ĐẠI HỌC HUẾ TRƯỜNG ĐẠI HỌC SƯ PHẠM NGUYỄN LÊ MỸ LINH NGHIÊN CỨU BIÊN TÍNH BENTONIT Cổ ĐỊNH VÀ ỨNG DUNG TRONG XUC TAC - HAP PHU ■■ CHUYÊN NGÀNH: HÓA LÝ THUYẾT VÀ HÓA LÝ MÃ SỐ: 62.44.01.19 LUÂN ÁN TIẾN SĨ HÓA HỌC NGƯỜI HƯỚNG DẪN KHOA HỌC: GS.TS NGUYỄN HỮU PHÚ HUẾ, 2016 LỜI CAM ĐOAN Tôi xin cam đoan công trình nghiên cứu riêng Các số liệu kết nghiên cứu nêu luận án trung thực, đồng tác giả cho phép sử dụng chưa công bố trong công trình khác Tác giả Nguyễn Lê Mỹ Linh Lời Cảm Ơn Trước kết/, xin/ tỏ tòng biết ơn sâu sắc đến GS.TS 'Nguyễn Hữu Phú/ TS Đinh/ Quang KKhiếu/, cáo thầy tận ttnh/ hướng dẫn, hỗ trợ và/ định hướng cho suốt thời gian thực luận án Thêm/ lời cảm ơn đặc biệt đến P 0) tăng entropi (AS > 0) Từ nghiên cứu nhận thấy bentonit hữu bentonit hữu - vô có triển vọng hấp phụ hợp chất hữu ô nhiễm có kích thước lớn ( > 15 Ả ) Vật liệu Fe-bentonit chất xúc tác tốt cho phản ứng alkyl hóa hợp chất thơm với độ chọn lọc độ chuyển hóa cao.Tốc độ phản ứng benzyl hóa ^-xylen xúc tác Febentonit tăng theo tỉ lệ mol chất tham gia phản ứng, hàm lượng xúc tác nhiệt độ Năng lượng hoạt hóa phản ứng xúc tác Fe-bentonit xác định 120,76 kJ/mol Điểm bật luận án xác định mô hình Langmuir-Hinshewood phù hợp với mô hình động học phản ứng benzyl hóa ^-xylen Kết mở triển vọng việc sử dụng bentonit Cổ Định chống polyme kim loại hay oligome kim loại làm chất xúc tác cho phản ứng Friedel-Crafts tương tự Các kết nghiên cứu cấu trúc, tính chất bề mặt vật liệu, nhiệt động học, động học hấp phụ phản ứng benzyl hóa ^-xylen chứng tỏ rằng, trình hấp phụ xúc tác xảy bề mặt mao quản trung bình hạt vật liệu Sự chèn ghép tác nhân (Fe3+, Al3+, CTAB) đóng vai trò thay đổi chất tâm xúc tác hấp phụ, định xứ “lộ” thành mao quản bề mặt hạt vật liệu, tạo tâm dễ “tiếp cận” tác nhân (phân tử, ion, ) tham gia trình hấp phụ xúc tác - DANH MỤC CÁC CÔNG TRÌNH KHOA HỌC ĐÃ CÔNG BỐ - LIÊN QUAN ĐÉN LUẬN ÁN Nguyen Le My Linh, Nguyen Thi Thuc Nhi, Đinh Quang Khieu, Nguyen Huu Phu (2011), “Modification of Co Dịnh bentonite with cetyltrimethylammonium bromide by ion exchange and sonication assisted ion exchange methods”, Tạp chí Hóa học, 49 (5AB), tr.715-720 Nguyen Le My Linh, Đinh Quang Khieu, Nguyen Huu Phu (2011), “Removal of phenol from aqueous solution by cetyltrimethylammonium functionalized bentonite”, Tạp chí Hóa học, 49 (5AB), tr.95-101 Nguyen Le My Linh, Nguyen Thi Thuc Nhi, Tran Xuan Mau, Dinh Quang Khieu, Nguyen Huu Phu (2013), “Synthesis of Fe-CTAB-bentonite complexes from Co Dinh bentonite by ion exchange and hydrothermal assisted ion exchange methods”, Tạp chí khoa học Đại học Huế, 84 (6), tr 55-63 Nguyễn Lê Mỹ Linh, Dương Tuấn Quang, Đinh Quang Khiếu, Nguyễn Hữu Phú (2015), “Nghiên cứu tổng hợp Al-bentonite Cổ định phương pháptrao đổi ion”, Tạp chí Xúc tác Hấp phụ, (4), tr 62-69 Nguyễn Lê Mỹ Linh, Nguyễn Thị Thanh Lai, Dương Tuấn Quang, Đinh Quang Khiếu, Nguyễn Hữu Phú (2015), “Nghiên cứu hấp phụ As(V) dung dịch nước vật liệu Fe-CTAB-bentonite”, Tạp chí Xúc tác Hấpphụ, (4), tr 70-77 Nguyễn Lê Mỹ Linh, Hoàng Văn Đức, Dương Tuấn Quang, Lê Thị Hòa, Đinh Quang Khiếu, Nguyễn Hữu Phú (2015), “Nghiên cứu phản ứng benzyl hóa p-xylene benzyl chloride xúc tác Fe-bentonite”, Tạp chí Hóa học, 53 (3E12), tr.213-217 Nguyễn Lê Mỹ Linh, Hoàng Văn Đức, Dương Tuấn Quang, Lê Thị Hòa, Đinh Quang Khiếu, Nguyễn Hữu Phú (2015), “Nghiên cứu hấp phụ As(V) trongdung dịch nước vật liệu Al-bentonite Al-CTAB-bentonite”, Tạp chí Hóa học, 53 (3E12), tr.296-302 Nguyễn Lê Mỹ Linh, Nguyễn Thị Anh Thư, Dương Tuấn Quang, Đinh Quang Khiếu Nguyễn Hữu Phú (2015), “Nghiên cứu động học đẳng nhiệt hấp phụ phenol đỏ vật liệu bentonite biến tính”, Tạp chí Hóa học, 53 (3E12), tr.303-309 Nguyễn Lê Mỹ Linh, Nguyễn Thị Thanh Lai, Dương Tuấn Quang, Đinh Quang Khiếu, Nguyễn Hữu Phú (2015), “Nghiên cứu hấp phụ As(V) trongdung dịch nước vật liệu Fe-bentonit”, Tạp chí Hóa học, 53 (3), tr.367-373 TÀI LIỆU THAM KHẢO - 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Tinh ch bentonit C nh, nghiờn cu thnh phn, cu trỳc v tớnh cht ca bentonit C nh - Nghiờn cu tng hp vt liu CTAB -bentonit, Fe -bentonit, Al -bentonit, Fe-CTABbentonit, Al-CTAB -bentonit v kho sỏt cỏc... thiabendazole bng Al -bentonit Quỏ trỡnh hp ph xy b mt ngoi ln trong cỏc vi mao qun ca Al -bentonit theo c ch tng tỏc tnh in Nhúm tỏc gi khỏc [31] tng hp Al -bentonit v Al/Febentonit dựng lm xỳc tỏc quỏ trỡnh phõn hy phm nhum tartrazine, vi lng Fe a vo bentonit cng nhiu, quỏ trỡnh phõn hy cng hiu qu Hin nay, nhiu nghiờn cu khụng ch tp trung vo bin tớnh bentonit bng mt kim loi m cũn hn hp nhiu kim loi, trong ú ỏng... tớch b mt trong c xỏc nh bi b mt ca khong khụng gian gia cỏc lp trong cu trỳc tinh th Do khong cỏch c bn gia cỏc lp b thay i ph thuc vo loi cation trao i gia cỏc lp, ph thuc vo cu trỳc v tớnh cht ca cht b hp ph, nờn b mt trong ca bentonit cng b thay i trong quỏ trỡnh hp ph Din tớch b mt ngoi c xỏc nh bi b mt ca cỏc mao qun hỡnh thnh gia cỏc ht bentonit Din tớch b mt ngoi ph thuc vo kớch thc ht bentonit. .. nhụm-oxit H2O2 [37] st I.3.2.2 Gii thiu v Me -bentonit (Me: Fe, Al) Vt liu Fe -bentonit hay Al -bentonit l sn phm ca quỏ trỡnh chốn cỏc polycation st hay nhụm vo bentonit Cỏc polycation ny c iu ch thụng qua quỏ trỡnh thy phõn cỏc cation Fe3+ hay Al3+ trong mụi trng kim S thy phõn cation Me3+ trong mụi trng kim tựy thuc vo iu kin thc nghim s thu c cỏc cu t chớnh trong dung dch to ra tr chng: cation monome... gian d 00i ca vt liu Al -bentonit thu c 17 - 19 Vt liu Al -bentonit tng hp trong iu kin nng huyn phự bentonit 47 g/l cú din tớch b mt (358 m /g) ln hn nhiu so vi bentonit ban u (85 m /g), ch yu l do 2 2 s tng din tớch vi mao qun Nhúm tỏc gi Aceman [20] iu ch ion Keggin Al t l mol OH-/Al3+ l 13 2.3, lỳc ny 80 - 95 % Al trong dung dch tn ti dng Al v dung dch ny cú 13 th bn trong 3 thỏng Theo cỏc ti... cu cho thy vt liu Al -bentonit cú din tớch b mt ln v cha nhiu tõm axit Lewis cng nh Bronsted, vỡ vy chỳng cú nhiu ng dng trong lnh vc hp ph v xỳc tỏc [4, 31, 70] Macias v cng s [110] tng hp vt liu Al -bentonit, Al/Labentonit ng dng trong phn ng dehydrat húa butanol Altunlu [25] ó tng hp vt liu Al -bentonit bng phng phỏp trao i ion, kt qu hp ph phenol, 2-chlorophenol tt hn nhiu so vi bentonit cha bin tớnh... b mt bentonit mang in tớch dng v nhúm OH tham gia vo phn ng trao i anion Ti cỏc giỏ tr pH > pHpzc, b mt bentonit mang in tớch õm v ion H+ tham gia vo phn ng trao i cation Dung lng trao i cation v anion ca bentonit thay i trong khong rng, ph thuc vo in tớch õm mng li v pH ca mụi trng trao i [13] Trong mụi trng kim, núi chung dung lng trao i cation ca bentonit l ln Dung lng trao i cation dao ng trong. .. vo v trớ oxy ỏy ca t din trong mng li tinh th bi lc Van der Walls hoc liờn kt hiro Vi cỏc cht hu c khụng phõn cc, cht cao phõn t v c bit l vi khun thỡ s hp ph ch xy ra trờn b mt ngoi ca bentonit Nh kh nng hp ph ln v a dng m bentonit c s dng rng rói trong cụng nghip cng nh trong nn kinh t quc dõn vi vai trũ l mt vt liu hp ph t nhiờn tiờu biu Vic nghiờn cu tớnh cht hp ph ca bentonit cú ý ngha khoa hc... 1.1.4 Ngun bentonit Vit Nam hin nay Vit Nam l nc cú ngun bentonit phong phỳ, a dng trong ú cú thnh phn chớnh l MMT Theo mt s ti liu a cht, hin nay nc ta ó phỏt hin c hn hai chc m v im qung sột bentonit Cỏc m cú trin vng v quy mụ ln u tp trung phớa nam Vit Nam (Lõm ng, Bỡnh Thun, Thnh ph H Chớ Minh ) phớa bc, bentonit tp trung ch yu vựng ng bng Bc B, Thanh Hoỏ v ch yu thuc nhúm smectit thp M bentonit