Kev muab cov peev txheej hluav taws xob uas ruaj khov yog ib qho ntawm cov teeb meem tseem ceeb tshaj plaws ntawm lub xyoo pua no. Cov chaw tshawb fawb hauv cov ntaub ntawv sau qoob loo los ntawm qhov kev txhawb siab no, suav nrog thermoelectric1, photovoltaic2 thiab thermophotovoltaics3. Txawm hais tias peb tsis muaj cov ntaub ntawv thiab cov khoom siv uas muaj peev xwm sau qoob loo hauv Joule ntau yam, cov ntaub ntawv pyroelectric uas tuaj yeem hloov lub zog hluav taws xob mus rau hauv kev hloov pauv kub tsis tu ncua yog suav tias yog sensors4 thiab energy harvesters5,6,7. Ntawm no peb tau tsim lub macroscopic thermal energy harvester hauv daim ntawv ntawm lub capacitor multilayer ua los ntawm 42 grams ntawm lead scandium tantalate, tsim 11.2 J ntawm lub zog hluav taws xob ib lub voj voog thermodynamic. Txhua lub pyroelectric module tuaj yeem tsim lub zog hluav taws xob ceev txog li 4.43 J cm-3 ib lub voj voog. Peb kuj qhia tau tias ob lub modules zoo li no hnyav 0.3 g yog txaus los txuas ntxiv lub zog autonomous energy harvesters nrog embedded microcontrollers thiab kub sensors. Thaum kawg, peb qhia tau tias rau qhov kub thiab txias ntawm 10 K, cov multilayer capacitors no tuaj yeem ncav cuag 40% Carnot efficiency. Cov khoom no yog vim (1) kev hloov pauv theem ferroelectric rau kev ua haujlwm zoo, (2) cov hluav taws xob xau qis kom tiv thaiv kev poob, thiab (3) qhov hluav taws xob tawg siab. Cov macroscopic, scalable thiab ua haujlwm tau zoo pyroelectric fais fab harvesters no rov xav txog kev tsim hluav taws xob thermoelectric.
Piv rau qhov kub thiab txias uas xav tau rau cov khoom siv thermoelectric, kev sau lub zog ntawm cov khoom siv thermoelectric xav tau kev hloov pauv kub dhau sijhawm. Qhov no txhais tau tias yog lub voj voog thermodynamic, uas piav qhia zoo tshaj plaws los ntawm daim duab entropy (S)-kub (T). Daim duab 1a qhia txog daim duab ST ib txwm muaj ntawm cov khoom siv pyroelectric tsis-linear (NLP) uas qhia txog kev hloov pauv theem ferroelectric-paraelectric hauv scandium lead tantalate (PST). Cov ntu xiav thiab ntsuab ntawm lub voj voog ntawm daim duab ST sib raug rau lub zog hluav taws xob hloov pauv hauv lub voj voog Olson (ob ntu isothermal thiab ob ntu isopole). Ntawm no peb xav txog ob lub voj voog nrog tib lub zog hluav taws xob hloov pauv (lub teb qhib thiab tawm) thiab kev hloov pauv kub ΔT, txawm tias muaj qhov kub pib sib txawv. Lub voj voog ntsuab tsis nyob hauv thaj chaw hloov pauv theem thiab yog li muaj thaj chaw me dua li lub voj voog xiav nyob hauv thaj chaw hloov pauv theem. Hauv daim duab ST, thaj chaw loj dua, lub zog sau ntau dua. Yog li ntawd, kev hloov pauv theem yuav tsum sau ntau lub zog. Qhov xav tau rau thaj chaw loj hauv NLP zoo ib yam li qhov xav tau rau kev siv hluav taws xob9, 10, 11, 12 qhov twg PST multilayer capacitors (MLCs) thiab PVDF-based terpolymers tau qhia txog kev ua haujlwm zoo heev. txias txias hauv lub voj voog 13, 14, 15, 16. Yog li ntawd, peb tau txheeb xyuas PST MLCs uas xav tau rau kev sau qoob loo thermal. Cov qauv no tau piav qhia tag nrho hauv cov txheej txheem thiab tau piav qhia hauv cov ntawv ntxiv 1 (scanning electron microscopy), 2 (X-ray diffraction) thiab 3 (calorimetry).
a, Kos duab ntawm daim duab kos entropy (S)-kub (T) nrog lub zog hluav taws xob qhib thiab kaw siv rau cov ntaub ntawv NLP qhia txog kev hloov pauv theem. Ob lub voj voog sau zog tau pom hauv ob thaj chaw kub sib txawv. Lub voj voog xiav thiab ntsuab tshwm sim sab hauv thiab sab nraud ntawm kev hloov pauv theem, feem, thiab xaus rau hauv thaj chaw sib txawv ntawm qhov chaw. b, ob lub nplhaib DE PST MLC unipolar, tuab 1 hli, ntsuas ntawm 0 thiab 155 kV cm-1 ntawm 20 ° C thiab 90 ° C, feem, thiab cov voj voog Olsen sib xws. Cov ntawv ABCD xa mus rau cov xeev sib txawv hauv lub voj voog Olson. AB: MLCs tau them rau 155 kV cm-1 ntawm 20 ° C. BC: MLC tau tswj hwm ntawm 155 kV cm-1 thiab qhov kub tau nce mus txog 90 ° C. CD: MLC tso tawm ntawm 90 ° C. DA: MLC txias rau 20 ° C hauv xoom teb. Thaj chaw xiav sib raug rau lub zog nkag uas xav tau los pib lub voj voog. Thaj chaw txiv kab ntxwv yog lub zog sau hauv ib lub voj voog. c, vaj huam sib luag sab saud, voltage (dub) thiab tam sim no (liab) piv rau lub sijhawm, taug qab thaum lub voj voog Olson tib yam li b. Ob lub ntxig sawv cev rau qhov kev nthuav dav ntawm voltage thiab tam sim no ntawm cov ntsiab lus tseem ceeb hauv lub voj voog. Hauv vaj huam sib luag qis dua, cov kab daj thiab ntsuab sawv cev rau cov kab kub thiab lub zog sib xws, rau 1 hli tuab MLC. Lub zog raug suav los ntawm cov kab tam sim no thiab voltage ntawm vaj huam sib luag sab saud. Lub zog tsis zoo sib xws rau lub zog sau. Cov kauj ruam sib xws rau cov ntawv loj hauv plaub tus lej zoo ib yam li hauv lub voj voog Olson. Lub voj voog AB'CD sib xws rau lub voj voog Stirling (ntxiv daim ntawv ceeb toom 7).
qhov twg E thiab D yog lub teb hluav taws xob thiab lub teb hluav taws xob hloov chaw, raws li. Nd tuaj yeem tau txais tsis ncaj qha los ntawm DE Circuit (Daim duab 1b) lossis ncaj qha los ntawm kev pib lub voj voog thermodynamic. Cov txheej txheem muaj txiaj ntsig zoo tshaj plaws tau piav qhia los ntawm Olsen hauv nws txoj haujlwm ua thawj coj ntawm kev sau cov zog pyroelectric hauv xyoo 1980s17.
Hauv daim duab 1b qhia ob lub voj voog DE monopolar ntawm 1 hli tuab PST-MLC qauv sib sau ua ke ntawm 20 ° C thiab 90 ° C, feem, hla ntau yam ntawm 0 txog 155 kV cm-1 (600 V). Ob lub voj voog no tuaj yeem siv los xam qhov tsis ncaj qha lub zog sau los ntawm Olson lub voj voog qhia hauv Daim Duab 1a. Qhov tseeb, lub voj voog Olsen muaj ob ceg isofield (ntawm no, xoom teb hauv ceg DA thiab 155 kV cm-1 hauv ceg BC) thiab ob ceg isothermal (ntawm no, 20 ° C thiab 20 ° C hauv ceg AB). C hauv ceg CD) Lub zog sau thaum lub voj voog sib raug rau thaj chaw txiv kab ntxwv thiab xiav (EdD integral). Lub zog sau Nd yog qhov sib txawv ntawm lub zog nkag thiab tso zis, piv txwv li tsuas yog thaj chaw txiv kab ntxwv hauv daim duab 1b. Lub voj voog Olson tshwj xeeb no muab Nd lub zog ceev ntawm 1.78 J cm-3. Lub voj voog Stirling yog lwm txoj hauv kev rau Olson lub voj voog (Supplementary Note 7). Vim tias theem them tas mus li (qhib hluav taws xob) yooj yim dua, qhov ceev ntawm lub zog uas rho tawm los ntawm daim duab 1b (lub voj voog AB'CD) ncav cuag 1.25 J cm-3. Qhov no tsuas yog 70% ntawm qhov uas lub voj voog Olson tuaj yeem sau tau, tab sis cov khoom siv sau qoob loo yooj yim ua nws.
Ntxiv rau, peb tau ntsuas lub zog uas tau sau thaum lub voj voog Olson los ntawm kev siv lub zog ntawm PST MLC siv theem tswj kub Linkam thiab lub ntsuas qhov chaw (txoj kev). Daim duab 1c ntawm sab saum toj thiab hauv cov duab qhia txog tam sim no (liab) thiab voltage (dub) uas tau sau rau ntawm tib lub PST MLC tuab 1 hli ib yam li rau lub voj voog DE uas mus dhau tib lub voj voog Olson. Tam sim no thiab voltage ua rau nws muaj peev xwm xam lub zog uas tau sau, thiab cov kab nkhaus tau pom hauv daim duab 1c, hauv qab (ntsuab) thiab kub (daj) thoob plaws hauv lub voj voog. Cov ntawv ABCD sawv cev rau tib lub voj voog Olson hauv daim duab 1. Kev them MLC tshwm sim thaum lub ceg AB thiab tau ua tiav ntawm qhov tam sim no qis (200 µA), yog li SourceMeter tuaj yeem tswj kev them kom zoo. Qhov tshwm sim ntawm qhov tam sim no pib tas li no yog tias qhov nkhaus voltage (kab nkhaus dub) tsis yog linear vim yog qhov tsis yog linear peev xwm hloov chaw teb D PST (Daim duab 1c, sab saum toj inset). Thaum kawg ntawm kev them, 30 mJ ntawm lub zog hluav taws xob khaws cia rau hauv MLC (taw tes B). Lub MLC ces ua kom sov thiab tam sim no tsis zoo (thiab yog li ntawd tam sim no tsis zoo) raug tsim tawm thaum lub zog tseem nyob ntawm 600 V. Tom qab 40 s, thaum qhov kub mus txog qhov siab tshaj plaws ntawm 90 ° C, tam sim no no tau them rov qab, txawm hais tias cov kauj ruam qauv tsim tawm hauv lub voj voog lub zog hluav taws xob ntawm 35 mJ thaum lub sijhawm isofield no (qhov thib ob inset hauv daim duab 1c, sab saum toj). Lub zog ntawm MLC (ceg CD) ces raug txo qis, ua rau muaj ntxiv 60 mJ ntawm kev ua haujlwm hluav taws xob. Tag nrho cov zog tso zis yog 95 mJ. Lub zog sau yog qhov sib txawv ntawm lub zog nkag thiab tso zis, uas muab 95 - 30 = 65 mJ. Qhov no sib xws rau lub zog ceev ntawm 1.84 J cm-3, uas ze heev rau Nd rho tawm los ntawm lub nplhaib DE. Qhov rov ua dua ntawm lub voj voog Olson no tau raug sim ntau yam (Supplementary Note 4). Los ntawm kev nce ntxiv ntawm qhov hluav taws xob thiab kub, peb tau ua tiav 4.43 J cm-3 siv Olsen lub voj voog hauv 0.5 hli tuab PST MLC dhau qhov kub thiab txias ntawm 750 V (195 kV cm-1) thiab 175 ° C (Ntxiv Lus Cim 5). Qhov no yog plaub npaug ntau dua li qhov kev ua tau zoo tshaj plaws tau tshaj tawm hauv cov ntaub ntawv rau Olson lub voj voog ncaj qha thiab tau txais ntawm cov yeeb yaj kiab nyias ntawm Pb (Mg, Nb) O3-PbTiO3 (PMN-PT) (1.06 J cm-3) 18 (cm. Ntxiv Lus Cim 1 rau ntau tus nqi hauv cov ntaub ntawv). Qhov kev ua tau zoo no tau raug ua tiav vim yog qhov xau qis heev ntawm cov MLCs no (<10−7 A ntawm 750 V thiab 180 ° C, saib cov ntsiab lus hauv Cov Lus Qhia Ntxiv 6) - ib qho tseem ceeb uas Smith et al.19 tau hais - piv rau cov ntaub ntawv siv hauv kev tshawb fawb ua ntej 17,20. Qhov kev ua tau zoo no tau raug ua tiav vim yog qhov xau qis heev ntawm cov MLCs no (<10−7 A ntawm 750 V thiab 180 ° C, saib cov ntsiab lus hauv Cov Lus Qhia Ntxiv 6) - ib qho tseem ceeb uas Smith et al.19 tau hais - piv rau cov ntaub ntawv siv hauv kev tshawb fawb ua ntej 17,20. Эти характеристики были достигнуты благодаря очень низкому току утечки этих MLC (<10–7 А при 750 Всму . подробности в дополнительном примечании 6) — критический момент, упомянутый Смитом и др. 19— в отличие от к материалам, использованным в более ранних исследованиях 17,20. Cov yam ntxwv no tau ua tiav vim yog qhov xau qis heev ntawm cov MLCs no (<10–7 A ntawm 750 V thiab 180 ° C, saib Cov Lus Qhia Ntxiv 6 kom paub meej) - ib qho tseem ceeb uas Smith et al. 19 tau hais - sib piv rau cov ntaub ntawv siv hauv kev tshawb fawb ua ntej 17,20.由于这些MLC 的泄漏电流非常低（在750 V 和180°C 时人<10-7 A，请参见补充说明6中的详篁毁斯明6）提到的关键点——相比之下，已经达到了这种性能到早期研究中使用的材料17,20.由于这些 mlc的泄漏非常（在在 750 V 和 180°C 时 <10-7 A，参见补充 说明 6 中详））人 19 提到关键 关键 点相比之下 相比之下 相比之下 相比之下 相比之下 相比之下 相比之下 相比之下 相比之下之下之下之下之下之下之下相比之下 相比之下 相比之下 相比之下 相比之下 相比之下，已经达到了这种性能到早期研究中使用的材料17.20. Поскольку ток утечки этих MLC очень низкий (<10–7 А при 750 В и 180°C, см. подробности в дополнитель) ключевой момент, упомянутый Смитом и др. 19—Yawmsaub has le hov, tug quaspuj hov tug quaspuj hab tug quaspuj. Vim tias qhov xau tam sim no ntawm cov MLCs no qis heev (<10–7 A ntawm 750 V thiab 180 °C, saib Cov Lus Qhia Ntxiv 6 kom paub meej) - ib qho tseem ceeb uas Smith et al. 19 tau hais - rau kev sib piv, cov kev ua tau zoo no tau ua tiav.rau cov ntaub ntawv siv hauv kev tshawb fawb ua ntej 17,20.
Cov xwm txheej zoo sib xws (600 V, 20–90 ° C) siv rau lub voj voog Stirling (Ntawv qhia ntxiv 7). Raws li xav tau los ntawm cov txiaj ntsig ntawm lub voj voog DE, qhov tso zis yog 41.0 mJ. Ib qho ntawm cov yam ntxwv tseem ceeb tshaj plaws ntawm Stirling voj voog yog lawv lub peev xwm los ua kom lub zog pib loj dua los ntawm cov nyhuv thermoelectric. Peb pom qhov nce hluav taws xob txog li 39 (los ntawm lub zog pib ntawm 15 V mus rau qhov kawg hluav taws xob txog li 590 V, saib Daim Duab Ntxiv 7.2).
Lwm qhov tshwj xeeb ntawm cov MLCs no yog tias lawv yog cov khoom macroscopic loj txaus los sau lub zog hauv joule ntau yam. Yog li ntawd, peb tau tsim ib qho prototype harvester (HARV1) siv 28 MLC PST 1 hli tuab, ua raws li tib lub phaj tsim qauv piav qhia los ntawm Torello et al.14, hauv 7 × 4 matrix raws li pom hauv daim duab. Cov kua dielectric nqa cua sov hauv manifold raug tshem tawm los ntawm lub twj tso kua mis peristaltic ntawm ob lub pas dej uas qhov kub ntawm cov kua dej tau khaws cia tas li (txoj kev). Sau txog li 3.1 J siv lub voj voog Olson piav qhia hauv daim duab 2a, thaj chaw isothermal ntawm 10 ° C thiab 125 ° C thiab thaj chaw isofield ntawm 0 thiab 750 V (195 kV cm-1). Qhov no sib raug rau lub zog ceev ntawm 3.14 J cm-3. Siv cov khoom sib xyaw no, kev ntsuas tau coj mus rau hauv ntau yam mob (Daim duab 2b). Nco ntsoov tias 1.8 J tau txais dhau qhov kub thiab txias ntawm 80 ° C thiab qhov hluav taws xob ntawm 600 V (155 kV cm-1). Qhov no yog qhov zoo sib xws nrog 65 mJ uas tau hais ua ntej rau 1 hli tuab PST MLC nyob rau hauv tib qho xwm txheej (28 × 65 = 1820 mJ).
a, Kev teeb tsa sim ntawm HARV1 prototype uas tau sib dhos ua ke raws li 28 MLC PSTs 1 hli tuab (4 kab × 7 kem) khiav ntawm Olson cycles. Rau txhua plaub kauj ruam ntawm lub voj voog, qhov kub thiab voltage tau muab rau hauv prototype. Lub khoos phis tawj tsav lub twj tso kua dej peristaltic uas ncig cov kua dej dielectric ntawm cov chaw khaws dej txias thiab kub, ob lub valve, thiab lub zog. Lub khoos phis tawj kuj siv cov thermocouples los sau cov ntaub ntawv ntawm qhov hluav taws xob thiab tam sim no muab rau prototype thiab qhov kub ntawm lub tshuab sib xyaw los ntawm lub zog muab. b, Zog (xim) sau los ntawm peb 4 × 7 MLC prototype piv rau qhov kub thiab txias (X-axis) thiab voltage (Y-axis) hauv kev sim sib txawv.
Ib qho loj dua ntawm lub tshuab sau qoob loo (HARV2) nrog 60 PST MLC 1 hli tuab thiab 160 PST MLC 0.5 hli tuab (41.7 g cov khoom siv pyroelectric nquag) tau muab 11.2 J (Nco Ntsoov Ntxiv 8). Xyoo 1984, Olsen tau ua lub tshuab sau qoob loo raws li 317 g ntawm cov khoom siv Pb (Zr, Ti) O3 uas muaj peev xwm tsim tau 6.23 J ntawm hluav taws xob ntawm qhov kub ntawm kwv yees li 150 ° C (ref. 21). Rau qhov kev sib xyaw ua ke no, qhov no yog tib qho nqi muaj nyob rau hauv joule ntau yam. Nws tau txais ntau dua ib nrab ntawm tus nqi peb tau ua tiav thiab yuav luag xya npaug ntawm qhov zoo. Qhov no txhais tau tias lub zog ceev ntawm HARV2 yog 13 npaug siab dua.
Lub sijhawm voj voog HARV1 yog 57 vib nas this. Qhov no tsim tau 54 mW ntawm lub zog nrog 4 kab ntawm 7 kem ntawm 1 hli tuab MLC teeb tsa. Txhawm rau coj nws mus ib kauj ruam ntxiv, peb tau tsim lub tshuab sib xyaw thib peb (HARV3) nrog 0.5 hli tuab PST MLC thiab kev teeb tsa zoo sib xws rau HARV1 thiab HARV2 (Nco Ntsoov Ntxiv 9). Peb ntsuas lub sijhawm thermalization ntawm 12.5 vib nas this. Qhov no sib raug rau lub sijhawm voj voog ntawm 25 s (Nco Ntsoov Ntxiv Daim Duab 9). Lub zog sau (47 mJ) muab lub zog hluav taws xob ntawm 1.95 mW ib MLC, uas ua rau peb xav tias HARV2 tsim tau 0.55 W (kwv yees li 1.95 mW × 280 PST MLC 0.5 hli tuab). Tsis tas li ntawd, peb tau simulated cua sov hloov pauv siv Finite Element Simulation (COMSOL, Nco Ntsoov Ntxiv 10 thiab Cov Lus Qhia Ntxiv 2–4) sib raug rau HARV1 kev sim. Kev tsim qauv ntawm cov khoom siv finite ua rau nws muaj peev xwm kwv yees cov nqi zog yuav luag ib qho kev txiav txim siab siab dua (430 mW) rau tib tus lej ntawm PST kem los ntawm kev ua kom MLC nyias mus rau 0.2 hli, siv dej ua cov dej txias, thiab rov qab kho lub matrix rau 7 kab. × 4 kem (ntxiv rau , muaj 960 mW thaum lub tank nyob ib sab ntawm qhov sib xyaw, Daim Duab Ntxiv 10b).
Txhawm rau qhia txog qhov muaj txiaj ntsig ntawm tus neeg sau no, lub voj voog Stirling tau siv rau lub tshuab ua qauv qhia uas muaj tsuas yog ob lub PST MLCs tuab 0.5 hli ua cov neeg sau cua sov, lub qhov hloov hluav taws xob siab, lub qhov hloov hluav taws xob qis nrog lub capacitor cia, lub DC / DC converter, lub microcontroller fais fab qis, ob lub thermocouples thiab boost converter (Nco Ntsoov Ntxiv 11). Lub voj voog xav kom lub capacitor cia yuav tsum tau them thawj zaug ntawm 9V thiab tom qab ntawd khiav nws tus kheej thaum qhov kub ntawm ob lub MLCs yog los ntawm -5 ° C txog 85 ° C, ntawm no hauv cov voj voog ntawm 160 s (ob peb lub voj voog tau qhia hauv Nco Ntsoov Ntxiv 11). Qhov zoo kawg nkaus, ob lub MLCs hnyav tsuas yog 0.3g tuaj yeem tswj hwm lub kaw lus loj no. Lwm qhov tshwj xeeb yog tias lub converter hluav taws xob qis muaj peev xwm hloov 400V mus rau 10-15V nrog 79% kev ua haujlwm (Nco Ntsoov Ntxiv 11 thiab Daim Duab Ntxiv 11.3).
Thaum kawg, peb tau soj ntsuam qhov ua tau zoo ntawm cov MLC modules no hauv kev hloov lub zog thermal mus rau hauv lub zog hluav taws xob. Qhov zoo ntawm qhov ua tau zoo yog txhais tias yog qhov sib piv ntawm qhov ceev ntawm lub zog hluav taws xob Nd sau rau qhov ceev ntawm cov cua sov muab Qin (Cov lus qhia ntxiv 12):
Cov duab 3a, b qhia txog kev ua haujlwm zoo η thiab kev ua haujlwm zoo sib xws ηr ntawm lub voj voog Olsen, raws li kev ua haujlwm ntawm qhov kub thiab txias ntawm 0.5 hli tuab PST MLC. Ob qho tib si cov ntaub ntawv teeb tsa tau muab rau lub teb hluav taws xob ntawm 195 kV cm-1. Kev ua haujlwm zoo \(\this\) ncav cuag 1.43%, uas yog sib npaug rau 18% ntawm ηr. Txawm li cas los xij, rau qhov kub thiab txias ntawm 10 K txij li 25 °C txog 35 °C, ηr ncav cuag cov nqi txog li 40% (kab xiav hauv daim duab 3b). Qhov no yog ob npaug ntawm tus nqi paub rau cov ntaub ntawv NLP kaw hauv PMN-PT zaj duab xis (ηr = 19%) hauv qhov kub thiab txias ntawm 10 K thiab 300 kV cm-1 (Ref. 18). Qhov kub thiab txias qis dua 10 K tsis tau txiav txim siab vim tias qhov thermal hysteresis ntawm PST MLC yog ntawm 5 thiab 8 K. Kev lees paub txog qhov cuam tshuam zoo ntawm kev hloov pauv theem ntawm kev ua haujlwm zoo yog qhov tseem ceeb. Qhov tseeb, cov nqi zoo tshaj plaws ntawm η thiab ηr yuav luag txhua tus tau txais ntawm qhov kub pib Ti = 25 ° C hauv Figs. 3a, b. Qhov no yog vim muaj kev hloov pauv theem ze thaum tsis muaj daim teb siv thiab Curie kub TC yog nyob ib puag ncig 20 ° C hauv cov MLCs no (Daim ntawv ntxiv 13).
a,b, qhov ua tau zoo η thiab qhov ua tau zoo ntawm Olson lub voj voog (a)\({\eta }_{{\rm{r}}}=\eta /{\eta}_{{\rm{Carnot}} rau qhov hluav taws xob siab tshaj plaws los ntawm ib daim teb ntawm 195 kV cm-1 thiab qhov kub pib sib txawv Ti, }}\,\)(b) rau MPC PST 0.5 hli tuab, nyob ntawm qhov kub thiab txias ΔTspan.
Qhov kev soj ntsuam tom kawg muaj ob qho tseem ceeb: (1) txhua qhov kev caij tsheb kauj vab zoo yuav tsum pib ntawm qhov kub siab dua TC rau qhov kev hloov pauv theem uas tshwm sim los ntawm thaj teb (los ntawm paraelectric mus rau ferroelectric) kom tshwm sim; (2) cov ntaub ntawv no ua haujlwm tau zoo dua ntawm lub sijhawm khiav ze rau TC. Txawm hais tias cov txiaj ntsig loj tau pom hauv peb qhov kev sim, qhov kub thiab txias txwv tsis pub peb ua tiav cov txiaj ntsig loj vim yog Carnot txwv (\ (\ Delta T / T \)). Txawm li cas los xij, qhov ua tau zoo heev uas tau pom los ntawm cov PST MLCs no ua pov thawj Olsen thaum nws hais tias "ib chav kawm zoo tagnrho 20 regenerative thermoelectric motor ua haujlwm ntawm qhov kub ntawm 50 ° C thiab 250 ° C tuaj yeem muaj kev ua haujlwm ntawm 30% "17. Txhawm rau kom ncav cuag cov nqi no thiab sim lub tswv yim, nws yuav muaj txiaj ntsig zoo siv cov PSTs doped nrog cov TCs sib txawv, raws li kawm los ntawm Shebanov thiab Borman. Lawv tau qhia tias TC hauv PST tuaj yeem sib txawv ntawm 3 ° C (Sb doping) txog 33 ° C (Ti doping) 22. Yog li ntawd, peb xav tias cov tiam tom ntej pyroelectric regenerators raws li doped PST MLCs lossis lwm yam khoom siv nrog thawj theem kev hloov pauv muaj zog tuaj yeem sib tw nrog cov khoom siv fais fab zoo tshaj plaws.
Hauv kev tshawb fawb no, peb tau tshawb nrhiav MLCs ua los ntawm PST. Cov khoom siv no muaj cov electrodes Pt thiab PST, uas ntau lub capacitors txuas nrog ua ke. PST tau raug xaiv vim nws yog cov khoom siv EC zoo heev thiab yog li ntawd cov khoom siv NLP zoo heev. Nws qhia txog kev hloov pauv theem ferroelectric-paraelectric thawj zaug nyob ib puag ncig 20 ° C, qhia tias nws cov kev hloov pauv entropy zoo ib yam li cov uas tau pom hauv daim duab 1. Cov MLCs zoo sib xws tau piav qhia tag nrho rau EC13,14 cov khoom siv. Hauv kev tshawb fawb no, peb tau siv 10.4 × 7.2 × 1 mm³ thiab 10.4 × 7.2 × 0.5 mm³ MLCs. MLCs nrog lub thickness ntawm 1 hli thiab 0.5 hli tau ua los ntawm 19 thiab 9 txheej ntawm PST nrog lub thickness ntawm 38.6 µm, feem. Hauv ob qho tib si, txheej PST sab hauv tau muab tso rau ntawm 2.05 µm tuab platinum electrodes. Tus qauv tsim ntawm cov MLCs no xav tias 55% ntawm PSTs yog cov nquag, sib raug rau qhov ntawm cov electrodes (Nco Ntsoov Ntxiv 1). Thaj chaw electrode nquag yog 48.7 mm2 (Nco Ntsoov Ntxiv 5). MLC PST tau npaj los ntawm cov tshuaj tiv thaiv theem khov kho thiab txoj kev casting. Cov ntsiab lus ntawm cov txheej txheem npaj tau piav qhia hauv tsab xov xwm dhau los14. Ib qho ntawm qhov sib txawv ntawm PST MLC thiab tsab xov xwm dhau los yog qhov kev txiav txim ntawm B-qhov chaw, uas cuam tshuam loj heev rau kev ua haujlwm ntawm EC hauv PST. Qhov kev txiav txim ntawm B-qhov chaw ntawm PST MLC yog 0.75 (Nco Ntsoov Ntxiv 2) tau txais los ntawm sintering ntawm 1400 ° C ua raws li ntau pua teev ntev annealing ntawm 1000 ° C. Yog xav paub ntxiv txog PST MLC, saib Cov Lus Qhia Ntxiv 1-3 thiab Cov Lus Qhia Ntxiv 5.
Lub tswv yim tseem ceeb ntawm txoj kev tshawb no yog raws li lub voj voog Olson (Daim Duab 1). Rau lub voj voog zoo li no, peb xav tau lub thawv kub thiab txias thiab lub hwj chim uas muaj peev xwm saib xyuas thiab tswj tau qhov hluav taws xob thiab tam sim no hauv ntau lub modules MLC. Cov voj voog ncaj qha no siv ob qho kev teeb tsa sib txawv, uas yog (1) Linkam modules cua sov thiab txias ib lub MLC txuas nrog lub zog Keithley 2410, thiab (2) peb lub prototypes (HARV1, HARV2 thiab HARV3) ua ke nrog tib lub zog. Hauv qhov xwm txheej tom kawg, cov kua dielectric (roj silicone nrog viscosity ntawm 5 cP ntawm 25 ° C, yuav los ntawm Sigma Aldrich) tau siv rau kev sib pauv cua sov ntawm ob lub thawv (kub thiab txias) thiab MLC. Lub thawv thermal muaj lub thawv iav puv nrog cov kua dielectric thiab muab tso rau saum lub phaj thermal. Kev khaws cia txias muaj lub dab dej nrog cov raj kua uas muaj cov kua dielectric hauv lub thawv yas loj uas puv nrog dej thiab dej khov. Ob lub qhov cua peb txoj kev (yuav los ntawm Bio-Chem Fluidics) tau muab tso rau ntawm txhua qhov kawg ntawm lub tshuab sib xyaw kom hloov cov kua dej ntawm ib lub pas dej mus rau lwm qhov (Daim Duab 2a). Txhawm rau kom ntseeg tau tias qhov sib npaug ntawm lub pob PST-MLC thiab cov dej txias, lub sijhawm voj voog tau ntev mus txog thaum cov thermocouples nkag thiab tawm (ze li sai tau rau pob PST-MLC) qhia tib qhov kub. Cov ntawv sau Python tswj hwm thiab sib dhos txhua yam twj paj nruag (qhov chaw ntsuas, twj tso kua mis, qhov cua, thiab thermocouples) kom khiav lub voj voog Olson kom raug, piv txwv li lub voj voog txias pib voj voog los ntawm PST pawg tom qab lub ntsuas qhov chaw raug them kom lawv kub ntawm qhov hluav taws xob xav tau rau lub voj voog Olson.
Los yog, peb tau lees paub cov kev ntsuas ncaj qha ntawm lub zog sau nrog cov txheej txheem tsis ncaj qha. Cov txheej txheem tsis ncaj qha no yog raws li kev hloov pauv hluav taws xob (D) - hluav taws xob teb (E) cov voj voog teb sau ntawm qhov kub sib txawv, thiab los ntawm kev xam thaj tsam ntawm ob lub voj voog DE, ib tus tuaj yeem kwv yees qhov tseeb tias muaj pes tsawg lub zog tuaj yeem sau tau, raws li pom hauv daim duab. hauv daim duab 2. .1b. Cov voj voog DE no kuj tau sau los ntawm kev siv Keithley qhov chaw ntsuas.
Nees nkaum yim lub PST MLCs uas tuab 1 hli tau sib sau ua ke hauv 4-kab, 7-kab sib luag raws li tus qauv tsim tau piav qhia hauv qhov siv. 14. Qhov sib txawv ntawm cov kua dej ntawm cov kab PST-MLC yog 0.75 hli. Qhov no ua tiav los ntawm kev ntxiv cov kab xev ob sab ua cov kua dej nyob ib puag ncig ntug ntawm PST MLC. PST MLC txuas nrog hluav taws xob sib luag nrog tus choj epoxy nyiaj uas sib cuag nrog cov hlau electrode. Tom qab ntawd, cov xov hlau tau nplaum nrog cov roj epoxy nyiaj rau txhua sab ntawm cov xov hlau electrode rau kev txuas rau lub zog fais fab. Thaum kawg, ntxig tag nrho cov qauv rau hauv lub raj polyolefin. Qhov tom kawg tau nplaum rau lub raj kua dej kom ntseeg tau tias muaj kev sib khi zoo. Thaum kawg, 0.25 hli tuab K-hom thermocouples tau tsim rau hauv txhua qhov kawg ntawm PST-MLC qauv los saib xyuas qhov kub ntawm cov kua dej nkag thiab tawm. Txhawm rau ua qhov no, lub raj yuav tsum tau perforated ua ntej. Tom qab txhim kho lub thermocouple, siv cov nplaum zoo ib yam li ua ntej ntawm lub raj thermocouple thiab hlau kom rov qab kho lub foob.
Yim daim qauv sib cais tau tsim, plaub ntawm lawv muaj 40 0.5 hli tuab MLC PSTs faib ua cov phaj sib luag nrog 5 kem thiab 8 kab, thiab plaub seem muaj 15 1 hli tuab MLC PSTs txhua. hauv 3-kab × 5-kab phaj sib luag. Tag nrho cov PST MLCs siv yog 220 (160 0.5 hli tuab thiab 60 PST MLC 1 hli tuab). Peb hu ob lub subunits no HARV2_160 thiab HARV2_60. Qhov sib txawv kua hauv daim qauv HARV2_160 muaj ob daim kab xev ob sab 0.25 hli tuab nrog ib txoj hlau 0.25 hli tuab ntawm lawv. Rau daim qauv HARV2_60, peb rov ua tib yam txheej txheem, tab sis siv txoj hlau 0.38 hli tuab. Rau kev sib npaug, HARV2_160 thiab HARV2_60 muaj lawv tus kheej cov kua dej, twj tso kua mis, li qub thiab sab txias (Supplementary Note 8). Ob lub HARV2 sib koom ib lub thawv cua sov, ib lub thawv 3 liv (30 cm x 20 cm x 5 cm) rau ntawm ob lub phaj kub nrog cov hlau nplaum tig. Tag nrho yim lub prototypes sib txuas ua ke hluav taws xob. Cov HARV2_160 thiab HARV2_60 subunits ua haujlwm tib lub sijhawm hauv Olson lub voj voog ua rau muaj zog sau tau 11.2 J.
Muab 0.5 hli tuab PST MLC rau hauv cov yeeb nkab polyolefin nrog daim kab xev ob sab thiab xov hlau ntawm ob sab kom tsim qhov chaw rau cov kua ntws. Vim nws me me, tus qauv tau muab tso rau ntawm ib sab ntawm lub qhov dej kub lossis txias, txo lub sijhawm voj voog.
Hauv PST MLC, lub zog hluav taws xob tas mus li raug siv los ntawm kev siv lub zog hluav taws xob tas mus li rau ceg cua sov. Yog li ntawd, lub zog hluav taws xob tsis zoo raug tsim thiab lub zog khaws cia. Tom qab cua sov PST MLC, lub zog raug tshem tawm (V = 0), thiab lub zog khaws cia rau hauv nws raug xa rov qab mus rau lub hauv paus, uas sib raug rau ib qho kev koom tes ntxiv ntawm lub zog sau. Thaum kawg, nrog lub zog hluav taws xob V = 0 siv, MLC PSTs raug txias rau lawv qhov kub pib kom lub voj voog tuaj yeem pib dua. Ntawm theem no, lub zog tsis raug sau. Peb tau khiav lub voj voog Olsen siv Keithley 2410 SourceMeter, them PST MLC los ntawm lub zog hluav taws xob thiab teeb tsa qhov sib phim tam sim no rau tus nqi tsim nyog kom cov ntsiab lus txaus tau sau thaum lub sijhawm them rau kev suav lub zog txhim khu kev qha.
Hauv Stirling lub voj voog, PST MLCs tau them rau hauv hom voltage ntawm tus nqi hluav taws xob pib (qhov voltage pib Vi > 0), qhov tam sim no xav tau kom cov kauj ruam them nqi siv sijhawm li 1 s (thiab cov ntsiab lus txaus tau sau rau kev suav qhov tseeb ntawm lub zog) thiab qhov kub txias. Hauv Stirling lub voj voog, PST MLCs tau them rau hauv hom voltage ntawm tus nqi hluav taws xob pib (qhov voltage pib Vi > 0), qhov tam sim no xav tau kom cov kauj ruam them nqi siv sijhawm li 1 s (thiab cov ntsiab lus txaus tau sau rau kev suav qhov tseeb ntawm lub zog) thiab qhov kub txias. В циклах Стирлинга PST MLC заряжались в режиме источника напряжения при начальном значении электрическогяжанектрическогя назад Vi > 0), желаемом податливом токе, так что этап зарядки занимает около 1 с (и набирается достаточное кое достаточное кое надежного расчета энергия) thiab холодная температура. Hauv Stirling PST MLC voj voog, lawv tau them rau hauv hom voltage qhov chaw ntawm tus nqi pib ntawm lub teb hluav taws xob (qhov voltage pib Vi > 0), qhov tam sim no xav tau, yog li ntawd theem them yuav siv sijhawm li 1 s (thiab muaj cov ntsiab lus txaus rau kev suav lub zog txhim khu kev qha) thiab qhov kub txias.在斯特林循环中， PST MLC 在电压源模式下以初始电场值（初始电压Vi > 0) 充电，所需的顺应电流使得充电步骤大约需要1秒（并且收集了足够的点以可靠地计算能量）和低温. Hauv lub voj voog tswj, PST MLC raug them ntawm tus nqi hluav taws xob pib (qhov hluav taws xob pib Vi > 0) hauv hom qhov hluav taws xob, yog li qhov tam sim no uas xav tau yuav siv sijhawm li 1 vib nas this rau kauj ruam them (thiab peb tau sau cov ntsiab lus txaus kom suav tau zoo (zog) thiab qhov kub qis. В цикле Стирлинга PST MLC заряжается в режиме источника напряжения с начальным значением электрическогьяжежения поля 0), требуемый ток податливости таков, что этап зарядки занимает около 1 с (и набирается достаточничте костаточничте надежно рассчитать энергию) thiab низкие температуры. Hauv lub voj voog Stirling, PST MLC raug them rau hauv hom voltage qhov chaw nrog tus nqi pib ntawm lub teb hluav taws xob (qhov hluav taws xob pib Vi > 0), qhov tam sim no xav tau yog xws li theem them yuav siv sijhawm li 1 s (thiab muaj cov ntsiab lus txaus los suav lub zog) thiab qhov kub qis.Ua ntej PST MLC kub, qhib lub voj voog los ntawm kev siv cov hluav taws xob sib phim ntawm I = 0 mA (qhov hluav taws xob sib phim tsawg kawg nkaus uas peb qhov chaw ntsuas tuaj yeem ua tau yog 10 nA). Yog li ntawd, tus nqi tseem nyob hauv PST ntawm MJK, thiab qhov hluav taws xob nce ntxiv thaum cov qauv kub. Tsis muaj zog sau rau hauv caj npab BC vim I = 0 mA. Tom qab mus txog qhov kub siab, qhov hluav taws xob hauv MLT FT nce (qee zaum ntau dua 30 zaug, saib ntxiv daim duab 7.2), MLK FT raug tso tawm (V = 0), thiab lub zog hluav taws xob khaws cia rau hauv lawv rau tib yam li lawv yog tus nqi pib. Tib qho kev sib raug zoo tam sim no raug xa rov qab mus rau qhov chaw ntsuas. Vim yog qhov nce hluav taws xob, lub zog khaws cia ntawm qhov kub siab siab dua li qhov tau muab thaum pib ntawm lub voj voog. Yog li ntawd, lub zog tau txais los ntawm kev hloov pauv cua sov mus rau hauv hluav taws xob.
Peb siv Keithley 2410 SourceMeter los saib xyuas qhov hluav taws xob thiab tam sim no siv rau PST MLC. Lub zog sib xws yog xam los ntawm kev koom ua ke cov khoom ntawm hluav taws xob thiab tam sim no nyeem los ntawm Keithley lub ntsuas qhov chaw, \ (E = {\int }_{0}^{\tau }{I}_({\rm {meas))}\left(t\ right){V}_{{\rm{meas}}(t)\), qhov twg τ yog lub sijhawm ntawm lub sijhawm. Ntawm peb cov kab hluav taws xob, cov nqi zog zoo txhais tau tias lub zog peb yuav tsum muab rau MLC PST, thiab cov nqi tsis zoo txhais tau tias lub zog peb rho tawm ntawm lawv thiab yog li ntawd lub zog tau txais. Lub zog sib piv rau ib lub voj voog sau tau txiav txim siab los ntawm kev faib lub zog sau los ntawm lub sijhawm τ ntawm tag nrho lub voj voog.
Tag nrho cov ntaub ntawv tau muab tso rau hauv cov ntawv tseem ceeb lossis cov ntaub ntawv ntxiv. Cov ntawv thiab cov lus thov rau cov ntaub ntawv yuav tsum raug xa mus rau qhov chaw ntawm cov ntaub ntawv AT lossis ED uas tau muab nrog tsab xov xwm no.
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Peb ua tsaug rau N. Furusawa, Y. Inoue, thiab K. Honda rau lawv txoj kev pab hauv kev tsim MLC. PL, AT, YN, AA, JL, UP, VK, OB thiab ED Ua tsaug rau Luxembourg National Research Foundation (FNR) rau kev txhawb nqa txoj haujlwm no los ntawm CAMELHEAT C17/MS/11703691/Defay, MASSENA PRIDE/15/10935404/Defay- Siebentritt, THERMODIMAT C20/MS/14718071/Defay thiab BRIDGES2021/MS/16282302/CECOHA/Defay.
Chav Haujlwm Tshawb Fawb Txog Cov Khoom Siv thiab Kev Siv Tshuab, Luxembourg Institute of Technology (LIST), Belvoir, Luxembourg