Nghiên cứu tổng hợp một số vật liệu rây phân tử MeAPO4 ứng dụng làm xúc tác cho phản ứng oxi hoá n parafin

....

BỘ GIÁO DỤC ĐÀO TẠO
TRƯỜNG ĐẠI HỌC BÁCH KHOA HÀ NỘI

Vũ Ngọc Quyền

NGHIÊN CỨU TỔNG HỢP MỘT SỐ VẬT LIỆU RÂY PHÂN TỬ
MeAPO4 ỨNG DỤNG LÀM XÚC TÁC CHO PHẢN ỨNG
OXI HOÁ n-PARAFIN

LUẬN ÁN TIẾN SĨ HOÁ HỌC

Hà Nội, 2012


BỘ GIÁO DỤC ĐÀO TẠO
TRƯỜNG ĐẠI HỌC BÁCH KHOA HÀ NỘI

Vũ Ngọc Quyền

NGHIÊN CỨU TỔNG HỢP MỘT SỐ VẬT LIỆU RÂY PHÂN
TỬ MeAPO4 ỨNG DỤNG LÀM XÚC TÁC CHO PHẢN ỨNG
OXI HỐ n-PARAFIN

Chun ngành: Hố dầu và xúc tác Hữu cơ
Mã số: 62.44.35.01

LUẬN ÁN TIẾN SĨ HOÁ HỌC

NGƯỜI HƯỚNG DẪN KHOA HỌC

1. PGS. TS Nguyễn Văn Phất
2. GS. TS Đào Văn Tường

Hà Nội - 2012


LỜi CAM ĐOAN
Tơi xin cam đoan đây là cơng trình nghiên cứu khoa học của riêng tôi, các
số liệu và kết quả nghiên cứu trong Luận án là trung thực và chưa từng được cơng
bố dưới bất kỳ hình thức nào.
Hà Nội, năm 2012
Nghiên cứu sinh

Vũ Ngọc Quyền


1
MỤC LỤC
LỜI MỞ ĐẦU ............................................................................................... 8
CHƯƠNG 1. TỔNG QUAN ................................................................... 10
1.1. Rây phân tử .................................................................................. 10
1.1.1. Khái niệm .............................................................................. 10
1.1.2. Phân loại rây phân tử............................................................. 10
1.2. Rây phân tử zeolit ........................................................................ 11
1.2.1. Khái niệm .............................................................................. 11
1.2.2. Phân loại ................................................................................ 11
1.2.3. Cấu trúc tinh thể .................................................................... 12
1.2.4. Tính chất................................................................................ 13
1.3. Rây phân tử aluminophosphat...................................................... 17

1.3.1. Khái niệm .............................................................................. 17
1.3.2. Phân loại và cấu trúc của rây phân tử AlPO4 ........................ 17
1.4. Rây phân tử metalaluminophotphate (MeAPO4) ......................... 19
1.4.1. Giới thiệu về rây phân tử MeAPO4 ....................................... 19
1.4.2. Thay thế đồng hình của Me................................................... 20
1.4.3. Ứng dụng và lý thuyết quá trình tổng hợp xúc tác MeAPO4:
......................................................................................................... 28
1.5. Tổng quan về phản ứng oxi hố. .................................................. 30
1.5.1. Phản ứng oxi hóa và phân loại .............................................. 30
1.5.2. Q trình oxi hố có xúc tác trong pha lỏng đồng thể .......... 31
1.5.3. Xúc tác dị thể ........................................................................ 33
1.5.4. Phản ứng oxi hóa n-parafin ................................................... 34
1.5.5. Một số kết quả đã nghiên cứu về oxi hoá n-parafin.............. 37
CHƯƠNG 2. THỰC NGHIỆM VÀ PHƯƠNG PHÁP .......................... 39
NGHIÊN CỨU ........................................................................................ 39
2.1. Tổng hợp MeAPO4 (Me = V, Ti, Fe) ........................................... 39
2.1.1 Nguyên tắc tổng hợp .............................................................. 39
2.1.2. Tiến hành tổng hợp ............................................................... 40
2.2. Các phương pháp nghiên cứu đặc trưng xúc tác và nghiên cứu
phản ứng oxi hóa n-hexan ................................................................. 42
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DANH MỤC CÁC CƠNG TRÌNH ĐÃ CƠNG BỐ
1.

2.

3.

4.

5.

6.

7.

Vũ Ngọc Quyền, Nguyễn Văn Phất, Hoàng Văn Hoan, Nguyễn
Thị Hà; Thử nghiệm sử dụng muối Natri của axit béo từ quá trình
oxi hố n-parafin làm chất tẩy rửa; Khoa học và cơng nghệ số 53/2011.p 53
Vũ Ngọc Quyền, Đào Quốc Tuỳ, Hoàng Thanh Bình, Nguyễn
Văn Phất; Nghiên cứu chuyển hố cao lanh Tun Quang thành
Zeolit;; Tạp chí Hố học số T.43 (5A), năm 2005, p107-111.
Vũ Ngọc Quyền, Nguyễn Văn Phất, Hoàng Văn Hoan, Ngô Xuân
Anh; Tổng hợp và ứng dụng xúc tác FeAPO trong phản ứng oxi
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Vũ Ngọc Quyền, Đào Quốc Tuỳ; Tổng hợp và đặc trương của
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