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An Organic Redox Flow Cell‐Inspired Paper‐Based Primary Battery Full Papers ChemSusChem doi.org/10.1002/cssc.201903511 An Organic Redox Flow Cell-Inspired Paper-Based Primary Battery Marina Navarro-Segarra+,[a] Perla Patricia Alday+,[a] DavidGarcia,[a] Omar A. Ibrahim,[b] Erik Kjeang,[b] Neus SabatØ,[a, c] and Juan Pablo Esquivel*[a] Aportable paper-basedorganic redox flow primary battery trolytesand provides the advantage to form aneutral or near- using sustainable quinone chemistry is presented. The com- neutralpHasthe electrolytes neutralize at the absorbent pad, pact prototype relies on the capillaryforces of the paper which allows asafe disposal after use. The effectsofthe device matrix to develop aquasi-steadyflow of the reactants through design parameters have been studied to enhance battery fea- apair of porous carbon electrodes withoutthe need of exter- tures such as poweroutput,operational time, and fuel utiliza- nal pumps. Co-laminar capillary flow allows operation Under tion. The device achieves afaradaic efficiency of upto98%, mixed-mediaconditions, in which an alkaline anolyte and an which is the highest reported in acapillary-based electrochem- acidic catholyte are employed. This feature enables higher ical power source, as well as acell capacity of up to 1 2 electrochemical cell voltages during discharge operation and 11.4 AhLÀ cmÀ ,comparable to state-of-the-art large-scale the utilization of awider range of available species and elec- redox flow cells. Introduction The increasing usage of small-sized portable electronic devices properly managed butnowadays is sent away to places in the in recent decades has led to astrong demand forminiaturized world where it can causeenvironmental and health prob- power sources. Moreover, such devices require batteries to be lems.[4] The problem is even more critical when this waste is adaptedtoproduct sizes and form factors that make their re- not even collected properly and ends up in landfillswhere, in cycling even more challenging, since it is much harder to sepa- many cases, it is incinerated. One of the most hazardous com- rate the battery from the device, thus aggravating the environ- ponents in e-waste is batteries, as they need special and dedi- mental impact associated to the generation of waste electrical cated recyclingprocesses.[5] To date, the portable energy and electronicequipment(WEEE). WEEE is rapidly becoming demand has been mostly fulfilled withinexpensive primary al- the largest waste stream worldwide.[1,2] According to areport kaline andbutton cell batteries. Unfortunately,these power from the World Economic Forum,the material value of our sources are disposed of after use, sometimes even before spent electronic devices globally amountsto$62.5 billion, being completely depleted, causing significantenergy waste which is three times more than the annual output of the and environmental damage if not properly collected and recy- world’s silver mines.[3] Indeed, WEEE can be asource of highly cled.[6–9] This is reflectedinthe percentage of primary batteries valuablematerials but still it will require energy and resources that are collectedfor recycling in Europe: in 2017, approxi- to manage, collect,process, and repurpose. WEEE should be mately 226 000 tons of portable batteries and accumulators were sold in the EU-28, whereas only about 100000 tons of waste portable batteries and accumulatorswere collected for [10] [a] M. Navarro-Segarra,+ Dr.P.P.Alday,+ D. Garcia,Prof. N. SabatØ, recycling, representing approximately 45 %. For this reason, Dr.J.P.Esquivel other alternatives for sustainable energy storage are being de- Instituto de MicroelectrónicadeBarcelona, IMB-CNM(CSIC) veloped, such as redox flow batteries, fuel cells, and, more re- C/ dels Til·lerssn, Campus UAB,08193 Bellaterra, Barcelona (Spain) cently,microfluidic fuel cells.[11–13] These devices rely on the use E-mail:[email protected] of liquid fuels that are either oxidized or reduced at the device [b] Dr.O.A.Ibrahim, Prof. E. Kjeang Fuel CellResearch Lab (FCReL), SchoolofMechatronic SystemsEngineering electrodes. Very often, these power sourcesmake use of Simon FraserUniversity, V3T 0A3 Surrey,BC(Canada) oxygen reduction as cathodic species, which allows them to [c] Prof. N. SabatØ become lighter and more efficient. CatalanInstitution for Research and Advanced Studies(ICREA) Concerning fuel choices, many chemistries have been tested PasseigLluísCompanys 23, 08010 Barcelona (Spain) with promisingresults; for example, methanol,ethanol, hydro- + [ ] These authors contributed equally to this work. gen or formic acid have been widely explored, owing to their Supporting Information and the ORCID identification number(s) for the promising theoretical specific energies. However,although author(s) of this article can be found under: https://doi.org/10.1002/cssc.201903511. these fuels are seen as benign, their operation often requires This publication is part of aSpecial Issue focusing on “Organic Batteries”. preciousmetals(e.g.,Pt, Pd, Ru) as catalysts, which excludes Please visit the issue at http://doi.org/10.1002/cssc.v13.9. them as primary battery replacements. In this sense, new ap- ChemSusChem 2020, 13,2394 –2401 2394 2020 Wiley-VCH Verlag GmbH &Co. KGaA, Weinheim Full Papers ChemSusChem doi.org/10.1002/cssc.201903511 proaches have been reported,inwhich catalyst-free redox Results and Discussion chemistries, such as all-vanadium,zinc/bromide, or polysulfide/ bromide,are used as fuel in fluidic systemsthat only require Device design and operation principle inexpensive carbon material electrodes to collect the cur- rent.[14] However,these inorganic compounds involvetoxic and The device presented herein is acompact andlightweight environmentally nonfriendly elements. For this reason, organic paper-based primary battery inspired in the workingoperation active specieshave arisen as amore sustainable alternative. In of aredox flow cell. Figure 1shows apictureofaready-to-use particular, quinones are organiccompounds that have been re- prototype. The device main structure consists of two parallel cently identified as suitable candidates because they are sus- tainable, benign, abundant,and inexpensive.[15,16] The devel- oped quinone-based redox batteries have already demonstrat- ed their viability for large-scale energy storageapplica- tions.[17–19] Portable approaches for theseorganic redox flow batteries were reported by Yang et al. in 2014 and Ibrahim et al. in 2017, both of which used water-based solutions of an anthraquinone as the negative electrode and benzoquinoneas the positive one, yielding powerdensities of around 2 [20,21] 4mWcmÀ with 0.6 Vopen circuit potential. Despite good performance, the vast majority of flow cells requireexternal pumps to maintain the flow of reactants. This factincreases the device complexity andreduces its integration capacity and overall energyefficiency.[22,23] Asmart way of overcoming this drawback has been assessed for micro-scale fuel cells with ca- pillary-based microfluidics, which rely on paper and other porousmatrices for fluid transport and thus eliminate the Figure 1. Paper-based capillary flow redox primary battery. Scale bar= 1cm. need for external pumps.[24–28] Paper-based microfluidic fuel cells have already demonstrated their feasibility with well- known fuels, such as methanol, ethanol, hydrogen, or formic paper strips connected to acircular paper pad. The prototype acid.[29–33] However,asmentioned above,the need for noble is designed to start operating by immersing one of its ends in metal catalysts prevents their usability as primarypower sour- areservoir that contains two small chambers with different sol- ces. Other paper-based approaches have used glucose as fuel, utionsofelectroactive species. The paper strip ends absorb which can be scavenged with enzymaticcatalysts.[34–36] Never- the fluids contained in the chambers establishing aconvective theless, their implementation in real environments is still chal- flow of reactants by capillary force. Acarbon electrode placed lenging,asbiocatalysts have restricted stability,lack reproduci- on each of the paper channels allows the redox speciesto bility,and yield very low power outputs. Afirst validation of a react (i.e.,oxidize and reduce) and thus enable energy genera- redox battery using quinone species in apaper matrix was re- tion. Asmall segmentofpaper connects both channels, acting ported in 2017 by Esquivel et al.,[37] who showedportable as asalt bridge between the electrodes. The device keeps power generation and abiotic degradation of the whole functioning until the round pad at the end is completely filled device. The reported approachcan potentially eliminate end- up. Depending on the size, material, and design of the absorb- of-life concerns posed by currentprimary battery technologies, ent pad, the operating time of the battery can expand from a as the devices are conceived to be discarded after use without few minutes to half an hour.Moreover,the battery can easily the need for any specific recycling facilities because of their be recharged by replacing the wet absorbent pad with adry all-organic nature, causingnoharm to the environment where component and refilling the fuel reservoir with additional elec- they are disposed of. The prototype, although promising,yield- troactivespecies.The capillary-based paper battery has been ed faradaic efficiencies below 3%,owing to its diffusion-driven designedasahand-sized device. A205mmpiece of paper, operation. formingaUshape, provides the inlet channels to the solutions The work presented herein
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