DSpace at VNU: Nghiên cứu tổng hợp vật liệu quang xúc tác nano hệ TiO2 -CeO2 và thăm dò khả năng ứng dụng trong xử lý môi trường

Nghiên cứu tổng hợp vật liệu quang xúc tác nano hệ TiO2-CeO2 thăm dò khả ứng dụng xử lý mơi trường Mạc Đình Thiết Trường Đại học Khoa học Tự nhiên Luận án TS Chuyên ngành: Hóa vô cơ; Mã số 62 44 25 01 Người hướng dẫn: PGS.TS Nguyễn Đình Bảng; PGS.TS Nghiêm Xuân Thung Năm bảo vệ: 2013 Abstract Nghiên cứu cách có hệ thống yếu tố có ảnh hưởng đến đặc trưng vật lý hoạt tính quang xúc tác mẫu xúc tác nano TiO2-CeO2 tổng hợp theo phương pháp: tẩm, sol-gel đồng kết tủa Lần tổng hợp vật liệu quang xúc tác nano hệ TiO2-CeO2 phương pháp khác tạo sản phẩm với chế pha tạp khác chế kích thích quang xúc tác khác Ce có vai trò khác bề mặt vào cấu trúc TiO2 trình quang xúc tác Bước đầu đánh giá khả ứng dụng thực tế vật liệu quang xúc tác nano hệ TiO2-CeO2 trình phân hủy, xử lý nước thải dệt nhuộm làng nghề Vạn Phúc – Quận Hà Đông – Hà Nội Kết cho thấy tính khả thi việc ứng dụng vật liệu quang xúc tác nano hệ TiO2-CeO2 tổng hợp xử lý môi trường Khả ứng dụng thực tiễn: Những kết nghiên cứu nhận từ luận án sở khoa học cho trình tổng hợp TiO2 biến tính kích thước nano có hoạt tính quang xúc tác cao với phân hủy chất hữu ô nhiễm, sử dụng tối đa nguồn lượng ánh sáng mặt trời tạo tiền đề cho ứng dụng sản phẩm vào lĩnh vực: xử lý mơi trường nước- khí, diệt khuẩn tạo nguồn lượng thân thiện với môi trường Đây hướng nhằm đưa nghiên cứu vào ứng dụng thực tiễn Keywords Hóa vơ cơ; Vật liệu quang xúc tác nano; Xử lý mơi trường; Hóa học Content MỞ ĐẦU TiO2 vật liệu quang xúc tác quan trọng, phát Fujishima Honda (năm 1972) qua khả phân tách nước thành oxi hyđro điện cực TiO2 [37] Quá trình quang xúc tác sở chất bán dẫn TiO2 q trình oxi hóa nâng cao đầy triển vọng việc phân hủy chất gây ô nhiễm môi trường, dùng để khử độc cho nước không khí… Vật liệu TiO2 có nhiều ưu so với chất bán dẫn có hoạt tính quang xúc tác khác, là: TiO2 có giá thành thấp, trơ hóa học, khả quang hoạt tự phục hồi cao, tái sử dụng dễ dàng [24, 70] Tuy nhiên, việc ứng dụng thực tế TiO2 lĩnh vực chưa mang lại hiệu cao, số hạn chế định: (i)- TiO2 có lượng vùng cấm Eg lớn (3,0 – 3,2 eV) tương ứng với lượng ánh sáng có bước sóng λ ≤ 400 nm Vì vậy, dùng nguồn lượng mặt trời (nguồn lượng vơ tận) q trình sử dụng xạ tử ngoại (UV), xạ UV chiếm trọng phần nhỏ (~ 5%) phổ xạ mặt trời; (ii)- Phản ứng tái hợp electron lỗ trống quang sinh (e-CB - h+VB) TiO2 diễn với tốc độ lớn, làm giảm mạnh hoạt tính xúc tác [12, 87] Để khắc phục hạn chế trên, cần: (i)- Giảm lượng vùng cấm (Eg) cho phép sử dụng mở rộng khả hoạt động quang xúc tác sang vùng khả kiến (Vis) phổ mặt trời; (ii)- Ngăn chặn tái hợp e-CB h+VB TiO2 sau xảy kích hoạt electron Nhiều nhóm tác giả tiến hành nghiên cứu làm giảm lượng vùng cấm TiO2, cách pha tạp kim loại chuyển tiếp khác V, Cr, Fe, Co, Ni, Cu, Tuy nhiên, có kết trái ngược đưa ra, với tăng [60, 61, 93, 157, 158] giảm [23] hoạt tính so sánh với TiO2 tinh khiết Gần đây, có nhiều nghiên cứu pha tạp nguyên tố đất La, Nd, Eu, Ce vào TiO2 cho thấy có hoạt tính vùng ánh sáng nhìn thấy [67, 68, 72, 133, 145, 146, 147] Hơn thế, có mặt nguyên tố đất TiO2 có tác dụng làm giảm tái hợp electron lỗ trống cách hiệu [67, 145, 147] Trong số nguyên tố đất hiếm, việc sử dụng xeri có thuận lợi nguyên tố đất phổ biến nhất, CeO2 sử dụng rộng rãi pin nhiên liệu ứng dụng xử lý ô nhiễm môi trường Trên giới, nghiên cứu biến tính TiO2 xeri mức độ thăm dò khẳng định việc biến tính TiO2 xeri có hiệu hoạt tính quang xúc tác vùng ánh sáng nhìn thấy [72, 108, 133], kết có từ cơng trình cơng bố cho thấy hoạt tính quang xúc tác hàm lượng xeri pha tạp tối ưu khác tùy thuộc vào phương pháp tổng hợp, việc so sánh lý giải đề cập Ở Việt Nam chưa có cơng trình nghiên cứu biến tính TiO2 xeri khảo sát cách hệ thống yếu tố ảnh hưởng đến hoạt tính quang xúc tác hệ TiO2-CeO2 phản ứng phân hủy chất hữu nhiễm Chính vậy, đề tài luận án “Nghiên cứu tổng hợp vật liệu quang xúc tác nano hệ TiO2-CeO2 thăm dò khả ứng dụng xử lý mơi trường” nhằm mục đích nghiên cứu lý thuyết tổng hợp chất xúc tác nano hệ TiO2-CeO2 có hoạt tính quang xúc tác vượt trội so với TiO2 tinh khiết tác động xạ mặt trời Với mục đích đó, nhiệm vụ mà luận án cần thực là: Tổng hợp xúc tác nano hệ TiO2-CeO2 số phương pháp (tẩm, sol-gel đồng kết tủa) Nghiên cứu đặc trưng sản phẩm XRD, EDX, UV-Vis, SEM, TEM, BET Trên sở đó, khẳng định làm rõ vai trò xeri việc thúc đẩy hoạt tính quang xúc tác TiO2 Khảo sát ảnh hưởng điều kiện tổng hợp đến cấu trúc tính chất quang xúc tác sản phẩm, từ lựa chọn điều kiện thích hợp cho trình tổng hợp xúc tác hệ TiO2-CeO2, đồng thời tìm phương pháp tổng hợp chất quang xúc tác hệ TiO2-CeO2 tốt Bước đầu khảo sát thăm dò ứng dụng hoạt tính quang xúc tác sản phẩm TiO2CeO2 xử lý nước thải dệt nhuộm Reference TÀI LIỆU THAM KHẢO Tiếng Việt [1] Vũ Đăng Độ, Triệu Thị Nguyệt (2008), Hóa học vơ cơ, Tập 2, NXB Giáo dục [2] Đặng Thanh Lê, Mai Đăng Khoa, Ngô Sĩ Lương (2008), “Khảo sát hoạt tính xúc tác quang bột TiO2 kích thước nano mét trình khử màu thuốc nhuộm”, Tạp chí Hóa học Tập 46 (2A), tr 139-143 [3] Ngô Sỹ Lương, Lê Diên Thân, 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