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ĐẠI HỌC HUẾ TRƯỜNG ĐẠI HỌC KHOA HỌC VẬT LIỆU TRÊN CƠ SỞ CARBON HOẠT TÍNH: TỔNG HỢP VÀ ỨNG DỤNG LUẬN ÁN TIẾN SĨ NGÀNH HÓA LÝ THUYẾT VÀ HÓA LÝ HUẾ – NĂM 2023 ĐẠI HỌC HUẾ TRƯỜNG ĐẠI HỌC KHOA HỌC VẬT LIỆU TRÊN CƠ SỞ CARBON HOẠT TÍNH: TỔNG HỢP VÀ ỨNG DỤNG Ngành: HĨA LÝ THUYẾT VÀ HÓA LÝ Mã số: 9.44.01.19 LUẬN ÁN TIẾN SĨ HOÁ LÝ THUYẾT VÀ HOÁ LÝ HUẾ – NĂM 2023 LỜI CAM ĐOAN Tôi xin cam đoan cơng trình nghiên cứu riêng tơi, số liệu kết nghiên cứu ghi luận án trung thực; Trong có số kết chung nhóm nghiên cứu hướng dẫn GS TS Thừa Thiên Huế, ngày 19 tháng 04 năm 2023 Tác giả luận án i LỜI CẢM ƠN Trước tiên, tơi xin bày tỏ lịng biết ơn chân thành sâu sắc đến thầy GS.TS tận tâm hướng dẫn, định hướng nghiên cứu để luận án hoàn thành Thầy truyền đạt kiến thức, kinh nghiệm cho tơi suốt q trình thực luận án Tôi xin trân trọng cảm ơn giúp đỡ, dạy nhiệt tình thầy TS Tơi xin chân thành cảm ơn q thầy Bộ mơn Hóa lý, q thầy Khoa Hóa học, Trường Đại học Khoa học, Đại học Huế, giúp đỡ, tạo điều kiện thuận lợi cho tơi q trình học tập, nghiên cứu, thực bảo vệ luận án Tôi xin chân thành cảm ơn quý thầy cô Khoa Khoa học tự nhiên Công nghệ, Trường Đại học Tây Nguyên, giúp đỡ, tạo điều kiện thuận lợi cho trình học tập, nghiên cứu, thực bảo vệ luận án Cùng với trân trọng đó, tơi chân thành cảm ơn Lãnh đạo Sở đồng chí quan Sở Giáo dục Đào tạo, Tỉnh Đăk Nông tạo điều kiện tốt cho tơi suốt q trình học tập nghiên cứu Cuối cùng, xin bày tỏ lời cảm ơn sâu sắc đến gia đình, người thân bạn bè ln quan tâm, khích lệ, động viên giúp đỡ suốt thời gian học tập vừa qua Thừa Thiên Huế, tháng 04 năm 2023 Tác giả luận án ii DANH MỤC CÁC CHỮ VIẾT TẮT, KÝ HIỆU Viết tắt Tiếng Anh Tiếng Việt AC Activated carbon Carbon hoạt tính ASV Anodic stripping voltammetry Volt-ampere hịa tan anode BET Brunauer-Emmett-Teller BIM Benzimidazolate Benzimidazolate BIOC Biochar Than sinh khối Britton-Robinson Buffer Dung dịch đệm Britton- Solution Robinson CB Conduction band Vùng dẫn cbIM Chlorobenzimidazolate Chlorobenzimidazolate CP Chloramphenicol Chloramphenicol CV Cyclic voltammetry Volt-ampere vòng DEF N,N-Diethylformamide N,N-Diethylformamide DP- Differential pulse anodic Volt-ampere hòa tan anode ASV stripping voltammetry xung vi phân DPV Differential pulse voltammetry Volt-ampere xung vi phân B-RBS EDX Eg Ep hay Up EtOH Energy-dispersive X-ray spectroscopy Phương pháp BrunauerEmmett-Teller Phổ tán xạ lượng tia X Energy of band gap Năng lượng vùng cấm Peak voltage Thế đỉnh Ethanol Ethanol iii Fourier-transform Phổ hồng ngoại biến đổi infrared spectroscopy Fourier GCE Glassy carbon electrode Điện cực than thủy tinh GO Graphene oxide Graphene oxide FTIR HPLC High-performance liquid chromatography Sắc ký lỏng hiệu cao Ideal adsorption solution Lý thuyết dung dịch hấp phụ theory lý tưởng Trichlosan's "IC25" toxin Tiêu chuẩn xác định độc tố standard "IC25" trichlosan Ip Dissolution peak current Dòng đỉnh hòa tan iPrOH i-Propyl alcohol i-Propyl alcohol IAST IC25 International Union of Pure and IUPAC Applied Chemistry Danh pháp IUPAC Nomenclature LOD Limit of detection Giới hạn phát LSV Linear sweep voltammetry MB Methylene blue Methylene blue MeCN Methyl cyanide Methyl cyanide MeOH Methanol Methanol mIM Methylimidazolate Methylimidazolate MO Methyl orange Methyl orange MOF Metal-organic framework Khung hữu – kim loại MR Methyl red Methyl red NMR Nuclear Magnetic Resonance Cộng hưởng từ hạt nhân iv Phương pháp volt-ampere qt tuyến tính Q trình oxy hóa xúc tác PCO Photo catalytic oxidation P-factor P-factor Yếu tố P pHPZC Point zero charge Điểm đẳng điện POM Polyoxometalate Polyoxometalate Photoinduced Tính siêu ưa nước quang superhydrophilicity tạo Pur Purinate Purinate RE Relative error Sai số tương đối Rev Recovery Độ thu hồi RH Rice husk Vỏ trấu RHAC Rice husk activated carbon Carbon hoạt tính từ vỏ trấu RHO Rhobohedral Rhobohedral RSD Relative standard deviation Độ lệch chuẩn tương đối SD Standard deviation Độ lệch chuẩn SEM Scanning electron microscopy Hiển vi điện tử quét SOD Sodalite Sodalite SSES Sum of squares Tổng bình phương Square-wave anodic stripping Volt-ampere hịa tan anode voltammetry sóng vng PSH SWASV TBAC Tetrabutyl ammonium chloride TCS Trichlosan TEM quang Tetrabutyl ammonium chloride Trichlosan Transmission electron microscopy v Hiển vi điện tử truyền qua Thermogravimetry/Differental Phương pháp phân tích nhiệt scanning calorimetry vi sai quét/Nhiệt khối lượng Ultraviolet-Visible absorption Phổ hấp thụ tử ngoại – spectroscopy khả kiến UV-Vis Ultraviolet-Visible diffuse Phổ phản xạ khuếch tán tử DRS Reflectance spectroscopy ngoại – khả kiến VB Valance band Vùng hóa trị WE Working electrode Điện cực làm việc X X-Ray Tia X XRD X-ray diffraction Nhiễu xạ tia X TG/DSC UV-Vis ZIF Zeolitic imidazolate framework vi Khung zeolite imidazole MỤC LỤC LỜI CAM ĐOAN i LỜI CẢM ƠN ii DANH MỤC CÁC CHỮ VIẾT TẮT, KÝ HIỆU iii MỤC LỤC vii DANH MỤC CÁC BẢNG x DANH MỤC SƠ ĐỒ xii DANH MỤC CÁC HÌNH xiii MỞ ĐẦU Chương TỔNG QUAN VỀ VẬT LIỆU 1.1 Than hoạt tính 1.1.1 Giới thiệu chung 1.1.2 Điều chế than hoạt tính 1.2 Vật liệu ZIF-11 10 1.3 Vật liệu bán dẫn TiO2 14 1.3.1 Vật liệu TiO2 14 1.3.2 Phức titanium hòa tan nước 17 1.4 Thuốc nhuộm methylene blue, methyl orange methyl red 21 1.4.1 Giới thiệu chung thuốc nhuộm 21 1.4.2 Thuốc nhuộm methylene blue 22 1.4.3 Thuốc nhuộm methyl orange 22 1.4.4 Thuốc nhuộm methyl red 23 1.5 Chloramphenicol trichlosan 24 1.5.1 Chloramphenicol 24 1.5.2 Trichlosan 25 1.6 Một số nghiên cứu ứng dụng composite sở than hoạt tính 27 1.7 Ứng dụng vật liệu sở carbon phân tích điện hóa xúc tác quang hóa 28 vii 1.7.1 Ứng dụng điện hóa 28 1.7.2 Ứng dụng hấp phụ phẩm màu 30 1.8 Nghiên cứu đẳng nhiệt hấp phụ đơn cấu tử đa cấu tử 32 1.8.1 Nghiên cứu đẳng nhiệt hấp phụ đơn cấu tử 32 1.8.2 Nghiên cứu đẳng nhiệt hấp phụ hệ đa cấu tử 34 Chương NỘI DUNG VÀ PHƯƠNG PHÁP NGHIÊN CỨU 40 2.1 Nội dung nghiên cứu 40 2.1.1 Nghiên cứu tổng hợp vật liệu carbon hoạt tính từ vỏ trấu (RHAC) ứng dụng để biến tính điện cực (RHAC/GCE) phân tích điện hóa xác định chloramphenicol mẫu nước hồ nuôi tôm 40 2.1.2 Nghiên cứu tổng hợp vật liệu ZIF-11/RHAC ứng dụng để biến tính điện cực (ZIF-11/RHAC/GCE) phân tích điện hóa xác định trichlosan mẫu mỹ phẩm 40 2.1.3 Nghiên cứu tổng hợp vật liệu TiO2/RHAC ứng dụng làm chất hấp phụ đồng thời ba cấu tử methylene blue, methyl orange methyl red tái sử dụng 40 2.2 Phương pháp nghiên cứu 40 2.2.1 Tổng hợp vật liệu 40 2.2.2 Phương pháp đặc trưng cấu trúc, tính chất khảo sát đặc tính hấp phụ vật liệu 53 Chương KẾT QUẢ VÀ THẢO LUẬN 62 3.1 TỔNG HỢP THAN HOẠT TÍNH TỪ VỎ TRẤU ĐỂ XÁC ĐỊNH CHLORAMPHENICOL 62 3.1.1 Tổng hợp than hoạt tính từ vỏ trấu 62 3.1.2 Xác định chloramphenicol điện cực biến tính RHAC/GCE 69 3.2 NGHIÊN CỨU TỔNG HỢP ĐIỆN CỰC BIẾN TÍNH BẰNG COMPOSITE ZIF-11/RHAC (ZIF-11/RHAC/GCE) ĐỂ XÁC ĐỊNH TRICHLOSAN 87 viii synthesis of RHO-type zeolitic imidazolate frameworks: synthesis and formation mechanism of ZIF-11 and ZIF-12 Dalt Trans 42(47):16608– 16613 48 Ho YS, McKay G (1998), A Comparison of 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