Three-dimensional (3D) printing has showed great potential for the construction of electrochemical sensor devices. However, reported 3D-printed biosensors are usually constructed by physical adsorption and needed immobilizing reagents on the surface of functional materials. To construct the 3D-printed biosensors, the simple modification of the 3D-printed device by non-expert is mandatory to take advantage of the remote, distributed 3D printing manufacturing. Here, a 3D-printed electrode was prepared by fused deposition modeling (FDM) 3D printing technique and activated by chemical and electrochemical methods. A glucose oxidase-based 3D-printed nanocarbon electrode was prepared by covalent linkage method to an enzyme on the surface of the 3D-printed electrode to enable biosensing. X-ray photoelectron spectroscopy and scanning electron microscopy were used to characterize the glucose oxidase-based biosensor. Direct electrochemistry glucose oxidase-based biosensor with higher stability was then chosen to detect the two biomarkers, hydrogen peroxide and glucose by chronoamperometry. The prepared glucose oxidase-based biosensor was further used for the detection of glucose in samples of apple cider. The covalently linked glucose oxidase 3D-printed nanocarbon electrode as a biosensor showed excellent stability. This work can open new doors for the covalent modification of 3D-printed electrodes in other electrochemistry fields such as biosensors, energy, and biocatalysis.

D Printing and Innovation Hub Department of Food Technology Mendel University in Brno Zemedelska 1 CZ 613 00 Brno Czech Republic

Department of Chemical and Biomolecular Engineering Yonsei University 50 Yonsei ro Seodaemungu Seoul 03722 South Korea

Department of Medical Research China Medical University Hospital China Medical University No 91 Hsueh Shih Road Taichung Taiwan

Future Energy and Innovation Laboratory Central European Institute of Technology Brno University of Technology 61200 Brno Czech Republic

School of Pharmacy Southwest Medical University Luzhou Sichuan 646000 People's Republic of China

Zobrazit více v PubMed

Choong YYC, Tan H, Patel DC, Choong WTN, Chen C, Low HY, Tan M, Patel CD, Chua CK (2020) The global rise of 3d printing during the COVID-19 pandemic. Nat Rev Mater 5:637–639 DOI

Ngo TD, Kashani A, Imbalzano G, Nguyen KTQ, Hui D (2018) Additive manufacturing (3D printing): a review of materials, methods, applications and challenges. Composites Part B 143:172–196 DOI

Wang L, Pumera M (2021) Recent advances of 3d printing in analytical chemistry: focus on microfluidic, separation, and extraction devices. TrAC Trends Anal Chem 135:116151 DOI

Browne MP, Redondo E, Pumera M (2020) 3D printing for electrochemical energy applications. Chem Rev 120:2783–2810 DOI

Muñoz J, Pumera M (2020) 3D-printed biosensors for electrochemical and optical applications. TrAC Trends Anal Chem 128:115933 DOI

Ambrosi A, Pumera M (2018) Sel-containedpolymer/metal 3D printed electrochemical platform for tailored water splitting. Adv Funct Mater 28:1700655

Ng S, Iffelsberger C, Sofer Z, Pumera M (2020) Tunable room-temperature synthesis of ReS DOI

Symes MD, Kitson PJ, Yan J, Richmond CJ, Cooper GJ, Bowman RW, Vilbrandt T, Cronin L (2012) Integrated 3D-printed reactionware for chemical synthesis and analysis. Nat Chem 4:349–354 DOI

Browne MP, Urbanova V, Plutnar J, Novotný F, Pumera M (2020) Inherent impurities in 3D-printed electrodes are responsible for catalysis towards water splitting. J Mater Chem A 8:1120–1126 DOI

Lee JY, An J, Chua CK (2017) Fundamentals and applications of 3D printing for novel materials. Appl Mater Today 7:120–133 DOI

Valot L, Martinez J, Mehdi A, Subra G (2019) Chemical insights into bioinks for 3D printing. Chem Soc Rev 48:4049–4086 DOI

Helú MAB, Liu L (2021) Fused deposition modeling (FDM) based 3D printing of microelectrodes and multi-electrode probes. Electrochim Acta 365:137279 DOI

Manzanares Palenzuela CL, Novotny F, Krupicka P, Sofer Z, Pumera M (2018) 3D-printedgraphene/polylactic acid electrodes promise high sensitivity in electroanalysis. Anal Chem 90:5753–5757

Bin Hamzah HH, Keattch O, Covill D, Patel BA (2018) The effects of printing orientation on the electrochemical behaviour of 3D printed acrylonitrile butadiene styrene (ABS)/carbon black electrodes. Sc Rep 8:1–8

Katic V, Dos Santos PL, Dos Santos MF, Pires BM, Loureiro HC, Lima AP, Queiroz JCM, Landers R, Munoz RAA, Bonacin JA (2019) 3D printed graphene electrodes modified with prussian blue: emerging electrochemical sensing platform for peroxide detection. ACS Appl Mater Interfaces 11:35068–35078 DOI

Munoz J, Redondo E, Pumera M (2021) Bistable (supra)molecular switches on 3D-printed responsive interfaces with electrical readout. ACS Appl Mater Interfaces 13:12649–12655 DOI

Richter EM, Rocha DP, Cardoso RM, Keefe EM, Foster CW, Munoz RAA, Banks CE (2019) Complete additively manufactured (3D-printed) electrochemical sensing platform. Anal Chem 91:12844–12851 DOI

Akshay Kumar KP, Ghosh K, Alduhaish O, Pumera M (2021) Dip-coating of mxene and transition metal dichalcogenides on 3D-printed nanocarbon electrodes for the hydrogen evolution reaction. Electrochem Commun 122:106890 DOI

Ng S, Iffelsberger C, Michalicka J, Pumera M (2021) Atomic layer deposition of electrocatalytic insulator Al DOI

Elbadawi M, Ong JJ, Pollard TD, Gaisford S, Basit AW (2021) Additive manufacturable materials for electrochemical biosensor electrodes. Adv Funct Mater 31:2006407 DOI

Gusmão R, Browne MP, Sofer Z, Pumera M (2019) The capacitance and electron transfer of 3D-printed graphene electrodes are dramatically influenced by the type of solvent used for pre-treatment. Electrochem Commun 102:83–88 DOI

Kalinke C, Neumsteir NV, Roberto de Oliveira P, Janegitz BC, Bonacin JA (2020) Sensing of L-methionine in biological samples through fully 3D-printed electrodes. Anal Chim Acta 1142:135–142 DOI

Tan C, Nasir MZM, Ambrosi A, Pumera M (2017) 3D printed electrodes for detection of nitroaromatic explosives and nerve agents. Anal Chem 89:8995–9001 DOI

Browne MP, Novotny F, Sofer Z, Pumera M (2018) 3D printed graphene electrodes' electrochemical activation. ACS Appl Mater Interfaces 10:40294–40301 DOI

Cardoso RM, Castro SVF, Silva MNT, Lima AP, Santana MHP, Nossol E, Silva RAB, Richter EM, Paixão TRLC, Muñoz RAA (2019) 3D-printed flexible device combining sampling and detection of explosives. Sensors Actuators B Chem 292:308–313 DOI

Cardoso RM, Silva PRL, Lima AP, Rocha DP, Oliveira TC, do Prado TM, Fava EL, Fatibello-Filho O, Richter EM, Muñoz RAA (2020) 3D-printedgraphene/polylactic acid electrode for bioanalysis: biosensing of glucose and simultaneous determination of uric acid and nitrite in biological fluids. Sensors Actuators B Chem 307:127621

Manzanares-Palenzuela CL, Hermanova S, Sofer Z, Pumera M (2019) Proteinase-sculptured 3D-printed graphene/polylactic acid electrodes as potential biosensing platforms: towards enzymatic modeling of 3D-printed structures. Nanoscale 11:12124–12131

Silva V, Fernandes-Junior WS, Rocha DP, Stefano JS, Munoz RAA, Bonacin JA, Janegitz BC (2020) 3D-printed reduced graphene oxide/polylactic acid electrodes: a new prototyped platform for sensing and biosensing applications. Biosens Bioelectron 170:112684 DOI

Lopez Marzo AM, Mayorga-Martinez CC, Pumera M (2020) 3D-printed graphene direct electron transfer enzyme biosensors. Biosens Bioelectron 151:111980 DOI

Luo Q, Zhong Z, Zheng Y, Gao D, Xia Z, Wang L (2021) Preparation and evaluation of a poly(n-isopropylacrylamide) derived graphene quantum dots based hydrophilic interaction and reversed-phase mixed-mode stationary phase for complex sample analysis. Talanta 224:121869 DOI

Supraja P, Tripathy S, Krishna Vanjari SR, Singh V, Singh SG (2019) Electrospun tin (IV) oxide nanofiber based electrochemical sensor for ultra-sensitive and selective detection of atrazine in water at trace levels. Biosens Bioelectron 141:111441 DOI

Kogularasu S, Govindasamy M, Chen SM, Lin SH, Akilarasan M, Mani V (2018) A novel synthesis of non-aggregated spinel nickel ferrite nanosheets for developing non-enzymatic reactive oxygen species sensor in biological samples. Sensors Actuators B Chem 266:655–663 DOI

Sakthivel K, Govindasamy M, Chen SM, Muthumariappan A, Mani V, Selvaraj S (2017) 3D graphene oxide-cobalt oxide polyhedrons for highly sensitive non-enzymatic electrochemical determination of hydrogen peroxide. Sensors Actuators B Chem 253:773–783 DOI

Lawal AT (2018) Progress in utilisation of graphene for electrochemical biosensors. Biosens Bioelectron 106:149–178 DOI

Liu Y, Wang M, Zhao F, Xu Z, Dong S (2005) The direct electron transfer of glucose oxidase and glucose biosensor based on carbon nanotubes/chitosan matrix. Biosens Bioelectron 21:984–988 DOI

Cai Y, Liang B, Chen S, Zhu Q, Tu T, Wu K, Cao Q, Fang L, Liang X, Ye X (2020)One-step modification of nano-polyaniline/glucose oxidase on double-side printed flexible electrode for continuous glucose monitoring: characterization, cytotoxicity evaluation and in vivo experiment. Biosens Bioelectron 165:112408 DOI

Guzsvány V, Anojčić J, Vajdle O, Radulović E, Madarász D, Kónya Z, Kalcher K (2019) Amperometric determination of glucose in white grape and in tablets as ingredient by screen-printed electrode modified with glucose oxidase and composite of platinum and multiwalled carbon nanotubes. Food Anal Methods 12:570–580 DOI

Zhang Z, Chen Z, Cheng F, Zhang Y, Chen L (2017) Highly sensitive on-site detection of glucose in human urine with naked eye based on enzymatic-like reaction mediated etching of gold nanorods. Biosens Bioelectron 89:932–936 DOI

Akilarasan M, Kogularasu S, Chen SM, Chen TW, Govidasamy M, Lou BS (2018) Effects of annealing temperature on crystal structure and glucose sensing properties of cuprous oxide. Sensors Actuators B Chem 266:655–663 DOI

Ikeda M, Tanida T, Yoshii T, Kurotani K, Onogi S, Urayama K, Hamachi I (2014) Installing logic-gate responses to a variety of biological substances in supramolecular hydrogel–enzyme hybrids. Nat Chem 6:511–518 DOI

Mani V, Devadas B, Chen SM (2013) Direct electrochemistry of glucose oxidase at electrochemically reduced graphene oxide-multiwalled carbon nanotubes hybrid material modified electrode for glucose biosensor. Biosens Bioelectron 41:309–315 DOI

Sanchez-Calvo A, Costa-Garcia A, Blanco-Lopez MC (2020)Paper-based electrodes modified with cobalt phthalocyanine colloid for the determination of hydrogen peroxide and glucose. Analyst 145:2716–2724 DOI

Salimi A, Compton RG, Hallaj R (2004) Glucose biosensor prepared by glucose oxidase encapsulated sol-gel and carbon-nanotube-modified basal plane pyrolytic graphite electrode. Anal Biochem 333:49–56 DOI

Hu G, Liu H, Zhu Y, Hernandez M, Koutchma T, Shao S (2018) Suppression of the formation of furan by antioxidants during UV-C light treatment of sugar solutions and apple cider. Food Chem 269:342–346 DOI