(Luận án tiến sĩ) khảo sát tính chất động lực học của một số hạt nano bằng phương pháp tương quan huỳnh quang trên hệ đo tự xây dựng

BỘ GIÁO DỤC VÀ ĐÀO TẠO VIỆN HÀN LÂM KHOA HỌC VÀ CÔNG NGHỆ VIỆT NAM HỌC VIỆN KHOA HỌC VÀ CÔNG NGHỆ - Nguyễn Thị Thanh Bảo KHẢO SÁT TÍNH CHẤT ĐỘNG LỰC HỌC CỦA MỘT SỐ HẠT NANO BẰNG PHƯƠNG PHÁP TƯƠNG QUAN HUỲNH QUANG TRÊN HỆ ĐO TỰ XÂY DỰNG LUẬN ÁN TIẾN SỸ HÓA HỌC Hà Nội – 2022 TIEU LUAN MOI download : skknchat@gmail.com BỘ GIÁO DỤC VÀ ĐÀO TẠO VIỆN HÀN LÂM KHOA HỌC VÀ CÔNG NGHỆ VIỆT NAM HỌC VIỆN KHOA HỌC VÀ CÔNG NGHỆ - Nguyễn Thị Thanh Bảo KHẢO SÁT TÍNH CHẤT ĐỘNG LỰC HỌC CỦA MỘT SỐ HẠT NANO BẰNG PHƯƠNG PHÁP TƯƠNG QUAN HUỲNH QUANG TRÊN HỆ ĐO TỰ XÂY DỰNG Chuyên ngành: Hóa lý thuyết Hóa lý Mã số: 9.44.01.19 LUẬN ÁN TIẾN SỸ HÓA HỌC NGƯỜI HƯỚNG DẪN KHOA HỌC: PGS.TS Đặng Tuyết Phương PGS.TS Đinh Văn Trung Hà Nội – 2022 TIEU LUAN MOI download : skknchat@gmail.com LỜI CAM ĐOAN Tôi xin cam đoan kết nghiên cứu hướng dẫn PGS.TS Đặng Tuyết Phương PGS.TS Đinh Văn Trung, khơng trùng lặp với cơng trình khoa học khác Các số liệu, kết luận án trung thực, chưa công bố tạp chí đến thời điểm ngồi cơng trình tác giả Hà Nội, ngày 20 tháng năm 2022 Tác giả luận án Nguyễn Thị Thanh Bảo TIEU LUAN MOI download : skknchat@gmail.com LỜI CẢM ƠN Tơi xin bày tỏ lịng kính trọng biết ơn sâu sắc tới PGS.TS Đặng Tuyết Phương, người tận tâm hướng dẫn, định hướng nghiên cứu, động viên khích lệ tạo điều kiện giúp đỡ cho tơi suốt q trình thực luận án Tơi xin gửi lời cảm ơn chân thành đến PGS.TS Đinh Văn Trung, thầy hướng dẫn đồng thời người đồng hành ngày tháng nghiên cứu vất vả Tôi xin chân thành cảm ơn tập thể cán bộ, nhân viên phịng Hóa học Bề mặt - Viện Hóa học, đồng nghiệp nhóm Quang phổ Laser nhóm Vật lý khí - Viện Vật lý hỗ trợ, giúp đỡ, ủng hộ, trao đổi khoa học tạo điều kiện tốt cho tơi q trình thực luận án Tơi xin trân trọng cảm ơn Ban lãnh đạo Viện Hóa học, Học viện Khoa học Công nghệ – Viện Hàn lâm Khoa học Công nghệ Việt Nam cán Viện, Học viện quan tâm giúp đỡ tạo điều kiện thuận lợi cho trình học tập nghiên cứu thực luận án Tôi xin trân trọng cảm ơn Ban lãnh đạo Viện Vật lý tạo điều kiện thời gian, vật chất để tơi hồn thành luận án Tôi xin gửi lời cảm ơn đến cô, chú, anh, chị bạn đồng nghiệp Trung tâm Điện tử học Lượng tử, Viện Vật lý quan tâm, giúp đỡ động viên thời gian thực luận án Cuối cùng, xin bày tỏ lời cảm ơn sâu sắc đến gia đình, người thân bạn bè ln dành cho tơi tình cảm chân thành, khích lệ, động viên chia sẻ với suốt thời gian thực luận án Nguyễn Thị Thanh Bảo TIEU LUAN MOI download : skknchat@gmail.com MỤC LỤC DANH MỤC CÁC KÝ HIỆU, CÁC CHỮ VIẾT TĂT i DANH MỤC CÁC BẢNG iii DANH MỤC CÁC HÌNH VẼ VÀ ĐỒ THỊ iv MỞ ĐẦU CHƯƠNG I TỔNG QUAN 1.1 Các hạt nano 1.1.1 Chấm lượng tử bán dẫn 1.1.1.1 Hiệu ứng giam giữ lượng tử 1.1.1.2 Cấu trúc chấm lượng tử 1.1.1.3 Tính chất quang chấm lượng tử 1.1.2 Nano silica 10 1.1.3 Cacbon nanodot (CND) 13 1.1.4 Nano bạc dạng lăng trụ tam giác 14 1.1.5 Ảnh hưởng kích thước hạt nano nghiên cứu y sinh 16 1.2 Phương pháp đo tương quan huỳnh quang FCS 19 1.2.1 Nguyên lý đo phương trình lý thuyết FCS 19 1.2.2 Các đối tượng phát quang đo đạc FCS 22 1.2.3 Cấu hình hệ đo FCS 23 1.2.4 Phương pháp FCS xác định tương tác phân tử 25 1.2.5 Hiệu ứng chống bó (antibunching) đơn phân tử đơn hạt phát quang 26 1.3 Tình hình nghiên cứu giới nước 27 1.3.1 Tình hình nghiên cứu giới 27 1.3.2 Tình hình nghiên cứu nước 30 1.4 Kết luận phần tổng quan 30 CHƯƠNG II THỰC NGHIỆM VÀ PHƯƠNG PHÁP NGHIÊN CỨU 2.1 Hoá chất dụng cụ thí nghiệm 32 TIEU LUAN MOI download : skknchat@gmail.com 2.2 Tổng hợp hạt nano 33 2.2.1 Tổng hợp nano silica 33 2.2.2 Tổng hợp cacbon nanodot 35 2.2.3 Tổng hợp nano bạc dạng lăng trụ 35 2.2.4 Tổng hợp chấm lượng tử CdTe/CdS 36 2.3 Thiết kế hệ đo đạc tương quan huỳnh quang FCS 37 2.3.1 Thiết kế hệ đo FCS 37 2.3.2 Xây dựng hệ điện tử thu nhận xử lý tín hiệu quang 38 2.3.3 Tính tốn đường tương quan thực nghiệm 41 2.3.4 Căn chỉnh hệ đo 41 2.3.5 Tương quan tán xạ SCS 42 2.3.6 Hiệu ứng chống bó 42 2.3.7 Chuẩn bị mẫu 43 2.4 Các phương pháp bổ trợ đặc trưng vật liệu 44 2.4.1 Phổ huỳnh quang 44 2.4.2 Phổ hấp thụ tử ngoại – khả kiến UV-VIS 44 2.4.3 Hiển vi điện tử truyền qua (TEM) 44 2.4.4 Tán xạ ánh sáng động (DLS) 44 CHƯƠNG III KẾT QUẢ VÀ THẢO LUẬN 3.1 Kết xây dựng đặc trưng hệ đo FCS 45 3.1.1 Cấu hình hệ đo FCS 45 3.1.2 Khảo sát kích thước thể tích đo 50 3.1.3 Hệ số khuếch tán chất màu R6G 52 3.1.4 Ảnh hưởng thay đổi nồng độ chất màu 56 3.1.5 Ảnh hưởng cường độ laze 57 3.2 FCS xác định tương tác phân tử sinh học 58 3.3 Xác định kích thước thủy động lực học chấm lượng tử bán dẫn 62 3.3.1 Xác định kích thước thủy động lực học chấm lượng tử CdTe/CdS 62 TIEU LUAN MOI download : skknchat@gmail.com 3.3.2 Xác định kích thước thủy động lực học chấm lượng tử CdTe 65 3.4 Nghiên cứu trình khuếch tán phân tử chất màu chấm lượng tử mơi trường có độ nhớt thay đổi 71 3.5 FCS nano silica mang tâm màu 76 3.6 FCS cacbon nanodot 83 3.7 Tương quan tán xạ SCS 87 3.7.1 Tương quan tán xạ nano bạc 87 3.7.2 Tương quan tán xạ nano silica không phát quang 89 3.8 Đo đạc đơn hạt/đơn phân tử Hiệu ứng chống bó đơn phân tử chất màu đơn hạt phát quang 91 KẾT LUẬN 94 NHỮNG ĐÓNG GÓP MỚI CỦA LUẬN ÁN 96 TÀI LIỆU THAM KHẢO 97 DANH MỤC CÁC CÔNG TRÌNH ĐÃ CƠNG BỐ 113 TIEU LUAN MOI download : skknchat@gmail.com i DANH MỤC CÁC KÝ HIỆU, CÁC CHỮ VIẾT TẮT Ký hiệu, chữ Tên tiếng Việt Tên tiếng Anh viết tắt  Thời gian trễ Delay Time D Thời gian khuếch tán Diffusion Time d Đường kính hạt Particle Diameter DT Hệ số khuếch tán Diffusion Coefficient Số phân tử trung bình Average number of molecules in the thể tích đo measurement volume Rh Bán kính thuỷ động lực học Hydrodynamic Radius G(0) Giá trị G()  = G() at  = ADN Axit deoxyribonucleic Deoxyribonucleic Acid AFM Hiển vi lực nguyên tử Atomic Force Microscopy AgNPr Nano bạc dạng lăng trụ Silver Nanoprism APD Photodiode thác lũ Avalanche Photodiode APTEOS 3-Aminopropyl trietoxy silan (3-Aminopropyl)triethoxysilane AUC Siêu ly tâm phân tích Analytical Ultracentrifuge BSA Albumin huyết bị Bovine Serum Albumin CND Cacbon nanodot Carbon Nanodot DLS Tán xạ ánh sáng động Dynamic Light Scattering DMSO Đimetyl sunfoxit Dimethyl sulfoxide FCS Phổ tương quan huỳnh quang Fluorescence Correlation Spectroscopy HBT Hanbury-Brown-Twiss Hanbury-Brown-Twiss HSA Albumin huyết người Human Serum Albumin N TIEU LUAN MOI download : skknchat@gmail.com ii MPA Axit 3-mecapto propionic 3-Mercaptopropionic Acid MSA Axit mecapto succinic Mercaptosuccinic Acid MTEOS Metyl trietoxy silan Methyltriethoxysilane PMT Ống nhân quang điện Photomultiplier Tube PVP Poly(vinyl pyroliđon) Polyvinylpyrrolidone RB Rođamin B Rhodamine B R6G Rođamin 6G Rhodamine 6G SCS Phổ tương quan tán xạ Scattering Correlation Spectroscopy SEC Sắc ký loại trừ kích thước Size Exclusive Chromatography TEM Hiển vi điện tử truyền qua Transmision Electron Microscopy TEOS Tetraetoxy silan Tetraethoxysilane TMCS Trimetylsilyl clorua Trimethylchlorosilane UV-VIS Tử ngoại – nhìn thấy Ultraviolet - Visible XRD Tán xạ tia X X-ray Diffraction TIEU LUAN MOI download : skknchat@gmail.com iii DANH MỤC CÁC BẢNG Trang Bảng 1.1 Phân loại chấm lượng tử Bảng 2.1 Danh mục hóa chất 32 Bảng 2.2 Danh mục dụng cụ thiết bị 32 Bảng 2.3 Điều kiện tổng hợp nano silica với nhóm chức bề mặt –OH 34 Bảng 2.4 Điều kiện tổng hợp nano silica với nhóm chức bề mặt khác 35 Bảng 3.1 Các thành phần hệ đo FCS xây dựng luận án 48 Bảng 3.2 Các giá trị đo FCS cho RB 52 Bảng 3.3 Các thông số thể tích đo 52 Bảng 3.4 Các giá trị đo FCS cho R6G 54 Bảng 3.5 Hệ số khuếch tán R6G nước so sánh với tài liệu tham khảo 54 Bảng 3.6 Kết đo đạc tương tác ADN sợi đơn phát quang ADN bổ trợ 61 Bảng 3.7 Kết đo FCS chấm lượng tử CdTe/CdS so sánh với RB 64 Bảng 3.8 Kích thước chấm lượng tử CdTe 69 Bảng 3.9 Hệ số khuếch tán kích thước nano silica phát quang có nhóm chức bề mặt – OH 78 Bảng 3.10 Kích thước nano silica phát quang có nhóm chức bề mặt khác 79 Bảng 3.11 Kích thước CND tổng hợp từ saccarozơ 85 Bảng 3.12 Kích thước AgNPr xác định theo phương pháp khác 89 Bảng 3.13 Đường kính hạt (nm) nano silica khơng phát quang xác định theo phương pháp khác 91 TIEU 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Việt nam Luận án ? ?Khảo sát tính chất động lực học số hạt nano phương pháp tương quan huỳnh quang hệ đo tự xây dựng? ?? có mục tiêu: Xây dựng hệ đo tương quan huỳnh quang Ứng dụng hệ để nghiên cứu... KHOA HỌC VÀ CÔNG NGHỆ VIỆT NAM HỌC VIỆN KHOA HỌC VÀ CÔNG NGHỆ - Nguyễn Thị Thanh Bảo KHẢO SÁT TÍNH CHẤT ĐỘNG LỰC HỌC CỦA MỘT SỐ HẠT NANO BẰNG PHƯƠNG PHÁP TƯƠNG QUAN HUỲNH QUANG TRÊN... nhớt cao phương pháp FCS sở hệ đo xây dựng - Khảo sát kích thước số loại hạt nano khác với chấm lượng tử phương pháp FCS (trên sở đo huỳnh quang) SCS (trên sở đo tán xạ) Các hạt bao gồm: nano silica