờu, húa cht v thit b nghiờn cu 2.2.1 Nguyờn liu 2.2.2 Cỏc hoỏ cht dựng nghiờn cu 2.2.3 Thit b cụng ngh dựng phõn tớch o c 2.3 Phng phỏp nghiờn cu 2.3.1 Phng phỏp to kớch thc ht than 2.3.2 Phng phỏp xỏc nh phõn b kớch thc v cu trỳc b mt 2.3.3 Phng phỏp xỏc nh t trng than hot tớnh 2.3.4 Phng phỏp hp ph ng nhit nit nhit (-196)0C 2.3.5 Phng phỏp hp ph benzen 2.3.6 Phng phỏp phõn tớch, xỏc nh hm lng cỏc cht hu c 39 39 39 39 40 41 41 42 44 45 49 51 Footer Page of 148 Header Page of 148 iv Chng - KT QU V THO LUN 3.1 c im nghiờn cu phõn b kth ca cỏc mu than hot tớnh siờu mn c ch to bng phng phỏp nghin bi 3.1.1 c im phõn b kth than siờu mn ch to t THT Tr Bc 3.1.2 c im phõn b kth than siờu mn ch to t THT TQ 3.1.3 c im phõn b kth than siờu mn ch to t THT tre 3.2 Xỏc nh tớnh cht, cu trỳc xp ca cỏc mu than sau nghin 3.2.1 ỏnh giỏ cu trỳc xp thụng qua hp ph nit 3.2.1.1 Kho sỏt s hp ph nit trờn THT Tr Bc 3.2.1.2 Kho sỏt s hp ph nit trờn THT Trung Quc 3.2.1.3 Kho sỏt s hp ph nit trờn THT Tre 3.2.2 Kh nng hp ph hi benzen ca cỏc loi THT 3.2.2.1 Kho sỏt kh nng hp ph benzen trờn THT Tr Bc 3.2.2.2 Kho sỏt kh nng hp ph benzen trờn THT Trung Quc 3.2.2.3 Kho sỏt kh nng hp ph benzen trờn THT Tre 3.3 Nghiờn cu quỏ trỡnh hp ph ng nhit v ng hc hp ph ca THT cú kớch thc siờu mn mụi trng nc 3.3.1 c im quỏ trỡnh hp ph MB trờn cỏc mu THT siờu mn 3.3.1.1 ng nhit hp ph MB trờn cỏc mu THT siờu mn 3.3.1.2 ng hc hp ph ca MB trờn cỏc mu THT siờu mn 3.3.2 c im quỏ trỡnh hp ph TNR trờn cỏc mu THT siờu mn 3.3.2.1 ng nhit hp ph TNR trờn cỏc mu THT siờu mn 3.3.2.2 ng hc hp ph vi TNR trờn cỏc mu THT siờu mn 3.3.3 c im quỏ trỡnh hp ph TNT trờn cỏc mu THT siờu mn 3.4 Nghiờn cu xut phng ỏn ỏp dng THT siờu mn cho cụng ngh x lý nc thi nhim TNT 3.4.1 Thit lp mụ hỡnh tớnh toỏn x lý nc thi nhim TNT theo m 3.4.2 C s cng ỏp dng THT siờu mn cho x lý nc thi nhim TNT theo m 3.4.3 Tớnh toỏn ỏp dng THT siờu mn cho x lý nc thi nhim TNT theo ng hc hp ph KT LUN DANH MC CC CễNG TRèNH CễNG B TI LIU THAM KHO Footer Page of 148 55 55 55 59 62 66 66 66 72 74 79 79 82 84 87 87 87 100 107 108 117 121 125 125 126 129 133 135 136 Header Page of 148 v DANH MC CC Kí HIU, CC CH VIT TT B Hng s cu trỳc xp theo Dubinin BET Brunauer-Emmett-Teller Ce Nng cht b hp ph t trng thỏi cõn bng C0 Nng cht b hp ph D Kớch thc ht d ng kớnh mao qun GC-MS Phng phỏp sc ký khớ ph HPLC Phng phỏp sc ký lng hiu nng cao KF, Hng s hp ph Freundlich KS Hng s hp ph Freundlich theo mụ hỡnh hp ph v KL Hng s hp ph Langmuir k1 Hng s hp ph bc k2 Hng s hp ph bc kth Kớch thc ht m Khi lng cht hp ph MB Methylthionine chloride (methylene blue) cũn gi l xanh mờtylen M Phõn t gam n H s m hp ph ca phng trỡnh Freundlich NA S Avogadro P; Ps áp suất áp suất bão hoà chất bị hấp phụ qe, qt Dung lng hp ph cõn bng v ti thi im t qmax Dung lng hp ph cc i r Bỏn kớnh mao qun SEM Hin vi in t quột (Scanning Electron Microscopy) SBET Din tớch b mt riờng ca than hot tớnh tớnh theo BET SBJH B mt ngoi ca mao qun trung bỡnh Stot B mt riờng tng cng SMicro B mt riờng ca mao qun nh SExt B mt riờng ngoi Footer Page of 148 Header Page of 148 vi S Din tớch b mt TB Tr Bc THT Than hot tớnh THT SM Than hot tớnh siờu mn TNR Trinitroresorxin cũn gi l styphnic axit TNT Trinitrotoluen TQ Trung Quc T Nhit K V Th tớch dung dch cht hp ph VBJH Th tớch mao qun trung bỡnh VMicro Th tớch mao qun trnh Vm Lng cht hp ph trng thỏi ngng t Vrn Th tớch phn cht rn Vtng Tng th tớch xp Vln Tng th tớch cỏc mao qun ln ca than hot tớnh Vnh Tng th tớch cỏc mao qun nh ca than hot tớnh Vtng Tng th tớch xp ca than hot tớnh Vtrung Tng th tớch cỏc mao qun trung bỡnh ca than hot tớnh Wo Th tớch khụng gian hp ph ca mao qun nh theo Dubinin t Khi lng riờng thc b Khi lng riờng biu kin Khi lng riờng Tit din ngang ca phõn t cht b hp ph Sc cng b mt t tng chiu dy t ca lp hp ph Vhp Th tớch cht hp ph tng theo c ch a lp l1, l2 Trng lng cỏc gi mu cõn Mark-Bell Vhp Th tớch cht hp ph tng theo c ch a lp Footer Page of 148 Header Page of 148 vii danh mục bảng Bng 1.1: Kớch thc ca GAC v PAC theo sng 18 Bng 3.1: Cỏc c trng cu trỳc ca cỏc mu THT Tr Bc 71 Bng 3.2 Cỏc c trng cu trỳc ca cỏc mu THT Trung Quc 74 Bng 3.3 Cỏc c trng cu trỳc ca cỏc mu THT tre 75 Bng 3.4 Cỏc thụng s c trng ca THT TB hp ph benzen 81 Bng 3.5 Cỏc thụng s c trng ca cỏc mu THT TQ hp ph benzen 82 Bng 3.6 Cỏc thụng s c trng ca cỏc mu THT tre hp ph benzen 84 Bng 3.7 Dung lng hp ph ca THT Tr Bc cú kth khỏc 88 Bng 3.8 Cỏc thụng s ca phng trỡnh ng nhit Freundlich i vi h MB/THT Tr Bc 90 Bng 3.9 Cỏc thụng s ca phng trỡnh ng nhit Langmuir i vi h MB/THT Tr Bc Bng 3.10 Dung lng hp ph ca THT TQ cú kth khỏc 91 94 Bng 3.11 Cỏc thụng s ca phng trỡnh ng nhit Freundlich i vi h MB/ THT Trung Quc 96 Bng 3.12 Cỏc thụng s ca phng trỡnh ng nhit Langmuir i vi h MB/THT Trung Quc 97 Bng 3.13 Cỏc thụng s phng trỡnh ng nhit Freundlich v Langmuir i vi h MB/THT tre 98 Bng 3.14 Mi quan h Ct, qe theo thi gian t quỏ trỡnh hp ph dung dch metylen xanh trờn cỏc mu THT Tr Bc cú kớch thc khỏc 100 Bng 3.15 Phng trỡnh thc nghim v hng s tc k2 ca THT Tr Bc cú kớch thc ht khỏc 102 Bng 3.16 Phng trỡnh thc nghim v hng s tc k2 ca THT Trung Quc cú kớch thc ht khỏc Footer Page of 148 104 Header Page 10 of 148 viii Bng 3.17 Phng trỡnh thc nghim v hng s tc k 106 Bng 3.18 Dung lng hp ph ca cỏc mu THT Tr Bc vi TNR 108 Bng 3.19 Cỏc thụng s c trng ca phng trỡnh Freundlich v Langmuir i vi h TNR/THT Tr Bc 111 Bng 3.20 Dung lng hp ph ca cỏc mu THT TQ vi TNR 113 Bng 3.21 Cỏc thụng s c trng ca phng trỡnh Freundlich v Langmuir i vi h MB/THT Trung Quc 115 Bng 3.22 Dung lng hp ph ca cỏc mu THT tre vi TNR 116 Bng 3.23 Cỏc thụng s Freundlich v Langmuir i vi TNR/THT tre 117 Bng 3.24 Phng trỡnh thc nghim v hng s tc k2 ca h TNR/ THT Tr Bc 118 Bng 3.25 Phng trỡnh thc nghim v hng s tc k2 ca h TNR/THT tre 120 Bng 3.26 Dung lng hp ph ca cỏc mu THT Tr Bc vi TNT 121 Bng 3.27 Dung lng hp ph ca cỏc mu THT TQ vi TNT 122 Bng 3.28 Dung lng hp ph ca cỏc mu THT tre vi TNT 122 Bng 3.29 Cỏc thụng s phng trỡnh ng nhit Freundlich i vi h TNT/THT Tr Bc 123 Bng 3.30 Cỏc thụng s phng trỡnh ng nhit Freundlich i vi h TNT/THT Trung Quc 123 Bng 3.31 Cỏc thụng s phng trỡnh ng nhit Freundlich i vi h TNT/THT tre 123 Bng 3.32 T l cht hp ph trờn cỏc loi than x lý TNT 127 Bng 3.33 c lng giỏ thnh x lý 1m3 TNT trờn cỏc loi THT SM 128 Bng 3.34 Tham s ca phng trỡnh ng hc biu kin bc hp ph TNT trờn than Tr Bc Footer Page 10 of 148 129 Header Page 144 of 148 132 Kt qu nghiờn cu ng hc hp ph dung dch lng ó chng minh c: hng s tc phn ng tng dn kớch thc ht THT gim v tng t bin kớch thc ht t n kớch thc siờu mn (di 10àm) v tuõn theo mụ hỡnh phn ng ng hc hp ph gi bc hai C th: cỏc mu THT cú kớch thc ht ln hn 50àm hng s tc phn ng k tng u v tuyn tớnh phm vi mt vi ln; kớch thc ht khong 10-50àm hng s tc phn ng tng nhanh hn, n hng chc ln; kớch thc ht t n siờu mn (di 10àm) thỡ hng s tc cú th tng n trm ln so vi mu cú kớch thc ht ln hn 120àm Cỏc kt qu nghiờn cu s hp ph cỏc hp cht hu c nh: MB, TNT, NTR dung dch trờn cỏc mu THT cú kớch thc siờu mn (SPAC) ca lun ỏn phự hp vi kt qu ngiờn cu ca cỏc tỏc gi nc ngoi [55], [89-96] Ngoi kh nng hp ph mao qun thỡ THT cú kớch thc siờu mn cũn tuõn theo mụ hỡnh hp ph b mt ngoi hay mụ hỡnh hp ph v ht (Shell Adsorption Model - SAM) Footer Page 144 of 148 Header Page 145 of 148 133 KT LUN Bng phng phỏp nghin bi cú th ch to THT cú kớch thc siờu mn T cỏc kt qu nghiờn cu c im quỏ trỡnh hp ph ca cỏc mu than Tr Bc, than Trung Quc, than tre i vi khớ nit, hi benzen v cỏc cht hu c dung dch nc, cho thy quỏ trỡnh nghin nh cỏc ht THT cú kớch thc ln, t hng nghỡn hoc hng trm àm, v kớch thc siờu mn, c chc àm, bng phng phỏp nghin c hc (nghin bi), khụng lm nh hng ỏng k n dung lng hp ph hay cu trỳc l xp THT: Phng phỏp nghin c hc phự hp vi cụng ngh ch to THT siờu mn phũng thớ nghim v cú th ỏp dng sn xut quy mụ cụng nghip ó kho sỏt c im quỏ trỡnh hp ph dung dch nc trờn THT siờu mn ca mt s hp cht hu c mang mu v cú tớnh n gc nitro thm Kt qu cho thy: Ngoi s ph thuc vo bn cht ca cỏc loi THT, kh nng hp ph cũn ph thuc vo kớch thc ht; kớch thc ht ca THT gim, hiu sut hp ph tng Kt qu nghiờn cu ng hc hp ph dung dch nc cho thy: Hng s tc phn ng tng dn kớch thc ht gim dn, tng t bin kớch thc ht t n kớch thc siờu mn v tuõn theo mụ hỡnh phn ng ng hc hp ph gi bc hai ó thit lp c cỏc phng trỡnh ng nhit hp ph mụi trng nc ca mt s cht hu c nh MB, TNR, TNT trờn cỏc h hp ph than hot tớnh bt mn v siờu mn Kt qu cho thy phng trỡnh ng nhit Frenudlich l thớch hp ỏp dng x lý s liu thc nghim cng nh tớnh toỏn cỏc thụng s cụng ngh x lý mụi trng bng phng phỏp hp ph mụi trng nc Footer Page 145 of 148 Header Page 146 of 148 134 ó ỏnh giỏ bc u mt s c tớnh kinh t k thut ca THT siờu mn ỏp dng vo mc ớch x lý nc thi nhim TNT * Nhng úng gúp mi ca lun ỏn - Nghiờn cu mt cỏch h thng cỏc liờn quan n ch to THT cú kớch thc siờu mn Phng phỏp nghin c hc khụng lm nh hng n cu trỳc l xp ca 03 loi THT: than Tr Bc, than Trung Quc, than tre v phng phỏp ny phự hp vi cụng ngh ch to THT siờu mn phũng thớ nghim - Thit lp cỏc phng trỡnh ng nhit v ng hc hp ph mụi trng nc ca cỏc cht MB, TNR, TNT trờn than hot tớnh bt mn v siờu mn Cỏc kt qu nghiờn cu cho thy: quỏ trỡnh hp ph ph thuc vo bn cht v kớch thc ht ca than THT cng mn thỡ hiu sut v tc hp ph cng cao - Xỏc nh quy trỡnh nghin khụng phỏ hy v cu trỳc mao qun v quỏ trỡnh hp ph phõn t ln ch yu xy b mt ngoi ca than hot tớnh Footer Page 146 of 148 Header Page 147 of 148 DANH MC CC CễNG TRèNH CễNG B Trn Quang Sỏng, Lờ Huy Du (2008), Kho sỏt kh nng hp ph mu xanh metylen ca than hot tớnh c iu ch t tre, Tp Nghiờn cu KHKT&CNQS s 22, Tr 54-57 Lờ Huy Du, Trn Quang Sỏng, Trn ng Mnh (2009), Nghiờn cu sn xut th than hot tớnh t tre lung bng lũ cụng nghip, Hi ngh Xỳc tỏc v Hp ph ton quc ln th 5, thỏng 11/2011, Tp Húa hc, Tp 47(6A), Tr 220-226 Trn Quang Sỏng, Ngc Khuờ, Lờ Huy Du (2011), Nghiờn cu nh hng ca kớch thc ht n kh nng hp ph than hot tớnh dng bt, Tp Húa hc, Tp 49(3), Tr 336-341 Trn Quang Sỏng, Ngc Khuờ (2011), nh hng ca kớch thc ht than hot tớnh n hiu qu hp ph axit styphnic lờn than hot tớnh Tr Bc, Tp Phõn tớch Húa Lý Sinh, Tp 16(4), tr 32-37 Trn Quang Sỏng, Ngc Khuờ, Lờ Huy Du (2011), nh hng ca kớch thc ht than ty mu n kh nng hp ph v tc hp ph, Hi ngh xỳc tỏc hp ph ton quc ln th 6, Tp Húa hc, Tp 49(5AB), Tr 116-123 Le Huy Du, Tran Kim Phuong, Tran Quang Sang, Tran Dang Mnh (2011), Testing Manufacture of Activated Carbon from Bamboo charcoal in the Industrial rotary furnace, The 1st International Conference on Energy, Environment and Climate changes (ICEC 2011), Ho Chi Minh University of Industry (HUI), Vietnam Trn Quang Sỏng, Ngc Khuờ, Lờ Huy Du (2014), nh hng ca kớch thc ht n hiu qu hp ph trinitrotoluen trờn than hot tớnh, Tp Xỳc tỏc v Hp ph, Tp 3(2), Tr 36-41 Footer Page 147 of 148 Header Page 148 of 148 136 TI LIU THAM KHO Nguyn Vit Bc v cng s (2007), Nghiờn cu vt liu ngy trang, nghi trang chng trinh sỏt rada, Bỏo cỏo kt qu ti thuc chng trỡnh KCB 02-08 BQP, H Ni Nguyn Hi Bng (2011), Nghiờn cu c im quỏ trỡnh hp ph ca cht n nhúm nitramin mụi trng nc v ng dng x lý mụi trng, Lun ỏn tin s húa hc, Vin KH-CNQS, H Ni Lờ Vn Cỏt (2002), Hp ph v trao i ion k thut x lý nc v nc thi NXB Thng kờ, H Ni Thõn Thnh Cụng (2006), Nghiờn cu phõn hu phosphin trờn than hot tớnh tm xỳc tỏc dựng hp lc c Lun ỏn tin s Trung tõm KHKT-CNQS, H Ni Phm Vn Cng (2013), X lý si cacbon dựng lm tng bn vt liu composite, K thut trang b, s 151, trang 45 Lờ Huy Du (1985), Nghiờn cu nh hng ca yu t hot hoỏ quỏ trỡnh iu ch than hot tớnh ộp viờn dựng mt n phũng c Lun ỏn phú tin s Hoỏ hc, Vin KTQS, H Ni Lờ Huy Du (2001), Nghiờn cu ch to vt liu hp ph súng rada t si polyme v oxyt kim loi, Bỏo cỏo kt qu ti BQP, tr 13-14 Lờ Ngc nh (1997), Nghiờn cu s suy gim bc x laser bng sol khớ, Lun ỏn tin s húa hc, Vin KTQS, H Ni Ngc Khuờ v cng s (2001), Hin trng cụng ngh x lý mt s cht thi c thự ca sn xut quc phũng, 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(1996), Manufacture of activated carbon fiber, Patent US 5521008 18 Alzaydien, A S., (2009), Adsorption of methylene blue from aqueous solution onto a low-cost natural Jordanian Tripoli, Am J Environ Sci 197208 19 Ana Rita Pereira Almendra (2011), The effect of water inorganic matrix in ibuprofen adsorption onto activated carbon for water and wastewater treatment New University of Lisbon, PhD 2011 20 Ana LiDia Serpa, et al., (2005), Adsorption onto Fluidized Powdered Activated Carbon Flocs-PACF, Environ Sci Technol 2005 , 39, pp 885 - 888 Footer Page 149 of 148 Header Page 150 of 148 138 21 A S Mestre, et al., (2007), Activated carbons for the adsorption of ibuprofen, Carbon, vol 45, pp 1979-1988 22 Ayeni K E., (2012), Adsorption of cadmium and chromium using activated carbon derived from carica papaya seed, Continental J Water, Air and Soil Pollution 3(1): pp 17 20 23 Ayoub Karimi-Jashni (1994), Effect of pH on Adsorption and Desorption Equilibria and Kinetics of 2-Nitrophenol and 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