Trong nghiên cứu này chúng tôi tiến hành tổng hợp polyme theo tỷ lệ mol hợp phần của
Pa với Py bao gồm (0 mM:160 mM); (40 mM:120 mM); (80 mM:80 mM); (120 mM:40
mM); (160 mM:0 mM). Hình 5.6 trình bày đáp ứng dòng-thế của điện cực SPCE được tổng
hợp màng polyme với tỷ lệ mol hợp phần Pa/Py khác nhau. Thông qua giá trị cường độ đỉnh
ôxy hóa hoặc đỉnh khử ta có thể đánh độ dẫn của màng polyme PPy-Ppa hình thành trên điện
cực làm việc. Kết quả cho thấy các màng PPy-PPa đều cho đáp ứng điện hóa tốt trong dung
dịch đo. Tuy nhiên, cường độ dòng đỉnh ôxy hóa và khử của chúng rất khác nhau và phụ
thuộc vào tỷ lệ hợp phần của Pa so với Py. Màng PPa thuần (số mol Py là 0) cho đáp ứng
điện hóa thấp nhất, không có sự xuất hiện đỉnh đỉnh ôxy hóa-khử. Khi tỷ lệ mol Pa so với
Py tăng lên thì cường độ dòng đỉnh ôxy hóa và khử đều giảm và vị trí đỉnh đỉnh có xu hướng
dịch về phía điện áp cao. Điều này có thể được giải thích là do sự có mặt của Pa đã làm tăng
tính thấm ướt bề mặt, giảm tính kỵ nước của Py và do độ dẫn của Pa thấp hơn so với Py. Tại
tỷ lệ hợp phần của Pa với Py là 1:3 (40 mM:120 mM) cho màng có độ dẫn cao nhất và đáp
ứng điện hóa tốt nhất với hai đỉnh ôxy hóa và khử rất rõ ràng tại điện áp lần lượt là +0,26 V
và -0,06 V vs. Ag/AgCl. Như vậy, tỷ lệ hợp phần này được lựa chọn để tổng hợp màng
polyme ứng dụng chế tạo cảm biến.
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3. Đỗ Thị Ngọc Trâm, Trương Thị Ngọc Liên (2018), Cảm biến điện hóa glucose sử
dụng cấu trúc đa lớp giữa polyme oxy hóa - khử Osmium và enzyme glucose oxidase.
Những tiến bộ trong Vật lý Kỹ thuật và Ứng dụng - CAEP V, ISBN 978-604-913-
232-2, tr.212-218.
4. Đỗ Thị Ngọc Trâm, Yoshiakia Ukita, Trương Thị Ngọc Liên (2018), Nghiên cứu
thiết kế chíp vi lưu li tâm tích hợp với điện cực mực in ứng dụng trong cảm biến sinh
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đăng 17/04/2018).
5. Trương Thị Ngọc Liên, Đỗ Thị Ngọc Trâm. Đăng kí sáng chế: “Quy trình tổng
hợp vật liệu lai cấu trúc nano hai chiều giữa polyme đồng trùng hợp
polypyrrole-polypyrrole carboxyl (PPy-PPa) và oxit graphene dạng khử điện
hóa (erGO) ứng dụng chế tạo cảm biến trong chẩn đoán bệnh sớm” (chấp
nhận đơn hợp lệ ngày 26/06/2018).
- 1 -
PHỤ LỤC
Phụ lục 1. Giá trị thành phần mạch tương đương Randles của cảm biến mAb
hCG/SAM(MHDA)/SPAuE
Nồng độ kháng nguyên
α-hCG (ng/mL)
Thành phần trong mạch Randles
Rs (k) Rct (k) Cdl (F)
0 1,60 ± 0,09 9,35 ± 1,8 3,04 ± 0,01
0,1 1,65 ± 0,10 9,41 ± 1,9 2,79 ± 0,02
4 1,66 ± 0,10 16,5 ± 2,9 2,46 ± 0,02
10 1,49 ± 0,09 19,8 ± 4,7 2,38 ± 0,01
20 1,69 ± 0,09 21,3 ± 2,4 2,05 ± 0,02
30 1,59 ± 0,10 24,7 ± 4,3 1,96 ± 0,02
70 1,55 ± 0,09 32,4 ± 2,5 1,90 ± 0,02
100 1,60 ± 0,09 38,1 ± 5,4 1,75 ± 0,02
Phụ lục 2. Giá trị thành phần mạch tương đương Randles cảm biến PSA-
aptamer/SAM(MHDA)/SPAuE với nồng độ aptamer (5 µg/mL, 50 µg/mL)
Nồng độ
kháng
nguyên
PSA
(ng/mL)
Giá trị thành phần của mạch tương đương Randles
5 µg/mL aptamer /MHDA/ SPAuE 50 µg/mL aptamer /MHDA/ SPAuE
Rs (kΩ) Rct (kΩ) Cdl (µF) Rs (kΩ) Rct (kΩ) Cdl (µF)
0 8,65 9,29 2,44 8,93 20,70 6,46
2 8,83 8,23 1,85 9,97 19,45 7,35
4 9,41 6,13 1,13 9,93 18,76 7,03
6 8,89 7,02 1,23 9,57 18,51 6,91
8 8,88 7,39 1,30 9,57 18,62 6,95
10 8,67 7,54 1,20 9,17 18,40 6,94
12 8,72 7,67 1,14 9,17 18,23 6,87
14 8,71 7,72 1,15 8,93 20,70 6,46
- 2 -
Phụ lục 3. Giá trị các thành phần mạch tương đương Randles của các cảm biến PSA-
aptamer/SAM(MHDA)/AuNPs-SPCE với 5 vòng quét tạo hạt nano vàng và các nồng độ aptamer
khác nhau (5 µg/mL, 10 µg/mL, 25 µg/mL, 50 µg/mL, 100 µg/mL).
PSA/aptamer/MHDA/5 CVs AuNPs-SPCE
Nồng
độ
PSA
ng/mL
Giá trị các thành phần mạch tương đương Randles
Aptamer
5 µg/mL
Aptamer
10 µg/mL
Aptamer
25 µg/mL
Aptamer
50 µg/mL
Aptamer
100 µg/mL
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
0 1,496 3,944 2,691 2,558 1,539 4,173 1,422 4,906 1,650 3,551
2 1,501 3,806 2,911 2,544 1,743 3,940 1,553 4,683 1,662 3,327
4 1,623 3,773 2,914 2,501 1,893 3,856 1,613 4,533 1,832 3,042
6 1,673 3,663 2,958 2,354 1,890 3,776 1,704 4,371 1,837 3,029
8 1,766 3,577 3,012 2,330 1,921 3,632 1,746 4,107 1,852 3,033
10 1,827 3,580 3,025 2,296 1,946 3,585 1,762 4,114 1,908 3,028
12 1,847 3,493 3,11 2,282 1,966 3,548 1,765 4,095 1,940 2,902
14 1,850 3,495 3,10 2,284 1,967 3,547 1,766 4,097 1,942 2,905
Phụ lục 4. Giá trị các thành phần mạch tương đương Randles của các cảm biến PSA-
aptamer/SAM(MHDA)/AuNPs-SPCE với 10 vòng quét tạo hạt nano vàng và các nồng độ aptamer
khác nhau (5 µg/mL, 10 µg/mL, 25 µg/mL, 50 µg/mL, 100 µg/mL).
PSA/aptamer/MHDA/10 CVs AuNPs-SPCE
Nồng
độ
PSA
ng/mL
Giá trị các thành phần mạch tương đương Randles
Aptamer
5 µg/mL
Aptamer
10 µg/mL
Aptamer
25 µg/mL
Aptamer
50 µg/mL
Aptamer
100 µg/mL
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
0 1,095 4,172 1,411 3,976 1,488 3,930 1,359 3,878 1,738 3,734
2 1,358 3,615 1,580 3,992 1,489 3,847 1,472 3,564 1,864 3,555
4 1,487 3,361 1,582 3,758 1,614 3,666 1,592 3,488 1,934 3,211
6 1,544 3,329 1,837 3,294 1,655 3,823 1,638 3,432 1,953 3,394
8 1,584 3,373 1,849 3,284 1,782 3,530 1,638 3,432 1,959 3,260
10 1,720 3,224 1,929 3,301 1,827 3,580 1,670 3,295 2,014 3,246
12 1,759 3,160 1,957 3,203 1,852 3,492 1,716 3,350 2,035 3,095
14 1,760 3,164 1,959 3,200 1,853 3,490 1,718 3,348 2,038 3,093
- 3 -
Phụ lục 5. Giá trị các thành phần mạch tương đương Randles của các cảm biến PSA-
aptamer/SAM(MHDA)/AuNPs-SPCE với 15 vòng quét tạo hạt nano vàng và các nồng độ aptamer
khác nhau (5 µg/mL, 10 µg/mL, 25 µg/mL, 50 µg/mL, 100 µg/mL).
Phụ lục 6. Giá trị các thành phần mạch tương đương Randles của các cảm biến MHDA/AuNPs-
modified SPCE với 20 vòng quét tạo hạt nano vàng và các nồng độ aptamer khác nhau (5 µg/mL, 10
µg/mL, 25 µg/mL, 50 µg/mL, 100 µg/mL).
PSA/aptamer/MHDA/20 CVs AuNPs-SPCE
Nồng
độ
PSA
ng/mL
Giá trị các thành phần mạch tương đương Randles
Aptamer
5 µg/mL
Aptamer
10 µg/mL
Aptamer
25 µg/mL
Aptamer
50 µg/mL
Aptamer
100 µg/mL
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
0 1,628 3,932 1,992 3,313 1,918 3,139 1,124 3,415 1,398 2,527
2 1,680 3,995 2,139 3,261 1,981 3,168 1,168 4,128 1,421 2,377
4 1,689 4,290 2,137 3,100 2,040 3,024 1,214 4,542 1,429 2,408
6 1,806 3,731 2,182 2,979 2,094 2,877 1,217 3,663 1,511 2,453
8 1,861 3,774 2,241 3,134 2,106 2,890 1,221 3,448 1,521 2,334
10 1,876 3,569 2,241 3,134 2,161 2,848 1,243 3,601 1,544 2,394
12 2,091 3,376 2,322 3,076 2,149 2,883 1,336 3,459 1,566 2,439
14 2,093 3,374 2,325 3,073 2,150 2,880 1,339 3,456 1,569 2,433
PSA/aptamer/MHDA/15Cvs AuNPs-SPCE
Nồng
độ
PSA
ng/mL
Giá trị các thành phần mạch tương đương Randles
Aptamer
5 µg/mL
Aptamer
10 µg/mL
Aptamer
25 µg/mL
Aptamer
50 µg/mL
Aptamer
100 µg/mL
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
Rct
(kΩ)
Cdl
(µF)
0 1,561 3,745 1,480 4,173 1,697 3,974 1,379 2,564 1,613 4,533
2 1,699 3,521 1,598 4,076 1,880 3,849 1,433 2,496 1,684 4,465
4 1,845 3,422 1,720 3,888 1,890 3,764 1,447 2,439 1,722 4,216
6 1,901 3,243 1,779 3,737 1,909 3,601 1,506 2,437 1,729 4,153
8 1,912 3,147 1,840 3,630 1,915 3,471 1,525 2,353 1,744 4,082
10 1,952 3,104 1,852 3,610 1,953 3,465 1,544 2,350 1,747 4,011
12 1,988 3,068 1,888 3,599 1,956 3,390 1,566 2,394 1,758 3,785
14 1,989 3,066 1,890 3,595 1,957 3,387 1,568 2,390 1,759 3,783
- 4 -
Phụ lục 7. Giá trị các thành phần mạch tương đương Randles của cảm biến được chế tạo với điều
kiện tối ưu: hạt nano vàng tổng hợp trên SPCE 10 CVs và nồng độ aptamer là 5 µg/mL
Nồng độ PSA
(ng/mL)
Giá trị các thành phần mạch tương đương Randles
PSA/aptamer/MHDA/AuNPs-SPCE
Rs (kΩ) Rct (kΩ) Cdl (µF)
0 2,66 1,34 4,58
2 2,67 1,48 4,17
4 2,66 1,60 4,08
6 2,67 1,72 3,90
8 2,66 1,78 3,74
10 2,66 1,87 3,60
12 2,66 1,88 3,54
14 2,66 1,89 3,61
Phụ lục 8. Giá trị các thành phần mạch tương đương Randles được cho bởi khảo sát độ đặc hiệu
PSA-Aptamer/SAM(MHDA)/AuNPs-SPCE
Nồng độ
kháng nguyên
(ng/mL)
Giá trị các thành phần mạch tương đương Randles
hCG Amylin Protein TAU
Rct (kΩ) Cdl (µF) Rct (kΩ) Cdl (µF) Rct (kΩ) Cdl (µF)
0 1,090 3,65 1,121 3,71 1,230 2,57
2 1,097 3,77 1,144 3,68 1,249 2,49
4 1,149 3,83 1,181 3,50 1,260 2,41
6 1,179 3,69 1,141 3,42 1,361 2,45
8 1,178 3,68 1,125 3,45 1,373 2,40
10 1,180 3,73 1,135 3,46 1,370 2,42
12 1,168 3,66 1,125 3,45 1,361 2,42
14 1,170 3,64 1,130 3,46 1,359 2,43
- 5 -
Phụ lục 9. Giá trị Rct của 03 cảm biến mAb AFP/PPy-PPa/SPCE độc lập chế tạo cùng quy trình
công nghệ sử dụng xây dựng đường đặc trưng chuẩn.
Nồng độ
kháng
nguyên
AFP
(ng/mL)
Rct () Rct ()
Giá trị trung
bình Rct M1 M2 M3 M1 M2 M3
0 891,2 945,9 866,2 0,0 0,0 0,0 0,0
5 1368,0 1308,0 1573,0 476,8 362,1 706,8 484,8 ± 111,0
10 1895,0 1430,0 1880,0 1003,8 484,1 1013,8 859,3 ± 187,6
20 2174,0 1811,0 2032,0 1282,8 865,1 1165,8 1149,1 ± 142,0
30 2443,0 2527,0 2540,0 1551,8 1581,1 1673,8 1679,8 ± 116,4
40 3145,0 3092,0 2800,0 2253,8 2146,1 1933,8 2095,3 ± 104,6
50 3358,0 3377,0 3094,0 2466,8 2431,1 2227,8 2414,6 ± 93,4
60 3820,0 3755,0 3293,0 2928,8 2809,1 2426,8 2831,1 ± 213,1
70 4050,0 3989,0 4024,0 3158,8 3043,1 3157,8 3187,8 ± 101,9
80 4166,0 4270,0 4538,0 3274,8 3324,1 3671,8 3447,1 ± 147,6
90 4072,0 4302,0 4340,0 3180,8 3356,1 3473,8 3465,6 ± 197,1
100 4071,0 4103,0 4242,0 3179,8 3157,1 3375,8 3315,3 ± 146,9
- 6 -
Phụ lục 10. Giá trị Rct của 03 cảm biến mAb AFP/PPy-PPa/erGO-SPCE độc lập chế tạo cùng quy
trình công nghệ sử dụng xây dựng đường đặc trưng chuẩn.
Nồng độ
kháng
nguyên
AFP
(ng/mL)
Rct () Rct ()
Giá trị trung
bình Rct M1 M2 M3 M1 M2 M3
0 286,7 276,4 290,7 0,0 0,0 0,0 0,0
0,1 426,6 465,3 458,4 139,9 188,9 167,7 171,0 ± 17,2
1 709,9 661,1 751,9 423,2 384,7 461,2 396,5 ± 45,7
5 1104,0 901,9 1160,0 817,3 625,5 869,3 725,5 ± 117,8
10 1307,0 1491,0 1354,0 1020,3 1214,6 1063,3 1006,4 ± 139,5
20 2088,0 1647,0 1829,0 1801,3 1370,6 1538,3 1630,9 ± 176,4
30 2527,0 2469,0 2408,0 2240,3 2192,6 2117,3 2262,6 ± 118,8
40 2984,0 2649,0 2436,0 2697,3 2372,6 2145,3 2469,4 ± 210,4
50 3633,0 3411,0 3127,0 3346,3 3134,6 2836,3 3199,4 ± 213,9
60 4241,0 4014,0 3894,0 3954,3 3737,6 3603,3 3723,1 ± 122,8
70 4593,0 4525,0 5076,0 4306,3 4248,6 4785,3 4425,6 ± 179,8
80 5173,0 4842,0 5403,0 4886,3 4565,6 5112,3 4780,9 ± 218,4
90 5657,0 6024,0 6089,0 5370,3 5747,6 5798,3 5576,1 ± 196,8
100 6207,0 5591,0 6494,0 5920,3 5314,6 6203,3 5804,6 ± 257,2
500 6384,0 6039,0 6839,0 6097,3 5762,6 6548,3 6213,1 ± 283,2
1000 6513,0 5597,0 6053,0 6226,3 5320,6 5756,3 5849,6 ± 311,2
Phụ lục 11. Giá trị Rct của các cảm biến mAb AFP/SAM(p-ATP)/AuNPs-SPCE xây dựng đường
chuẩn
Nồng độ kháng nguyên
AFP (ng/mL)
Rct () Rct () Giá trị trung bình
Rct M1 M2 M3 M1 M2 M3
0 601,5 627,4 596,8 0,0 0,0 0,0 0,0
1 819,4 891,2 854,0 217,9 263,8 257,2 246,3 ± 18,9
10 1199,0 1186,0 1344,0 597,5 558,6 747,2 634,4 ± 75,2
20 1553,0 1453,0 1555,0 951,5 825,6 958,2 911,8 ± 57,4
30 2141,0 1853,0 1755,0 1539,5 1225,6 1158,2 1307,8 ± 154,5
40 2460,0 2267,0 2178,0 1858,5 1639,6 1581,2 1693,1 ± 110,3
50 2593,0 2694,0 2442,0 1991,5 2066,6 1845,2 1967,8 ± 81,7
60 2843,0 3094,0 2814,0 2241,5 2466,6 2217,2 2308,4 ± 105,4
70 2983,0 3328,0 3171,0 2381,5 2700,6 2574,2 2552,1 ± 113,7
80 3291,0 3678,0 3661,0 2689,5 3050,6 3064,2 2934,8 ± 163,5
90 3223,0 3273,0 3464,0 2621,5 2645,6 2867,2 2711,4 ± 103,8
100 3151,0 3181,0 3264,0 2549,5 2553,6 2667,2 2590,1 ± 51,4
- 7 -
Phụ lục 12. Giá trị Rct của các cảm biến mAb AFP/poly(p-ATP)/AuNPs-SPCE xây dựng đường
chuẩn
Nồng độ kháng nguyên
AFP (ng/mL)
Rct (k) Rct (k)
Giá trị trung bình Rct
M1 M2 M3 M1 M2 M3
0 5,65 5,59 5,62 0,00 0,00 0,00 0,0
1 7,81 9,11 9,89 2,16 3,52 4,26 3,31 ± 0,77
10 12,29 13,01 18,43 6,64 7,42 12,81 8,96 ± 2,57
20 24,57 21,98 30,70 18,92 16,39 25,08 20,13 ± 3,29
30 37,27 30,09 34,09 31,62 24,50 28,47 28,19 ± 2,46
40 43,12 37,39 48,49 37,47 31,80 42,87 37,38 ± 3,72
50 50,61 44,31 51,04 44,96 38,72 45,42 43,03 ± 2,873
60 55,04 46,90 55,99 49,39 41,31 50,37 47,02 ± 3,81
70 61,78 54,04 58,99 56,13 48,45 53,37 52,65 ± 2,79
80 65,04 61,78 75,58 59,39 56,19 69,96 61,85 ± 5,41
90 70,76 73,40 81,53 65,11 67,81 75,91 69,61 ± 4,19
100 74,73 75,58 82,51 69,08 69,99 76,89 71,98 ± 3,27