Luận án tiến sĩ 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 - PHẠM VĂN LÂM 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 …… ….***………… PHẠM VĂN LÂM 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 HĨA HỌC Chun 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, tơi xin bày tỏ lịng kính trọng biết ơn sâu sắc tới cố PGS.TS Vũ Anh Tuấn, người anh, người thầy tận tình hướng dẫn tơi thực cơng trình nghiên cứu Tơi xin trân trọng cảm ơn GS.TS Trần Đại Lâm, người thầy tiếp tục hướng dẫn tơi hồn thành luận án Tôi xin trân trọng cảm ơn lãnh đạo Viện Hàn lâm Khoa học Công 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 suốt trình thực luận án Nghiên cứu sinh Phạm Văn Lâm 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 Phạm Văn Lâm 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 .1 CHƯƠNG TỔNG QUAN .3 1.1 Quá trình hấp phụ loại bỏ chất ô nhiễm nước 1.1.1 Các chất ô nhiễm chủ yếu cần ưu tiên xử lý nước 1.1.2 Các công nghệ phổ biến để loại bỏ chất ô nhiễm 1.1.3 Quá trình hấp phụ để loại bỏ chất ô nhiễm nước 10 1.2 Vật liệu hấp phụ nano, nanocomposite xử lý nước 14 1.2.1 Vật liệu nano với vai trò chất hấp phụ nano xử lý nước 15 1.2.2 Vật liệu hấp phụ nanocomposite xử lý nước 17 1.3 Những vấn đề liên quan trực tiếp đến nội dung nghiên cứu luận án 20 1.3.1 Khoáng sét bentonite - vật liệu nguồn chế tạo nanocomposite 20 1.3.2 Phương pháp tổng hợp nanocomposite Fe3O4/bentonite 23 1.3.3 Tình hình nghiên cứu chế tạo ứng dụng FB xử lý nước 25 1.3.4 Nano sắt hóa trị không (nZVI) oxit phức hợp Fe-Mn .28 1.3.5 Hydrogel nanocomposite sở chitosan .31 1.3.6 Polyme in dấu phân tử ứng dụng xử lý nước nước thải 34 CHƯƠNG THỰC NGHIỆM 37 2.1 Tổng hợp vật liệu 37 2.1.1 Nguyên liệu, hóa chất 37 2.1.2 Tổng hợp vật liệu FB .37 2.1.3 Tổng hợp vật liệu IFMB 39 2.1.4 Tổng hợp vật liệu CAB/CGA 42 2.2 Nghiên cứu khả hấp phụ vật liệu 44 2.2.1 Khả hấp phụ vật liệu FB 44 2.2.2 Khả hấp phụ vật liệu IFMB – Hấp phụ RY-145 .46 2.2.3 Khả hấp phụ vật liệu CAB/CGA – Hấp phụ amoni 47 2.3 Nghiên cứu khả tái sử dụng vật liệu 47 2.4 Các phương pháp xác định đặc trưng vật liệu phân tích đánh giá kết hấp phụ .48 2.4.1 Nhiễu xạ tia X (XRD) 48 2.4.2 Phổ hồng ngoại (FTIR) 48 2.4.3 Hiển vi điện tử quét phát xạ trường (FE-SEM) .49 2.4.4 Hiển vi điện tử truyền qua (TEM) 49 2.4.5 Tán xạ ánh sáng .49 2.4.6 Đẳng nhiệt hấp phụ khí nitơ 49 2.4.7 Phổ tán sắc lượng tia X (EDX) .49 2.4.8 Phương pháp đo đường cong từ hoá 49 2.4.9 Phân tích nhiệt (TG-DTA) 49 2.4.10 Phương pháp dịch chuyển pH (pH drift method) 49 2.4.11 Xác định độ trương nở vật liệu CAB/CGA 50 2.4.12 Hấp thụ nguyên tử AAS .50 2.4.13 Phương pháp đo phổ UV-Vis .50 2.4.14 Phương pháp so màu xác định nồng độ amoni 51 2.4.15 Phương pháp phân tích xác định tiêu COD 51 2.4.16 Phương pháp phân tích xác định tiêu TOC 51 CHƯƠNG KẾT QUẢ VÀ THẢO LUẬN 52 3.1 Vật liệu FB .52 3.1.1 Nghiên cứu lựa chọn thành phần FB chế độ nung 52 3.1.2 Các đặc trưng vật liệu 53 3.1.3 Khả hấp phụ vật liệu 61 3.2 Vật liệu IFMB 74 3.2.1 Tối ưu hóa thành phần IFMB 74 3.2.2 Các đặc trưng vật liệu 80 3.2.3 Khả hấp phụ thuốc nhuộm RY-145 IFMB 83 3.2.4 Tái sử dụng vật liệu 89 3.3 Vật liệu CAB/CGA 91 3.3.1 Tổng hợp vật liệu 91 3.3.2 Các đặc trưng vật liệu CAB/CGA 98 3.3.3 Khả hấp phụ amoni CAB/CGA 101 3.3.4 Tái sử dụng vật liệu 106 KẾT LUẬN .108 NHỮNG ĐÓNG GÓP 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 ngun tử AOPs Q trình oxy hóa nâng cao BOD Nhu cầu oxy sinh học CAB CTS-g - poly(acrylic acid)/bentonite CAB/CGA Hydrogel composite mạng xen kẽ CTS-g-poly(acrylic 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 1.1: Ưu, nhược điểm kỹ thuật sử dụng để loại bỏ chất ô nhiễm Bảng 1.2 Một số nghiên cứu tổng hợp FB, chất gây ô nhiễm mục tiêu 27 trình loại bỏ chúng Bảng 2.1 Nồng độ dung dịch tiền chất tổng hợp IFMB 40 Bảng 2.2 Điều kiện thí nghiệm xác định thơng số quy trình tổng hợp CAB 44 Bảng 3.1 Hiệu suất hấp phụ As(V) mẫu vật liệu có thành phần khác 53 Bảng 3.2 Hiệu suất hấp phụ As(V) mẫu vật liệu nung nhiệt 53 độ khác Bảng 3.3 Độ bền hóa học mẫu vật liệu 53 Bảng 3.4 Kết phân tích EDX mẫu FB75-500 58 Bảng 3.5 Diện tích bề mặt số mẫu vật liệu 58 Bảng 3.6 Số liệu đẳng nhiệt hấp phụ As(V) As(III) FB100-80 64 Bảng 3.7 Số liệu đẳng nhiệt hấp phụ As(III) As(V) FB75-500 64 Bảng 3.8 Dung lượng hấp phụ As cực đại theo Langmuir vật liệu FB 66 Bảng 3.9 Số liệu đẳng nhiệt hấp phụ Pb2+ Cd2+ vật liệu FB thơng số 69 mơ hình đẳng nhiệt hấp phụ Bảng 3.10 So sánh dung lượng hấp phụ Pb2+ Cd2+ số vật liệu 70 Bảng 3.11 So sánh dung lượng hấp phụ RR195 số vật liệu 74 Bảng 3.12 Bảng ma trận thí nghiệm tối ưu hóa 75 Bảng 3.13 Thành phần 15 mẫu IFMB tổng hợp 75 Bảng 3.14 Bảng mã hóa giá trị biến khảo sát 76 Bảng 3.15 Các hệ số phương trình hồi quy 77 Bảng 3.16 Kết kiểm tra tính tương thích mơ hình 80 Bảng 3.17 Diện tích bề mặt riêng bentonite, FMB IFMB 82 Bảng 3.18 Kết phân tích EDX mẫu IFMB 82 Bảng 3.19 Thay đổi pH dung dịch trình hấp phụ RY-145 84 IFMB 112 TÀI LIỆU THAM KHẢO René P Schwarzenbach, Bernhard Wehrli et al., Global Water Pollution and Human Health, Annu Rev Environ Resour, 2010, 35, 109-136 Chang Min Park, Yeomin Yoon et al., Removal of heavy metals from water sources in the developing world using low-cost materials: A review, Chemosphere, 2019, 229, 142e159 M Wołowiec, T Bajda et al., Removal of Heavy Metals and Metalloids fromWater Using DrinkingWater Treatment Residuals as Adsorbents: A Review, Minerals 2019, 9, 487 E Marón, L Castrillon et al., Removal of ammonium from aqueous solutions with volcanic tuff J Hazard Mater., 2006, 137, 1402-1409 J Huang, P.R Teasdale, Removing ammonium from water and wastewater using cost-effective adsorbents: A review J Env Sci., 2018, 63, 174-197 Javier Mateo-Sagasta, Sara Marjani Zadeh, Hugh Turral, Water pollution from agriculture: a global review Executive summary, 2017, FAO and IWMI P A Rezagama, M Hibbaan, Ammonia-Nitrogen (NH3-N) and AmmoniumNitrogen (NH4+-N) Equilibrium on The Process of Removing Nitrogen By Using Tubular Plastic Media, J Mater Environ Sci., 2017, (S), 4915-4922 W Gong, X Meng, X Tang, P Ji, Core-shell MnO2-SiO2 nanorods for catalyzing the removal of dyes from water, Catalysts, 2017, 7, 19 K.A Adegoke, O.S Bello, Dye sequestration using agricultural wastes as adsorbents, Water Resour Indus., 2015, 12, 8–24 10 Tara, N., Asiri et al., A M Nano-engineered adsorbent for removal of dyes from water: A review Current Current Analytical Chemistry, 2020, 16, 14-40 11 Christie, R.M., Environmental aspects of textile dyeing, Wood head Publishing; ISBN: Cambridge, 2017, p 1845691156 12 Sen, T.K.; Afroze, S.; Ang, H., Equilibrium, kinetics and mechanism of removal of methylene blue from aqueous solution by adsorption onto pine cone biomass of Pinusradiate, Water Air Soil Pollut., 2011, 218, 499-515 13 M T Yagub, H.M Ang et al., Dye and its removal from aqueous solution by adsorption: A review, Adv Colloid Interface Sci., 2014, 209, 172-184 113 14 R Breton, A Boxall "Pharmaceuticals and personal care products in the environment: regulatory drivers and research needs." 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