journal article·2015-07Open access

Interfacial assembly of mesoporous nanopyramids as ultrasensitive cellular interfaces featuring efficient direct electrochemistry

Biao Kong, Debabrata Sikdar, Jing Tang, Yang Liu, Malin Premaratne, Wei Zhang, Yunke Jing, Gengfeng Zheng, Cordelia Selomulya, Dongyuan Zhao

NPG Asia Materials· Volume 7· Issue 7

Abstract

A general method for assembling patterned interfaces of uniform, flexible mesoporous iron oxide nanopyramid islands (NPIs) is presented. The three-dimensional (3D) mesoporous iron oxide–NPI interfaces possess a unique mesostructure that features a large surface area (~158 m2 g−1), a large pore size (~18 nm) and excellent flexibility (can be folded 100 times). Furthermore, the 3D mesoporous Au–NPI interfaces allow efficient immobilization of cytochrome c (Cyt c; more than 165-fold increase) and a significant enhancement of localized surface plasmon resonance (~26-fold at 625 nm) compared with that of two-dimensional (2D) planar iron oxide films without nanopores. More importantly, the ultrasensitive integrated interfaces demonstrate over 1000-fold enhancement of the photocurrent variation on the 3D mesostructures based on the switchable direct electrochemistry of Cyt c. The strategy of interfacial assembly offers new possibilities for the chemical design of patterned mesoporous semiconductors with high flexibility and tailored photocatalytic characteristics. This investigation provides a novel paradigm for an unconventional 3D porous biointerface that can be used for sub-nanomolar level recognition of biomolecules (~0.2 nM for H2O2) and suggests the new concept of large-surface-area 3D mesostructure–protein interfaces as a step toward using direct electrochemistry for biomedical applications. Flexible lab-on-a-chip devices containing iron oxide nanopyramids may kick start new approaches to sub-nanomolar detection of biomolecules. A team of Chinese and Australian researchers led by Dongyuan Zhao from Fudan University used lithographic techniques to pattern surfaces with pointy iron oxide nanopyramids and gold nanoparticles and then loaded the protein cytochrome c (Cyt c). The three-dimensional, mesoporous cavities inside the nanopyramids boosted both cell attachment onto the device and the surface plasmon signals used for biosensing. When the team exposed the biointerface to solar light to initiate the Cyt c redox cycle, they saw a 1,000-fold enhancement in the photoelectrochemical current over typical interfaces. The magnitude of such solar-driven currents makes the device extremely sensitive — the researchers foresee direct monitoring of electrochemical transfer between proteins for real-time disease diagnostics. A general method for assembling patterned interfaces of uniform, flexible mesoporous iron oxide nanopyramid islands is presented. The 3D porous interfaces possess a unique mesostructure that features a large surface area, a large pore size and excellent flexibility. Furthermore, the 3D porous Au–NPI interfaces allow efficient immobilization of cytochrome c and a significant enhancement of localized surface plasmon resonance. More importantly, the ultrasensitive integrated interfaces demonstrate over 1000-fold enhancement of the photocurrent variation on the 3D mesostructures based on the switchable direct electrochemistry cytochrome c. The strategy of interfacial assembly offers new possibilities for the chemical design of patterned mesoporous semiconductors with high flexibility and tailored photocatalytic characteristics.
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Research context

OpenAlex topics: Advanced biosensing and bioanalysis techniques · Iron oxide chemistry and applications · Anodic Oxide Films and Nanostructures

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (55)

Show source-provided references
1. Jiang, S., Cheng, R., Wang, X., Xue, T., Liu, Y., Nel, A., Huang, Y. & Duan, X. Real-time electrical detection of nitric oxide in biological systems with sub-nanomolar sensitivity. Nat. Commun. 4, 2225 (2013).10.1038/ncomms3225 ↗
2. Cui, Y., Wei, Q., Park, H. & Lieber, C. M. Nanowire nanosensors for highly sensitive and selective detection of biological and chemical species. Science 293, 1289–1292 (2001).10.1126/science.1062711 ↗
3. Wu, H.-J., Henzie, J., Lin, W. C., Rhodes, C., Li, Z., Sartorel, E., Thorner, J., Yang, P. & Groves, J. T. Membrane-protein binding measured with solution-phase plasmonic nanocube sensors. Nat. Methods 9, 1189–1191 (2012).10.1038/nmeth.2211 ↗
4. Liu, X., Chen, L., Liu, H., Yang, G., Zhang, P., Han, D., Wang, S. & Jiang, L. Bio-inspired soft polystyrene nanotube substrate for rapid and highly efficient breast cancer-cell capture. NPG Asia Mater. 5, e63. doi:10.1038/am.2013.43 (2013).10.1038/am.2013.43 ↗
5. Wang, H., Meng, F., Cai, Y., Zheng, L., Li, Y., Liu, Y., Jiang, Y., Wang, X. & Chen, X. Sericin for resistance switching device with multilevel nonvolatile memory. Adv. Mater. 25, 5498–5503 (2013).10.1002/adma.201301983 ↗
6. Tang, J., Zhang, Y., Kong, B., Wang, Y., Da, P., Li, J., Elzatahry, A. A., Zhao, D., Gong, X. & Zheng, G. Solar-driven photoelectrochemical probing of nanodot/nanowire/cell interface. Nano Lett. 14, 2702–2708 (2014).10.1021/nl500608w ↗
7. Chen, H., Shao, L., Li, Q. & Wang, J. Gold nanorods and their plasmonic properties. Chem. Soc. Rev. 42, 2679–2724 (2013).10.1039/C2CS35367A ↗
8. Meng, F., Hervault, Y. M., Shao, Q., Hu, B., Norel, L., Rigaut, S. & Chen, X. Orthogonally modulated molecular transport junctions for resettable electronic logic gates. Nat. Commun. 5, 3023 (2014).10.1038/ncomms4023 ↗
9. Xia, F., Feng, L., Wang, S., Sun, T., Song, W., Jiang, W. & Jiang, L. Dual-responsive surfaces that switch between superhydrophilicity and superhydrophobicity. Adv. Mater. 18, 432–436 (2006).10.1002/adma.200501772 ↗
10. Liu, H., Li, Y., Sun, K., Fan, J., Zhang, P., Meng, J., Wang, S. & Jiang, L. Dual-responsive surfaces modified with phenylboronic acid-containing polymer brush to reversibly capture and release cancer cells. J. Am. Chem. Soc. 135, 7603–7609 (2013).10.1021/ja401000m ↗
11. Liu, X., Zhang, F., Wang, Q., Gao, J., Meng, J., Wang, S., Yang, Z. & Jiang, L. Platelet-Inspired multiscaled cytophilic interfaces with high specificity and efficiency toward point-of-care cancer diagnosis. Small 10, 4677–4683 (2014).10.1002/smll.201401530 ↗
12. Liang, K., Such, G. K., Johnston, A. P., Zhu, Z., Ejima, H., Richardson, J. J., Cui, J. & Caruso, F. Endocytic pH-triggered degradation of nanoengineered multilayer capsules. Adv. Mater. 26, 1901–1905 (2014).10.1002/adma.201305144 ↗
13. Guillet-Nicolas, R., Popat, A., Bridot, J. L., Monteith, G., Qiao, S. Z. & Kleitz, F. pH-Responsive nutraceutical–mesoporous silica nanoconjugates with enhanced colloidal stability. Angew. Chem. Int. Ed. 52, 2318–2322 (2013).10.1002/anie.201208840 ↗
14. Zhu, A., Luo, Y. & Tian, Y. Switching the direction of plasmon-induced photocurrents by cytochrome c at Au–TiO2 nanocomposites. Chem. Commun. 42, 6448–6450 (2009).10.1039/b911344d ↗
15. Zhu, A., Luo, Y. & Tian, Y. Plasmon-induced enhancement in analytical performance based on gold nanoparticles deposited on TiO2 film. Anal. Chem. 81, 7243–7247 (2009).10.1021/ac900894p ↗
16. Freeman, R., Finder, T. & Willner, I. Multiplexed analysis of Hg2+ and Ag+ ions by nucleic acid functionalized CdSe/ZnS quantum dots and their use for logic gate operations. Angew. Chem. Int. Ed. 48, 7818–7821 (2009).10.1002/anie.200902395 ↗
17. Gill, R., Patolsky, F., Katz, E. & Willner, I. Electrochemical control of the photocurrent direction in intercalated DNA/CdS nanoparticle systems. Angew. Chem. Int. Ed. 44, 4554–4557 (2005).10.1002/anie.200500830 ↗
18. Halik, M., Klauk, H., Zschieschang, U., Schmid, G., Dehm, C., Schütz, M., Maisch, S., Effenberger, F., Brunnbauer, M. & Stellacci, F. Low-voltage organic transistors with an amorphous molecular gate dielectric. Nature 431, 963–966 (2004).10.1038/nature02987 ↗
19. Duan, X., Huang, Y. & Lieber, C. M. Nonvolatile memory and programmable logic from molecule-gated nanowires. Nano Lett. 2, 487–490 (2002).10.1021/nl025532n ↗
20. Kovtyukhova, N. I. & Mallouk, T. E. Nanowires as building blocks for self-assembling logic and memory circuits. Chem. Eur. J. 8, 4354–4363 (2002).10.1002/1521-3765(20021004)8:19<4354::AID-CHEM4354>3.0.CO;2-1 ↗
21. Javey, A., Kim, H., Brink, M., Wang, Q., Ural, A., Guo, J., McIntyre, P., McEuen, P., Lundstrom, M. & Dai, H. High-κ dielectrics for advanced carbon-nanotube transistors and logic gates. Nat. Mater. 1, 241–246 (2002).10.1038/nmat769 ↗
22. Wei, H., Wang, Z., Tian, X., Käll, M. & Xu, H. Cascaded logic gates in nanophotonic plasmon networks. Nat. Commun. 2, 387 (2011).10.1038/ncomms1388 ↗
23. Long, R., Mao, K., Gong, M., Zhou, S., Hu, J., Zhi, M., You, Y., Bai, S., Jiang, J., Zhang, Q., Wu, X. & Xiong, Y. Tunable oxygen activation for catalytic organic oxidation: schottky iunction versus plasmonic effects. Angew. Chem. Int. Ed. 53, 3205–3209 (2014).10.1002/anie.201309660 ↗
24. Wang, X., Liow, C., Qi, D., Zhu, B., Leow, W. R., Wang, H., Xue, C., Chen, X. & Li, S. Programmable photo-electrochemical hydrogen evolution based on multi-segmented CdS-Au nanorod arrays. Adv. Mater. 26, 3506–3512 (2014).10.1002/adma.201306201 ↗
25. Liang, M. & Guo, L.-H. Photoelectrochemical DNA sensor for the rapid detection of DNA damage induced by styrene oxide and the fenton reaction. Environ. Sci. Technol. 41, 658–664 (2006).10.1021/es0617688 ↗
26. Liu, S., Li, C., Cheng, J. & Zhou, Y. Selective photoelectrochemical detection of DNA with high-affinity metallointercalator and tin oxide nanoparticle electrode. Anal.Chem. 78, 4722–4726 (2006).10.1021/ac052022f ↗
27. Zhang, X., Zhao, Y., Zhou, H. & Qu, B. A new strategy for photoelectrochemical DNA biosensor using chemiluminescence reaction as light source. Biosens. Bioelectron. 26, 2737–2741 (2011).10.1016/j.bios.2010.09.051 ↗
28. Kang, Q., Yang, L., Chen, Y., Luo, S., Wen, L., Cai, Q. & Yao, S. Photoelectrochemical detection of pentachlorophenol with a multiple hybrid CdSexTe1−x/TiO2 nanotube structure-based label-free immunosensor. Anal. Chem. 82, 9749–9754 (2010).10.1021/ac101798t ↗
29. Feng, H., Zhou, L., Li, J., Tran, T. T., Wang, N., Yuan, L., Yan, Z. & Cai, Q. A photoelectrochemical immunosensor for tris (2, 3-dibromopropyl) isocyanurate detection with a multiple hybrid CdTe/Au–TiO2 nanotube arrays. Analyst 138, 5726–5733 (2013).10.1039/c3an00956d ↗
30. Li, Y. J., Ma, M. J., Yin, G., Kong, Y. & Zhu, J. J. Phthalocyanine-sensitized graphene–CdS nanocomposites: an enhanced photoelectrochemical immunosensing platform. Chem. Eur. J. 19, 4496–4505 (2013).10.1002/chem.201203521 ↗
31. Fan, G., Han, L., Zhu, H., Zhang, J. & Zhu, J.-J. Ultrasensitive photoelectrochemical immunoassay for matrix metalloproteinase-2 detection based on CdS: Mn/CdTe co-sensitized TiO2 nanotubes and signal amplification of SiO2@Ab2 conjugates. Anal. Chem. 86, 12398–12405 (2014).10.1021/ac504027d ↗
32. Zhao, W.-W., Yu, P.-P., Xu, J.-J. & Chen, H.-Y. Ultrasensitive photoelectrochemical biosensing based on biocatalytic deposition. Electrochem. Commun. 13, 495–497 (2011).10.1016/j.elecom.2011.02.031 ↗
33. Zhao, W.-W., Xu, J.-J. & Chen, H.-Y. Photoelectrochemical bioanalysis: the state of the art. Chem. Soc. Rev. 44, 729–741 (2015).10.1039/C4CS00228H ↗
34. Zhao, W.-W., Xu, J.-J. & Chen, H.-Y. Photoelectrochemical DNA biosensors. Chem. Rev. 114, 7421–7441 (2014).10.1021/cr500100j ↗
35. Stoll, C., Kudera, S., Parak, W. J. & Lisdat, F. Quantum dots on gold: electrodes for photoswitchable cytochrome c electrochemistry. Small 2, 741–743 (2006).10.1002/smll.200500441 ↗
36. Zhu, A., Luo, Y. & Tian, Y. Switching the direction of plasmon-induced photocurrents by cytochrome c at Au-TiO2 nanocomposites. Chem. Commun. 6448–6450 (2009).10.1039/b911344d ↗
37. Zhu, Y., Cao, H., Tang, L., Yang, X. & Li, C. Immobilization of horseradish peroxidase in three-dimensional macroporous TiO2 matrices for biosensor applications. Electrochim. Acta 54, 2823–2827 (2009).10.1016/j.electacta.2008.11.025 ↗
38. Zhou, H., Gan, X., Wang, J., Zhu, X. & Li, G. Hemoglobin-based hydrogen peroxide biosensor tuned by the photovoltaic effect of nano titanium dioxide. Anal. Chem. 77, 6102–6104 (2005).10.1021/ac050924a ↗
39. Zhu, X., Yuri, I., Gan, X., Suzuki, I. & Li, G. Electrochemical study of the effect of nano-zinc oxide on microperoxidase and its application to more sensitive hydrogen peroxide biosensor preparation. Biosens. Bioelectron. 22, 1600–1604 (2007).10.1016/j.bios.2006.07.007 ↗
40. Ren, X., Chen, D., Meng, X., Tang, F., Hou, X., Han, D. & Zhang, L. Zinc oxide nanoparticles/glucose oxidase photoelectrochemical system for the fabrication of biosensor. J. Colloid Interf. Sci. 334, 183–187 (2009).10.1016/j.jcis.2009.02.043 ↗
41. Tang, J., Wang, Y., Li, J., Da, P., Geng, J. & Zheng, G. Sensitive enzymatic glucose detection by TiO2 nanowire photoelectrochemical biosensors. J. Mater. Chem. A 2, 6153–6157 (2014).10.1039/C3TA14173J ↗
42. Kong, B., Tang, J., Zhang, Y., Selomulya, C., Gong, X., Liu, Y., Zhang, W., Yang, J., Wang, W., Sun, X., Wang, Y., Zheng, G. & Zhao, D. Branched artificial nanofinger arrays by mesoporous interfacial atomic rearrangement. J. Am. Chem. Soc. 137, 4260–4266 (2015).10.1021/jacs.5b01747 ↗
43. Hu, B., Shi, W., Wu, Y. L., Leow, W. R., Cai, P., Li, S. & Chen, X. Orthogonally engineering matrix topography and rigidity to regulate multicellular morphology. Adv. Mater. 26, 5786–5793 (2014).10.1002/adma.201402489 ↗
44. Li, Y. Q., Zhu, B., Li, Y., Leow, W. R., Goh, R., Ma, B., Fong, E., Tang, M. & Chen, X. A synergistic capture strategy for enhanced detection and elimination of bacteria. Angew. Chem. Int. Ed. 53, 5837–5841 (2014).10.1002/anie.201310135 ↗
45. Kong, B., Tang, J., Wu, Z., Wei, J., Wu, H., Wang, Y., Zheng, G. & Zhao, D. Ultralight mesoporous magnetic frameworks by interfacial assembly of Prussian blue nanocubes. Angew. Chem. Int. Ed. 53, 2888–2892 (2014).10.1002/anie.201308625 ↗
46. Kong, B., Tang, J., Selomulya, C., Li, W., Wei, J., Fang, Y., Wang, Y., Zheng, G. & Zhao, D. Oriented mesoporous nanopyramids as versatile plasmon enhanced interfaces. J. Am. Chem. Soc. 136, 6822–6825 (2014).10.1021/ja501517h ↗
47. Lu, A.-H., Nitz, J. J., Comotti, M., Weidenthaler, C., Schlichte, K., Lehmann, C. W., Terasaki, O. & Schüth, F. Spatially and size selective synthesis of Fe-based nanoparticles on ordered mesoporous supports as highly active and stable catalysts for ammonia decomposition. J. Am. Chem. Soc. 132, 14152–14162 (2010).10.1021/ja105308e ↗
48. Linic, S., Christopher, P. & Ingram, D. B. Plasmonic-metal nanostructures for efficient conversion of solar to chemical energy. Nat. Mater. 10, 911–921 (2011).10.1038/nmat3151 ↗
49. Zou, C., Larisika, M., Nagy, G., Srajer, J., Oostenbrink, C., Chen, X., Knoll, W., Liedberg, B. & Nowak, C. Two-dimensional heterospectral correlation analysis of the redox-induced conformational transition in cytochrome c using surface-enhanced raman and infrared absorption spectroscopies on a two-layer gold surface. J. Phys. Chem. B 117, 9606–9614 (2013).10.1021/jp404573q ↗
50. Page, C. C., Moser, C. C., Chen, X. & Dutton, P. L. Natural engineering principles of electron tunnelling in biological oxidation–reduction. Nature 402, 47–52 (1999).10.1038/46972 ↗
51. Shimizu, S., Narita, M. & Tsujimoto, Y. Bcl-2 family proteins regulate the release of apoptogenic cytochrome c by the mitochondrial channel VDAC. Nature 399, 483–487 (1999).10.1038/20959 ↗
52. Wang, Y., Tang, J., Peng, Z., Wang, Y., Jia, D., Kong, B., Elzatahry, A. A., Zhao, D. & Zheng, G. Fully solar-powered photoelectrochemical conversion for simultaneous energy storage and chemical sensing. Nano Lett. 14, 3668–3673 (2014).10.1021/nl5014579 ↗
53. Kong, B., Tang, J., Wu, Z., Selomulya, C., Wang, H., Wei, J., Wang, Y., Zheng, G. & Zhao, D. Y. Bio-inspired porous antenna-like nanocube/nanowire heterostructure as ultra-sensitive cellular interfaces. NPG Asia Mater. 6, e117. doi:10.1038/am.2014.56 (2014).10.1038/am.2014.56 ↗
54. Gao, H., Liu, C., Jeong, H. E. & Yang, P. Plasmon-enhanced photocatalytic activity of iron oxide on gold nanopillars. ACS Nano 6, 234–240 (2011).10.1021/nn203457a ↗
55. Sikdar, D., Rukhlenko, I. D., Cheng, W. & Premaratne, M. Tunable broadband optical responses of substrate-supported metal/dielectric/metal nanospheres. Plasmonics 9, 659–672 (2014).10.1007/s11468-014-9681-8 ↗