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Controlled Insertion of Silver Nanoparticles in LbL Nanostructures: Fine-Tuning the Sensing Units of an Impedimetric E-Tongue

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CHEMOSENSORS 2024年第6期12卷 87页

作者： Goncalves, Maria Helena Braunger, Maria Luisa de Barros, Anerise Hensel, Rafael C. Dalafini, Julianna G. Mazali, Italo O. Correa, Leonardo M. Ugarte, Daniel Riul Jr, Antonio Rodrigues, Varlei Univ Estadual Campinas Inst Fis Gleb Wataghin BR-13083859 Campinas Brazil Univ Estadual Campinas Inst Chem BR-13083970 Campinas Brazil Univ Sao Paulo Sao Carlos Inst Phys BR-13566590 Sao Carlos Brazil

Silver nanoparticles (AgNPs) possess unique characteristics ideal for enhancing device sensitivity, primarily due to their high surface-to-volume ratio facilitating heightened interaction with analytes. Integrating AgNPs into polymers or carbon-based materials results in nanocomposites with synergistic properties, enabling the detection of minute changes in the environment across various applications. In this study, we investigate the adsorption kinetics of AgNPs within multilayered layer-by-layer (LbL) structures, specifically examining the impact of AgNPs concentration in the LbL film formation that is further explored as sensing units in an impedimetric microfluidic e-tongue. Although absorption kinetic studies are infrequent, they are crucial to optimize the AgNPs adsorption and distribution within LbL structures, significantly influencing upcoming applications. Through systematic variation of AgNPs concentration within identical LbL architectures, we applied the films as sensing units in a microfluidic e-tongue capable of distinguishing food enhancers sharing the umami taste profile. Across all tested scenarios, our approach consistently achieves robust sample separation, evidenced by silhouette coefficient, principal component analyses, and long-term stability. This work contributes to exploring controlled nanomaterial-based developments, emphasizing the importance of precise parameter control for enhanced sensor performance across diverse analytical applications.

关键词： e-tongue metal nanoparticles layer-by-layer films impedance measurements microfluidics multisensor array

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Hole-matrixed carbonylated graphene: Synthesis, properties, and highly-selective ammonia gas sensing

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CARBON 2021年 172卷 236-247页

作者： Rabchinskii, M. K. Varezhnikov, A. S. Sysoev, V. V. Solomatin, M. A. Ryzhkov, Sergei A. Baidakova, M. V. Stolyarova, D. Yu Shnitov, V. V. Pavlov, Sergei S. Kirilenko, D. A. Shvidchenko, A. V. Lobanova, E. Yu Gudkov, M. V. Smirnov, D. A. Kislenko, V. A. Pavlov, S. V. Kislenko, S. A. Struchkov, N. S. Bobrinetskiy, I. I. Emelianov, A. V. Liang, P. Liu, Z. Brunkov, P. N. Ioffe Inst 26 Politekh Skaya St St Petersburg 194021 Russia Yuri Gagarin State Tech Univ Saratov 77 Polytech Skaya St Saratov 410054 Russia ITMO Univ 49 Kronverksky Pr St Petersburg 197101 Russia NRC Kurchatov Inst 1 1 Akad Kurchatova Pl Moscow 123182 Russia Russian Acad Sci NN Semenov Fed Res Ctr Chem Phys 4 Kosygina St Moscow 119991 Russia Tech Univ Dresden Inst Festkorper & Mat Phys D-01062 Dresden Germany RAS Joint Inst High Temp 13-2 Izhorskaya St Moscow 125412 Russia Skolkovo Inst Sci & Technol Skolkovo Innovat Ctr 3 Nobel St Moscow 143026 Russia Moscow Inst Phys & Technol 9 Inst Per Dolgoprudnyi 141701 Russia Natl Res Univ Elect Technol Bld 1Shokin Sq Moscow 124498 Russia Res & Dev Inst Informat Technol Biosyst BioSense Inst Zorana Dind 1 Novi Sad 21000 Serbia China Jiliang Univ 258 Xueyuan St Hangzhou 310018 Zhejiang Peoples R China

Here, the synthesis of holey carbonylated (C-ny) graphene derivative and its application for gas sensing is demonstrated. The carbonylation of graphene oxide leads to the 3-fold increase in the concentration of carbonyl groups' up to 9 at.% with a substantial elimination of other oxygen functionalities. Such a chemical modification is accompanied by the perforation of the graphene layer with the appearance of matrices of nanoscale holes, leading to corrugation of the layer and its sectioning into localized domains of the is-conjugated network. Combined with the predominant presence of carbonyls, granting the specificity in gas molecules adsorption, these features result in the enhanced gas sensing properties of Cny graphene at room temperature with a selective response to NH3. Opposite chemiresistive response towards ammonia when compared to other analytes, such as ethanol, acetone, CO2, is demonstrated for the C-ny graphene layer both in humid and dry air background. Moreover, a selective discrimination of all of the studied analytes is further approached by employing a vector signal generated by C-ny multi electrode chip. Comparing the experimental results with the calculations performed in framework of density functional theory, we clarify the effect of partial charge transfer caused by water and ammonia adsorption on the chemiresistive response. (C) 2020 Elsevier Ltd. All rights reserved.

关键词： Graphene Graphene chemical derivatives Gas sensors Ammonia VOCs multisensor array

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Towards electronic smelling of ketones and alcohols at sub- and low ppms by pinky-sized on-chip sensor array with SnO2 mesoporous layer gradually engineered by near IR-laser

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CHEMICAL ENGINEERING JOURNAL 2023年 474卷

作者： Solomatin, Maksim A. Radovic, Marko Petrunin, Alexander A. Kirilenko, Demid A. Varezhnikov, Alexey S. Dubourg, Georges Vasilkov, Mikhail Yu. Bainyashev, Alexey M. Nesterovic, Andrea Kiselev, Ilia Kostin, Konstantin B. Martynyuk, Yuri P. V. Gorokhovsky, Alexander Volchkov, Sergey S. Zimnyakov, Dmitry A. Ushakov, Nikolay M. Goffman, Vladimir G. Rabchinskii, Maxim K. Glukhova, Olga E. Sysoev, Victor V. Yuri Gagarin State Tech Univ Saratov Ul Polytech Skaya 77 Saratov 410054 Russia RAS Saratov Branch Kotelnikov Inst Radioengn & Elect Saratov 410019 Russia Univ Novi Sad Biosense Inst Ctr Sensor Technol Novi Sad 21102 Serbia Saratov NG Chernyshevskii State Univ Astrakhanskaya Str 83 Saratov 410012 Russia Ioffe Inst 26 Politekhn Skaya St St Petersburg 194021 Russia Univ Novi Sad Fac Technol Novi Sad 21102 Serbia Breitmeier Messtechn GmbH Englerstr 27 D-76275 Ettlingen Germany A Baitursynov Kostanay Reg Univ Baitursynov Str 47 Kostanai 110000 Kazakhstan

We consider an on-chip sensor array based on a mesoporous layer of SnO2 nanoparticles to be screen printed on the multielectrode-supplied Si/SiO2 substrate as a chemiresistive building platform for portable and personalized in situ instruments. To differentiate the local oxide layer properties we apply Nd:YAG laser whose scanning etched various layer areas at varied power driven by working current in 24.8 A-26.7 A range. As a result, the SnO2 layer has dual-grad modified properties as, (i) a spatial modification of thickness down to nm-range, and (ii) the change of oxidation state with appearance of traces of SnO, which both result in a great varying of gas -sensing properties of local sensor elements over the array. To test the functionality of the chip, we could detect vapors of four ketones (acetone, cyclopentanone, cyclohexanone, 2-octanone) and four alcohols (methanol, ethanol, isopropanol, butanol), at sub-, down to ca. 100 ppb, and low, up to 10, ppm concentrations with their selective recognition via processing the array's vector signal by linear discriminant algorithm. Primarily, we show differences in the interaction of ketones and alcohols with SnO2 surface by first-principle calculations in frames of density functional theory to serve as fundamental receptor pre-requisites for the analyte's selective discrimination by the oxide layer under the multisensor concept to employ here. We consistently show that two modes of the sensor operation could be rather equally applied to the array as, (i) UV LED, 366 nm wavelength, irradiation at room temperature, and (ii) heating up to approx. 583 K. While the heating provides faster and higher chemiresistive responses, the UV-excited mode provides more selective vector signals, lower energy consumption, and a higher signal-to-noise ratio.

关键词： Metal oxide Gas sensor DFT Electronic nose VOC multisensor array

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Electrochemical multisensor systems and arrays in the era of artificial intelligence

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CURRENT OPINION IN ELECTROCHEMISTRY 2023年 42卷

作者： Voitechovic, Edita Pauliukaite, Rasa Ctr Phys Sci & Technol FTMC Savanoriu Ave 231 LT-02300 Vilnius Lithuania

Current trends in analytical research seem almost impossible without the implementation of artificial intelligence. This short review is a summary of recent research and opinions of leading scientists regarding the transformation of common electrochemical multisensor systems and arrays in the imme-diate future. The review includes the aspects of the develop-ment of artificial intelligence-assisted (bio)electrochemical multisensor systems and arrays, the main bottlenecks, and successful smart analytical platforms. The promising applica-tions of so-called smart multisensor systems and arrays are shown in medicine, physical activity tracking, veterinary, pharmaceutical industry, forensic science, food industry, agri-culture, and ecology.

关键词： Artificial intelligence Machine learning multisensor array Systems Electrochemical Agriculture Wearable Medicine

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The Ti0.2V1.8C MXene Ink-Prepared Chemiresistor: From Theory to Tests with Humidity versus VOCs

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CHEMOSENSORS 2023年第1期11卷 7页

作者： Simonenko, Nikolay P. Glukhova, Olga E. Plugin, Ilya A. Kolosov, Dmitry A. Nagornov, Ilya A. Simonenko, Tatiana L. Varezhnikov, Alexey S. Simonenko, Elizaveta P. Sysoev, Victor V. Kuznetsov, Nikolay T. Russian Acad Sci Kurnakov Inst Gen & Inorgan Chem 31 Leninsky pr Moscow 119991 Russia Saratov NG Chernyshevskii State Univ Inst Phys Saratov 410012 Russia Yuri Gagarin State Tech Univ Saratov Dept Phys 77 Polytech Skaya str Saratov 410054 Russia

The 2D structure of MXenes attracts wide research attention toward an application of these materials in gas sensors. These structures are extremely sensitive to minor variations in their composition, which are employed for tuning their functional properties. Here, we consider the partially substituted MXenes of the composition of TixV2-xC, where x = 0.2, via quantum chemical calculations, and test their chemiresistive characteristics as a receptor component of the planar-type sensor and on-chip multisensor array. We thoroughly discuss the synthesis process of Ti0.2V1.8AlC MAX-phase and the corresponding MXenes, to prepare functional inks and, furthermore, deposit the films by microextrusion printing over an array of planar multi-electrode structures at the surface of a pen-sized chip. The crystal structure of the obtained materials is evaluated via X-ray diffraction analysis. The developed chip has been exposed upon few gaseous analytes, of alcohol VOCs, NH3, and H2O, of a 500-16,000 ppm concentration, at room temperature to ensure that we could observe the positive chemiresistive effect matured from resistance enhancing, with up to 10% vs. water vapors. The calculations carried in the framework of the density-functional theory for V2C, Ti2C, and Ti0.2V1.8C crystals ensured that the variations in their electronic structure were almost consistent with the experiment fundings: the most prominent effect is observed in relation to the H2O vapors. Therefore, these Ti0.2V1.8C structures could be considered for applying them in room temperature-operated hygrometers.

关键词： MXene Ti2C V2C Ti0 2V1 8C gas sensor multisensor array microextrusion printing humidity ethanol DFT

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Energy-Efficient Chemiresistive Sensor array Based on SWCNT Networks, WO3 Nanochannels and SWCNT-Pt Heterojunctions for NH3 Detection against the Background Humidity

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CHEMOSENSORS 2022年第11期10卷 476页

作者： Romashkin, Alexey V. V. Lashkov, Andrey V. V. Sysoev, Victor V. V. Struchkov, Nikolay S. S. Alexandrov, Evgeny V. V. Levin, Denis D. D. Natl Res Univ Elect Technol Ctr Probe Microscopy & Nanotechnol Moscow 124498 Russia Yuri Gagarin State Tech Univ Saratov Dept Phys Saratov 410054 Russia

Recently, promising results have been achieved in improving the sensitivity to ammonia in gas sensors through the use of structures composed of heterojunctions or nanochannels. However, their sensitivity is highly dependent on the background humidity under air conditions. The sensor structures which could ensure selective ammonia detection with a low detection limit, despite interference from changing background humidity, remain highly demanded. In this work, we consider sensing units containing (i) nanochannels formed by a continuous tungsten oxide nanolayer to appear in contact between single-walled carbon nanotubes (SWCNTs) and a Pt sublayer and (ii) SWCNT-Pt junctions in frames of mass-scale microelectronic technologies. SWCNTs were deposited by spray-coating on a thin WO3/Pt/W sublayer formed by a photolithographic pattern to be accompanied by satellite samples with just SWCNTs for reference purposes. We elucidate the specific differences that appeared in the response of sensors based on SWCNT-Pt junctions and WO3 nanochannels relative to satellite SWCNT samples with a similar SWCNT network density. Particularly, while a similar response to NH3 vapors mixed with dry air is observed for each sensor type, the response to NH3 is reduced significantly in the presence of background humidity, of 45 rel.%, especially in the case of WO3 nanochannel structures even at room temperature. A multisensor array based on the four various sensing structures involving SWCNT-Pt junctions, WO3 nanochannels, and their satellite-only-SWCNT ones allowed us to determine a correct ammonia concentration via utilizing the linear discriminant analysis despite the presence of background air humidity. Thus, such an energy-efficient multisensor system can be used for environmental monitoring of ammonia content, health monitoring, and other applications.

关键词： carbon nanotube nanochannel tungsten oxide heterojunction multisensor array ammonia gas sensor spray deposition

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Toward a Selective Analysis of Heavy Metal Salts in Aqueous Media with a Fluorescent Probe array

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SENSORS 2022年第4期22卷 1465-1465页

作者： Melnikov, Andrey G. Bykov, Denis A. Varezhnikov, Alexey S. Sysoev, Victor V. Melnikov, Gennady V. Yuri Gagarin State Tech Univ Saratov Dept Phys Saratov 410054 Russia

Detection of heavy meals in aqueous media challenges worldwide research in developing particularly fast and affordable methods. Fluorescent sensors look to be an appropriate instrument for such a task, as recently they have been found to have made large progress in the detection of chemical analytes, primarily in the environment, along with biological fluids, which still suffer from not enough selectivity. In this work, we propose a new fluorescent method to selectively recognize heavy metals in an aqueous solution via employing an array of several fluorescent probes: acridine yellow, eosin, and methylene blue, which were taken as examples, being sensitive to a microsurrounding of the probe molecules. The exemplary sensor array generated six channels of spectral information through the use of various combinations of excitation and detection wavelengths. Following the known multisensor approach, we applied a linear discriminant analysis to selectively distinguish the vector signals from the sensor array from salts of heavy metals-Cu, Pb, Zn, Cd, and Cz-at the concentration ranges of 2.41 x 10(-6)-1.07 x 10(-5) M, 2.8 x 10(-5)-5.87 x 10(-4) M, 1.46 x 10(-6)-6.46 x 10(-6) M, 1.17 x 10(-8)-5.2 x 10(-8) M, and 2.11 x 10(-6)-9.33 x 10(-6) M, respectively. The suggested approach was found to be promising due to it employing only one cuvette containing the test solution, simplifying a sample preparation when compared to preparing a variety of solutions in tests with single fluorescence probes.

关键词： fluorescence sensor heavy metal multisensor array selectivity

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UV-Light-Tunable p-/n-Type Chemiresistive Gas Sensors Based on Quasi-1D TiS3 Nanoribbons: Detection of Isopropanol at ppm Concentrations

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SENSORS 2022年第24期22卷 9815-9815页

作者： Sysoev, Victor V. V. Lashkov, Andrey V. V. Lipatov, Alexey Plugin, Ilya A. A. Bruns, Michael Fuchs, Dirk Varezhnikov, Alexey S. S. Adib, Mustahsin Sommer, Martin Sinitskii, Alexander Yuri Gagarin State Tech Univ Saratov Dept Phys Saratov 410054 Russia Natl Res Univ Elect Technol Ctr Probe Microscopy & Nanotechnol Moscow 124498 Russia South Dakota Sch Mines & Technol Dept Chem Biol & Hlth Sci 501 E St Joseph St Rapid City SD 57701 USA Karlsruhe Inst Technol KIT Inst Appl Mat & Karlsruhe Nano Micro Facil Hermann Von Helmholtz Pl 1 D-76344 Eggenstein Leopoldshafen Germany Karlsruhe Inst Technol KIT Inst Quantum Mat & Technol Hermann Von Helmholtz Pl 1 D-76344 Eggenstein Leopoldshafen Germany Karlsruhe Inst Technol KIT Inst Microstruct Technol D-76344 Eggenstein Leopoldshafen Germany Univ Nebraska Lincoln Dept Chem Lincoln NE 68588 USA

The growing demand of society for gas sensors for energy-efficient environmental sensing stimulates studies of new electronic materials. Here, we investigated quasi-one-dimensional titanium trisulfide (TiS3) crystals for possible applications in chemiresistors and on-chip multisensor arrays. TiS3 nanoribbons were placed as a mat over a multielectrode chip to form an array of chemiresistive gas sensors. These sensors were exposed to isopropanol as a model analyte, which was mixed with air at low concentrations of 1-100 ppm that are below the Occupational Safety and Health Administration (OSHA) permissible exposure limit. The tests were performed at room temperature (RT), as well as with heating up to 110 degrees C, and under an ultraviolet (UV) radiation at lambda = 345 nm. We found that the RT/UV conditions result in a n-type chemiresistive response to isopropanol, which seems to be governed by its redox reactions with chemisorbed oxygen species. In contrast, the RT conditions without a UV exposure produced a p-type response that is possibly caused by the enhancement of the electron transport scattering due to the analyte adsorption. By analyzing the vector signal from the entire on-chip multisensor array, we could distinguish isopropanol from benzene, both of which produced similar responses on individual sensors. We found that the heating up to 110 degrees C reduces both the sensitivity and selectivity of the sensor array.

关键词： gas sensor multisensor array alcohol room temperature UV radiation benzene titanium trisulfide

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Printing Technologies as an Emerging Approach in Gas Sensors: Survey of Literature

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SENSORS 2022年第9期22卷 3473-3473页

作者： Simonenko, Nikolay P. Fisenko, Nikita A. Fedorov, Fedor S. Simonenko, Tatiana L. Mokrushin, Artem S. Simonenko, Elizaveta P. Korotcenkov, Ghenadii Sysoev, Victor V. Sevastyanov, Vladimir G. Kuznetsov, Nikolay T. Russian Acad Sci Kurnakov Inst Gen & Inorgan Chem 31 Leninsky Pr Moscow 119991 Russia Russian Acad Sci D Mendeleev Univ Chem Technol Russia Higher Chem Coll 9 Miusskaya Sq Moscow 125047 Russia Skolkovo Inst Sci & Technol Lab Nanomat 3 Nobel Str Moscow 121205 Russia Moldova State Univ Dept Theoret Phys Kishinev 2009 Moldova Yuri Gagarin State Tech Univ Saratov Dept Phys 77 Polytech Skaya Str Saratov 410054 Russia

Herein, we review printing technologies which are commonly approbated at recent time in the course of fabricating gas sensors and multisensor arrays, mainly of chemiresistive type. The most important characteristics of the receptor materials, which need to be addressed in order to achieve a high efficiency of chemisensor devices, are considered. The printing technologies are comparatively analyzed with regard to, (i) the rheological properties of the employed inks representing both reagent solutions or organometallic precursors and disperse systems, (ii) the printing speed and resolution, and (iii) the thickness of the formed coatings to highlight benefits and drawbacks of the methods. Particular attention is given to protocols suitable for manufacturing single miniature devices with unique characteristics under a large-scale production of gas sensors where the receptor materials could be rather quickly tuned to modify their geometry and morphology. We address the most convenient approaches to the rapid printing single-crystal multisensor arrays at lab-on-chip paradigm with sufficiently high resolution, employing receptor layers with various chemical composition which could replace in nearest future the single-sensor units for advancing a selectivity.

关键词： gas sensor additive manufacturing deposition film coating ink lab-on-chip multisensor array

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Partially Oxidized Ti3C2Tx MXenes for Fast and Selective Detection of Organic Vapors at Part-per-Million Concentrations

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ACS APPLIED NANO MATERIALS 2020年第4期3卷 3195-3204页

作者： Pazniak, Hanna Plugin, Ilya A. Loes, Michael J. Inerbaev, Talgat M. Burmistrov, Igor N. Gorshenkov, Michail Polcak, Josef Varezhnikov, Alexey S. Sommer, Martin Kuznetsov, Denis, V Bruns, Michael Fedorov, Fedor S. Vorobeva, Nataliia S. Sinitskii, Alexander Sysoev, Victor V. Natl Univ Sci & Technol MISiS Dept Funct Nanosyst & High Temp Mat Moscow 119049 Russia Yuri Gavin State Tech Univ Saratov Dept Phys Saratov 410054 Russia Univ Nebraska Dept Chem Lincoln NE 68588 USA VS Sobolev Inst Geol & Mineral SB RAS Novosibirsk 630090 Russia LN Gumilyov Eurasian Natl Univ Astana 010008 Kazakhstan Plekhanov Russian Univ Econ Engn Ctr Dept Chem Innovat Mat & Technol Moscow 117997 Russia Brno Univ Technol CEITEC Cent European Inst Technol Brno 61600 Czech Republic Brno Univ Technol Inst Phys Engn Brno 61600 Czech Republic Yuri Gagarin State Tech Univ Saratov Dept Phys Saratov 410054 Russia Karlsruhe Inst Technol Inst Microstruct Technol D-76344 Eggenstein Leopoldshafen Germany Karlsruhe Inst Technol Inst Appl Mat D-76344 Eggenstein Leopoldshafen Germany Skolkovo Inst Sci & Technol Moscow 121205 Russia

MXenes, two-dimensional transition metal carbides or nitrides, have recently shown great promise for gas sensing applications. We demonstrate that the sensitivity of intrinsically metallic Ti3C2Tx MXene can be considerably improved via its partial oxidation in air at 350 degrees C. The annealed films of MXene sheets remain electrically conductive, while their decoration with semiconducting TiO2, considerably improves their chemiresistive response to organic analytes at low-ppm concentrations in dry air, which was used to emulate practical sensing environments. We demonstrate that partially oxidized MXene has a faster and a qualitatively different sensor response to volatile analytes compared to pristine Ti3C2Tx We fabricated multisensor arrays of partially oxidized Ti3C2Tx MXene devices and demonstrate that in addition to their high sensitivity they enable a selective recognition of analytes of nearly the same chemical nature, such as low molecular weight alcohols. We investigated the oxidation behavior of Ti3C2Tx in air in a wide temperature range and discuss the mechanism of sensor response of partially oxidized MXene films, which is qualitatively different from that of pristine Ti3C2Tx.

关键词： MXene titanium carbide gas sensor multisensor array chemiresistive response titanium dioxide work function

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