{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,4,1]],"date-time":"2026-04-01T10:31:56Z","timestamp":1775039516286,"version":"3.50.1"},"reference-count":54,"publisher":"MDPI AG","issue":"14","license":[{"start":{"date-parts":[[2019,7,10]],"date-time":"2019-07-10T00:00:00Z","timestamp":1562716800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"name":"Development of Reliability Technology of Standard Measurement for Hydrogen Convergence Station program of the Korea Research Institute of Standards and Science","award":["KRISS \u2013 2018 \u2013 GP2018-0011"],"award-info":[{"award-number":["KRISS \u2013 2018 \u2013 GP2018-0011"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Sensors"],"abstract":"<jats:p>Paper-based sensors fabricated using the pencil-on-paper method are expected to find wide usage in many fields owing to their low cost and high reproducibility. Here, hydrogen (H2) detection was realized by applying palladium (Pd) nanoparticles (NPs) to electronic circuits printed on paper using a metal mask and a pencil. We confirmed that multilayered graphene was produced by the pencil, and then characterized Pd NPs were added to the pencil marks. To evaluate the gas-sensing ability of the sensor, its sensitivities and reaction rates in the presence and absence of H2 were measured. In addition, sensing tests performed over a wide range of H2 concentrations confirmed that the sensor had a detection limit as low as 1 ppm. Furthermore, the sensor reacted within approximately 50 s at all H2 concentrations tested. The recovery time of the sensor was 32 s at 1 ppm and 78 s at 1000 ppm. Sensing tests were also performed using Pd NPs of different sizes to elucidate the relationship between the sensing rate and catalyst size. The experimental results confirmed the possibility of fabricating paper-based gas sensors with a superior sensing capability and response rate.<\/jats:p>","DOI":"10.3390\/s19143050","type":"journal-article","created":{"date-parts":[[2019,7,10]],"date-time":"2019-07-10T11:56:51Z","timestamp":1562759811000},"page":"3050","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Hydrogen Sensing Using Paper Sensors with Pencil Marks Decorated with Palladium"],"prefix":"10.3390","volume":"19","author":[{"given":"Nam Hee","family":"Lee","sequence":"first","affiliation":[{"name":"Department of Chemistry, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Korea"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Un-Bong","family":"Baek","sequence":"additional","affiliation":[{"name":"Energy Materials Metrology, Korea Research Institute of Standards and Science, 267 Gajeong-ro, Yuseong-gu, Daejeon 34113, Korea"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Seung-Hoon","family":"Nahm","sequence":"additional","affiliation":[{"name":"Energy Materials Metrology, Korea Research Institute of Standards and Science, 267 Gajeong-ro, Yuseong-gu, Daejeon 34113, Korea"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"1968","published-online":{"date-parts":[[2019,7,10]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"15","DOI":"10.1016\/j.synthmet.2004.09.013","article-title":"Hydrogen sensors based on carbon nanotubes thin films","volume":"148","author":"Sayago","year":"2005","journal-title":"Synth. Met."},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"2518","DOI":"10.1016\/j.ijhydene.2006.11.015","article-title":"Palladium dispersed multiwalled carbon nanotube based hydrogen sensor for fuel cell applications","volume":"32","author":"Ramaprabhu","year":"2007","journal-title":"Int. J. Hydrog. Energy"},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"329","DOI":"10.1016\/j.snb.2011.04.070","article-title":"Hydrogen sensors\u2014A review","volume":"157","author":"Blackb","year":"2011","journal-title":"Sens. Actuators B"},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"2743","DOI":"10.1039\/c2an16029c","article-title":"Advances in materials for room temperature hydrogen sensors","volume":"137","author":"Arya","year":"2012","journal-title":"Analyst"},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"1","DOI":"10.1016\/j.snb.2014.05.052","article-title":"Pt\/NiO ring gate based Schottky diode hydrogen sensors with enhanced sensitivity and thermal stability","volume":"202","author":"Vankoa","year":"2014","journal-title":"Sens. Actuators B"},{"key":"ref_6","doi-asserted-by":"crossref","first-page":"234","DOI":"10.1016\/j.snb.2011.06.078","article-title":"Hydrogen sensor based on Pd-functionalized film bulk acoustic resonator","volume":"159","author":"Chena","year":"2011","journal-title":"Sens. Actuators B"},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"16343","DOI":"10.1016\/j.ceramint.2014.07.073","article-title":"A room-temperature hydrogen sensor based on Pd nanoparticles doped TiO2 nanotubes","volume":"128","author":"Xianga","year":"2014","journal-title":"Ceram. Int."},{"key":"ref_8","doi-asserted-by":"crossref","first-page":"14831","DOI":"10.1016\/j.ijhydene.2011.12.075","article-title":"Hydrogen absorption in Pd nanoparticles of different shapes","volume":"37","author":"Crespo","year":"2012","journal-title":"Int. J. Hydrog. Energy."},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"1487","DOI":"10.1016\/S0038-1101(02)00495-1","article-title":"Comparison of Pt\/GaN and Pt\/4H-SiC gas sensors","volume":"47","author":"Kim","year":"2003","journal-title":"Solid State Electron."},{"key":"ref_10","doi-asserted-by":"crossref","first-page":"739","DOI":"10.1063\/1.1541944","article-title":"Reversible barrier height changes in hydrogen-sensitive Pd\/GaN and Pt\/GaN diodes","volume":"82","author":"Kim","year":"2003","journal-title":"Appl. Phys. Lett."},{"key":"ref_11","doi-asserted-by":"crossref","first-page":"338","DOI":"10.1016\/S0925-4005(03)00222-3","article-title":"Hydrogen sensing using titania nanotube","volume":"93","author":"Varghese","year":"2003","journal-title":"Sens. Actuators B"},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"586","DOI":"10.1016\/j.cplett.2005.11.040","article-title":"Hydrogen and ethanol sensors based on ZnO nanorods, nanowires and nanotubes","volume":"418","author":"Rout","year":"2006","journal-title":"Chem. Phys. Lett."},{"key":"ref_13","doi-asserted-by":"crossref","first-page":"6643","DOI":"10.1021\/jp8003147","article-title":"Fabrication of a SnO2 nanowire gas sensor and sensor performance for hydrogen","volume":"112","author":"Wang","year":"2008","journal-title":"J. Phys. Chem. C"},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"48","DOI":"10.1016\/j.snb.2010.03.024","article-title":"Catalyst supported growth of In2O3 nanostructures and their hydrogen gas sensing properties","volume":"147","author":"Qurashia","year":"2010","journal-title":"Sens. Actuators B"},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"5194","DOI":"10.1016\/j.ijhydene.2014.01.066","article-title":"Hydrogen sensing properties of ZnO nanorods: Effects of annealing, temperature and electrode structure","volume":"39","author":"Torun","year":"2014","journal-title":"Int. J. Hydrog. Energy"},{"key":"ref_16","doi-asserted-by":"crossref","first-page":"729","DOI":"10.1016\/j.ijhydene.2014.10.142","article-title":"Hydrogen sensing performance of a nickel oxide (NiO) thin film-based device","volume":"40","author":"Chou","year":"2015","journal-title":"Int. J. Hydrog. Energy"},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"109","DOI":"10.1016\/j.snb.2009.04.004","article-title":"High-temperature resistive hydrogen sensor based on thin nanoporous rutile TiO2 film on anodic aluminum oxide","volume":"140","author":"Lu","year":"2009","journal-title":"Sens. Actuators B"},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"249","DOI":"10.1149\/1.2043887","article-title":"Solid-state hydrogen sensors using palladium\u2013nickel alloys: Effect of alloy composition on sensor response","volume":"142","author":"Hughes","year":"1995","journal-title":"J. Electrochem. Soc."},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"379","DOI":"10.1016\/S0925-8388(99)00374-6","article-title":"Kinetics and morphology of the reverse \u03b2 \u2192 \u03b1 hydride transformation in thermodynamically open Pd\u2013H system","volume":"293\u2013295","author":"Goltsova","year":"1999","journal-title":"J. Alloys. Compd."},{"key":"ref_20","doi-asserted-by":"crossref","first-page":"11","DOI":"10.1002\/adem.200300557","article-title":"Hydrogen in nano-sized metals","volume":"6","author":"Pundt","year":"2004","journal-title":"Adv. Eng. Mater."},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"880","DOI":"10.1016\/j.tsf.2010.07.122","article-title":"Hydrogen gas sensing performance of Pd\u2013Ni alloy thin films","volume":"519","author":"Lee","year":"2010","journal-title":"Thin. Solid. Films"},{"key":"ref_22","doi-asserted-by":"crossref","first-page":"6984","DOI":"10.1016\/j.ijhydene.2010.04.051","article-title":"Hysteresis behavior of electrical resistance in Pd thin films during the process of absorption and desorption of hydrogen gas","volume":"35","author":"Lee","year":"2010","journal-title":"Int. J. Hydrog. Energy."},{"key":"ref_23","doi-asserted-by":"crossref","first-page":"1422","DOI":"10.1002\/smll.201000145","article-title":"Joule heating a palladium nanowire sensor for accelerated response and recovery to hydrogen gas","volume":"6","author":"Yang","year":"2010","journal-title":"Small"},{"key":"ref_24","doi-asserted-by":"crossref","first-page":"269","DOI":"10.1146\/annurev.ms.21.080191.001413","article-title":"The palladium\u2013hydrogen system","volume":"21","author":"Flanagan","year":"1991","journal-title":"Annu. Rev. Mater. Sci."},{"key":"ref_25","doi-asserted-by":"crossref","first-page":"1384","DOI":"10.1002\/1521-4095(200109)13:18<1384::AID-ADMA1384>3.0.CO;2-8","article-title":"Functionalized carbon nanotubes for molecular hydrogen sensors","volume":"13","author":"Kong","year":"2001","journal-title":"Adv. Mater."},{"key":"ref_26","doi-asserted-by":"crossref","first-page":"2218","DOI":"10.1088\/0957-4484\/16\/10\/040","article-title":"Carbon nanotube films for room temperature hydrogen sensing","volume":"16","author":"Wang","year":"2005","journal-title":"Nanotechnology"},{"key":"ref_27","doi-asserted-by":"crossref","first-page":"6321","DOI":"10.1021\/jp067716m","article-title":"Palladium nanoparticles decorated single-walled carbon nanotube hydrogen sensor","volume":"11","author":"Mubeen","year":"2007","journal-title":"J. Phys. Chem. C"},{"key":"ref_28","doi-asserted-by":"crossref","first-page":"2177","DOI":"10.1021\/nl9008474","article-title":"Fast, sensitive hydrogen gas detection using single palladium nanowires that resist fracture","volume":"9","author":"Yang","year":"2009","journal-title":"Nano. Lett."},{"key":"ref_29","doi-asserted-by":"crossref","first-page":"223110","DOI":"10.1063\/1.3132064","article-title":"Ultralow-power hydrogen sensing with single palladium nanowires","volume":"94","author":"Offermans","year":"2009","journal-title":"Appl. Phys. Lett."},{"key":"ref_30","doi-asserted-by":"crossref","first-page":"135502","DOI":"10.1088\/0957-4484\/20\/13\/135502","article-title":"Individual Pd nanowire hydrogen sensors fabricated by electron-beam lithography","volume":"20","author":"Jeon","year":"2009","journal-title":"Nanotechnology"},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"2227","DOI":"10.1126\/science.1063189","article-title":"Hydrogen sensors and switches from electrodeposited palladium mesowire arrays","volume":"293","author":"Favier","year":"2001","journal-title":"Science"},{"key":"ref_32","doi-asserted-by":"crossref","first-page":"3345","DOI":"10.1021\/cm048191i","article-title":"Fabrication of palladium nanotubes and their application in hydrogen sensing","volume":"17","author":"Yu","year":"2005","journal-title":"Chem. Mater."},{"key":"ref_33","doi-asserted-by":"crossref","first-page":"3707","DOI":"10.1016\/j.electacta.2010.10.078","article-title":"Hydrogen sensor based on a graphene-palladium nanocomposite","volume":"56","author":"Lange","year":"2011","journal-title":"Electrochim. Acta."},{"key":"ref_34","doi-asserted-by":"crossref","first-page":"4877","DOI":"10.1002\/adma.201001798","article-title":"Hydrogen sensing using pd-functionalized multi-layer graphene nanoribbon networks","volume":"22","author":"Johnson","year":"2010","journal-title":"Adv. Mater."},{"key":"ref_35","doi-asserted-by":"crossref","first-page":"8044","DOI":"10.1039\/C5NJ01673H","article-title":"Hydrogen-gas sensors based on graphene functionalized palladium nanoparticles: Impedance response as a valuable sensor","volume":"39","year":"2015","journal-title":"New J. Chem."},{"key":"ref_36","doi-asserted-by":"crossref","first-page":"20294","DOI":"10.1016\/j.ijhydene.2014.10.006","article-title":"Reliability of hydrogen sensing based on bimetallic Ni\u2013Pd\/graphene composites","volume":"39","author":"Phan","year":"2014","journal-title":"Int. J. Hydrog. Energy."},{"key":"ref_37","doi-asserted-by":"crossref","first-page":"437","DOI":"10.1016\/j.snb.2014.07.120","article-title":"Effects of Pd nanocube size of Pd nanocube-graphene hybrid on hydrogen sensing properties","volume":"204","author":"Phan","year":"2014","journal-title":"Sens. Actuators B"},{"key":"ref_38","doi-asserted-by":"crossref","first-page":"13293","DOI":"10.1021\/am503105s","article-title":"Palladium-decorated hydrogen-gas sensors using periodically aligned graphene nanoribbons","volume":"6","author":"Pak","year":"2014","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_39","doi-asserted-by":"crossref","first-page":"599","DOI":"10.1016\/j.carbon.2013.09.047","article-title":"Single wall carbon nanotubes loaded with Pd and NiPd nanoparticles for H2 sensing at room temperature","volume":"66","year":"2014","journal-title":"Carbon"},{"key":"ref_40","doi-asserted-by":"crossref","first-page":"2395","DOI":"10.1002\/adfm.201500094","article-title":"Flexible and highly sensitive strain sensors fabricated by pencil drawn for wearable monitor","volume":"25","author":"Liao","year":"2015","journal-title":"Adv. Funct. Mater."},{"key":"ref_41","doi-asserted-by":"crossref","first-page":"29140","DOI":"10.1021\/acsami.7b08737","article-title":"Cheap, flexible, and thermal-sensitive paper sensor through writing with ionic liquids containing pencil leads","volume":"9","author":"Sun","year":"2017","journal-title":"ACS Appl. Mater. Inter."},{"key":"ref_42","doi-asserted-by":"crossref","first-page":"143101","DOI":"10.1063\/1.4917063","article-title":"Pencil-trace on printed silver interdigitated electrodes for paper-based NO2 gas sensors","volume":"106","author":"Zhang","year":"2015","journal-title":"Appl. Phys. Lett."},{"key":"ref_43","doi-asserted-by":"crossref","first-page":"1","DOI":"10.1016\/j.pmatsci.2014.10.004","article-title":"Graphene-based materials: Synthesis and gas sorption, storage and separation","volume":"69","author":"Gadipelli","year":"2015","journal-title":"Prog. Mater. Sci."},{"key":"ref_44","doi-asserted-by":"crossref","first-page":"1704","DOI":"10.1039\/c0ee00759e","article-title":"To draw an air electrode of a Li\u2013air battery by pencil","volume":"4","author":"Wang","year":"2011","journal-title":"Energy Environ. Sci."},{"key":"ref_45","doi-asserted-by":"crossref","first-page":"315101","DOI":"10.1088\/0022-3727\/47\/31\/315101","article-title":"Direct growth of large-area graphene films onto oxygen plasma-etched quartz for nitrogen dioxide gas detection","volume":"47","author":"Yang","year":"2014","journal-title":"J. Phys. D Appl. Phys."},{"key":"ref_46","doi-asserted-by":"crossref","first-page":"55","DOI":"10.1016\/S0368-2048(98)00312-0","article-title":"XPS, AES and Auger parameter of Pd and PdO","volume":"104","author":"Brun","year":"1999","journal-title":"J. Electron. Spectrosc. Relat. Phenom."},{"key":"ref_47","doi-asserted-by":"crossref","first-page":"3368","DOI":"10.1039\/c1ee01853a","article-title":"Paper supercapacitors by a solvent-free drawing method","volume":"4","author":"Zheng","year":"2011","journal-title":"Energy. Environ. Sci."},{"key":"ref_48","doi-asserted-by":"crossref","first-page":"3812","DOI":"10.1038\/srep03812","article-title":"Pencil drawn strain gauges and chemiresistors on paper","volume":"4","author":"Lin","year":"2014","journal-title":"Sci. Rep."},{"key":"ref_49","doi-asserted-by":"crossref","first-page":"668","DOI":"10.1039\/C0EE00295J","article-title":"Graphene-based nanomaterials for energy storage","volume":"4","author":"Pumera","year":"2011","journal-title":"Energy. Environ. Sci."},{"key":"ref_50","doi-asserted-by":"crossref","first-page":"10078","DOI":"10.1039\/c3ta11774j","article-title":"Graphene-based gas sensors","volume":"1","author":"Yuan","year":"2013","journal-title":"J. Mater. Chem. A"},{"key":"ref_51","unstructured":"Yu, P.Y., and Cardona, M. (2005). Fundamentals of Semiconductors: Physics and Materials Properties, Springer. [4th ed.]."},{"key":"ref_52","unstructured":"Masel, R.I. (1996). Principles of Adsorption and Reaction on Solid Surfaces, Wiley."},{"key":"ref_53","doi-asserted-by":"crossref","first-page":"296","DOI":"10.1016\/j.snb.2010.06.070","article-title":"Wafer-scale synthesis of graphene by chemical vapor deposition and its application in hydrogen sensing","volume":"150","author":"Wu","year":"2010","journal-title":"Sens. Actuators B"},{"key":"ref_54","doi-asserted-by":"crossref","first-page":"79","DOI":"10.1023\/A:1019078419537","article-title":"Hydrogen absorption in palladium films sensed by changes in their resistivity","volume":"45","author":"Cabrera","year":"1997","journal-title":"Catal. Lett."}],"container-title":["Sensors"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/1424-8220\/19\/14\/3050\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,10,11]],"date-time":"2025-10-11T13:04:24Z","timestamp":1760187864000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/1424-8220\/19\/14\/3050"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2019,7,10]]},"references-count":54,"journal-issue":{"issue":"14","published-online":{"date-parts":[[2019,7]]}},"alternative-id":["s19143050"],"URL":"https:\/\/doi.org\/10.3390\/s19143050","relation":{},"ISSN":["1424-8220"],"issn-type":[{"value":"1424-8220","type":"electronic"}],"subject":[],"published":{"date-parts":[[2019,7,10]]}}}