Co-reporter:Jiying Liang;Xue Yu;Tiangang Yang;Menglu Li;Li Shen;Yue Jin
Physical Chemistry Chemical Physics 2017 vol. 19(Issue 33) pp:22472-22481
Publication Date(Web):2017/08/23
DOI:10.1039/C7CP04030J
In this paper, poly(N-isopropylacrylamide-co-3-aminophenylboronic acid) (P(NIPAM-co-APBA)) copolymer films were successfully electropolymerized on the Au electrode surface. The electroactive probe ferrocene carboxylic acid (FCA) in solution showed reversible thermal-, glucose- and pH-responsive on–off cyclic voltammetric (CV) behaviors at the film electrodes. The comparative experiments demonstrated that the thermo-responsive property of the film electrode was ascribed to the PNIPAM component of the films, whereas the glucose- and pH-sensitive behaviors came from the PAPBA constituent. The reduced form of nicotinamide adenine dinucleotide (NADH) could be electrocatalytically oxidized by FCA at the film electrodes, which would greatly amplify the multi-responsive CV signal difference between the on and off states. On the basis of these results, a binary 4-input/4-output logic circuit was fabricated with temperature, glucose, pH and NADH as inputs and the CV responses at 4 different levels as outputs. Moreover, a ternary CONSENSUS logic circuit was established on the same platform, which was the first report on the combination of ternary logic gate and bioelectrocatalysis without using enzymes. This work provided a novel idea for constructing complicated biocomputing systems by increasing the number of inputs/outputs with multi-sensitive interfaces and by designing new types of multi-valued logic gates on the basis of bioelectrocatalysis.
Co-reporter:Lei Wang;Wenjing Lian
Chemistry - A European Journal 2016 Volume 22( Issue 14) pp:4825-4832
Publication Date(Web):
DOI:10.1002/chem.201504812
Abstract
A closed bipolar electrode (BPE) system was developed with electrochromic poly(3-methylthiophene) (PMT) films electropolymerized on the ITO/rGO electrode as one pole of BPE in the reporting reservoir and the bare ITO electrode as another pole of BPE in the analyte reservoir, in which rGO represents reduced graphene oxide. Under a suitable driving voltage (Vtot), the electrochemical reduction/oxidation of electroactive probes, such as H2O2/glutathione (Glu), in the analyte reservoir could induce the reversible color change of PMT films in the reporting reservoir between blue and red. Based on this, a keypad lock with H2O2, Glu, and Vtot=−3.0 V as the three inputs and the color change of PMT films as the visible output was established. This system was easily operated and did not need to synthesize the complex compounds or DNA molecules. The security system was easy to reset and could be used repeatedly.
Co-reporter:Lei Wang, Wenjing Lian, Huiqin Yao, and Hongyun Liu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 9) pp:5168
Publication Date(Web):February 16, 2015
DOI:10.1021/am5075002
In the present work, reduced graphene oxide (rGO)/poly(N-isopropylacrylamide) (PNIPAA) composite films were electrodeposited onto the surface of Au electrodes in a fast and one-step manner from an aqueous mixture of a graphene oxide (GO) dispersion and N-isopropylacrylamide (NIPAA) monomer solutions. Reflection–absorption infrared (IR) and Raman spectroscopies were employed to characterize the successful construction of the rGO/PNIPAA composite films. The rGO/PNIPAA composite films exhibited reversible potential-, pH-, temperature-, and sulfate-sensitive cyclic voltammetric (CV) on–off behavior to the electroactive probe ferrocenedicarboxylic acid (Fc(COOH)2). For instance, after the composite films were treated at −0.7 V for 7 min, the CV responses of Fc(COOH)2 at the rGO/PNIPAA electrodes were quite large at pH 8.0, exhibiting the on state. However, after the films were treated at 0 V for 30 min, the CV peak currents became much smaller, demonstrating the off state. The mechanism of the multiple-stimuli switchable behaviors for the system was investigated not only by electrochemical methods but also by scanning electron microscopy and X-ray photoelectron spectroscopy. The potential-responsive behavior for this system was mainly attributed to the transformation between rGO and GO in the films at different potentials. The film system was further used to realize multiple-stimuli responsive bioelectrocatalysis of glucose catalyzed by the enzyme of glucose oxidase and mediated by the electroactive probe of Fc(COOH)2 in solution. On the basis of this, a four-input enabled OR (EnOR) logic gate network was established.Keywords: bioelectrocatalysis; logic gates; multiple-stimuli responsive; poly(N-isopropylacrylamide); reduced graphene oxide
Co-reporter:Shuang Liu, Menglu Li, Xue Yu, Chen-Zhong Li and Hongyun Liu
Chemical Communications 2015 vol. 51(Issue 67) pp:13185-13188
Publication Date(Web):07 Jul 2015
DOI:10.1039/C5CC04412J
Based on the damage of natural DNA, a 3-input/4-output logic gate system and other biomacromolecular devices, such as a 2-to-1 encoder, a 1-to-2 decoder and a keypad lock, were developed using simultaneously obtained electrochemiluminescence (ECL) and cyclic voltammetry (CV) signals as outputs in the presence of Ru(bpy)32+.
Co-reporter:Shuang Liu;Lei Wang;Wenjing Lian;Dr. Hongyun Liu; Chen-Zhong Li
Chemistry – An Asian Journal 2015 Volume 10( Issue 1) pp:225-230
Publication Date(Web):
DOI:10.1002/asia.201402927
Abstract
A logic-gate system with three outputs and three inputs was developed based on the bioelectrocatalysis of glucose by glucose oxidase (GOx) entrapped in chitosan films on the electrode surface by means of ferrocenedicarboxylic acid (Fc(COOH)2). Cyclic voltammetric (CV) signals of Fc(COOH)2 exhibited pH-triggered on/off behavior owing to electrostatic interactions between the film and the probe at different pH levels. The addition of glucose greatly increased the oxidation peak current (Ipa) through the electrocatalytic reaction. pH and glucose were selected as two inputs. As a reversible inhibitor of GOx, Cu2+ was chosen as the third input. The combination of three inputs led to Ipa with different values according to different mechanisms, which were defined as three outputs with two thresholds. The logic gate with three outputs by using one type of enzyme provided a novel model to build logic circuits based on biomacromolecules, which might be applied to the intelligent medical diagnostics as smart biosensors in the future.
Co-reporter:Wenjing Lian
The Journal of Physical Chemistry C 2015 Volume 119(Issue 34) pp:20003-20010
Publication Date(Web):August 10, 2015
DOI:10.1021/acs.jpcc.5b06456
A series of biomacromolecular logic gates and functional devices with cyclic voltammetric (CV) and electrochemiluminescence (ECL) responses as output signals were established on the basis of molecularly imprinted polymer (MIP) film electrodes. The MIP films were electropolymerized on the surface of Au electrodes with o-phenylenediamine (OPD) as the monomer and chloramphenicol (CP) as the template molecule. The simultaneous CV and ECL signals of Ru(bpy)32+ were significantly enhanced by the addition of natural DNA in solution at the MIP film electrodes after CP removal. The CV and ECL responses of the Ru(bpy)32+–DNA system at the MIP film electrodes were greatly influenced by CP removal and rebinding. Moreover, the addition of ferrocene methanol (FcMeOH) to the solution led to substantial quenching of the ECL signal and produced a new CV peak pair. On the basis of these results, 3-input/3-output and 3-input/5-output biomacromolecular logic gate systems were established with DNA, CP, and FcMeOH as inputs and the ECL responses at different levels or CV responses at different potentials as outputs. After an elaborate reconfiguration of inputs and outputs, the functional non-Boolean logic devices such as a 2-to-1 encoder, a 1-to-2 decoder, and a 1-to-2 demultiplexer were also constructed on the same platform.
Co-reporter:Peng Wang, Shuang Liu, and Hongyun Liu
The Journal of Physical Chemistry B 2014 Volume 118(Issue 24) pp:6653-6661
Publication Date(Web):May 29, 2014
DOI:10.1021/jp501624y
In the present work, N,N-diethylacrylamide (DEA) and methyl acrylic acid (MAA) monomers were copolymerized into P(DEA-co-MAA) thin films on the electrode surface with a simple one-step polymerization method at ambient temperature and pressure, and the enzyme glucose oxidase (GOD) was entrapped in the films, designed as P(DEA-co-MAA)-GOD. The cyclic voltammetric (CV) response of ferrocene dicarboxylic acid (Fc(COOH)2) at the film electrodes was very sensitive to environmental stimuli, such as temperature, pH, the identity and concentration of anions, and the concentration of CO2 in solution. This multiresponsive CV behavior of the system could be further employed to switch the electrochemical oxidation of glucose catalyzed by GOD entrapped in the films with Fc(COOH)2 as the mediator in solution, demonstrating the amplification effect. The SEM and stereomicroscopy results showed that the multisensitive behaviors of the system were attributed to the structure change of the copolymer films with the stimuli. Specifically, the synergistic effect of temperature and pH was observed, and the hydrogen bonding between PDEA and PMAA components in the copolymer played a key role for this. The present system could be performed under physiological conditions at 37 °C and pH 7.4, which may offer numerous possibilities not only to design new multiswitchable biosensors based on bioelectrocatalysis but also to establish foundations for controlled drug delivery and other medical applications.
Co-reporter:Huiqin Yao;Ling Lin;Peng Wang
Applied Biochemistry and Biotechnology 2014 Volume 173( Issue 8) pp:2005-2018
Publication Date(Web):2014 August
DOI:10.1007/s12010-014-0987-y
Dual-responsive poly(N,N-diethylacrylamide) (PDEA) hydrogel films with entrapped horseradish peroxidase (HRP) and glucose oxidase (GOD) were successfully prepared on electrode surface with a simple one-step polymerization procedure under mild conditions, designated as PDEA-HRP-GOD. Cyclic voltammetric (CV) response of electroactive probe K3Fe(CN)6 at the film electrodes displayed reversible thermo- and sulfate-responsive switching behavior. For example, at 25 °C, the K3Fe(CN)6 demonstrated a well-defined CV peak pair with large peak currents for the films, showing the on state, while at 40 °C, the CV response was greatly suppressed and the system was at the off state. The influence of temperature and Na2SO4 concentration on the switching behavior of the film system was not independent or separated, but was synergetic. The responsive mechanism of the system was ascribed to the structure change of PDEA component in the films with temperature and sulfate concentration. This switching property of the PDEA-HRP-GOD films could be further used to realize dual-responsive catalytic oxidation of glucose sequentially by HRP and GOD entrapped in the films with Fe(CN)63− as the mediator through changing the surrounding temperature and Na2SO4 concentration. This system may establish a foundation for fabricating a new type of multi-switchable electrochemical biosensors based on bienzyme electrocatalysis.
Co-reporter:Kaina Zhang, Yan Liang, Dan Liu, Hongyun Liu
Sensors and Actuators B: Chemical 2012 173() pp: 367-376
Publication Date(Web):
DOI:10.1016/j.snb.2012.07.016
Co-reporter:Yi Xie, Naifei Hu, Hongyun Liu
Journal of Electroanalytical Chemistry 2009 630(1–2) pp: 63-68
Publication Date(Web):
DOI:10.1016/j.jelechem.2009.02.017
Co-reporter:Shuang Liu, Menglu Li, Xue Yu, Chen-Zhong Li and Hongyun Liu
Chemical Communications 2015 - vol. 51(Issue 67) pp:NaN13188-13188
Publication Date(Web):2015/07/07
DOI:10.1039/C5CC04412J
Based on the damage of natural DNA, a 3-input/4-output logic gate system and other biomacromolecular devices, such as a 2-to-1 encoder, a 1-to-2 decoder and a keypad lock, were developed using simultaneously obtained electrochemiluminescence (ECL) and cyclic voltammetry (CV) signals as outputs in the presence of Ru(bpy)32+.
