Nghiên cứu chế tạo một số vật liệu nano vô cơ hiệu năng cao định hướng ứng dụng trong xử lý nước

BỘ GIÁO DỤC VÀ ĐÀO TẠO VIỆN HÀN LÂM KHOA HỌC VÀ CÔNG NGHỆ VIỆT NAM HỌC VIỆN KHOA HỌC VÀ CÔNG NGHỆ - NGHIÊN CỨU CHẾ TẠO MỘT SỐ VẬT LIỆU NANO VÔ CƠ HIỆU NĂNG CAO ĐỊNH HƯỚNG ỨNG DỤNG TRONG XỬ LÝ NƯỚC LUẬN ÁN TIẾN SĨ HÓA HỌC HÀ NỘI - 2022 VIỆN HÀN LÂM KHOA HỌC VÀ CÔNG NGHỆ VIỆT NAM HỌC VIỆN KHOA HỌC VÀ CÔNG NGHỆ …… … ***………… NGHIÊN CỨU CHẾ TẠO MỘT SỐ VẬT LIỆU NANO VÔ CƠ HIỆU NĂNG CAO ĐỊNH HƯỚNG ỨNG DỤNG TRONG XỬ LÝ NƯỚC LUẬN ÁN TIẾN SĨ HÓA HỌC Chuyên ngành: Hóa vơ Mã số: 44 01 13 Người hướng dẫn khoa học GS TS TRẦN ĐẠI LÂM Hà Nội - 2022 LỜI CẢM ƠN Lời đầu tiên, xin bày tỏ lịng kính trọng biết ơn sâu sắc tới cố PGS TS Vũ Anh Tuấn, người anh, người thầy tận tình hướng dẫ n tơi th ự c hi ệ n cơng trình nghiên c ứ u Tôi xin trân trọng cảm ơn GS TS Trần Đại Lâm, người thầy tiếp tục hướng dẫn tơi hồn thành luận án Tơi xin trân trọng cảm ơn lãnh đạo Viện Hàn lâm Khoa học Cơng nghệ Việt Nam, ban lãnh đạo viện Hóa học, Học viện Khoa học Công nghệ - Viện Hàn lâm Khoa học Công nghệ Việt Nam tạo điều kiện thuận lợi để tơi thực hồn thành cơng trình nghiên cứu Xin chân thành cảm ơn bạn bè, đồng nghiệp gia đình động viên, tạo điều kiện giúp đỡ tơi suốt q trình thực luận án Nghiên cứu sinh LỜI CAM ĐOAN Tôi xin cam đoan, cơng trình nghiên cứu độc lập tơi hướng dẫn người thầy Hầu hết số liệu, kết luận án nội dung từ báo xuất thành viên tập thể khoa học, đồng tác giả cho phép sử dụng Các số liệu, kết nghiên cứu trình bày trình bày luận án trung thực chưa tác giả khác công bố cơng trình Tác giả luận án NCS MỤC LỤC DANH MỤC CÁC KÍ HIỆU VÀ CHỮ VIẾT TẮT i DANH MỤC BẢNG iii DANH MỤC HÌNH VÀ ĐỒ THỊ v MỞ ĐẦU CHƯƠNG TỔNG QUAN 1 Quá trình hấp phụ loại bỏ chất ô nhiễm nước 1 Các chất ô nhiễm chủ yếu cần ưu tiên xử lý nước 1 Các công nghệ phổ biến để loại bỏ chất ô nhiễm 1 Quá trình hấp phụ để loại bỏ chất ô nhiễm nước Vật liệu hấp phụ nano, nanocomposite xử lý nước 10 14 Vật liệu nano với vai trò chất hấp phụ nano xử lý nước 15 2 Vật liệu hấp phụ nanocomposite xử lý nước 17 Những vấn đề liên quan trực tiếp đến nội dung nghiên cứu luận án 20 Khoáng sét bentonite - vật liệu nguồn chế tạo nanocomposite 20 Phương pháp tổng hợp nanocomposite Fe3O4/bentonite 23 3 Tình hình nghiên cứu chế tạo ứng dụng FB xử lý nước 25 Nano sắt hóa trị khơng (nZVI) oxit phức hợp Fe-Mn 28 Hydrogel nanocomposite sở chitosan 31 Polyme in dấu phân tử ứng dụng xử lý nước nước thải 34 CHƯƠNG THỰC NGHIỆM Tổng hợp vật liệu 37 37 1 Nguyên liệu, hóa chất 37 2 Tổng hợp vật liệu FB 37 Tổng hợp vật liệu IFMB 39 Tổng hợp vật liệu CAB/CGA 42 2 Nghiên cứu khả hấp phụ vật liệu 44 2 Khả hấp phụ vật liệu FB 44 2 Khả hấp phụ vật liệu IFMB – Hấp phụ RY-145 46 2 Khả hấp phụ vật liệu CAB/CGA – Hấp phụ amoni Nghiên cứu khả tái sử dụng vật liệu 47 47 Các phương pháp xác định đặc trưng vật liệu phân tích đánh giá kết hấp phụ 48 Nhiễu xạ tia X (XRD) 48 Phổ hồng ngoại (FTIR) 48 Hiển vi điện tử quét phát xạ trường (FE-SEM) 49 4 Hiển vi điện tử truyền qua (TEM) 49 Tán xạ ánh sáng 49 Đẳng nhiệt hấp phụ khí nitơ 49 Phổ tán sắc lượng tia X (EDX) 49 Phương pháp đo đường cong từ hoá 49 Phân tích nhiệt (TG-DTA) 49 10 Phương pháp dịch chuyển pH (pH drift method) 49 11 Xác định độ trương nở vật liệu CAB/CGA 50 12 Hấp thụ nguyên tử AAS 50 13 Phương pháp đo phổ UV-Vis 50 14 Phương pháp so màu xác định nồng độ amoni 51 15 Phương pháp phân tích xác định tiêu COD 51 16 Phương pháp phân tích xác định tiêu TOC CHƯƠNG KẾT QUẢ VÀ THẢO LUẬN Vật liệu FB 51 52 52 1 Nghiên cứu lựa chọn thành phần FB chế độ nung 52 Các đặc trưng vật liệu 53 3 Khả hấp phụ vật liệu 61 Vật liệu IFMB 74 Tối ưu hóa thành phần IFMB 74 2 Các đặc trưng vật liệu 80 3 Khả hấp phụ thuốc nhuộm RY-145 IFMB 83 Tái sử dụng vật liệu 3 Vật liệu CAB/CGA 89 91 3 Tổng hợp vật liệu 91 3 Các đặc trưng vật liệu CAB/CGA 98 3 Khả hấp phụ amoni CAB/CGA 101 3 Tái sử dụng vật liệu 106 KẾT LUẬN 108 NHỮNG ĐĨNG GĨP MỚI CỦA LUẬN ÁN 110 CÁC CƠNG TRÌNH CƠNG BỐ LIÊN QUAN ĐẾN LUẬN ÁN 111 TÀI LIỆU THAM KHẢO 112 i DANH MỤC CÁC KÍ HIỆU VÀ CHỮ VIẾT TẮT AA Acrylic axit AAS Phương pháp quang phổ hấp thụ nguyên tử AOPs Quá trình oxy hóa nâng cao BOD Nhu cầu oxy sinh học CAB CTS-g - poly(acrylic acid)/bentonite Hydrogel composite mạng xen kẽ CTS-g-poly(acrylic CAB/CGA acid)/bentonite với CTS-GA COD Nhu cầu oxy hóa học CTS Chitosan FB Nanocomposite Fe3O4/bentonite FMB Composite oxit phức hợp Fe – Mn bentonite FMO Oxit phức hợp Fe - Mn GA Glutaraldehyde HG Hydrogel HC Hydrogel composite HM Kim loại nặng IFMB Vật liệu composite nZVI/oxit phức hợp (Fe-Mn)/bentonite KPS Kali persulphate MBA N,N’-methylene bisacrylamide MIPs Polyme in dấu phân tử MMT Montmorillonite MNCs Nanocomposite kim loại MONCs Nanocomposite oxit kim loại MONPs Nano oxit kim loại NC Nanocomposite NOCs Chất hữu tự nhiên nZVI Vật liệu nano sắt không nZVI/B Vật liệu nano sắt không bentonite PAA Polyacrylic axit PEG Polyethylene glycol ii PNCs Polyme nanocomposite PZC Điểm điện tích khơng RSM Phương pháp đáp ứng bề mặt SOCs Chất hữu tổng hợp TB Tinh bột TOC Tổng lượng carbon hữu iii DANH MỤC BẢNG Trang Bảng 1: Ưu, nhược điểm kỹ thuật sử dụng để loại bỏ chất ô nhiễm Bảng Một số nghiên cứu tổng hợp FB, chất gây ô nhiễm mục tiêu 27 trình loại bỏ chúng Bảng Nồng độ dung dịch tiền chất tổng hợp IFMB 40 Bảng 2 Điều kiện thí nghiệm xác định thơng số quy trình tổng hợp CAB 44 Bảng Hiệu suất hấp phụ As(V) mẫu vật liệu có thành phần khác 53 Bảng Hiệu suất hấp phụ As(V) mẫu vật liệu nung nhiệt 53 độ khác Bảng 3 Độ bền hóa học mẫu vật liệu 53 Bảng Kết phân tích EDX mẫu FB75-500 58 Bảng Diện tích bề mặt số mẫu vật liệu 58 Bảng Số liệu đẳng nhiệt hấp phụ As(V) As(III) FB100-80 64 Bảng Số liệu đẳng nhiệt hấp phụ As(III) As(V) FB75-500 64 Bảng Dung lượng hấp phụ As cực đại theo Langmuir vật liệu FB 66 Bảng Số liệu đẳng nhiệt hấp phụ Pb2+ Cd2+ vật liệu FB thông số 69 mơ hình đẳng nhiệt hấp phụ Bảng 10 So sánh dung lượng hấp phụ Pb2+ Cd2+ số vật liệu 70 Bảng 11 So sánh dung lượng hấp phụ RR195 số vật liệu 74 Bảng 12 Bảng ma trận thí nghiệm tối ưu hóa 75 Bảng 13 Thành phần 15 mẫu IFMB tổng hợp 75 Bảng 14 Bảng 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LUẬN ÁN TIẾN SĨ HÓA HỌC Chuyên ngành: Hóa vơ Mã số: 44 01 13 Người hướng dẫn khoa... nhiều vật liệu nano, nanocomposite khác đã, nghiên cứu chế tạo sử dụng chất xúc tác, hấp phụ hiệu để loại bỏ chất ô nhiễm nước [37] Vật liệu nano với vai trò chất hấp phụ nano xử lý nước Lớp vật liệu. .. nghệ nano ứng dụng xử lý nước từ phịng thí nghiệm đến ứng dụng quy mô lớn thực tế [58] 2 Vật liệu hấp phụ nanocomposite xử lý nước Ngày nay, vật liệu NC lên lựa chọn thay để khắc phục hạn chế vật