All in one transitional flow-based integrated self-powered catechol sensor using BiFeO3 nanoparticles

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Highlights

  • Proposed a novel transitional flow-based self-powered catechol sensor (TFPNG-SPCS).

  • Hollow tubular-shaped BiFeO3 piezoelectric nanogenerator delivers ≈2.624 mW/m2.

  • The TFPNG-SPCS sensor has good selectivity and detection limits down to 10.2 μM.

  • The TFPNG-SPCS can work as a micro-power source as well as an active biosensor.

Abstract

A highly reliable transitional flow-based integrated self-powered catechol sensor (SPCS) proposed for the detection of organic contaminants in water samples. Here the cost-effective hollow tube-shaped piezoelectric nanogenerator (TFPNG-SPCS) by the BiFeO3 nanoparticles works as an SPCS. The obtained ferroelectric remnant polarization and coercive voltages are 0.089 μC/cm2 and 223 V at 1 Hz frequency. The TFPNG device delivers an instantaneous peak-to-peak power density of 2.624 mW/m2 at 500 MΩ. The classification between physical and chemical stimuli is possible through in-tunnel transitional flow and converts them into a readable electrical signal. The proposed TFPNG-SPCS sensor has good selectivity, reasonable sensitivity, eco-friendly, and detection limits down to 10.2 μM, having a linear relationship with catechol concentrations.

Introduction

Electrochemical sensors (ECS), play a vital role in investigation of the oxidizable chemical compounds in environment/industry sectors. The major parts in ECS are the sensing element, transducer, power supply, data processing unit, and establishment of the closed-circuit during the measurement. Over the few years, the utility of conventional ECS drastically spread into various fields such as pharmaceuticals, medicine, chemical plants, materials design, biotechnology, environmental monitoring, and military applications. However, the advanced ECS mainly depends on the development of miniaturized sensors with multi-functionality, low power consumption, automation, flexible materials, robustness, cost-effective and clean fabrication procedures [1]. Recently, the energy harvesting technologies such as enzymatic fuel cell (EFC), microbial fuel cells (MFC), thermoelectric generators (TEG), piezoelectric/pyroelectric (PENG/PyNG) and triboelectric nanogenerators (TENG) were well developed [2,3]. All these approaches exhibited the possibility of multi-functionality and self-powered (no external power supply) concepts with the reduction of device size, cost-effectiveness, and stability. The device fabrication trend needs to change with better functionality and effectiveness for overcoming these issues.

As we know, multiferroic materials has more than one ferroic properties among ferroelectricity, ferromagnetism, and ferroelasticity and it’s been a fascinating subject of research in fields related to sensors, memory and energy [4]. Among the perovskite-based multiferroics, bismuth ferrite (BiFeO3) is one of the superior material because of its large polarization with good chemical stability [5,6]. The usage of BiFeO3 in many fields explored recently, but the sensing application for orgonic molecules was not tested widely. Moreover, the BiFeO3 has excellent properties such as biocompatibility, low-dielectric constant, reasonable piezoelectric/ferroelectric properties make it a potential material to apply in the piezoelectric system [7,8].

The catechol is a significant isomer of phenolic compounds used in medicines, flavouring agents, insecticides, cosmetics, and photography dyes [9,10]. But it perceived as significant environmental pollutants because of their low degradability and high toxicity in the ecological environment [11]. Catechol is promptly absorbed from the gastrointestinal tract, causing liver failure, cancers, neurodegenerative diseases, and renal tube deterioration, besides accumulating in the bone marrow. The quantification of catechol along these areas improved lot, and different strategies have been executed to detect and estimate catechol, for example, gas chromatography, mass spectrometry, voltammetry, and high-performance liquid chromatography and fluorescence methods [12]. But these methods require large space, high manufacturing and installation cost, complex working procedures, extensive sample preparation, not available for on field detection due to the need of high-pressure carrier gas. Therefore, the quantification of catechol by alternative chemical sensor methods with better functional material, zero-power supply is highly necessary.

To overcome the mentioned issues, we applied multiferroic BiFeO3 in the transitional flow-based piezoelectric nanogenerator (TFPNG), it also acts as an integrated biosensing unit demonstrated to analyze the oxidizable compounds, i.e., catechol. The device design contains a hollow tube, which is flexible, along with the specific interactive holes in particular positions these hollow structure and interactive sites combine to promote the capability of multi-functionality (piezoelectricity + chemical sensing). The device is miniaturized, flexible, and have continuous monitoring capability without external power supply and changes in the sensing element. An alternative approach by implementing a cost-effective direct current (I)-voltage(V) technique for the quantitative analysis of organic molecules.

Here, the distinguish of physical and chemical stimuli is possible through in-tunnel transitional flow and converts them into a readable electrical signal. TFPNG excludes the necessity of external sensing and power supply unit for a potential characteristic application. The transitional flow of catechol solution in TFPNG induces the piezoelectric effect (through the stress-induced process), and the interaction of catechol, BiFeO3 through the interactive holes provides the catechol sensing (through chemisorption interaction). This work promotes a novel working mechanism in the detection of biomolecules with a vast range of analytes that can be resolved based on different responses and incredibly propels the applicability of self-powered devices.

Section snippets

Synthesis of bismuth ferrite

Single-phase crystalline BiFeO3 nanoparticles synthesized by a solvent evaporation method, which effectively suppressed the formation of multiple secondary phases (Bi2O3, Bi2Fe4O9) and improved the overall quality of the formed microstructures. The stoichiometric ratio of metal nitrates used with tartaric acid as a precipitating agent. 0.1 M Fe(NO3)3.9H2O (iron nitrate nonahydrate) and 0.01 M Bi(NO3)3.5H2O(Bismuth nitrate pentahydrate) were dissolved in 2 N HNO3 (65 % nitric acid), which acts

Physiochemical analysis of BiFeO3 nanoparticles and catechol sensor response

The schematic of the proposed catechol sensor and the device layers depicted in Fig. 1a. The inset shows the optical image of the catechol sensor fabricated by the spin-coated perovskite BiFeO3 nanoparticles. Before going to the sensor studies, the crystalline phase, active phonon modes, morphology of BiFeO3 were systematically evaluated, and the corresponding results depicted in Fig. (1 b, c, and S2). The XRD pattern confirms the existence of a single-phase along with the rhombohedral crystal

Conclusion

In summary, a transitional flow-based self-powered, the self-signaled bio-sensing device was systematically reported, which is an entirely novel and disruptive approach by merging piezoelectric nanogenerator and bio-chemical sensing with sensitivity to lower concentrations. The TFPNG device configuration was able to distinguish the physical stimuli response and bio-chemical sensor response successfully by modulating the device layers. The dual functionality role of the present device was a

Supplementary files

Fig. S1- Synthesis of BiFeO3 by solvent evaporation technique. Fig. S2 presents the EDS mapping, spectra of as formed pure phase BiFeO3. Fig. S3 shows the frequency dependent dielectric loss and dielectric constant of the BiFeO3 pellets sintered at 550 °C. Fig. S4 represents the surface morphology of the PDMS mold (a) before and (b) after Plasma etching. Fig. S5-S9 shows the electrical response of TFPNG and TFPNG-SPCS devices output upon various conditions. Table 1. Comparison of analytical

CRediT authorship contribution statement

Abisegapriyan K S: Investigation, Methodology, Writing - original draft. Nirmal Prashanth Maria Joseph Raj: Validation, Formal analysis, Data curation. Nagamalleswara Rao Alluri: Writing - review & editing. Arunkumar Chandrasekhar: Validation, Visualization. Sang-Jae Kim: Supervision, Funding acquisition.

Declaration of Competing Interests

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgment

The Basic Science Research Program supported this work through the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (2018R1A4A1025998, 2019R1A2C3009747).

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