Flexible aqueous Zn–S battery based on an S-decorated Ti3C2Tx cathode

ARTICLE OPEN Flexible aqueous Zn–S ba e y based on an S-deco a ed Ti 3 C 2 T x ca hode Ke al K. Soniga a 1 , Jay aj V. Vaghasiya 2 , Ca men C. Mayo ga-Ma inez 2 and Ma in Pume a 1,2,3,4 ✉ Flexible aqueous zinc-ion ba e ies can s o e ene gy sa ely and a a low cos , which benefi s wea able elec onic gadge s; howe e , cu en ly used ca hodes es ic hese de ices wi h a low specific capaci y and ene gy densi y. He ein, we de eloped a flexible zinc- sul u (Zn–S) ba e y cons uc ed by Ti 3 C 2 T x deco a ed wi h sul u (S@Ti 3 C 2 T x ) as a ca hode and Zn me al anode wi h iodine-added amphiphilic gel elec oly e (AGE). Benefi ing om he confinemen syne gy o S@Ti 3 C 2 T x ca hode, he Zn-S ba e y exhibi ed a high s o age capaci y o 772.7 mAh g −1 a 300 mA g −1 , which is highe han a con en ional S-deco a ed ca bon ca hode (491.7 mAh g −1 ). Mo e specially, he flexible de ice o e s good cycling s abili y (82.7%) and excellen mechanical s abili y wi h 91% capaci y e en ion a e 90° bending (500 cycles). To demons a e eal applica ions, he flexible Zn–S ba e ies we e in eg a ed in se ies o powe elec ical gadge s (e.g., digi al clock, ligh -emi ing diode, and obo ). I exhibi s excep ional flexibili y o sus ain di e en de o ma ions and main ains a s eady supply o powe o un he wea able elec onic gadge . These findings o e a esh s a ing poin o flexible ene gy s o age echnologies and show he p omising po en ial o he Zn–S ba e y in eal-wo ld applica ions. npj 2D Ma e ials and Applica ions (2023) 7:45 ; h ps://doi.o g/10.1038/s41699-023-00411-2 INTRODUCTION The aqueous zinc-ion ba e y (ZIB) eme ges as a sus ainable ene gy s o age de ice due o i s low-cos componen s and en i onmen al iendliness 1–4 . I is also he mos in es iga ed flexible ene gy s o age de ice due o i s sa e wea abili y. Howe e , many ZIB de ices a e cons uc ed using me al oxide-/polyme - based in e cala ion- ype ca hodes (e.g., Mn, Ni, Ti, V, and polyaniline) 5–8 , which limi s hei pe o mance due o hei low heo e ical capaci y. Recen ly, sul u (S) ca hodes eme ged as an inexpensi e al e na i e o he abo e ca hodes in ZIBs due o hei low-cos , high heo e ical con e sion capaci y, and sa e Zn–S con e sion po en ial in aqueous elec oly es 9–12 . Howe e , Zn–S ba e ies a e s ill unde pe o ming in e ms o con e sion kine ics and s abili y due o he insula ing na u e o sul u , sluggish Zn–S con e sion eac ion, and he o ma ion o byp oduc s ha esul in he loss o ac i e ma e ial 13,14 . To o e come he abo e issues, a ew a emp s ha e been epo ed o imp o e he pe o mance o sul u ca hodes by confining composi es wi h po ous ca bon 15,16 , ca bon nano ubes 17 , ca bon nanofibe s 18 , Fe(CN) 64− -doped poly- aniline 19 , S@FeN 4 single si es/ni ogen-doped ca bon 20 , and sul u in ionic liquid films 21 . Along wi h his, e o s ha e also been made wi h modifica ions in elec oly es, i.e., adding ca aly ic iodine edox addi i e 17 , mixing u ea as a co-media o 22 , sol a ion agen s a egy by using eu ec ic elec oly e 23 , and using co-sol en s like e aglyme 24 and e hylene glycol 18,25 . These e o s success ully imp o ed he e e sibili y o Zn–S con e sion wi h a educed ene gy ba ie . To make he Zn–S ba e y a e sa ile componen , mo e e o is needed o implemen e ficien ca hode confinemen wi h ad anced s a egies and solid/gel- ype elec oly es ins ead o liquid elec oly es ha could se e o de elop u u e flexible ba e ies. Recen ly, he wo-dimensional (2D) ansi ion me al ca bide (MXenes) ma e ials ha e eme ged as po en ial elec odes and conduc i e confinemen ma e ials o imp o e ca hode pe o mance in ZIBs due o hei high conduc i i y, la ge su ace a ea, and di e se su ace unc ionali ies 26,27 . The model MXene, Ti 3 C 2 T x , was ound as an e ficien bu e medium o inc ease Zn 2+ s o age in polyaniline ca hodes due o i s 2D nanoshee mo phology, which p o ides a pla o m o as di usion pa h- ways 28 . The confinemen o MXenes (e.g., Ti 3 C 2 T x and V 2 CT x ) wi h a ious me al oxide composi e ca hodes (e.g., MnO 229 ,V 2 O 530,31 , ZnMn 2 O 432 , and H 2 V 3 O 833 ) g ea ly imp o ed he in e cala ion pe o mance in ZIBs by enhanced conduc i i y and he impac o su ace g oups. Li e al. epo ed aqueous I2=I edox kine ics boos ed by MXene conduc i e confinemen o Zn-I 2 con e sion chemis y benefi ed om he confinemen e ec and as e cha ge ans e 34 . Looking a he e sa ili y o MXenes, i is possible o design an MXene-confined sul u ca hode composi e ha will enhance he Zn–S ba e y’s chemis y by p o iding conduc i e confinemen o he sul u ca hode and inc easing he ac i i y o edox addi i es like iodide– iiodide. De eloping a flexible Zn–S ba e y wi h high pe o mance. He ein, we p epa ed a flexible Zn–S ba e y using S@Ti 3 C 2 T x as ca hode and AGE as gel elec oly e. The 2D mo phology and me allic p ope y o Ti 3 C 2 T x o e conduc i e confinemen o he sul u ca hode o imp o ed Zn–S edox kine ics and quick di usion pa hs o he Zn 2+ ions. On he o he hand, he amphiphilic na u e o AGE helps o de elop obus in e aces wi h elec odes and es ic s he shu le o iodide species so hey can benefi om egula ed sel -discha ge. The as- ab ica ed Zn–S ba e y wi h S@Ti 3 C 2 T x ca hode o e s high powe capaci y, good cycling s abili y, and excellen capaci y e en ion upon mul iple bending modes. To demons a e a eal applica ion, he Zn–S ba e ies we e connec ed in se ies o powe a digi al clock, ed- 1 Fu u e Ene gy and Inno a ion Labo a o y, Cen al Eu opean Ins i u e o Technology, B no Uni e si y o Technology, B no, Czech Republic. 2 Cen e o Ad anced Func ional Nano obo s, Depa men o Ino ganic Chemis y, Facul y o Chemical Technology, Uni e si y o Chemis y and Technology P ague, P ague, Czech Republic. 3 Facul y o Elec ical Enginee ing and Compu e Science, VSB - Technical Uni e si y o Os a a, Os a a, Czech Republic. 4 Depa men o Medical Resea ch, China Medical Uni e si y Hospi al, China Medical Uni e si y, Taichung, Taiwan. ✉email: [email p o ec ed]om www.na u e.com/npj2dma e ials Published in pa ne ship wi h FCT NOVA wi h he suppo o E-MRS 1234567890():,; ligh -emi ing diode, and obo o p o ide a s eady powe supply in a ious de o ma ions. To he bes o ou knowledge, his is an exclusi e wo k o a Ti 3 C 2 T x -assis ed flexible Zn-S (aqueous) ba e y has been epo ed. RESULTS AND DISCUSSIONS Syn hesis and mo phology s udy o S@Ti 3 C 2 T x To de elop an e ficien ca hode elec ode, S@Ti 3 C 2 T x was p epa ed by liquid shea in si u sul u deco a ion o ex olia ed Ti 3 C 2 T x in he p esence o su ac an by s ong mechanical blending (Fig. 1a). Mo e de ails a e gi en in he expe imen al sec ion. This me hod a oids ene gy-consuming high- empe a u e me hods, which a e commonly used o blend S wi h hos ma e ials 15–17 . A e ha , ca bon clo h was used as a conduc i e subs a e o c ea e a flexible S@Ti 3 C 2 T x ca hode elec ode (Fig. 1b, c). Finally, a flexible aqueous Zn–S ba e y was de eloped by employing S@Ti 3 C 2 T x as a ca hode, Zn oil as an anode, and AGE as an elec oly e, which shows significan applica ions o powe a ious elec onic de ices (Fig. 1d, e). The ba e y wo ks wi h a epo ed hyb id mechanism 17,24 du ing he discha ge p ocess:Zn2þþSþI 3þ4e!ZnS þ3Iand du - ing he cha ging p ocess, ZnS þ3I!I 3þSþZn2þþ4e.He e, he p oposed highly conduc i e Ti 3 C 2 T X as ca hode composi e p o ides confinemen syne gy o ac i a e he insula ed sul u and iodine o as e and acile edox eac ions and alle ia e he conduc i e channels o Zn ion di usion. On he o he side, he e hylene oxide and p opylene oxide g oups o he AGE ma ix allow he good dissolu ion o iodine and also es ic he di usion o iodides 35,36 . Be o e examining he S@Ti 3 C 2 T x ca hode’s ole in flexible Zn–S ba e ies and hei ac ual applica ion o powe elec ical de ices, i is c ucial o fi s look a he s uc u al, mo phological, and elec ochemical p ope ies o S@Ti 3 C 2 T x com- posi e and AGE. He e, he S@Ti 3 C 2 T x composi e was cha ac e ized sys ema ically by he mog a ime ic analysis (TGA), X- ay di ac ion (XRD), scanning elec on mic oscopy (SEM), scanning ansmission elec on mic oscopy (STEM), ene gy-dispe si e X- ay spec oscopy (EDS), ansmission elec on mic oscopy (TEM), and high- esolu ion scanning ansmission elec on mic oscopy (HR-STEM) o alida e he successi e composi ion p epa a ion. The SEM image o p is ine Ti 3 C 2 T x in Fig. 2a shows an o de ed a angemen o 2D nanoshee s ack clus e s wi h a size o ~5–6 µm leng h and a isible gap be ween he shee s. The EDS elemen a y mapping (Supplemen a y Fig. 1) o hese nanoshee s acks confi ms he p esence o elemen s Ti, C, F, and O. Fu he , solu ion-shea ed Ti 3 C 2 T x was analyzed by STEM and ound o con ain well-dispe sed Ti 3 C 2 T x nanoshee s (Fig. 2b) simila in size o he s acks. TEM and HR-TEM images (Fig. 2c, d) o ew-laye nanoshee s show good c ys allini y as confi med by selec ed a ea elec on di ac ion (SAED, inse o Fig. 2d), indica ing nea spli s in he Ti 3 C 2 T x s acks du ing solu ion shea ing. The STEM image and co esponding EDS elemen a y mapping o shea ed S@Ti 3 C 2 T X a e p esen ed in Fig. 2e. We can see clea ly ha S is e enly a ached o he su ace o he Ti 3 C 2 T x nanoshee s, c ea ing a uni o m S@Ti 3 C 2 T x laye s uc u e. The EDS mappings alida ed he p esence o S, Ti, and C dis ibu ion. TGA analysis conduc ed unde a ni ogen a mosphe e es i- ma ed he sul u p opo ion o ~60 w % in he composi e p epa ed using he solu ion shea ing me hod (Supplemen a y Fig. 2). XRD was used o examine he c ys alline p ope ies o S@Ti 3 C 2 T x composi es (Supplemen a y Fig. 3). The XRD pa e n o Ti 3 C 2 T X indica es he b oad di ac ion peak a 2θ=~8° (002), ep esen ing he e ficien spli s o nanoshee s h ough he shea ing me hod 28 . In he composi e samples, Ti 3 C 2 T x peaks eme ge in s ong peaks o S and he ep esen a i e peak o Ti 3 C 2 T x , s ill isible below 2θ=8°, indica es a la ge dis ance be ween he Ti 3 C 2 T x nanoshee s by e ec i e in si u S deco a ion. S@Ti3C2Tx ca hode Zinc Anode Amphiphilic Gel Elec oly e Sul u Ti3C2Tx Zn2+ = Ti = C= O, OH, F Polyme Iodides abc d e Fig. 1 Schema ic illus a ion o p epa ing flexible Zn-S ba e y ca hode based on S@Ti 3 C 2 T x o powe ing a down-scaled obo . aSyn hesis o S@Ti 3 C 2 T x by solu ion shea -assis ed me hod. bMolecula schema ic o S@Ti 3 C 2 T x composi e. cDeposi ion on ca bon clo h. dFlexible Zn–S ba e y wi h S@Ti 3 C 2 T x ca hode, Zn anode, and amphiphilic gel elec oly e-in used cellulose as a sepa a o . eDown-scaled obo powe ed by he p oduced wea able Zn–S ba e y. K.K. Soniga a e al. 2 npj 2D Ma e ials and Applica ions (2023) 45 Published in pa ne ship wi h FCT NOVA wi h he suppo o E-MRS 1234567890():,; XRD s udy sugges s an e ec i e physical blending o Ti 3 C 2 T x wi h S wi hou oxida ion o chemical eac ions. The quali y and ex en o he S@Ti 3 C 2 T x can be s udied om he su ace a ea o he ma e ials. BET analysis o Ti 3 C 2 T x and S@Ti 3 C 2 T x was ca ied ou o s udy he specific su ace a ea, which is an impo an pa ame e o he quali y o elec odes. The adso p ion–deso p ion iso he m o bo h ma e ials is p o ided in Supplemen a y Fig. 4. I is no iced ha he su ace a ea o Ti 3 C 2 T x was 17.34 m 2 g −1 , which dec eased when blended wi h S (10.04 m 2 g −1 ), hus confi ming he compac physical mo phology o he ca hode’s composi ion 37 . This can be beneficial o be e di usion o Zn ions by imp o ed conduc i i y in he p esence o Ti 3 C 2 T x and good adso p ion o iodides du ing cha ge–discha ge. Elec ochemical s o age s udy o S@Ti 3 C 2 T x When imp o ing he elec ochemical s o age capabili ies o p epa ed S@Ti 3 C 2 T x ca hodes wi h an aqueous sys em, he selec ion o he cu en collec o and elec oly e is e y impo an . In he p esen case, we ha e adop ed hyd ophobic ca bon clo h as a cu en collec o due o he non-pola p ope ies o elemen al sul u . The elec oly e de eloped he e wi h zinc ace a e, iodine, and he block copolyme is amphiphilic and possesses a sol–gel- ype na u e o ensu e good in e acial con ac o ma ion (Supplemen a y Fig. 5a); his is inspi ed by polyme hyd ogel elec oly e om plu onic polyme , which p o ed excellen o ZIBs 38 . To confi m he in e acial compa ibili y o he ca hode, we compa ed he op ical obse a ion o a d op o liquid elec oly e on op o ca bon clo h coa ed wi h p is ine Ti 3 C 2 T x and S@Ti 3 C 2 T x . The elec ode su ace o S@Ti 3 C 2 T x composi ion becomes highly hyd ophobic compa ed o he o me and seems incon enien o he sys em (Supplemen a y Fig. 5b). The issue is sol ed by he compac in e ace c ea ed due o he AGE elec oly e’s amphi- philic and he mo- e e sible p ope ies, which allows i o be well- we ed on he S@Ti 3 C 2 T x ca hode in he sol phase be o e u ning in o a gel (Supplemen a y Fig. 5b). AGE is also esponsible o he acile dissolu ion o iodine due o he p esence o polyme in he ma ix; hence, i helps o m a acile I − /I 3 − edox couple. Supplemen a y Figu e 6 shows he na u e o iodine dissolu ion in compa ison o elec oly es wi h and wi hou polyme and e eals a clea solu ion wi h polyme by as e dissolu ion. The AGE main ains good ionic conduc i i y o 4.01 S cm −1 (Supple- men a y Fig. 7 and supplemen a y equa ion 1) and shows a zinc- ion ans e ence numbe o 0.45 measu ed om DC pola iza ion be ween zinc-blocking elec odes (Supplemen a y Fig. 8 and supplemen a y equa ion 2). The zinc s ipping–pla ing cycles o AGE conduc ed be ween symme ical zinc elec odes esul in a s abilized ol age p ofile o 100 cycles, indica ing he good elec ochemical sui abili y o AGE (Supplemen a y Fig. 9). No ably, AGE also shows a wide elec ochemical ope a ional ol age window up o 2.0 V s. Zn sui able o sa e aqueous sys ems (Supplemen a y Figu e 10). Fu he , he gel p ope y o AGE also benefi s he flexibili y o he de ice 39 . To e alua e he elec ochemical pe o mance o S@Ti 3 C 2 T x and S@C (S confined wi h ca bon nanopowde ) ca hodes, h ee- elec ode cyclic ol amme y (CV) was conduc ed in he I=I 3 solu ion (Supplemen a y Fig. 11). I is obse ed ha bo h S ca hodes show e e sible edox peaks o I=I 3, simila ly e e enced o glassy ca bon elec odes. Besides, educed cu en densi y was obse ed on bo h ca hodes due o he p esence o insula ing S. Howe e , S@Ti 3 C 2 T x shows a highe elec ochemical esponse wi h low pola iza ion compa ed o S@C, which indica es he supe io conduc i i y and su ace o S@Ti 3 C 2 T x .Fu he ,Zn–S ba e ies we e ab ica ed in CR2032 coin cells wi h he configu a ion o Zn/AGE- cellulose sepa a o /S@Ti 3 C 2 T x -ca bon clo h. The ab ica ed de ice builds up a s able open ci cui po en ial (OCP) o 1.068 ± 0.010 V s. Zn/Zn 2+ , sligh ly de ia ing om he heo e ical OCP o he Zn–S sys em explained elsewhe e (1.044 V s. Zn 2+ /Zn) 23 . This de ia ion may be assigned o he composi e con ibu ion o a modified ca hode and elec oly e sys em. Figu e 3a shows he CV scans o he ca hodes S@Ti 3 C 2 T x and S@C be ween 0.05 and 1.6 V a 0.1 mV s −1 scan speed, e ealing a ba e y- ype quasi- e e sible cha ac e is ic. The ca hodic peak eco ded a 0.5 V s. Zn/Zn 2+ belongs o he ZnS o ma ion and he anodic peak a 1.47 V s. Zn/Zn 2+ is o he e o ma ion o sul u om ZnS in aqueous elec ochemis y 19,24 .The edox peaks o S@Ti 3 C 2 T x a e sha p and include a la ge s o age a ea compa ed o b oad and educed S@C peaks, indica ing he supe io confinemen e ec and as e zinc con e sion s o age. Figu e 3b illus a es he gal anos a ic cha ging–discha ging (GCD) ol age p ofile o bo h elec odes wi h simila ol age ange a a cu en densi y o 300 mA g −1 . The S@Ti 3 C 2 T x deli e ed highe Zn s o age and an imp o ed elec ochemical p ofile wi h a lowe pola iza ion ol age window compa ed o he ca bon sca old. The deli e ed specific capaci y o S@Ti 3 C 2 T x is 772.7 mAh g −1 , which is highe han he con en ional S@C ca hode (491.7 mAh g −1 ). He e, Ti 3 C 2 T x could p o ide a be e -conduc ing en i onmen and Zn ion anspo flux ha leads he enhanced s o age pe o mance. The capaci y o he S@Ti 3 C 2 T x /AGE-based de ice is imp o ed compa ed o a ailable epo s o gel-based Zn-S ba e y as lis ed in Fig. 3h 18,19,21 and also eaches an imp essi e ene gy densi y o 363.16 Wh kg −1 , which is abo e he epo ed solid-s a e ZIBs 38–43 . Supplemen a y Figu e 12 enlis s he capaci y o a ious epo ed MXene-suppo ed ca hodes o he ZIBs 28–34,40–43 as S@Ti 3 C 2 T x ca hodes b eak he specific capaci y limi a ion o such ca hodes. 5 µm 5 µm 200 nm 1 µm 1 µm 1 µm 1 µm TiSC abc e d 100 nm Fig. 2 Mo phology s udy. a SEM image o p is ine Ti 3 C 2 T X. bSTEM image o shea ed Ti 3 C 2 T X nanoshee . cTEM image o Ti 3 C 2 T X nanoshee . dHR-TEM image o Ti 3 C 2 T X nanoshee (inse ep esen s SAED pa e n). eSTEM o shea ed S@Ti 3 C 2 T X and co esponding EDS elemen a y mapping. K.K. Soniga a e al. 3 Published in pa ne ship wi h FCT NOVA wi h he suppo o E-MRS npj 2D Ma e ials and Applica ions (2023) 45 This indica es ha he combina ion o S and MXene can be a p omising high-capaci y ca hode compa ed o o he combina- ions wi h MXenes. To unde s and he edox kine ics in hese wo di e en en i onmen s, he cha ge ans e and ion di usion in he elec ode a e s udied using elec ochemical impedance spec o- scopy (EIS). The ob ained Nyquis plo s om EIS a e shown in Fig. 3c and he inse is he Randles equi alen ci cui used o ex ac he esis ance pa ame e s 44 . The S@Ti 3 C 2 T x ca hode elec ode shows low bulk esis ance (R s =11.12 Ω) and cha ge ans e esis ance (R c =16.83 Ω), whe eas he S@C elec ode shows R s =14.77 Ωand R c =45.47 Ω, indica ing a good conduc- i e pla o m and as e cha ge ans e in MXene confinemen . The kine ics o Zn 2+ ions in he elec ode ma ix can be es ima ed by he Wa bu g ac o , which is ob ained om he ela ionship o Z eal and he low- equency egion o he EIS spec um eflec ed as a s aigh line 44 . Figu e 3d illus a es he ela ionship be ween Z eal and he low- equency egion o he EIS spec um, and he slope o his g aph is he Wa bu g ac o based on supplemen a y equa ions (3) and (4) in he Supplemen a y In o ma ion, and i is in e sely p opo ional o he di usion. The lowe alue o he Wa bu g ac o o S@Ti 3 C 2 T x (σ=5.69) sugges s as e di usion kine ics o Zn 2+ ions due o acile confinemen suppo o a 2D mo phology belonging o la ge mic o-size Ti 3 C 2 T x (3.40 ± 1.2 µm). The S@C ealizes a high Wa bu g ac o (σ=6.42), meaning a slowe di usion ha may be ela ed o he small pa icle size o he ca bon (0.72 ± 0.2 µm) su ounded wi h ine sul u 45 . Fu he , he S@Ti 3 C 2 T x de ice was cycled a highe a es o 500, 700, and 1000 mA g −1 and s ill deli e ed a capaci y o 344, 263, and 187 mAh g −1 , espec i ely, while e aining coulombic e ficiency abo e 90% (Fig. 3e). The pola iza ion ol age inc eased significan ly a he high cu en a e ha may be ela ed o ising in esis ance con ibu ion. The a e capabili y was analyzed o 50 cycles by applying an inc emen al a e o 300 o 1000 mA g −1 ollowed by a e u n o 300 mAh g −1 (Fig. 3 ). De ice capaci y declined o 137.2 mAh g −1 a 1000 mA g −1 and e u ned o he same pe o - mance a he ini ial a e, indica ing acile and well-con olled ene gy s o age. Fu he , he de ice shows s able pe o mance o 300 cycles and e ained capaci y e en ion o 92.8% excep o a ew ini ial cycles (Fig. 3g). The ade in capaci y obse ed he e is o en associa ed wi h he loss o ac i e sul u in aqueous media due o he o ma ion o sul a e byp oduc s a he ca hode su ace (2ZnS þ4H2Oþ10e!2Zn2þþSO2 4þSþ8Hþ) 20,22,24 .The XPS spec a o he p is ine and cycled ca hode confi m he p esence o sul a e and zinc in he ca hode as e idenced by byp oduc s on he cycled ca hode (Supplemen a y Fig. 13). The highe ac i e ma e ial-loaded de ices we e ab ica ed o explo e he possibili y o scaling o he Zn–S ba e y. I can also deli e a capaci y o 522 mAh g −1 and 400 mAh g −1 o loading o 3.0 and 5.0 mg cm −2 , espec i ely (Supplemen a y Fig. 14). I was ound ha he capaci y is linea ill 1.5 mg cm −2 , bu shows significan decay in capaci y a loading abo e 2 mg cm −2 due o possible inc eased in e nal esis ance and a longe di usion pa hway 46 (Supplemen a y Fig. 15). I should be no ed ha de ice pe o mance is also capaci i ely con ibu ed by Ti 3 C 2 T x , conduc i e ca bon, and ca bon clo h. Fo he compa ison, he de ice wi h Ti 3 C 2 T x as a ca hode elec ode was ab ica ed and es ed simila ly on he abo e de ices. A a 300 mA g −1 a e, he Ti 3 C 2 T x can deli e a capaci y o 65.2 mAh g −1 (Supplemen a y Fig. 16). Fo he sake o compa ison, he de ice was also p epa ed wi h a liquid elec oly e wi h modifica ion in polyme con en . The Zn–S ba e y wi h 5 w % polyme con en elec oly e exhibi s a discha ge capaci y o 1016 mA g −1 a 300 mA g −1 , wi h supe io ac i a ion compa ed o Fig. 3 Elec ochemical s udy o S@Ti 3 C 2 T x ca hodes in Zn-S ba e y. a CV o S@Ti 3 C 2 T x and S@C elec ode a a scan a e o 0.1 mV s −1 and bGCD cu es a 300 mA g −1 .c,dNyquis plo s o S@Ti 3 C 2 T x and S@C, and co esponding cha ac e is ic o Z eal o high- equency ela ionship. e, GCD cu es o S@Ti 3 C 2 T x a di e en a es and a e capabili y. gS abili y measu emen o S@Ti 3 C 2 T x a 500 mA g −1 o 300 cycles. hCompa ison o he specific capaci y pe o mance o S@Ti 3 C 2 T x a 300 mA g −1 wi h epo ed Zn–S ba e ies wi h gel elec oly es. K.K. Soniga a e al. 4 npj 2D Ma e ials and Applica ions (2023) 45 Published in pa ne ship wi h FCT NOVA wi h he suppo o E-MRS AGE due o high conduc i i y (Supplemen a y Fig. 17). Howe e , liquid elec oly e su e s om issues ela ed o di ficul sealing and leakage p oblems, and may no be sui able o a obus flexible de ice. In es iga ion o zinc-ion s o age in S@Ti 3 C 2 T x To in es iga e he cha ge–discha ge mechanism o Zn s o age, an ex si u spec oscopy s udy was adop ed o iden i y he chemical s o age con e sion in he S@Ti 3 C 2 T x ca hode by XRD, Raman, and FT-IR (Fou ie - ans o m in a ed) echniques. Figu e 4a shows he ypical cha ge–discha ge ol age p ofile o a Zn-S ba e y wi h selec ed ol age poin s o ace he S o ZnS ans o ma ion and ice e sa by XRD. The co esponding eco ded X- ay di ac ion pa e ns a e p o ided in Fig. 4b. The ep esen a i e XRD peak o S can be iden ified a 2θ=23° on he ca bon clo h, whe e he b oad cha ac e is ic a 2θ=20–30° a ises om he ca bon clo h subs a e as compa ed in he s udy. Fi s , he discha ge analysis is ooled a a discha ge ol age o 0.4, 0.2, and 0.05 V, whe e he S peak is con inuously dec eased while he new peaks ha a ise a 28°, 48°, and 56° belong o ZnS o ma ion. This obse a ion is in good ag eemen wi h p e iously epo ed Zn–S sys ems 19,23 . F om 0.4 V o 0.2 V, ZnS o ma ion s a s and a 0.05 V he peaks a e mo e in ensely isible. While in cha ging mode om 1.3 V o 1.6 V, he ZnS peaks nea ly disappea wi h he e o ma ion o he sul u peak. He e, he sul u peak is no in ense as i was in beginning, which could be ela ed o sul u loss du ing he side eac ion and sul a e o ma ion obse ed in he XPS s udy. This ac also co ela es wi h he ep esen a i e b oad peak o Ti 3 C 2 T x nanoshee composi ion in he ca hode, which is isible in he discha ged s a e bu is also isible in a ully cha ged s a e a 1.6 V. These changes a e also obse ed in Raman spec oscopy whe e he ini ial abso p ion cha ac e is ic o he ca hode being consumed in he discha ge s a e and e o med again in he cha ge s a e belongs o he consump ion and e o ma ion o S (Supplemen a y Fig. 18). The FT-IR spec a p o ided in Fig. 4c show he p ofiles o subsequen ini ial discha ge, cha ge, and second discha ge, which alida e he e e sible cha ge–discha ge cha ac e is ics om he iden ified peaks o ZnS (1624, 1376, and 1103 cm −1 ) 19,47 . Those peaks a e o med du ing he fi s discha ge, pa ially disappea du ing cha ging, and hen e o m again du ing he second cha ge. STEM and EDS analyses we e pe o med o his cycled elec ode o obse e he dis ibu ion o discha ged p oduc s and composi ions. Figu e 4d p esen s a STEM image o he discha ged p oduc o cycled ca hode and co esponding EDS elemen al mapping o a simila a ea iden ifies he dis ibu ion o Ti, Zn, and S elemen s. I can be no ed ha he scanning o he Zn elemen is iden ical o he S elemen scanning. This is e iden and suppo s he p e ious obse a ion o sul u consump ion and ZnS o ma ion obse ed in spec oscopic me hods. Usually, Zn–S aqueous ene gy s o age is benefi ed om sulfide shu le- ee elec ochemis y compa ed o he Zn–MnO 2 sys em 23 , bu he use o addi i es like I=I 3in elec oly es may impac he ba e y wi h iodide di usion and leads o sel -discha ge. Howe e , he p esen Zn–S ba e y ealizes 98.1% capaci y e en ion a e es ing 27 h sel -discha ge es by con olling e y well he di usion, which may be by he combined e ec o AGE and Ti 3 C 2 T x (Supplemen a y Fig. 19). To unde s and he ole o AGE and Ti 3 C 2 T x on he con olling sel -di usion o iodide, liquid-s a e Zn–S ba e ies o S@Ti 3 C 2 T x and S@C a e p epa ed wi h liquid elec oly e and s udied he sel -di usion in de ices a e he cha ging o 1.6 V (Supplemen a y Fig. 20a, b). The obse ed capaci y e en ion o bo h ca hodes is 86.01% and 90.23% o S@C and S@Ti 3 C 2 T x , espec i ely, which is qui e a bi lowe han AGE-based de ices. The lowe decay obse ed in he S@Ti 3 C 2 T x sugges s pola su aces can play an impo an ole in holding he iodides simila ly obse ed in Zn–I 2 and Li–S ba e ies 34,48 .To isualize he di usion phenomena, a liquid elec oly e-based beake cell and an AGE-based la e al de ice we e ab ica ed on a glass subs a e, and biased cons an a 1.6 V o moni o he iodide o ma ion and di usion. Supplemen a y Fig. 21 shows he g adual o ma ion o iodides ha la e on di used h ough he elec oly e and a eled o he Zn oil. In he case o AGE-based de ice, iodide colo change was only ealized a he in e ace o he elec ode and AGE (Supplemen a y Fig. 22). The mic o-le el pho og aph can isualize he colo o ma ion e y clea ly, which is in a e y sho ange. Fu he , he compa ibili y o Zn me al was compa ed wi h AGE and liquid-based elec oly es o he S@Ti 3 C 2 T x ca hode o iden i y he ole o AGE in s abilizing he Zn anode. Zn anode mo phology was analyzed by SEM a he ini ial and hen cycled in Fig. 4 Ex si u cha ac e iza ion o cha ged and discha ged sul u ca hode. a,bGCD and ol age poin s o XRD measu ed du ing one cycle. cFT-IR spec oscopy o wo cycles. dSTEM and co esponding EDS elemen al analysis o he discha ged S@Ti 3 C 2 T x ca hode. K.K. Soniga a e al. 5 Published in pa ne ship wi h FCT NOVA wi h he suppo o E-MRS npj 2D Ma e ials and Applica ions (2023) 45 bo h elec oly es (Supplemen a y Fig. 23). The Zn anode in AGE shows a uni o m su ace a he ini ial s a e ha becomes laye ed a e long- e m cycling due o Zn s ipping and pla ing e en s. This indica es ha he elec oly e is much mo e sui able wi h a Zn anode. In he case o liquid elec oly es, he SEM image o Zn was obse ed wi h une enly g own solid clus e s on he su ace. This obse a ion sugges s ha he AGE and Ti 3 C 2 T x e ec i ely con ibu e o ad ancing he Zn-S ba e y. Flexible Zn–S ba e y and applica ions To e alua e he flexibili y o his de ice, he ab ica ion o a Zn–S flexible ba e y was p epa ed by a aching Zn oil o he flexible plas ic subs a e o p o ide a flexible backbone. Figu e 5a shows he a e capabili y o flexible Zn–S ba e y a di e en cu en densi ies anging om 500 mA g −1 o 2000 mA g −1 . The capaci y dec eases wi h inc easing cu en densi y, eaching up o 325 mA g −1 a a slow a e and 137 mA g −1 a a as e a e. The flexible ba e y shows he ideal cha ge–discha ge edox p ofile obse ed in he model coin cell de ice (Fig. 3e). Du ing he long- e m s abili y a 700 mA g −1 , i akes nea ly 20 cycles o achie e s able pe o mance and hen e ains 82.7% capaci y wi h a e age coulombic e ficiency o 98.3% (Fig. 5b). The as e cu en a e along wi h scaled elec odes makes an impac on deg ada ion in capaci y belonging o possible enhanced side eac ions and cha ge losses. The pe o mance and s abili y o he flexible Zn–S ba e y a e qui e supe io and compa able o ha epo ed o flexible solid-s a e ZIBs wi h me al oxide ca hodes and sul u ca hodes (Supplemen a y Tables 1 and 2). Flexibili y analysis was pe o med by cycling he ba e y de ice a 90° and 180° bending condi ions wi h a 500 mA g −1 a e whe e capaci y pe o mance was e ained a 81% and 72%, espec i ely, compa ed o he fla de ice (Fig. 5c). Figu e 5d illus a es he demons a ion o he p ac icali y o a flexible de ice wi h fla , ben in an upwa d and down di ec ions, and wis ed while powe ing a digi al clock wi h i (Supplemen a y Mo ie 1). The de ice an undis u bed du ing he ope a ion, which sugges s he compac - ness o he elec odes/elec oly e in e aces. To alida e flexibili y in e ms o ene gy s o age pe o mance, he de ice was e alua ed by moni o ing he OCP and specific capaci y a 90° o 500 bending cycles (Fig. 5e, ). I e ains i s OCP e y well wi h s able Fig. 5 Flexible Zn-S ba e y and eal-wo ld applica ions. a Cha ge–discha ge p ofile o flexible Zn–S ba e y a di e en a es. bS abili y p ofile o he flexible Zn–S ba e y. cSpecific capaci y o he flexible Zn–S ba e y a fla , 90°, and 180° bending. dPowe ing o a digi al clock upon di e en bending ope a ion o flexible Zn–S ba e y. e–hFlexibili y analysis o de ices a long- e m bending cycles in e ms o OCP and capaci y e en ion. iDischa ge p ofile o se ies-connec ed flexible Zn–S ba e ies. jDigi al pho og aphs showing he ol age o se ies- connec ed flexible Zn–S ba e y. Real-wo ld applica ions o flexible Zn-S ba e y. kPowe ing o LED gadge wi h flexible Zn–S ba e y module. lDC mo o -ope a ed oy obo powe ed wi h Zn-S ba e y module. K.K. Soniga a e al. 6 npj 2D Ma e ials and Applica ions (2023) 45 Published in pa ne ship wi h FCT NOVA wi h he suppo o E-MRS capaci y measu ed a e e y 100 in e als and finally eaches 91% capaci y e en ion. Fu he , he de ice was subjec ed o ex eme 180° bending o mo e han 300 cycles and s ill achie ed 86% capaci y e en ion (Fig. 5g, h). O e all, he de ice demons a ed good flexibili y and elec ochemical pe o mance. The de eloped flexible Zn–S ba e y has he po en ial o wea able applica ions and o un elec onic gadge s due o i s high capaci y and flexibili y. Owing o good ene gy densi y, he discha ge ol age o his ba e y ealizes deli e ing powe a a e y low ol age, which may limi he applicabili y. To enable i o p ac ical applica ion, we in es iga ed a Zn–S ba e y module p epa ed by se ies connec ion o cells o achie e highe ou pu ol age. The p epa ed module possesses good flexibili y as demons a ed (Supplemen a y Fig. 24). Se ies-connec ed de ices discha ge cu es and co esponding OCP a e p o ided in Fig. 5i, j. In compa ison o a single de ice wi h a wo king ol age o 1.065 V, he wo and h ee de ices connec ed in se ies exhibi 2.1 V and 3.2 V, espec i ely, wi h simila discha ge imes. The discha ge ol age p ofile also showed pe iodic enhancemen in he ol age, mainly imp o ed ini ially, which could be help ul o igge high- ol age gadge s. Howe e , he quick ol age decay a e ini ial gain may a ibu e o he inc eased ex e nal esis ance o module de ices. Fo he demons a ion, a wea able w is bel o wo se ies-connec ed Zn–S ba e ies was p epa ed o success ully illumina e a ed-colo ed LED indica o and powe i o o e 5 min (Fig. 5k). Nowadays, au omo i e obo ics un on DC mo o s powe ed by igid li hium-ion ba e ies ha limi po abili y and p esen sa e y and cos issues. He e, o demons a ion and o highligh he po en ial o a flexible Zn–S ba e y wi h low-cos componen s, we powe ed a oy obo equipped wi h a 1.5 V DC mo o . The flexible Zn–S ba e y module designed he e can powe and un he oy obo o 30–60 s wi h wo de ices (Fig. 5l and Supplemen a y Mo ie 2). This demons a ion applica ion p o es ha sys ema ic la ge-scale module design and de elopmen could e ficien ly sol e he powe ing o obo ics wi h his low-cos , flexible Zn–S ba e y. In his wo k, Ti 3 C 2 T x was deco a ed wi h S o use as ca hode along wi h AGE o imp o e he pe o mance o flexible Zn-S ba e ies. Illus a ions o wo composi ions o S@Ti 3 C 2 T x and S@C elucida e he impac o Ti 3 C 2 T x in Zn–S edox imp o emen whe e i plays an impo an ole o inc ease he edox kine ics, con olling soluble iodide shu ling by pola su ace and p o iding a backbone o as e Zn 2+ di usion channels. I is concluded ha he AGE coupled wi h S@Ti 3 C 2 T x ca hode enables con ol o sel - discha ge and also p o ec s he Zn anode agains co osion. The de ice o he S@Ti 3 C 2 T x ca hode pe o ms wi h a high ene gy densi y o 363.16 Wh kg −1 , which is imp essi e compa ed o me al oxide-based in e cala ion ca hodes popula o ZIBs. The flexibili y and bending s udy showed good pe o mance a e many de o ma ions wi hou significan de e io a ion o capaci y. Fo he fi s ime, s a egic eal-scale applica ions o he flexible and wea able Zn–S ba e y modules a e demons a ed o un an LED display and powe a mo o ized ab ica ed down-scale obo by connec ing Zn–S ba e ies in se ies. This case s udy and wo k ep esen a low-cos op ion o u u e wea able de ices and also a g een sou ce o ene gy o au omo i e obo ics. METHODS P epa a ion o S@Ti 3 C 2 T x composi es S@Ti 3 C 2 Tx composi e (60 w % S) was p epa ed by in si u solu ion- shea ed me hod by modifica ion in he p e iously epo ed me hod 49 . Fi s , su ac an solu ion was p epa ed in mixed sol en me hanol (40 %) and chlo o o m (60 %) by adding su ac an sodium chola e (2 mg/mL). Acco ding o he equi emen o S and Ti 3 C 2 T x composi ion, he weigh o bo h componen s in w /w % was added o he su ac an solu ion whe e he concen a ion o Ti 3 C 2 T x was kep a 3 mg/mL. The esul an solu ion was shea ed a 15,000 pm o 45 min (15 min, 3 imes a 10-min in e als) in an ice ba h wi h a s ainless s eel blade s i e om IKA. The blended solu ion was hen aken o sol en e apo a ion unde s i ing a 50 °C. The d ied mass was pou ed in o he me hanol and washed h ee imes o emo e sodium chola e om he composi e ollowed by d ying o 12 h a 60 °C. The d ied mass con ains he p opo ional composi ion weigh added o he solu ion. A simila p ocedu e was used o p epa e he S@C ( ~ 60 w % S) sample by eplacing ca bon powde wi h Ti 3 C 2 T x . P epa a ion o amphiphilic gel elec oly e (AGE) Amphiphilic gel elec oly e was p epa ed by ollowing ou p e ious me hod 33 . 1 M aqueous zinc ace a e solu ion was p epa ed wi h 0.20 w % iodine addi i e and mixed wi h 30 w % (w/w) P123 plu onic block-copolyme 37,38 . B iefly, he polyme was allowed o dissol e in solu ion o 3 h ollowed by gen le mixing wi h a spa ula. Fu he , he gel was subjec ed o h ee cooling–hea ing cycles (0 °C/25 °C) o sol-gel ansi ions o achie e a uni o m gel phase elec oly e. Fo he ba e y applica ion, a cellulose sepa a o was in used in he sol s a e o achie e a uni o mly coa ed sepa a o a oom empe a u e in he gel s a e. Fab ica ion o elec odes and ba e y The ca hode was p epa ed on ca bon clo h using a slu y coa ing me hod. A fi s , as-p epa ed ac i e ma e ial (80 w %) and ca bon black (10 w %) we e mixed well in a mo a o 30 min, and hen he slu y was p epa ed in NMP wi h PVDF (10 w %) o a u he 30 min o mixing. The homogenized slu y was doc o -bladed on he ca bon clo h and d ied a 70 °C o 24 h. The d ied elec ode was hen uni o mly p essed well and cu in o a 1 cm 2 -sized piece. The ac i e S loading o elec odes a ied om 0.8 o 1.0 mg cm −2 o low loading, 3.0 o 5.0 mg cm −2 o high loading, and 1.0 o 1.5 mg cm −2 o he flexible ba e y and modules. The Zn oil was used as an anode and polished o emo e he oxide laye . The ba e y cell was ab ica ed in 2032 coin cells whe ein he fi s - placed Zn oil was ollowed by a d op o sol-phase elec oly e and elec oly e-in used sepa a o . Finally, he ca hode was placed on op o he sepa a o and he de ice was sealed. Fu he , wo cooling–hea ing cycles (0 °C/25 °C) we e applied o achie e enough pene a ion o elec oly e and uni o m in e aces. In he flexible de ice ab ica ion elec odes we e scaled o 3 cm 2 .An anode was s uck on he flexible PET subs a e ollowed by he placemen o he gel-in used sepa a o s and ca hode. The sandwich assembly was sealed wi h glue ape wi h h ee laye s o make i leak-p oo . The de ice was allowed o s abilize o 12 h be o e obse ing measu emen s. 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We acknowledge P o . Ma in T unec, CEITEC BUT o he mog a ime ic analysis. AUTHOR CONTRIBUTIONS K.K.S.: ma e ial p epa a ion, de ice ab ica ion, elec ochemis y, da a analysis o BET, XRD, TEM, and Raman (measu ed a UCT cen al acili y), XPS measu emen and analysis (CEITEC Nano), and w i ing he o iginal d a ; J.V.V.: SEM and EDS measu emen s, gadge esou ces, and w i ing o iginal d a ; C.C.M.-M.: concep ualiza- ion, supe ision, and e ised o iginal d a ; M.P.: financial suppo , me hodology, supe ision, ini ia ed and o e saw he p ojec . All au ho s con ibu ed o w i ing he manusc ip . COMPETING INTERESTS The au ho s decla e no compe ing in e es s. ADDITIONAL INFORMATION Supplemen a y in o ma ion The online e sion con ains supplemen a y ma e ial a ailable a h ps://doi.o g/10.1038/s41699-023-00411-2. Co espondence and eques s o ma e ials should be add essed o Ma in Pume a. Rep in s and pe mission in o ma ion is a ailable a h p://www.na u e.com/ ep in s K.K. Soniga a e al. 8 npj 2D Ma e ials and Applica ions (2023) 45 Published in pa ne ship wi h FCT NOVA wi h he suppo o E-MRS Publishe ’s no e Sp inge Na u e emains neu al wi h ega d o ju isdic ional claims in published maps and ins i u ional a filia ions. Open Access This a icle is licensed unde a C ea i e Commons A ibu ion 4.0 In e na ional License, which pe mi s use, sha ing, adap a ion, dis ibu ion and ep oduc ion in any medium o o ma , as long as you gi e app op ia e c edi o he o iginal au ho (s) and he sou ce, p o ide a link o he C ea i e Commons license, and indica e i changes we e made. The images o o he hi d pa y ma e ial in his a icle a e included in he a icle’s C ea i e Commons license, unless indica ed o he wise in a c edi line o he ma e ial. I ma e ial is no included in he a icle’s C ea i e Commons license and you in ended use is no pe mi ed by s a u o y egula ion o exceeds he pe mi ed use, you will need o ob ain pe mission di ec ly om he copy igh holde . To iew a copy o his license, isi h p:// c ea i ecommons.o g/licenses/by/4.0/. © The Au ho (s) 2023 K.K. Soniga a e al. 9 Published in pa ne ship wi h FCT NOVA wi h he suppo o E-MRS npj 2D Ma e ials and Applica ions (2023) 45