Luận án Tiến sĩ Hóa học: Tổng hợp vật liệu composite trên cơ sở g-C3N4, ứng dụng trong điện hóa và quang xúc tác

Luận án Tiến sĩ Hóa học Tổng hợp vật liệu composite trên cơ sở g-C3N4, ứng dụng trong điện hóa và quang xúc tác trình bày các nội dung chính sau: Tổng hợp được các composite trên cơ sở vật liệu g-C3N4 bao gồm ZIF-67/gC3N4, ZIF-67/Fe2O3/g-C3N4, TiO2/g-C3N4, ứng dụng trong điện hóa và có hoạt tính xúc tác quang tốt.

ĐẠI HỌC HUẾ TRƯỜNG ĐẠI HỌC KHOA HỌC ĐẶNG THỊ NGỌC HOA TỔNG HỢP VẬT LIỆU COMPOSITE TRÊN CƠ SỞ g-C3N4, ỨNG DỤNG TRONG ĐIỆN HÓA VÀ QUANG XÚC TÁC LUẬN ÁN TIẾN SĨ HÓA HỌC HUẾ, 2022 ĐẠI HỌC HUẾ TRƯỜNG ĐẠI HỌC KHOA HỌC ĐẶNG THỊ NGỌC HOA TỔNG HỢP VẬT LIỆU COMPOSITE TRÊN CƠ SỞ g-C3N4, ỨNG DỤNG TRONG ĐIỆN HĨA VÀ QUANG XÚC TÁC Ngành: Hóa lý thuyết Hóa lý Mã số: 944.01.19 LUẬN ÁN TIẾN SĨ HÓA HỌC Người hướng dẫn khoa học: GS TS Đi h g hiế TS Phạm Lê Minh Thông HUẾ, 2022 LỜI CAM ĐOAN Tôi xin cam đoan luận án cơng trình nghiên cứu riêng tôi, hướng dẫn GS TS Đinh Quang Khiếu TS Phạm Lê Minh Thông Các số liệu kết nghiên cứu nêu luận án trung thực, đồng tác giả cho phép sử dụng chưa công bố cơng trình khác Tác giả luận án Đặng Thị Ngọc Hoa i LỜI CẢM ƠN Lời đầu tiên, tơi xin bày tỏ lịng biết ơn chân thành sâu sắc đến GS.TS Đinh Quang Khiếu tận tâm hướng dẫn, truyền đạt kiến thức kinh nghiệm cho tơi suốt q trình thực luận án Tôi xin cảm ơn TS Phạm Lê Minh Thơng hướng dẫn để tơi hồn thành luận án Tôi xin trân trọng cảm ơn giúp đỡ, dạy nhiệt tình PGS.TS Nguyễn Hải Phong, Bộ mơn Hố phân tích, Trường Đại học Khoa học, Đại học Huế Tôi xin chân thành cảm ơn Quý Thầy Cô Bộ mơn Hóa lý, Q Thầy Cơ Khoa Hóa học, anh chị em Nghiên cứu sinh, Học viên Cao học em sinh viên Khoa Hóa học, Trường Đại học Khoa học, Đại học Huế giúp đỡ, tạo điều kiện thuận lợi cho thời gian học tập, nghiên cứu bảo vệ luận án Tôi xin chân thành cảm ơn Ban Giám hiệu, Ban chủ nhiệm Khoa Cơ đồng nghiệp Bộ mơn Hóa học – Lý sinh, Khoa Cơ bản, Trường Đại học Y Dược, Đại học Huế giúp đỡ tạo điều kiện tốt cho suốt q trình học tập Cuối cùng, tơi xin bày tỏ lời cảm ơn sâu sắc đến người thân gia đình, bạn bè ln quan tâm, khích lệ động viên tơi suốt thời gian học tập nghiên cứu Tôi xin trân trọng cảm ơn! Thành phố Huế, ngày 25 tháng năm 2022 Tác giả luận án Đặng Thị Ngọc Hoa ii DANH MỤC CÁC CHỮ VIẾT TẮT, KÝ HIỆU Viết tắt Tiếng Anh Tiếng Việt AdSV Adsorptive anodic stripping Volt-Ampere hấp phụ hịa tan voltammetry anode AO Auramine O Vàng ASV Anodic stripping voltammetry Volt-Ampere hòa tan anode BET Brunauer-Emmett-Teller Brunauer-Emmett-Teller B-RBS Britton-Robinson Buffer Solution Dung dịch đệm Britton-Robinson CB Conduction band Vùng dẫn COD Chemical oxygen demand Nhu cầu oxygen hóa học CV Cyclic voltammetry Volt-Ampere vịng DCF Diclofenac Diclofenac DP-ASV Differential pulse anodic stripping Volt-Ampere hòa tan anode xung voltammetry vi phân Energy - dispersive X-ray Phổ tán xạ lượng tia X EDX spectroscopy Eg Energy of band gap Năng lượng vùng cấm EtOH Ethanol Ethanol FTIR Fourier transform infrared Phổ hồng ngoại biến đổi Fourier iii GCE Glassy carbon electrode Điện cực than thủy tinh HmIM 2-methyl imidazolate 2-methyl imidazolate HPLC High performance liquid Sắc ký lỏng hiệu cao chromatography IM Imidazolate Imidazolate M Metal Kim loại MB Methylene blue Methylene blue MeOH Methanol Methanol MG Malachite green Malachite green MOFs Metal-organic frameworks Khung hữu - kim loại MR Methyl red Methyl red MS Mass spectroscopy Phổ khối MyB Methyl blue Methyl blue NHE Normal hydrogen electrode Điện cực hydrogen chuẩn PZC Point of zero charge Điểm đẳng điện RE Relative error Độ lệch tương đối Rev Recovery Độ thu hồi RSD Relative standard deviation Độ lệch chuẩn tương đối SEM Scanning electron microscopy Hiển vi điện tử quét iv SV Stripping voltammetry Volt-Ampere hòa tan TEM Transmission electron microscopy Hiển vi điện tử truyền qua UV-Vis Ultraviolet - Visible absorption Phổ hấp thụ tử ngoại – khả kiến spectroscopy UV-Vis Ultraviolet - Visible diffuse Phổ phản xạ khuếch tán tử ngoại - DRS reflectance spectroscopy khả kiến VB Valance band Vùng hóa trị WE Working electrode Điện cực làm việc XPS X-ray photoelectron spectroscopy Phổ quang điện tử tia X XRD X-ray diffraction Nhiễu xạ tia X ZIFs Zeolitic imidazolate frameworks Khung zeolite imidazole v MỤC LỤC Trang LỜI CAM ĐOAN i LỜI CẢM ƠN ii DANH MỤC CÁC KÍ HIỆU, CÁC CHỮ VIẾT TẮT iii MỤC LỤC vi DANH MỤC CÁC BẢNG, SƠ ĐỒ ix DANH MỤC CÁC HÌNH xi MỞ ĐẦU Chương TỔNG QUAN TÀI LIỆU 1.1 T GQ VỀ VẬT LIỆU g-C3N4 1.1.1 Tính chất cấu trúc tinh thể 1.1.2 Phương pháp tổng hợp 11 1.1.3 ng dụng 14 1.2 VẬT LIỆU B T H g-C3N4 V ZIF-67 15 1.2.1 Vật liệu ZIF-67 15 1.2.2 Vật liệu g-C3N4 với -67, Fe2O3 ứng dụng phân tích điện hóa .19 1.3 VẬT LIỆU B T H g-C3N4 V TiO2 23 1.3.1 Vật liệu TiO2 hòa tan .23 1.3.2 Vật liệu g-C3N4 với TiO2 ứng dụng xúc tác quang hóa 26 1.4 GI I THIỆU VỀ O, DC VÀ MB 30 Chương NỘI DUNG VÀ PHƯƠNG PHÁP NGHIÊN CỨU 34 vi 2.1 Ộ D G GH Ê C 34 2.2 PHƯƠ G PHÁP GH Ê C 34 2.2.1 Các phương pháp nghiên cứu đặc trưng vật liệu 34 2.2.2 Phương pháp sắc ký lỏng hiệu cao (HPLC) 43 2.2.3 Sắc ký lỏng hiệu cao ghép nối khối phổ (HPLC-MS) 44 2.2.4 Phương pháp Volt-Ampere hòa tan (SV) 45 2.3 THỰC NGHIỆM 46 2.3.1 Hóa chất 46 2.3.2 Tổng hợp vật liệu 47 2.3.3 Biến tính điện cực GCE vật liệu ZIF-67/Fe2O3/g-C3N4 để xác định AO, vật liệu ZIF-6/g-C3N4 để xác định DCF 51 2.3.4 ghiên cứu hoạt tính quang xúc tác phân hủy MB TiO2/g-C3N4 54 Chương KẾT QUẢ VÀ THẢO LUẬN .59 3.1 GH Ê C T G H P VẬT LIỆU ZIF-67/g-C3N4 VÀ GD TRO G PHÂ T CH Đ Ệ HÓ XÁC ĐỊNH DCF TRO G Ư C T G 59 3.1.1 Tổng hợp vật liệu ZIF-67/g-C3N4 59 3.1.2 Phân tích điện hóa DC điện cực biến tính ( ) -67/g-C3N4 65 3.1.3 Phân tích mẫu thật 73 3.2 D GH Ê G Đ BI C T T G H P VẬT LIỆU ZIF-67/Fe2O3/g-C3N4 VÀ H Đ ỆN CỰC TRO G PHÂ T CH Đ Ệ HÓ G XÁC ĐỊNH AO TRO G THỰC PHẨM 75 3.2.1 Tổng hợp vật liệu ZIF-67/Fe2O3/g-C3N4 .75 3.2.2 Phân tích O điện cực biến tính -67/Fe2O3/g-C3N4 79 3.2.3 Phân tích mẫu thật 87 vii 3.3 GH Ê C LÝ MB DƯ T G H P VẬT LIỆU TiO2/g-C3N4 VÀ NG D NG XỬ Á H SÁ G KHẢ KI N 88 3.3.1 Tổng hợp phức peroxo­hydroxo titanium tan nước .88 3.3.2 Tổng hợp composite TiO2/g-C3N4 90 3.3.3 Hoạt tính xúc tác quang vật liệu TiO2/g-C3N4 96 KẾT LUẬN VÀ 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NGỌC HOA TỔNG HỢP VẬT LIỆU COMPOSITE TRÊN CƠ SỞ g-C3N4, ỨNG DỤNG TRONG ĐIỆN HÓA VÀ QUANG XÚC TÁC Ngành: Hóa lý thuyết Hóa lý Mã số: 944.01.19 LUẬN ÁN TIẾN SĨ HÓA HỌC Người hướng dẫn khoa học: GS... tác? ?? Mục tiêu luận án Tổng hợp composite sở vật liệu g-C3N4 bao gồm ZIF-67/gC3N4, ZIF-67/Fe2O3 /g-C3N4, TiO2 /g-C3N4, ứng dụng điện hóa có hoạt tính xúc tác quang tốt Những óng góp luận án Đã tổng. .. kiếm vật liệu tiên tiến để phát triển điện cực dùng phương pháp nhiều nhà khoa học quan tâm Dựa vào lý trên, chọn đề tài luận án ? ?Tổng hợp vật liệu composite sở g-C3N4, ứng dụng iện hóa quang xúc