{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,13]],"date-time":"2026-10-13T20:45:03Z","timestamp":1791924303558,"version":"4.3.4"},"reference-count":106,"publisher":"American Chemical Society (ACS)","issue":"40","license":[{"start":{"date-parts":[[2026,10,2]],"date-time":"2026-10-02T00:00:00Z","timestamp":1790899200000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100007392","name":"Instituto Nacional de Ci??ncia e Tecnologia em Nanomateriais de Carbono","doi-asserted-by":"publisher","id":[{"id":"10.13039\/501100007392","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100004901","name":"Funda????o de Amparo ?? 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However, in TEMPO-oxidized nanocellulose (TOCNF), water uptake also releases Na+ counterions from carboxylate residues, enabling interfacial polarization via image-charge interactions that can modulate junction-limited electronic transport. Here, we formulate aqueous inks in which TOCNF disperses pristine (nonfunctionalized) multiwalled carbon nanotubes (MWCNT) without covalent modification, yielding homogeneous, spray-processable composite films. Using DC electrical measurements under controlled relative humidity, impedance spectroscopy, scanning probe microscopy, and a mean-field electrostatic model for counterion-mediated polarization, we show that percolated TOCNF\/MWCNT films exhibit reproducible resistance gains, reaching up to \u223c270%, that are inconsistent with a swelling mechanism alone. To support this view, a control based on nonoxidized nanocellulose (with a negligible amount of dissociable counterions) was designed, which shows only modest changes at high humidity, thereby sustaining an important, counterion-mediated interfacial route. The impedance data indicate predominantly electronic transport and a humidity-dependent low-frequency reactive response near the percolation threshold. The DC measurements establish a reproducible steady-state behavior and within-session cycling, while intrinsic response times and long-term stability remain to be more explored. The model rationalizes how increased counterion concentration under humidification can induce polarizing charges at the nanotube surface, driving electrostatic repulsion and relative reorientation that weaken conductive CNT-CNT junctions across the network. Invoking the Derjaguin approximation, an effective, counterion-induced repulsive interaction between CNT surfaces is computed, which prevents the building-up of large connecting junctions across the network, thus reducing their ability to assemble percolating pathways. These findings establish an overlooked counterion-mediated design principle to tune mixed ionic-electronic transport in sustainable CNT\/nanocellulose electronic composites operating under humid or electrolyte-adjacent conditions.<\/jats:p>","DOI":"10.1021\/acsomega.6c04065","type":"journal-article","created":{"date-parts":[[2026,10,2]],"date-time":"2026-10-02T15:01:32Z","timestamp":1790953292000},"page":"60831-60847","source":"Crossref","is-referenced-by-count":0,"title":["Counterion-Mediated\nHumidity Modulation of Electronic\nTransport in Pristine MWCNT\/TOCNF Composites"],"prefix":"10.1021","volume":"11","author":[{"given":"Andreza J.","family":"Siqueira","sequence":"first","affiliation":[{"name":"Universidade Federal de Ouro Preto , , , ,","place":["Ouro Preto, MG, Brazil, 35400-000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wflander M.","family":"Souza","sequence":"additional","affiliation":[{"name":"Universidade Federal de Ouro Preto , , , ,","place":["Ouro Preto, MG, Brazil, 35400-000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rayssa O.","family":"Matos","sequence":"additional","affiliation":[{"name":"Universidade Federal de Ouro Preto , , , ,","place":["Ouro Preto, MG, Brazil, 35400-000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hana H.","family":"Koga","sequence":"additional","affiliation":[{"name":"Universidade Federal de Ouro Preto , , , ,","place":["Ouro Preto, MG, Brazil, 35400-000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3636-7272","authenticated-orcid":true,"given":"Vinicius","family":"Ornelas","sequence":"additional","affiliation":[{"name":"Universidade Federal de Minas Gerais , , , ,","place":["Belo Horizonte, MG, Brazil, 31270-901"]},{"name":"Universidade Federal de Minas Gerais , , , ,","place":["Belo Horizonte, MG, Brazil, 31270-901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Claudio","family":"Laudares","sequence":"additional","affiliation":[{"name":"Universidade Federal de Minas Gerais , , , ,","place":["Belo Horizonte, MG, Brazil, 31270-901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dalila C.","family":"Sicupira","sequence":"additional","affiliation":[{"name":"Universidade Federal de Ouro Preto , , , ,","place":["Ouro Preto, MG, Brazil, 35400-000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0620-9564","authenticated-orcid":true,"given":"Thiago","family":"Colla","sequence":"additional","affiliation":[{"name":"Universidade Federal de Ouro Preto , , , ,","place":["Ouro Preto, MG, Brazil, 35400-000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4040-1373","authenticated-orcid":true,"given":"Ive","family":"Silvestre","sequence":"additional","affiliation":[{"name":"Universidade Federal de Ouro Preto , , , ,","place":["Ouro Preto, MG, Brazil, 35400-000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1807-971X","authenticated-orcid":true,"given":"Ana Paula M.","family":"Barboza","sequence":"additional","affiliation":[{"name":"Universidade Federal de Ouro Preto , , , ,","place":["Ouro Preto, MG, Brazil, 35400-000"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,2]]},"reference":[{"key":"2026101315094221200_cit1","doi-asserted-by":"publisher","first-page":"2777","DOI":"10.1039\/D3AY02258G","article-title":"Paper-based\nsensors: affordable, versatile, and emerging analyte detection platforms","volume":"16","author":"Malik","year":"2024","journal-title":"Anal. 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Interfaces"},{"key":"2026101315094221200_cit5","doi-asserted-by":"publisher","first-page":"1110","DOI":"10.3390\/nano13061110","article-title":"Paper-Based\nHumidity Sensors as Promising Flexible Devices: State of the Art:\nPart 1. General Consideration","volume":"13","author":"Korotcenkov","year":"2023","journal-title":"Nanomaterials"},{"key":"2026101315094221200_cit6","doi-asserted-by":"crossref","first-page":"8232","DOI":"10.1021\/acs.langmuir.2c00566","article-title":"Self-Powered Carbon\nInk\/Filter Paper Flexible Humidity Sensor","volume":"38","author":"Li","year":"2022","journal-title":"Langmuir"},{"key":"2026101315094221200_cit7","doi-asserted-by":"publisher","first-page":"5721","DOI":"10.1021\/acsami.1c20918","article-title":"A Printed\nFlexible Humidity Sensor\nwith High Sensitivity and Fast Response Using a Cellulose Nanofiber\/Carbon\nBlack Composite","volume":"14","author":"Tachibana","year":"2022","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"2026101315094221200_cit8","doi-asserted-by":"publisher","first-page":"7877","DOI":"10.1007\/s10570-021-04026-y","article-title":"Robust cellulose-carbon\nnanotube conductive fibers for electrical\nheating and humidity sensing","volume":"28","author":"Ma","year":"2021","journal-title":"Cellulose"},{"key":"2026101315094221200_cit9","doi-asserted-by":"crossref","first-page":"4834","DOI":"10.1021\/acs.langmuir.8b04259","article-title":"Flexible and\nHighly Sensitive Humidity Sensor Based on Cellulose Nanofiber\/Carbon\nNanotube Composite Film","volume":"35","author":"Zhu","year":"2019","journal-title":"Langmuir"},{"key":"2026101315094221200_cit10","doi-asserted-by":"publisher","DOI":"10.1016\/j.sna.2024.115064","article-title":"Graphene Oxide\/Cellulose Nanofiber-Based Capacitive\nHumidity Sensor with High Sensitivity","volume":"368","author":"Li","year":"2024","journal-title":"Sens.\nActuators, A"},{"key":"2026101315094221200_cit11","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2020.127105","article-title":"Electrostatic self-assembly\nenabled\nflexible paper-based humidity sensor with high sensitivity and superior\ndurability","volume":"404","author":"Zhu","year":"2021","journal-title":"Chem. Eng. J."},{"key":"2026101315094221200_cit12","doi-asserted-by":"publisher","first-page":"3941","DOI":"10.1039\/c0cs00108b","article-title":"Cellulose\nnanomaterials review: structure, properties and nanocomposites","volume":"40","author":"Moon","year":"2011","journal-title":"Chem. Soc. Rev."},{"key":"2026101315094221200_cit13","doi-asserted-by":"publisher","first-page":"169","DOI":"10.1016\/j.progpolymsci.2015.07.003","article-title":"Recent advances in regenerated cellulose materials","volume":"53","author":"Wang","year":"2016","journal-title":"Prog. Polym. Sci."},{"key":"2026101315094221200_cit14","doi-asserted-by":"publisher","DOI":"10.1002\/cben.202300069","article-title":"Applications of\nCellulose-Based Nanomaterials for Sustainability\nand Therapeutics: A Review","volume":"11","author":"Sariboga","year":"2024","journal-title":"ChemBioEng. Rev."},{"key":"2026101315094221200_cit15","doi-asserted-by":"publisher","first-page":"61","DOI":"10.1007\/s10570-023-05616-8","article-title":"An overview of the development status\nand applications of cellulose-based\nfunctional materials","volume":"31","author":"Li","year":"2024","journal-title":"Cellulose"},{"key":"2026101315094221200_cit16","doi-asserted-by":"publisher","first-page":"11575","DOI":"10.1021\/acs.chemrev.7b00627","article-title":"Nanocellulose, a Versatile\nGreen Platform: From Biosources to Materials and Their Applications","volume":"118","author":"Thomas","year":"2018","journal-title":"Chem. Rev."},{"key":"2026101315094221200_cit17","doi-asserted-by":"publisher","first-page":"420","DOI":"10.3389\/fchem.2020.00420","article-title":"Current State of Applications\nof Nanocellulose in Flexible Energy\nand Electronic Devices","volume":"8","author":"Dias","year":"2020","journal-title":"Front. 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Rep."},{"key":"2026101315094221200_cit24","doi-asserted-by":"publisher","first-page":"2016","DOI":"10.1021\/acs.chemrev.2c00477","article-title":"Cellulose: A Review\nof Water Interactions, Applications in Composites, and Water Treatment","volume":"123","author":"Etale","year":"2023","journal-title":"Chem. Rev."},{"key":"2026101315094221200_cit25","doi-asserted-by":"publisher","first-page":"1925","DOI":"10.1021\/acs.chemrev.2c00611","article-title":"Understanding Nanocellulose\u2013Water\nInteractions: Turning a Detriment into an Asset","volume":"123","author":"Solhi","year":"2023","journal-title":"Chem. Rev."},{"key":"2026101315094221200_cit26","doi-asserted-by":"publisher","first-page":"2951","DOI":"10.1021\/acs.biomac.7b00890","article-title":"Interfacial\nMechanisms of Water Vapor Sorption into Cellulose Nanofibril Films\nas Revealed by Quantitative Models","volume":"18","author":"Hakalahti","year":"2017","journal-title":"Biomacromolecules"},{"key":"2026101315094221200_cit27","doi-asserted-by":"publisher","first-page":"1148","DOI":"10.1021\/acs.biomac.1c01446","article-title":"Humidity Response\nof Cellulose Thin Films","volume":"23","author":"Reishofer","year":"2022","journal-title":"Biomacromolecules"},{"key":"2026101315094221200_cit28","doi-asserted-by":"publisher","first-page":"119","DOI":"10.3390\/polym17010119","article-title":"Carbon Nanotube\/Polymer Composites\nfor Functional Applications","volume":"17","author":"Yim","year":"2025","journal-title":"Polymers"},{"key":"2026101315094221200_cit29","doi-asserted-by":"publisher","DOI":"10.1002\/admt.202200855","article-title":"Carbon\nNanotube-Based Strain Sensors: Structures, Fabrication,\nand Applications","volume":"8","author":"Wang","year":"2023","journal-title":"Adv. Mater. Technol."},{"key":"2026101315094221200_cit30","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbpol.2021.118385","article-title":"Green and sustainable cellulose-derived humidity sensors:\nA review","volume":"270","author":"Li","year":"2021","journal-title":"Carbohydr. Polym."},{"key":"2026101315094221200_cit31","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbpol.2024.122059","article-title":"Surface charge manipulation\nfor improved humidity sensing of TEMPO-oxidized cellulose nanofibrils","volume":"335","author":"Zhu","year":"2024","journal-title":"Carbohydr. Polym."},{"key":"2026101315094221200_cit32","doi-asserted-by":"publisher","first-page":"28248","DOI":"10.1021\/acsami.3c04283","article-title":"Flexible Humidity Sensor with High\nSensitivity and Durability for\nRespiratory Monitoring Using Near-Field Electrohydrodynamic Direct-Writing\nMethod","volume":"15","author":"Pan","year":"2023","journal-title":"ACS Appl. Mater. 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Electron.\nMater."},{"key":"2026101315094221200_cit39","doi-asserted-by":"publisher","DOI":"10.1063\/5.0302165","article-title":"High-Sensitivity\nFBG Humidity Sensors Enabled by Electrohydrodynamically\nPrinted Carbon-Nanofiber Functionalized Gratings","volume":"16","author":"Yu","year":"2026","journal-title":"AIP Adv."},{"key":"2026101315094221200_cit40","doi-asserted-by":"publisher","first-page":"37","DOI":"10.1016\/j.cis.2006.11.007","article-title":"The Role of\nSurfactants in Dispersion\nof Carbon Nanotubes","volume":"128\u2013130","author":"Vaisman","year":"2006","journal-title":"Adv. Colloid Interface\nSci."},{"key":"2026101315094221200_cit41","doi-asserted-by":"publisher","DOI":"10.1016\/j.mtchem.2021.100477","article-title":"Functionalization\nas a Way to Enhance Dispersion of Carbon Nanotubes in Matrices: A\nReview","volume":"20","author":"Lavagna","year":"2021","journal-title":"Mater. Today Chem."},{"key":"2026101315094221200_cit42","doi-asserted-by":"publisher","first-page":"1664","DOI":"10.3390\/polym16121664","article-title":"Nanocellulose:\nThe Ultimate Green Aqueous Dispersant for Nanomaterials","volume":"16","author":"Calvo","year":"2024","journal-title":"Polymers"},{"key":"2026101315094221200_cit43","doi-asserted-by":"publisher","first-page":"1439","DOI":"10.1021\/acs.nanolett.6b04405","article-title":"Understanding\nthe dispersive action of nanocellulose for carbon nanomaterials","volume":"17","author":"Hajian","year":"2017","journal-title":"Nano Lett."},{"key":"2026101315094221200_cit44","doi-asserted-by":"publisher","first-page":"357","DOI":"10.1016\/j.progpolymsci.2009.09.003","article-title":"Carbon nanotube-polymer\ncomposites: Chemistry, processing, mechanical and electrical properties","volume":"35","author":"Spitalsky","year":"2010","journal-title":"Prog. Polym. Sci."},{"key":"2026101315094221200_cit45","doi-asserted-by":"publisher","first-page":"149","DOI":"10.1016\/j.compositesa.2018.08.021","article-title":"Interfacial characteristics of carbon\nnanotube-polymer composites: A review","volume":"114","author":"Chen","year":"2018","journal-title":"Composites,\nPart A"},{"key":"2026101315094221200_cit46","doi-asserted-by":"publisher","first-page":"1200","DOI":"10.1016\/j.jcis.2022.05.041","article-title":"Scalable production of high-quality carbon nanotube dispersion in\naqueous solution using cellulose as dispersant by a freezing\/thawing\nprocess","volume":"623","author":"Qiao","year":"2022","journal-title":"J. Colloid Interface Sci."},{"key":"2026101315094221200_cit47","doi-asserted-by":"publisher","first-page":"2467","DOI":"10.1021\/nn4060368","article-title":"Highly Conducting, Strong Nanocomposites Based on Nanocellulose-Assisted\nAqueous Dispersions of Single-Wall Carbon Nanotubes","volume":"8","author":"Hamedi","year":"2014","journal-title":"ACS Nano"},{"key":"2026101315094221200_cit48","doi-asserted-by":"publisher","first-page":"3806","DOI":"10.1021\/acs.biomac.3c00449","article-title":"Protein Adsorption and Its Effects\non Electroanalytical Performance of Nanocellulose\/Carbon Nanotube\nComposite Electrodes","volume":"24","author":"Liljestro\u0308m","year":"2023","journal-title":"Biomacromolecules"},{"key":"2026101315094221200_cit49","doi-asserted-by":"publisher","first-page":"36647","DOI":"10.1021\/acsami.3c03906","article-title":"Dynamic\nAssembly of Strong and Conductive\nCarbon Nanotube\/Nanocellulose Composite Filaments and Their Application\nin Resistive Liquid Sensing","volume":"15","author":"Wise","year":"2023","journal-title":"ACS Appl. Mater.\nInterfaces"},{"key":"2026101315094221200_cit50","doi-asserted-by":"publisher","first-page":"50281","DOI":"10.1021\/acsami.1c16828","article-title":"Self-Recovery, Fatigue-Resistant,\nand Multifunctional Sensor Assembled by a Nanocellulose\/Carbon Nanotube\nNanocomplex-Mediated Hydrogel","volume":"13","author":"Lu","year":"2021","journal-title":"ACS Appl. Mater.\nInterfaces"},{"key":"2026101315094221200_cit51","doi-asserted-by":"publisher","first-page":"2180","DOI":"10.1103\/PhysRevB.21.2180","article-title":"Fluctuation-induced\ntunneling conduction in disordered materials","volume":"21","author":"Sheng","year":"1980","journal-title":"Phys. Rev. B"},{"key":"2026101315094221200_cit52","doi-asserted-by":"publisher","first-page":"17","DOI":"10.1002\/adma.200500928","article-title":"Polymer\nNanofibers and Nanotubes: Charge Transport and Device Applications","volume":"18","author":"Aleshin","year":"2006","journal-title":"Adv. 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