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A simple approach to the mass production of nanoporous gold electrode arrays on cellulose membranes for electrochemical sensing of oxygen using ionic liquid (IL) electrolytes was established. The approach, combining the inkjet printing of gold nanoparticle (GNP) patterns with the self-catalytic growth of these patterns into conducting layers, can fabricate hundreds of self-designed gold arrays on cellulose membranes within several hours using an inexpensive inkjet printer. The resulting paper-based gold electrode arrays (PGEAs) had several unique properties as thin-film sensor platforms, including good conductivity, excellent flexibility, high integration, and low cost. The porous nature of PGEAs also allowed the addition of electrolytes from the back cellulose membrane side and controllably produced large three-phase electrolyte/electrode/gas interfaces at the front electrode side. A novel paper-based solid-state electrochemical oxygen (O(2)) sensor was therefore developed using an IL electrolyte, 1-butyl-3-methylimidazolium hexafluorophosphate (BMIMPF(6)). The sensor looked like a piece of paper but possessed high sensitivity for O(2) in a linear range from 0.054 to 0.177 v/v %, along with a low detection limit of 0.0075% and a short response time of less than 10 s, foreseeing its promising applications in developing cost-effective and environment-friendly paper-based electrochemical gas sensors.

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Ultrasensitive multiplexed detection of biomarkers on a single electrode is usually a great challenge for electrochemical sensors. Here, a light addressable photoelectrochemical sensor (LAPECS) for the sensitive detection of multiple DNA biomarkers on a single electrode was reported. The sensor was constructed through four steps: (1) immobilization of capture DNA (C-DNA) of different targets on different areas of a single large-sized gold film electrode, (2) recognition of each target DNA (T-DNA) and the corresponding biotin-labeled probe DNA (P-DNA) through hybridization, (3) reaction of the biotin-labeled probe DNA with a streptavidin-labeled all-carbon PEC bioprobe, and (4) PEC detection of multiple DNA targets one by one via a light addressing strategy. Through this principle, the LAPECS can achieve ultrasensitive detection of three DNA sequences related to hepatitis B (HBV), hepatitis C (HCV) and human immunodeficiency (HIV) viruses with a similar wide calibration range of 1.0 pM ∼ 0.01 μM and a low detection limit of 0.7 pM by using one kind of PEC bioprobe. Moreover, the detection throughput of LAPECS may be conveniently expanded by simply enlarging the size of the substrate electrode or reducing the size of the sensing arrays and the light beam. The present work thus demonstrates the promising applications of LAPECS in developing portable, sensitive, high-throughput, and cost-effective biosensing systems.

Carbon nanotubes (CNTs) have received considerable attention in the field of electrochemical sensing, due to their unique structural, electronic and chemical properties, for instance, unique tubular nanostructure, large specific surface, excellent conductivity, modifiable sidewall, high conductivity, good biocompatibility, and so on. Here, we tried to give a comprehensive review on some important aspects of the applications of CNT-based electrochemical sensors in biomedical systems, including the electrochemical nature of CNTs, the methods for dispersing CNTs in solution, the approaches to the immobilization of functional CNT sensing films on electrodes, and the extensive biomedical applications of the CNT-based electrochemical sensors. In the last section, we mainly focused on the applications of CNT-based electrochemical sensors in the analysis of various biological substances and drugs, the methods for constructing enzyme-based electrochemical biosensors and the direct electron transfer of redox proteins on CNTs. Because several crucial factors (e.g., the surface properties of carbon nanotubes, the methods for constructing carbon nanotube electrodes and the manners for electrochemical sensing applications) predominated the analytical performances of carbon nanotube electrodes, a systematical comprehension of the related knowledge was essential to the acquaintance, mastery and development of carbon nanotube-based electrochemical sensors.

A novel enzyme-free and all-carbon photoelectrochemical (PEC) bioprobe, based on carboxylated multiwalled carbon nanotube-Congo red-fullerene nanohybrids (MWNTCOOH-CR-C60), for the ultrasensitive immunosensing of carcinoembryonic antigen (CEA) was reported. The MWNTCOOH-CR-C60 nanohybrids, prepared by mechanically grinding a mixture of MWNTCOOH, C60, and CR at a certain mass ratio, had good water dispersibility and high PEC conversion efficiency in visible light ranges. Covalent binding of the detection antibody of CEA on the MWNTCOOH-CR-C60 nanohybrids produced a sensitive PEC bioprobe for detection of CEA by sandwich immunosensing. The corresponding immunosensor, employing an inexpensive and portable green laser light, possessed a wide calibration range of 1.0 pg/mL~100.0 ng/mL and a low detection limit of 0.1 pg/mL (calculated 5 zmol for a 10.0 μL sample solution) (S/N = 3), which was successfully applied to the detection of CEA in serum samples from both healthy people and cancer patients. The present work thus demonstrated the promising application of fullerene-based nanocomposites in developing highly sensitive, environmentally friendly, and cost-effective PEC biosensors.

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