Synthesis and Electrochemical Biosensing Properties of Pyridine Dicarboxylic Acid Decorated Rare-earth-incorporatedTellurotungstates

doi:10.7503/cjcu20210561

Abstract

Abstract:

A family of rare 2，6-pyridinedicarboxylic acid decorated rare-earth（RE）-incorporated Keggin-type tellurotungstates（TTs）（PTEA）₇H₃K［RE₂（B-α-TeW₉O₃₃）₃W₃O₅（H₂O）₃（HDPA）］·22H₂O［RE=Ce³⁺（1）， Pr³⁺（2）， Nd³⁺（3）， Sm³⁺（4）； H₂DPA=2，6-pyridinedicarboxylic acid； PTEA=protonated triethanolamine］ were synthesized by the one-step self-assembly strategy in NaAc aqueous solution via microwave heating method. The polyanion of isomorphic compounds 1—4 consists of three trivacant Keggin ［B-α-TeW₉O₃₃］^8- building blocks linked by a ｛RE₂W₃O₅（H₂O）₃（HDPA）｝¹³⁺ heterometallic cluster. In this heterometallic cluster， HDPA as quadridentate ligand coordinates with two RE ions（RE1 and RE2） to form planar tri-heterocycle structure， which is perpendicular to the planar constructed by W2， W2A and W16 centers. Additionally， compound 1 can combinate with carboxylic multi-walled carbon nanotube（CMWCNT） to produce the 1-CMWCNT composite， which was then used as electrode material to establish electrochemical biosensor for detecting sequence-specific DNA.

Key words: Polyoxometalate, Tellurotungstate, Electrochemical biosensing

CLC Number:

O614

TrendMD:

JIANG Jun, GONG Tiantian, ZHANG Chengpeng, LIU Xiaoqian, ZHAO Junwei. Synthesis and Electrochemical Biosensing Properties of Pyridine Dicarboxylic Acid Decorated Rare-earth-incorporatedTellurotungstates[J]. Chem. J. Chinese Universities, 2022, 43(1): 20210561.

Figures/Tables 8

Fig.1 Trimeric [Sm2(B?α?TeW9O33)3W3O5(H2O)3(HDPA)]11– polyanion(A), three {TeW9} building blocks(B), isosceles triangle formed by three {TeW9} units(C), top view of the {Sm2W3O5(H2O)3(HDPA)}13+ central cluster(D), isosceles triangle constructed by three {WOn} atoms in the central cluster(E), reversely arrayed fashion of two isosceles triangles(F), side view of the {Sm2W3O5(H2O)3(HDPA)}13+ central cluster(G), highlight of the “anthracene”?like ring plane being perpendicular to the isosceles triangle defined by three W atoms(W16, W2 and W2A) in the central cluster(H), coordination geometry of the Sm13+ ion(I), coordination geometry of the Sm23+ ion(J)The atoms with the suffix A are generated by the symmetry operation: x, 0.5-y, z. C: black, N: blue, O: red, RE: amaranth, Te: atrovirens, W: orange; H: green, {WO6}: orange.

Fig.2 Packing architecture of the polyanions of 4 with a regular —ABAB— fashion in ab plane(A), four spatial orientations of the polyanions of 4(B), layer A in the bc plane(C), layer B in the bc plane(D), simplified layer A(E), simplified layer B(F), 3D stacking of the polyanions of 4 in the bc plane(G), simplified 3D stacking of the polyanions of 4 in the bc plane(H)The water or PTEA+ cations are omitted for clarity.

Fig.3 SEM images of CMWCNT(A, B), 1?CMWCNT composite(C, D), Au?1?CMWCNT composite(E, F) and EDS of CMWCNT(G), 1?CMWCNT composite(H) and Au?1?CMWCNT composite(I)

Fig.4 Preparation of the 1?CMWCNT composite(A), the 1?CMWCNT composite was dropped on GCE(B), schematic of Au?1?CMWCNT GCE(C), schematic of CP?Au?1?CMWCNT GCE(D), MCH blocking nonspecific binding sites on CP?Au?1?CMWCNT GCE(E), schematic of TD?CP?Au?1?CMWCNT GCE(F), schematic of MB?TD?CP?Au?1?CMWCNT GCE(G) and detection curves of MB?TD?CP?Au?1?CMWCNT GCE(H)

Fig.5 CV curves of different electrodes(A), DPV curves of Au?1?CMWCNT GCEs in different electrodeposition times(t=20, 40, 60, 80, 100, 120 s)(B) and the plot of DPV peak current of Au?1?CMWCNT GCEs versus electrodeposition time(t=20, 40, 60, 80, 100, 120 s)(C)(A) Bare GCE(purple), CMWCNT GCE(orange), 1?CMWCNT GCE(green), Au?1?CMWCNT GCE(red), CP?Au?1?CMWCNT GCE(cyan) and TD?CP?Au?1?CMWCNT GCE(yellow).

Fig.6 DPV curves of CP?Au?1?CMWCNT GCEs with different reaction times between CP and Au NPs(t= 0.5, 1, 1.5, 2, 2.5, 3 h)(A), plot of DPV peak current of CP?Au?1?CMWCNT GCEs versus reaction time between CP and Au NPs(t=0.5, 1, 1.5, 2, 2.5, 3 h)(B), DPV curves of MB?TD?CP?Au?1?CMWCNT GCEs with different hybridization times between CP and TD(t=0.5, 1, 1.5, 2, 2.5, 3 h)(C), plot of DPV peak current of MB?TD?CP?Au?1?CMWCNT GCEs versus hybridization time between CP and TD(t=0.5, 1, 1.5, 2, 2.5, 3 h)(D), DPV curves of MB?TD?CP?Au?1?CMWCNT GCEs with different incubation times in MB solution(t=5, 10, 15, 20, 25, 30 min)(E), and plot of DPV peak current of MB?TD?CP?Au?1?CMWCNT GCEs versus incubation time in MB solution(t=5, 10, 15, 20, 25, 30 min)(F)

Fig.7 DPV curves of MB?TD?CP?Au?1?CMWCNT GCEs with TD concentrations of 10?14—10?7 mol/L(A) and plot of the DPV peak current of MB?TD?CP?Au?1?CMWCNT GCEs versus the logarithm of the TD concentration in the range of 10?14—10?7 mol/L(B)

Fig.8 Comparison of DPV peak currents of MB?TD?CP?Au?1?CMWCNT GCE(a), MB?1MT?CP?Au?1?CMWCNT GCE(b), MB?3MT?CP?Au?1?CMWCNT GCE(c) and MB?NC?CP?Au?1?CMWCNT GCE(d)(A), comparison of DPV peak currents of six different MB?TD?CP?Au?1?CMWCNT GCEs for detecting 10?8 mol/L TD(B) and comparison of DPV peak currents of MB?TD?CP?Au?1?CMWCNT GCEs established immediately(a) and after 7 d(b—f)(C)

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