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Chifukwa cha kuchuluka kwa sodium, mabatire a sodium-ion (NIBs) ndi njira ina yabwino yosungira mphamvu zamagetsi. Pakadali pano, chopinga chachikulu pakukula kwa ukadaulo wa NIB ndi kusowa kwa zinthu zama electrode zomwe zimatha kusunga/kutulutsa ma ayoni a sodium kwa nthawi yayitali. Chifukwa chake, cholinga cha kafukufukuyu ndikufufuza mwanzeru zotsatira za kuwonjezera kwa glycerol pa polyvinyl alcohol (PVA) ndi sodium alginate (NaAlg) blends ngati zinthu zama electrode a NIB. Kafukufukuyu akuyang'ana kwambiri pa ma electrolyte a electrolyte a polymer, kutentha, ndi kuchuluka kwa structure-activity (QSAR) kutengera PVA, sodium alginate, ndi glycerol blends. Makhalidwe amenewa amafufuzidwa pogwiritsa ntchito njira za semi-empirical ndi density functional theory (DFT). Popeza kusanthula kwa kapangidwe kake kunavumbula tsatanetsatane wa kuyanjana pakati pa PVA/alginate ndi glycerol, mphamvu ya band gap (Eg) idafufuzidwa. Zotsatira zake zikuwonetsa kuti kuwonjezera kwa glycerol kumapangitsa kuti Eg value ichepe kufika pa 0.2814 eV. Malo ozungulira a electrostatic potential (MESP) akuwonetsa kufalikira kwa madera olemera ndi opanda ma electron komanso ma electron charges mu dongosolo lonse la electrolyte. Ma parameter a kutentha omwe adaphunziridwa akuphatikizapo enthalpy (H), entropy (ΔS), mphamvu ya kutentha (Cp), mphamvu ya Gibbs free (G) ndi kutentha kwa mapangidwe. Kuphatikiza apo, ma descriptor angapo a quantitative structure-activity relationship (QSAR) monga total dipole moment (TDM), total energy (E), ionization potential (IP), Log P ndi polarizability adafufuzidwa mu kafukufukuyu. Zotsatira zake zidawonetsa kuti H, ΔS, Cp, G ndi TDM zidakwera ndi kutentha komwe kumawonjezeka ndi kuchuluka kwa glycerol. Pakadali pano, kutentha kwa mapangidwe, IP ndi E kudachepa, zomwe zidapangitsa kuti reactivity ndi polarizability ziwonjezeke. Kuphatikiza apo, powonjezera glycerol, voteji ya selo idakwera kufika pa 2.488 V. DFT ndi PM6 mawerengedwe kutengera ma electrolyte a PVA/Na Alg glycerol otsika mtengo akuwonetsa kuti amatha kusintha mabatire a lithiamu-ion pang'ono chifukwa cha magwiridwe antchito awo ambiri, koma kusintha kwina ndi kafukufuku zikufunika.
Ngakhale mabatire a lithiamu-ion (LIBs) amagwiritsidwa ntchito kwambiri, kugwiritsa ntchito kwawo kumakumana ndi zopinga zambiri chifukwa cha moyo wawo waufupi, mtengo wake wokwera, komanso nkhawa zachitetezo. Mabatire a Sodium-ion (SIBs) akhoza kukhala njira ina yabwino m'malo mwa LIBs chifukwa cha kupezeka kwawo kwakukulu, mtengo wake wotsika, komanso kusakhala ndi poizoni wa sodium element. Mabatire a Sodium-ion (SIBs) akukhala njira yofunika kwambiri yosungira mphamvu zamagetsi zamagetsi1. Mabatire a Sodium-ion amadalira kwambiri ma electrolyte kuti athandize kunyamula ma ion ndikupanga magetsi2,3. Ma electrolyte amadzimadzi amapangidwa makamaka ndi mchere wachitsulo ndi zosungunulira zachilengedwe. Kugwiritsa ntchito kofunikira kumafuna kuganizira mosamala za chitetezo cha ma electrolyte amadzimadzi, makamaka pamene batire ili ndi kutentha kapena kupsinjika kwamagetsi4.
Mabatire a Sodium-ion (SIBs) akuyembekezeka kusintha mabatire a lithiamu-ion posachedwa chifukwa cha kuchuluka kwa malo awo osungiramo madzi m'nyanja, kusakhala ndi poizoni, komanso mtengo wotsika wa zinthu. Kupanga kwa zinthu za nanomaterial kwathandizira chitukuko cha kusungira deta, zida zamagetsi, ndi zowunikira. Mabuku ambiri awonetsa kugwiritsa ntchito kwa zinthu zosiyanasiyana za nanostructures (monga zitsulo zosungunuka, graphene, nanotubes, ndi fullerenes) m'mabatire a sodium-ion. Kafukufuku wayang'ana kwambiri pakupanga zinthu za anode, kuphatikizapo ma polima, pamabatire a sodium-ion chifukwa cha kusinthasintha kwawo komanso kukonda chilengedwe. Chidwi chofufuza m'munda wa mabatire a polima omwe angadzazidwenso ntchito mosakayikira chidzawonjezeka. Zipangizo zatsopano za polima electrode zokhala ndi kapangidwe ndi zinthu zapadera zitha kutsegulira njira ukadaulo wosungira mphamvu wosamalira chilengedwe. Ngakhale kuti zipangizo zosiyanasiyana za polima electrode zafufuzidwa kuti zigwiritsidwe ntchito m'mabatire a sodium-ion, gawoli likadali kumayambiriro kwa chitukuko. Kwa mabatire a sodium-ion, zipangizo zambiri za polima zokhala ndi mawonekedwe osiyanasiyana ziyenera kufufuzidwa. Kutengera ndi chidziwitso chathu cha momwe timasungira ma ayoni a sodium muzinthu zama electrode a polymer, zitha kuganiziridwa kuti magulu a carbonyl, ma free radicals, ndi ma heteroatoms mu dongosolo lolumikizidwa amatha kukhala malo ogwirira ntchito polumikizana ndi ma ayoni a sodium. Chifukwa chake, ndikofunikira kupanga ma polima atsopano okhala ndi kuchuluka kwakukulu kwa malo ogwirira ntchito awa. Gel polymer electrolyte (GPE) ndi ukadaulo wina womwe umathandizira kudalirika kwa batri, kuyendetsa bwino ma ayoni, kusatulutsa madzi, kusinthasintha kwakukulu, komanso magwiridwe antchito abwino12.
Ma polymer matrices amaphatikizapo zinthu monga PVA ndi polyethylene oxide (PEO)13. Gel permeable polymer (GPE) imaletsa madzi a electrolyte mu polymer matrix, zomwe zimachepetsa chiopsezo cha kutuluka kwa madzi poyerekeza ndi zolekanitsa zamalonda14. PVA ndi polymer yopangidwa ndi zinthu zowola. Ili ndi permittivity yayikulu, ndi yotsika mtengo komanso yopanda poizoni. Zinthuzo zimadziwika ndi mphamvu zake zopangira filimu, kukhazikika kwa mankhwala komanso kumamatira. Ilinso ndi magulu ogwira ntchito (OH) komanso kuchuluka kwakukulu kwa cross-linking potential15,16,17. Kusakaniza kwa polymer, kuwonjezera pulasitiki, kuphatikiza kwa composite ndi njira zopopera polymerization zagwiritsidwa ntchito kuti ziwongolere kuyendetsa bwino kwa ma electrolyte a polymer ochokera ku PVA kuti achepetse matrix crystallinity ndikuwonjezera kusinthasintha kwa unyolo18,19,20.
Kusakaniza ndi njira yofunika kwambiri popanga zinthu zopangidwa ndi polymeric kuti zigwiritsidwe ntchito m'mafakitale. Zosakaniza za polymer nthawi zambiri zimagwiritsidwa ntchito: (1) kukonza mphamvu zogwiritsira ntchito ma polima achilengedwe m'mafakitale; (2) kukonza mphamvu zamakemikolo, zakuthupi, ndi zamakanika za zinthu zomwe zimatha kuwonongeka; ndi (3) kusintha kufunikira kwa zinthu zatsopano zomwe zikusintha mwachangu mumakampani opaka chakudya. Mosiyana ndi copolymerization, kusakaniza kwa polymer ndi njira yotsika mtengo yomwe imagwiritsa ntchito njira zosavuta zakuthupi m'malo mwa njira zovuta zamakemikolo kuti ikwaniritse zomwe mukufuna21. Kuti apange ma homopolymer, ma polima osiyanasiyana amatha kuyanjana kudzera mu mphamvu za dipole-dipole, ma hydrogen bonds, kapena ma charge-transfer complexes22,23. Zosakaniza zopangidwa kuchokera ku ma polima achilengedwe ndi opangidwa zimatha kuphatikiza biocompatibility yabwino ndi mphamvu zabwino zamakanika, ndikupanga chinthu chapamwamba pamtengo wotsika wopanga24,25. Chifukwa chake, pakhala chidwi chachikulu popanga zinthu zopangidwa ndi polymeric mwa kusakaniza ma polima opangidwa ndi achilengedwe. PVA ikhoza kuphatikizidwa ndi sodium alginate (NaAlg), cellulose, chitosan ndi starch26.
Sodium alginate ndi polysaccharide yachilengedwe ya polymer ndi anionic yochokera ku algae yakuda ya m'nyanja. Sodium alginate imakhala ndi β-(1-4)-linked D-mannuronic acid (M) ndi α-(1-4)-linked L-guluronic acid (G) yokonzedwa m'mitundu ya homopolymeric (poly-M ndi poly-G) ndi heteropolymeric blocks (MG kapena GM)27. Kuchuluka ndi chiŵerengero cha M ndi G blocks zimakhudza kwambiri mankhwala ndi thupi la alginate28,29. Sodium alginate imagwiritsidwa ntchito kwambiri ndipo imaphunziridwa chifukwa cha kuwonongeka kwake, kuyanjana ndi thupi, mtengo wotsika, mphamvu zabwino zopangira filimu, komanso kusapha poizoni. Komabe, magulu ambiri a free hydroxyl (OH) ndi carboxylate (COO) mu unyolo wa alginate amapangitsa alginate kukhala yokonda madzi kwambiri. Komabe, alginate ili ndi mphamvu zochepa zamakanika chifukwa cha kufooka kwake komanso kuuma kwake. Chifukwa chake, alginate ikhoza kuphatikizidwa ndi zinthu zina zopangira kuti ziwongolere kukhudzidwa kwa madzi ndi mphamvu zamakina30,31.
Asanapange zipangizo zatsopano za electrode, mawerengedwe a DFT nthawi zambiri amagwiritsidwa ntchito poyesa kuthekera kwa kupanga zinthu zatsopano. Kuphatikiza apo, asayansi amagwiritsa ntchito ma molecular modeling kuti atsimikizire ndikulosera zotsatira zoyesera, kusunga nthawi, kuchepetsa zinyalala za mankhwala, ndi kulosera machitidwe oyanjana32. Ma molecular modeling akhala nthambi yamphamvu komanso yofunika kwambiri ya sayansi m'magawo ambiri, kuphatikiza sayansi ya zinthu, nanomaterials, chemistry ya makompyuta, ndi kupeza mankhwala33,34. Pogwiritsa ntchito mapulogalamu a ma modeling, asayansi amatha kupeza mwachindunji deta ya ma molecular, kuphatikiza mphamvu (kutentha kwa mapangidwe, ionization potential, activation energy, etc.) ndi geometry (ma bond angles, bond lengths, ndi torsion angles)35. Kuphatikiza apo, katundu wamagetsi (charge, HOMO ndi LUMO band gap energy, electron affinity), katundu wa ma spectral (ma characteristic vibrational modes and intensities monga FTIR spectra), ndi katundu wambiri (volume, diffusion, viscosity, modulus, etc.)36 akhoza kuwerengedwa.
LiNiPO4 ikuwonetsa zabwino zomwe zingatheke popikisana ndi zinthu za lithiamu-ion batire positive electrode chifukwa cha kuchuluka kwake kwa mphamvu (voltage yogwira ntchito ya pafupifupi 5.1 V). Kuti agwiritse ntchito bwino ubwino wa LiNiPO4 m'dera la high-voltage, voltage yogwira ntchito iyenera kuchepetsedwa chifukwa electrolyte yapamwamba yomwe yapangidwa pakadali pano ingakhale yokhazikika pa voltages pansi pa 4.8 V. Zhang et al. adafufuza za doping ya zitsulo zonse za 3d, 4d, ndi 5d transition pamalo a Ni a LiNiPO4, adasankha njira zopangira doping zomwe zili ndi magwiridwe antchito abwino kwambiri a electrochemical, ndipo adasintha voltage yogwira ntchito ya LiNiPO4 pomwe akusunga kukhazikika kwa magwiridwe antchito ake a electrochemical. Voltage yogwira ntchito yotsika kwambiri yomwe adapeza inali 4.21, 3.76, ndi 3.5037 ya Ti, Nb, ndi Ta-doped LiNiPO4, motsatana.
Chifukwa chake, cholinga cha kafukufukuyu ndikufufuza mwachiphunzitso momwe glycerol imagwirira ntchito ngati pulasitiki pamagetsi, mafotokozedwe a QSAR ndi mawonekedwe a kutentha kwa PVA/NaAlg system pogwiritsa ntchito mawerengedwe a quantum mechanical kuti igwiritsidwe ntchito m'mabatire a ion-ion omwe angadzazidwenso. Kuyanjana kwa mamolekyulu pakati pa chitsanzo cha PVA/NaAlg ndi glycerol kunasanthulidwa pogwiritsa ntchito chiphunzitso cha Bader cha quantum atomic of molecules (QTAIM).
Chitsanzo cha molekyulu chomwe chikuyimira kuyanjana kwa PVA ndi NaAlg kenako ndi glycerol chinakonzedwa bwino pogwiritsa ntchito DFT. Chitsanzocho chinawerengedwa pogwiritsa ntchito pulogalamu ya Gaussian 0938 ku Spectroscopy Department, National Research Center, Cairo, Egypt. Zitsanzozo zinakonzedwa bwino pogwiritsa ntchito DFT pa B3LYP/6-311G(d, p) level39,40,41,42. Kuti atsimikizire kuyanjana pakati pa zitsanzo zomwe zaphunziridwa, maphunziro a pafupipafupi omwe amachitika pamlingo womwewo wa chiphunzitso akuwonetsa kukhazikika kwa geometry yokonzedwa bwino. Kusowa kwa ma frequency oipa pakati pa ma frequency onse omwe ayesedwa kukuwonetsa kapangidwe kamene kaganiziridwa mu minima yeniyeni yabwino pamwamba pa mphamvu yomwe ingakhalepo. Ma parameter a thupi monga TDM, HOMO/LUMO band gap energy ndi MESP adawerengedwa pamlingo womwewo wa quantum mechanical wa chiphunzitso. Kuphatikiza apo, magawo ena a kutentha monga kutentha komaliza kwa kapangidwe, mphamvu yaulere, entropy, enthalpy ndi mphamvu ya kutentha adawerengedwa pogwiritsa ntchito njira zomwe zaperekedwa mu Gome 1. Ma model omwe adaphunziridwa adayesedwa ndi chiphunzitso cha quantum cha ma atomu mu mamolekyu (QTAIM) kuti adziwe momwe zinthu zimachitikira pamwamba pa kapangidwe kamene kaphunziridwa. Mawerengedwe awa adachitika pogwiritsa ntchito lamulo la "output=wfn" mu code ya pulogalamu ya Gaussian 09 kenako adawonetsedwa pogwiritsa ntchito code ya pulogalamu ya Avogadro43.
Pamene E ndi mphamvu yamkati, P ndi mphamvu, V ndi voliyumu, Q ndi kusinthana kwa kutentha pakati pa dongosolo ndi malo ake, T ndi kutentha, ΔH ndi kusintha kwa enthalpy, ΔG ndi kusintha kwa mphamvu yaulere, ΔS ndi kusintha kwa entropy, a ndi b ndi magawo ogwedezeka, q ndi mphamvu ya atomiki, ndipo C ndi kuchuluka kwa ma electron a atomiki44,45. Pomaliza, mapangidwe omwewo adakonzedwa bwino ndipo magawo a QSAR adawerengedwa pamlingo wa PM6 pogwiritsa ntchito SCIGRESS software code46 ku Spectroscopy Department of the National Research Center ku Cairo, Egypt.
Mu ntchito yathu yapitayi47, tinayesa chitsanzo chomwe chingakhale chotheka kwambiri chofotokoza momwe mayunitsi atatu a PVA amagwirira ntchito ndi mayunitsi awiri a NaAlg, pomwe glycerol imagwira ntchito ngati pulasitiki. Monga tafotokozera pamwambapa, pali njira ziwiri zomwe PVA ndi NaAlg zingagwirizanitsire ntchito. Mitundu iwiriyi, yomwe imatchedwa 3PVA-2Na Alg (yochokera pa nambala ya kaboni 10) ndi Term 1Na Alg-3PVA-Mid 1Na Alg, ili ndi kusiyana kochepa kwambiri kwa mphamvu48 poyerekeza ndi kapangidwe kena komwe kaganiziridwa. Chifukwa chake, zotsatira za kuwonjezera kwa Gly pa chitsanzo chomwe chingakhale chotheka kwambiri cha polymer yosakaniza ya PVA/Na Alg zidafufuzidwa pogwiritsa ntchito mapangidwe awiri omaliza: 3PVA-(C10)2Na Alg (yotchedwa 3PVA-2Na Alg potanthauza kuphweka) ndi Term 1 Na Alg − 3PVA-Mid 1 Na Alg. Malinga ndi mabuku, PVA, NaAlg ndi glycerol zimatha kupanga ma hydrogen bond ofooka pakati pa magulu ogwira ntchito a hydroxyl. Popeza PVA trimer ndi NaAlg ndi glycerol dimer zonse zili ndi magulu angapo a OH, kukhudzanako kumatha kuchitika kudzera m'gulu limodzi la OH. Chithunzi 1 chikuwonetsa kuyanjana pakati pa molekyulu ya glycerol ya chitsanzo ndi molekyulu ya chitsanzo 3PVA-2Na Alg, ndipo Chithunzi 2 chikuwonetsa chitsanzo chomangidwa cha kuyanjana pakati pa molekyulu ya chitsanzo Term 1Na Alg-3PVA-Mid 1Na Alg ndi kuchuluka kosiyanasiyana kwa glycerol.
Kapangidwe kokonzedwa bwino: (a) Gly ndi 3PVA − 2Na Alg zimagwirizana ndi (b) 1 Gly, (c) 2 Gly, (d) 3 Gly, (e) 4 Gly, ndi (f) 5 Gly.
Kapangidwe kabwino ka Term 1Na Alg- 3PVA –Mid 1Na Alg yolumikizana ndi (a) 1 Gly, (b) 2 Gly, (c) 3 Gly, (d) 4 Gly, (e) 5 Gly, ndi (f) 6 Gly.
Mphamvu ya electron band gap ndi chinthu chofunikira kuganizira pophunzira reactivity ya electrode iliyonse. Chifukwa imafotokoza momwe ma electron amagwirira ntchito pamene zinthuzo zikusinthidwa ndi zinthu zakunja. Chifukwa chake, ndikofunikira kuyerekeza mphamvu ya electron band gap ya HOMO/LUMO pa kapangidwe kake konse komwe kaphunziridwa. Gome 2 likuwonetsa kusintha kwa mphamvu za HOMO/LUMO za 3PVA-(C10)2Na Alg ndi Term 1Na Alg − 3PVA-Mid 1Na Alg chifukwa cha kuwonjezera kwa glycerol. Malinga ndi ref47, Eg value ya 3PVA-(C10)2Na Alg ndi 0.2908 eV, pomwe Eg value ya kapangidwe kake ikuwonetsa kuthekera kwa kuyanjana kwachiwiri (mwachitsanzo, Term 1Na Alg − 3PVA-Mid 1Na Alg) ndi 0.5706 eV.
Komabe, zinapezeka kuti kuwonjezera kwa glycerol kunapangitsa kusintha pang'ono kwa Eg value ya 3PVA-(C10)2Na Alg. Pamene 3PVA-(C10)2NaAlg inalumikizana ndi mayunitsi a glycerol 1, 2, 3, 4 ndi 5, ma Eg values ​​​​ake anakhala 0.302, 0.299, 0.308, 0.289 ndi 0.281 eV, motsatana. Komabe, pali chidziwitso chofunikira kuti pambuyo powonjezera mayunitsi atatu a glycerol, Eg value inakhala yocheperapo kuposa ya 3PVA-(C10)2Na Alg. Chitsanzo chomwe chikuyimira kuyanjana kwa 3PVA-(C10)2Na Alg ndi mayunitsi asanu a glycerol ndiye chitsanzo chogwirizana kwambiri. Izi zikutanthauza kuti pamene chiwerengero cha mayunitsi a glycerol chikuwonjezeka, mwayi wokhudzana nawo umawonjezekanso.
Pakadali pano, pa kuthekera kwachiwiri kogwirizana, mphamvu za HOMO/LUMO za mamolekyu a chitsanzo omwe akuyimira Term 1Na Alg − 3PVA –Mid 1Na Alg- 1Gly, Term 1Na Alg − 3PVA –Mid 1Na Alg- 2Gly, Term 1Na Alg − 3PVA –Mid 1Na Alg- 3Gly, Term 1Na Alg − 3PVA –Mid 1Na Alg- 4Gly, Term 1Na Alg − 3PVA –Mid 1Na Alg- 5Gly ndi Term 1Na Alg − 3PVA –Mid 1Na Alg- 6Gly zimakhala 1.343, 1.34 7, 0.976, 0.607, 0.348 ndi 0.496 eV, motsatana. Gome 2 likuwonetsa mphamvu zowerengera za HOMO/LUMO band gap za kapangidwe kake konse. Komanso, khalidwe lomwelo la kuthekera kwa kuyanjana kwa gulu loyamba likubwerezedwanso pano.
Chiphunzitso cha gulu mu fizikisi ya boma lolimba chimati pamene mpata wa gulu la zinthu za electrode ukuchepa, mphamvu yamagetsi ya zinthuzo imawonjezeka. Kupopera ndi njira yodziwika bwino yochepetsera mpata wa gulu la zinthu za sodium-ion cathode. Jiang ndi anzake adagwiritsa ntchito Cu doping kuti akonze mphamvu yamagetsi ya zinthu za β-NaMnO2. Pogwiritsa ntchito mawerengedwe a DFT, adapeza kuti kupopera ndi doping kunachepetsa mpata wa gulu la zinthuzo kuchokera pa 0.7 eV mpaka 0.3 eV. Izi zikusonyeza kuti kupopera ndi Cu doping kumakonza mphamvu yamagetsi ya zinthu za β-NaMnO2.
MESP imatanthauzidwa ngati mphamvu yolumikizirana pakati pa kugawa kwa ma molekyulu ndi mphamvu imodzi yabwino. MESP imaonedwa kuti ndi chida chothandiza kumvetsetsa ndi kutanthauzira makhalidwe a mankhwala ndi reactivity. MESP ingagwiritsidwe ntchito kumvetsetsa njira zolumikizirana pakati pa zinthu za polymeric. MESP imafotokoza kugawa kwa ma charge mkati mwa chinthu chomwe chikuphunziridwa. Kuphatikiza apo, MESP imapereka chidziwitso chokhudza malo ogwira ntchito muzinthu zomwe zikuphunziridwa32. Chithunzi 3 chikuwonetsa ma MESP plots a 3PVA-(C10) 2Na Alg, 3PVA-(C10) 2Na Alg − 1Gly, 3PVA-(C10) 2Na Alg − 2Gly, 3PVA-(C10) 2Na Alg − 3Gly, 3PVA-(C10) 2Na Alg − 4Gly, ndi 3PVA-(C10) 2Na Alg − 5Gly yoloseredwa pamlingo wa B3LYP/6-311G(d, p) wa chiphunzitso.
Ma contour a MESP owerengedwa ndi B3LYP/6-311 g(d, p) a (a) Gly ndi 3PVA − 2Na Alg yolumikizana ndi (b) 1 Gly, (c) 2 Gly, (d) 3 Gly, (e) 4 Gly, ndi (f) 5 Gly.
Pakadali pano, Chithunzi 4 chikuwonetsa zotsatira zowerengedwa za MESP za Term 1Na Alg-3PVA – Mid 1Na Alg, Term 1Na Alg-3PVA – Mid 1Na Alg-1Gly, Term 1Na Alg-3PVA – Mid 1Na Alg − 2Gly, Term 1Na Alg-3PVA – Mid 1Na Alg − 3gly, Term 1Na Alg-3PVA – Mid 1Na Alg − 4Gly, Term 1Na Alg-3PVA – Mid 1Na Alg-5gly ndi Term 1Na Alg-3PVA – Mid 1Na Alg − 6Gly, motsatana. MESP yowerengedwa imayimiridwa ngati khalidwe la contour. Mizere ya contour imayimiridwa ndi mitundu yosiyanasiyana. Mtundu uliwonse umayimira mtengo wosiyana wa electronegativity. Mtundu wofiira umasonyeza malo omwe ali ndi electronegative kwambiri kapena reactive. Pakadali pano, mtundu wachikasu umayimira malo osalowerera ndale 49, 50, 51 mu kapangidwe kake. Zotsatira za MESP zasonyeza kuti reactivity ya 3PVA-(C10)2Na Alg inakula ndi kuwonjezeka kwa mtundu wofiira kuzungulira mitundu yomwe yaphunziridwa. Pakadali pano, mphamvu ya mtundu wofiira mu mapu a MESP a molekyulu ya Term 1Na Alg-3PVA - Mid 1Na Alg imachepa chifukwa cha kuyanjana ndi kuchuluka kwa glycerol. Kusintha kwa kugawa kwa mtundu wofiira kuzungulira kapangidwe komwe kwaperekedwa kukuwonetsa reactivity, pomwe kuwonjezeka kwa mphamvu kumatsimikizira kuwonjezeka kwa electronegativity ya molekyulu ya 3PVA-(C10)2Na Alg chifukwa cha kuchuluka kwa glycerol.
B3LYP/6-311 g(d, p) inawerengedwa MESP Nthawi ya 1Na Alg-3PVA-Mid 1Na Alg yolumikizana ndi (a) 1 Gly, (b) 2 Gly, (c) 3 Gly, (d) 4 Gly, (e) 5 Gly, ndi (f) 6 Gly.
Mapangidwe onse omwe akuganiziridwa ali ndi magawo awo a kutentha monga enthalpy, entropy, mphamvu ya kutentha, mphamvu yaulere ndi kutentha kwa mapangidwe owerengedwa pa kutentha kosiyanasiyana kuyambira 200 K mpaka 500 K. Pofotokoza momwe machitidwe a thupi amagwirira ntchito, kuwonjezera pa kuphunzira machitidwe awo amagetsi, ndikofunikiranso kuphunzira momwe kutentha kumagwirira ntchito ngati kutentha chifukwa cha kuyanjana kwawo, komwe kumatha kuwerengedwa pogwiritsa ntchito ma equation omwe aperekedwa mu Table 1. Kuphunzira magawo a kutentha awa kumaonedwa ngati chizindikiro chofunikira cha kuyankha ndi kukhazikika kwa machitidwe a thupi otere pa kutentha kosiyanasiyana.
Ponena za enthalpy ya PVA trimer, imayamba kugwira ntchito ndi NaAlg dimer, kenako kudzera mu gulu la OH lomwe limalumikizidwa ku atomu ya kaboni #10, ndipo pomaliza ndi glycerol. Enthalpy ndi muyeso wa mphamvu mu dongosolo la thermodynamic. Enthalpy ndi yofanana ndi kutentha konse mu dongosolo, komwe kuli kofanana ndi mphamvu yamkati ya dongosolo kuphatikiza zomwe zimapangidwa ndi voliyumu yake ndi kupanikizika kwake. Mwanjira ina, enthalpy imasonyeza kuchuluka kwa kutentha ndi ntchito zomwe zimawonjezeredwa kapena kuchotsedwa ku chinthu52.
Chithunzi 5 chikuwonetsa kusintha kwa enthalpy panthawi ya 3PVA-(C10)2Na Alg yokhala ndi kuchuluka kosiyanasiyana kwa glycerol. Mafupikitsidwe A0, A1, A2, A3, A4, ndi A5 akuyimira mamolekyu a chitsanzo 3PVA-(C10)2Na Alg, 3PVA-(C10)2Na Alg − 1 Gly, 3PVA-(C10)2Na Alg − 2Gly, 3PVA-(C10)2Na Alg − 3Gly, 3PVA-(C10)2Na Alg − 4Gly, ndi 3PVA-(C10)2Na Alg − 5Gly, motsatana. Chithunzi 5a chikuwonetsa kuti enthalpy imawonjezeka ndi kutentha komwe kumawonjezeka komanso kuchuluka kwa glycerol. Enthalpy ya kapangidwe kamene kakuyimira 3PVA-(C10)2NaAlg − 5Gly (mwachitsanzo, A5) pa 200 K ndi 27.966 cal/mol, pomwe enthalpy ya kapangidwe kamene kakuyimira 3PVA-2NaAlg pa 200 K ndi 13.490 cal/mol. Pomaliza, popeza enthalpy ndi yabwino, izi zimachitika ngati endothermic.
Entropy imatanthauzidwa ngati muyeso wa mphamvu zomwe sizikupezeka mu dongosolo lotsekedwa la thermodynamic ndipo nthawi zambiri imaonedwa ngati muyeso wa kusokonezeka kwa dongosolo. Chithunzi 5b chikuwonetsa kusintha kwa entropy ya 3PVA-(C10)2NaAlg ndi kutentha komanso momwe imagwirira ntchito ndi mayunitsi osiyanasiyana a glycerol. Chithunzichi chikuwonetsa kuti entropy imasintha molunjika pamene kutentha kukukwera kuchokera pa 200 K mpaka 500 K. Chithunzi 5b chikuwonetsa momveka bwino kuti entropy ya chitsanzo cha 3PVA-(C10)2Na Alg imakhala ndi 200 cal/K/mol pa 200 K chifukwa chitsanzo cha 3PVA-(C10)2Na Alg chikuwonetsa kusokonezeka kochepa kwa lattice. Pamene kutentha kukukwera, chitsanzo cha 3PVA-(C10)2Na Alg chimasokonekera ndipo chimafotokoza kuwonjezeka kwa entropy ndi kutentha kukukwera. Komanso, n'zoonekeratu kuti kapangidwe ka 3PVA-C10 2Na Alg-5 Gly kali ndi entropy yapamwamba kwambiri.
Khalidwe lomweli likuwonetsedwa mu Chithunzi 5c, chomwe chikuwonetsa kusintha kwa mphamvu ya kutentha ndi kutentha. Mphamvu ya kutentha ndi kuchuluka kwa kutentha komwe kumafunika kuti musinthe kutentha kwa chinthu china ndi 1 °C47. Chithunzi 5c chikuwonetsa kusintha kwa mphamvu ya kutentha kwa molekyulu ya chitsanzo 3PVA-(C10)2NaAlg chifukwa cha kuyanjana ndi mayunitsi a glycerol 1, 2, 3, 4, ndi 5. Chithunzichi chikuwonetsa kuti mphamvu ya kutentha ya chitsanzo 3PVA-(C10)2NaAlg imawonjezeka motsatizana ndi kutentha. Kuwonjezeka kwa mphamvu ya kutentha komwe kumawonekera ndi kutentha kowonjezereka kumachitika chifukwa cha kugwedezeka kwa kutentha kwa phonon. Kuphatikiza apo, pali umboni wakuti kuwonjezereka kwa glycerol kumabweretsa kuwonjezeka kwa mphamvu ya kutentha ya chitsanzo 3PVA-(C10)2NaAlg. Kuphatikiza apo, kapangidwe kake kakuwonetsa kuti 3PVA-(C10)2NaAlg−5Gly ili ndi mphamvu yamphamvu kwambiri ya kutentha poyerekeza ndi kapangidwe kena.
Ma parameter ena monga mphamvu yaulere ndi kutentha komaliza kwa kapangidwe kake adawerengedwa pa kapangidwe kake ndipo akuwonetsedwa mu Chithunzi 5d ndi e, motsatana. Kutentha komaliza kwa kapangidwe kake ndi kutentha komwe kumatulutsidwa kapena kuyamwa panthawi yopangidwa kwa chinthu choyera kuchokera ku zinthu zake zomwe zimakhala pansi pa kupanikizika kosalekeza. Mphamvu yaulere ikhoza kutanthauziridwa ngati katundu wofanana ndi mphamvu, mwachitsanzo, mtengo wake umadalira kuchuluka kwa chinthucho mu mkhalidwe uliwonse wa thermodynamic. Mphamvu yaulere ndi kutentha kwa kapangidwe ka 3PVA-(C10)2NaAlg−5Gly zinali zotsika kwambiri ndipo zinali -1318.338 ndi -1628.154 kcal/mol, motsatana. Mosiyana ndi zimenezi, kapangidwe ka 3PVA-(C10)2NaAlg kali ndi mphamvu yaulere komanso kutentha kwa kapangidwe kake ka -690.340 ndi -830.673 kcal/mol, motsatana, poyerekeza ndi kapangidwe kake. Monga momwe zasonyezedwera mu Chithunzi 5, mitundu yosiyanasiyana ya kutentha imasinthidwa chifukwa cha kuyanjana ndi glycerol. Mphamvu yaulere ya Gibbs ndi yoyipa, zomwe zikusonyeza kuti kapangidwe kamene kakuperekedwako ndi kokhazikika.
PM6 inawerengera magawo a kutentha a 3PVA- (C10) 2Na Alg (chitsanzo A0), 3PVA- (C10) 2Na Alg − 1 Gly (chitsanzo A1), 3PVA- (C10) 2Na Alg − 2 Gly (chitsanzo A2), 3PVA- (C10) 2Na Alg − 3 Gly (chitsanzo A3), 3PVA- (C10) 2Na Alg − 4 Gly (chitsanzo A4), ndi 3PVA- (C10) 2Na Alg − 5 Gly (chitsanzo A5), komwe (a) ndi enthalpy, (b) entropy, (c) mphamvu ya kutentha, (d) mphamvu yaulere, ndi (e) kutentha kwa mapangidwe.
Kumbali inayi, njira yachiwiri yolumikizirana pakati pa PVA trimer ndi dimeric NaAlg imachitika m'magulu a terminal ndi apakati a OH mu kapangidwe ka PVA trimer. Monga momwe zinalili m'gulu loyamba, magawo a kutentha adawerengedwa pogwiritsa ntchito mulingo womwewo wa chiphunzitso. Chithunzi 6a-e chikuwonetsa kusiyanasiyana kwa enthalpy, entropy, mphamvu yotentha, mphamvu yaulere, komanso, pamapeto pake, kutentha kwa mapangidwe. Zithunzi 6a-c zikuwonetsa kuti enthalpy, entropy ndi mphamvu yotentha ya Term 1 NaAlg-3PVA-Mid 1 NaAlg zikuwonetsa khalidwe lomwelo monga gulu loyamba polumikizana ndi mayunitsi a glycerol 1, 2, 3, 4, 5 ndi 6. Kuphatikiza apo, mitengo yawo imawonjezeka pang'onopang'ono kutentha kukukwera. Kuphatikiza apo, mu Term 1 Na Alg − 3PVA-Mid 1 Na Alg yomwe ikuperekedwa, mitengo ya enthalpy, entropy ndi mphamvu yotentha idakwera ndi kuwonjezeka kwa kuchuluka kwa glycerol. Mafupikitsidwe a B0, B1, B2, B3, B4, B5 ndi B6 akuyimira mapangidwe otsatirawa motsatana: Term 1 Na Alg − 3PVA- Mid 1 Na Alg, Term 1 Na Alg- 3PVA- Mid 1 Na Alg − 1 Gly, Term 1 Na Alg- 3PVA- Mid 1 Na Alg − 2gly, Term 1 Na Alg- 3PVA- Mid 1 Na Alg − 3gly, Term 1 Na Alg- 3PVA- Mid 1 Na Alg − 4 Gly, Term 1 Na Alg- 3PVA- Mid 1 Na Alg − 5 Gly ndi Term 1 Na Alg- 3PVA- Mid 1 Na Alg − 6 Gly. Monga momwe zasonyezedwera mu Chithunzi 6a–c, n'zoonekeratu kuti kuchuluka kwa enthalpy, entropy ndi mphamvu ya kutentha kumawonjezeka pamene chiwerengero cha mayunitsi a glycerol chikukwera kuchoka pa 1 mpaka 6.
PM6 inawerengera magawo a kutentha kwa Term 1 Na Alg-3PVA- Mid 1 Na Alg (chitsanzo B0), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 1 Gly (chitsanzo B1), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 2 Gly (chitsanzo B2), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 3 Gly (chitsanzo B3), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 4 Gly (chitsanzo B4), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 5 Gly (chitsanzo B5), ndi Term 1 Na Alg-3PVA- Mid 1 Na Alg – 6 Gly (chitsanzo B6), kuphatikizapo (a) enthalpy, (b) entropy, (c) mphamvu ya kutentha, (d) mphamvu yaulere, ndi (e) kutentha kwa mapangidwe.
Kuphatikiza apo, kapangidwe kamene kakuyimira Term 1 Na Alg-3PVA- Mid 1 Na Alg-6 Gly kali ndi mphamvu yapamwamba kwambiri ya enthalpy, entropy ndi kutentha poyerekeza ndi kapangidwe kena. Pakati pawo, mphamvu zawo zinakwera kuchoka pa 16.703 cal/mol, 257.990 cal/mol/K ndi 131.323 kcal/mol mu Term 1 Na Alg − 3PVA- Mid 1 Na Alg mpaka 33.223 cal/mol, 420.038 cal/mol/K ndi 275.923 kcal/mol mu Term 1 Na Alg − 3PVA- Mid 1 Na Alg − 6 Gly, motsatana.
Komabe, Zithunzi 6d ndi e zikuwonetsa kudalira kutentha kwa mphamvu yaulere ndi kutentha komaliza kwa kapangidwe (HF). HF ikhoza kutanthauzidwa ngati kusintha kwa enthalpy komwe kumachitika pamene mole imodzi ya chinthu imapangidwa kuchokera ku zinthu zake pansi pa mikhalidwe yachilengedwe komanso yokhazikika. Zikuwonekera kuchokera pachithunzichi kuti mphamvu yaulere ndi kutentha komaliza kwa kapangidwe ka mapangidwe onse omwe aphunziridwa zikuwonetsa kudalira kolunjika pa kutentha, mwachitsanzo, zimawonjezeka pang'onopang'ono komanso molunjika ndi kutentha kowonjezereka. Kuphatikiza apo, chithunzichi chinatsimikiziranso kuti kapangidwe kamene kakuyimira Term 1 Na Alg − 3PVA- Mid 1 Na Alg − 6 Gly kali ndi mphamvu yaulere yotsika kwambiri komanso HF yotsika kwambiri. Ma parameter onsewa adatsika kuchoka pa -758.337 kufika pa -899.741 K cal/mol mu term 1 Na Alg − 3PVA- Mid 1 Na Alg − 6 Gly kufika pa -1,476.591 ndi -1,828.523 K cal/mol. Kuchokera ku zotsatira zake, zikuwoneka kuti HF imachepa ndi kuchuluka kwa mayunitsi a glycerol. Izi zikutanthauza kuti chifukwa cha kuchuluka kwa magulu ogwira ntchito, reactivity imawonjezekanso ndipo motero mphamvu zochepa zimafunika kuti tichite reaction. Izi zikutsimikizira kuti PVA/NaAlg yopangidwa ndi pulasitiki ingagwiritsidwe ntchito m'mabatire chifukwa cha reactivity yake yambiri.
Kawirikawiri, zotsatira za kutentha zimagawidwa m'mitundu iwiri: zotsatira za kutentha kochepa ndi zotsatira za kutentha kwambiri. Zotsatira za kutentha kochepa zimamveka makamaka m'maiko omwe ali m'malo okwera kwambiri, monga Greenland, Canada, ndi Russia. M'nyengo yozizira, kutentha kwa mpweya wakunja m'malo awa kumakhala pansi pa zero digiri Celsius. Moyo ndi magwiridwe antchito a mabatire a lithiamu-ion zimatha kukhudzidwa ndi kutentha kochepa, makamaka omwe amagwiritsidwa ntchito m'magalimoto amagetsi osakanikirana, magalimoto amagetsi oyera, ndi magalimoto amagetsi osakanikirana. Kuyenda mumlengalenga ndi malo ena ozizira omwe amafunikira mabatire a lithiamu-ion. Mwachitsanzo, kutentha kwa Mars kumatha kutsika kufika pa -120 digiri Celsius, zomwe zimapangitsa kuti pakhale chopinga chachikulu pakugwiritsa ntchito mabatire a lithiamu-ion mumlengalenga. Kutentha kotsika kungayambitse kuchepa kwa chiwongola dzanja chosinthira ndi zochita za mankhwala zamabatire a lithiamu-ion, zomwe zimapangitsa kuti chiwongola dzanja chofalikira cha lithiamu ions mkati mwa electrode ndi ionic conductivity mu electrolyte chichepe. Kuwonongeka kumeneku kumabweretsa kuchepa kwa mphamvu ndi mphamvu, ndipo nthawi zina ngakhale kuchepa kwa magwiridwe antchito53.
Kutentha kwakukulu kumachitika m'malo osiyanasiyana ogwiritsidwa ntchito, kuphatikizapo kutentha kwakukulu ndi kochepa, pomwe kutentha kochepa kumangokhala kokha m'malo ogwiritsidwa ntchito kutentha kochepa. Kutentha kochepa kumatsimikiziridwa makamaka ndi kutentha kozungulira, pomwe kutentha kwakukulu nthawi zambiri kumalumikizidwa molondola ndi kutentha kwakukulu mkati mwa batri ya lithiamu-ion panthawi yogwira ntchito.
Mabatire a lithiamu-ion amapanga kutentha pansi pa mikhalidwe yamphamvu yamagetsi (kuphatikizapo kuchaja mwachangu ndi kutulutsa mwachangu), zomwe zimapangitsa kutentha kwamkati kukwera. Kukhudzidwa ndi kutentha kwakukulu kungayambitsenso kuwonongeka kwa magwiridwe antchito a batri, kuphatikizapo kutayika kwa mphamvu ndi mphamvu. Nthawi zambiri, kutayika kwa lithiamu ndi kubwezeretsa zinthu zogwira ntchito kutentha kwambiri kumabweretsa kutayika kwa mphamvu, ndipo kutayika kwa mphamvu kumachitika chifukwa cha kuwonjezeka kwa kukana kwamkati. Ngati kutentha sikulamulirika, kutentha kumachitika, komwe nthawi zina kungayambitse kuyaka mwadzidzidzi kapena kuphulika.
Kuwerengera kwa QSAR ndi njira yowerengera kapena masamu yomwe imagwiritsidwa ntchito kuzindikira ubale pakati pa zochita zamoyo ndi kapangidwe ka zinthu zomwe zimapangidwa. Mamolekyu onse opangidwa adakonzedwa bwino ndipo zina mwa zinthu za QSAR zidawerengedwa pamlingo wa PM6. Gome 3 limalemba zina mwa zofotokozera za QSAR zomwe zidawerengedwa. Zitsanzo za zofotokozera zotere ndi charge, TDM, total energy (E), ionization potential (IP), Log P, ndi polarizability (onani Gome 1 kuti mudziwe njira zodziwira IP ndi Log P).
Zotsatira za kuwerengera zikusonyeza kuti mphamvu yonse ya kapangidwe kamene kaphunziridwa ndi zero chifukwa kali mu nthaka. Pa mwayi woyamba wokhudzana ndi kuyanjana, TDM ya glycerol inali 2.788 Debye ndi 6.840 Debye ya 3PVA-(C10) 2Na Alg, pomwe mitengo ya TDM idakwezedwa kufika pa 17.990 Debye, 8.848 Debye, 5.874 Debye, 7.568 Debye ndi 12.779 Debye pamene 3PVA-(C10) 2Na Alg idalumikizana ndi mayunitsi 1, 2, 3, 4 ndi 5 a glycerol, motsatana. Mtengo wa TDM ukakwera, umakweza momwe imagwirira ntchito ndi chilengedwe.
Mphamvu yonse (E) inawerengedwanso, ndipo ma E a glycerol ndi 3PVA-(C10)2 NaAlg anapezeka kuti ndi -141.833 eV ndi -200092.503 eV, motsatana. Pakadali pano, kapangidwe ka 3PVA-(C10)2 NaAlg kamalumikizana ndi mayunitsi a glycerol 1, 2, 3, 4 ndi 5; E imakhala -996.837, -1108.440, -1238.740, -1372.075 ndi -1548.031 eV, motsatana. Kuwonjezeka kwa glycerol kumabweretsa kuchepa kwa mphamvu yonse motero kumawonjezera reactivity. Kutengera kuwerengera mphamvu yonse, kunatsimikiziridwa kuti molekyulu ya chitsanzo, yomwe ndi 3PVA-2Na Alg-5 Gly, ndi yogwira ntchito kwambiri kuposa mamolekyu ena a chitsanzo. Chochitikachi chikugwirizana ndi kapangidwe kawo. 3PVA-(C10)2NaAlg ili ndi magulu awiri okha a -COONa, pomwe mapangidwe ena ali ndi magulu awiri a -COONa koma ali ndi magulu angapo a OH, zomwe zikutanthauza kuti kuchita kwawo zinthu zachilengedwe kumawonjezeka.
Kuphatikiza apo, mphamvu za ionization (IE) za kapangidwe kake zonse zaganiziridwa mu kafukufukuyu. Mphamvu ya ionization ndi gawo lofunikira poyesa reactivity ya chitsanzo chomwe chaphunziridwa. Mphamvu yofunikira kuti isunthe elekitironi kuchokera pamalo amodzi a molekyulu kupita ku infinity imatchedwa ionization energy. Imayimira mulingo wa ionization (kutanthauza reactivity) ya molekyulu. Mphamvu ya ionization ikakwera, reactivity imachepa. Zotsatira za IE za 3PVA-(C10)2NaAlg zomwe zimagwirizana ndi 1, 2, 3, 4 ndi 5 glycerol units zinali -9.256, -9.393, -9.393, -9.248 ndi -9.323 eV, motsatana, pomwe ma IE a glycerol ndi 3PVA-(C10)2NaAlg anali -5.157 ndi -9.341 eV, motsatana. Popeza kuwonjezera kwa glycerol kunapangitsa kuti phindu la IP lichepe, reactivity ya mamolekyulu inakula, zomwe zimapangitsa kuti molekyulu ya PVA/NaAlg/glycerol igwiritsidwe ntchito bwino muzipangizo zamagetsi.
Chofotokozera chachisanu mu Table 3 ndi Log P, yomwe ndi logarithm ya coefficient yogawa ndipo imagwiritsidwa ntchito kufotokoza ngati kapangidwe kamene kakuphunziridwa ndi kokonda madzi kapena kokonda madzi. Mtengo wa Log P woipa umasonyeza molekyulu yokonda madzi, kutanthauza kuti imasungunuka mosavuta m'madzi ndipo imasungunuka bwino mu zosungunulira zachilengedwe. Mtengo wabwino umasonyeza njira yosiyana.
Kutengera ndi zotsatira zomwe zapezeka, zitha kutsimikiziridwa kuti mapangidwe onse ndi okonda madzi, popeza ma Log P values ​​​​awo (3PVA-(C10)2Na Alg − 1Gly, 3PVA-(C10)2Na Alg − 2Gly, 3PVA-(C10)2Na Alg − 3Gly, 3PVA-(C10)2Na Alg − 4Gly ndi 3PVA-(C10)2Na Alg − 5Gly) ndi -3.537, -5.261, -6.342, -7.423 ndi -8.504, motsatana, pomwe Log P value ya glycerol ndi -1.081 yokha ndi 3PVA-(C10)2Na Alg ndi -3.100 yokha. Izi zikutanthauza kuti mawonekedwe a kapangidwe kamene kakuphunziridwa adzasintha pamene mamolekyu amadzi aphatikizidwa mu kapangidwe kake.
Pomaliza, kuchuluka kwa polarizability kwa kapangidwe kake konse kumawerengedwanso pamlingo wa PM6 pogwiritsa ntchito njira yofanana ndi yoyeserera. Poyamba zidanenedwa kuti kuchuluka kwa polarizability kwa zinthu zambiri kumadalira zinthu zosiyanasiyana. Chofunika kwambiri ndi kuchuluka kwa kapangidwe komwe kakuphunziridwa. Pa kapangidwe kake konse komwe kakukhudzana ndi mtundu woyamba wa kuyanjana pakati pa 3PVA ndi 2NaAlg (kuyanjana kumachitika kudzera mu atomu ya kaboni nambala 10), kuchuluka kwa polarizability kumawonjezeka powonjezera glycerol. Kuchuluka kwa polarizability kumawonjezeka kuchokera pa 29.690 Å mpaka 35.076, 40.665, 45.177, 50.239 ndi 54.638 Å chifukwa cha kuyanjana ndi mayunitsi a glycerol 1, 2, 3, 4 ndi 5. Motero, zinapezeka kuti molekyulu ya chitsanzo yomwe ili ndi polarizability yayikulu kwambiri ndi 3PVA-(C10)2NaAlg−5Gly, pomwe molekyulu ya chitsanzo yomwe ili ndi polarizability yotsika kwambiri ndi 3PVA-(C10)2NaAlg, yomwe ndi 29.690 Å.
Kuwunika kwa mafotokozedwe a QSAR kunawonetsa kuti kapangidwe ka 3PVA-(C10)2NaAlg − 5Gly ndiye kogwira mtima kwambiri pa kuyanjana koyamba komwe kwaperekedwa.
Pa njira yachiwiri yolumikizirana pakati pa PVA trimer ndi NaAlg dimer, zotsatira zake zikusonyeza kuti ma charge awo ndi ofanana ndi omwe adaperekedwa mu gawo lapitalo la kuyanjana koyamba. Mapangidwe onse ali ndi zero electronic charge, zomwe zikutanthauza kuti onse ali pansi.
Monga momwe zasonyezedwera mu Table 4, ma TDM values ​​​​(owerengedwa pa mulingo wa PM6) a Term 1 Na Alg − 3PVA-Mid 1 Na Alg adakwera kuchokera pa 11.581 Debye kufika pa 15.756, 19.720, 21.756, 22.732, 15.507, ndi 15.756 pamene Term 1 Na Alg − 3PVA-Mid 1 Na Alg idayankha ndi mayunitsi 1, 2, 3, 4, 5, ndi 6 a glycerol. Komabe, mphamvu yonse imachepa ndi kuchuluka kwa mayunitsi a glycerol, ndipo pamene Term 1 Na Alg − 3PVA- Mid 1 Na Alg ikugwirizana ndi mayunitsi enaake a glycerol (1 mpaka 6), mphamvu yonse ndi − 996.985, − 1129.013, − 1267.211, − 1321.775, − 1418.964, ndi − 1637.432 eV, motsatana.
Pa mwayi wachiwiri wokhudzana ndi kuyanjana, IP, Log P ndi polarizability zimawerengedwanso pamlingo wa PM6 wa chiphunzitso. Chifukwa chake, adaganizira zofotokozera zitatu zamphamvu kwambiri za reactivity ya mamolekyu. Pa kapangidwe kamene kakuyimira End 1 Na Alg-3PVA-Mid 1 Na Alg komwe kamagwirizana ndi mayunitsi a glycerol 1, 2, 3, 4, 5 ndi 6, IP imawonjezeka kuchokera ku −9.385 eV mpaka −8.946, −8.848, −8.430, −9.537, −7.997 ndi −8.900 eV. Komabe, mtengo wowerengedwa wa Log P unali wotsika chifukwa cha pulasitiki ya End 1 Na Alg-3PVA-Mid 1 Na Alg yokhala ndi glycerol. Pamene kuchuluka kwa glycerol kukukwera kuchoka pa 1 mpaka 6, mitengo yake imakhala -5.334, -6.415, -7.496, -9.096, -9.861 ndi -10.53 m'malo mwa -3.643. Pomaliza, deta ya polarizability inasonyeza kuti kuwonjezera kuchuluka kwa glycerol kunapangitsa kuti polarizability ya Term 1 Na Alg-3PVA-Mid 1 Na Alg ikule. Kuchuluka kwa polarizability ya molekyulu ya chitsanzo Term 1 Na Alg-3PVA-Mid 1 Na Alg kwawonjezeka kuchoka pa 31.703 Å kufika pa 63.198 Å pambuyo poyanjana ndi mayunitsi 6 a glycerol. Ndikofunika kuzindikira kuti kuwonjezera kuchuluka kwa mayunitsi a glycerol mu mwayi wachiwiri wolumikizana kumachitika kuti zitsimikizire kuti ngakhale pali maatomu ambiri ndi kapangidwe kovuta, magwiridwe antchito akadali bwino ndi kuwonjezeka kwa kuchuluka kwa glycerol. Motero, tinganene kuti chitsanzo cha PVA/Na Alg/glycerin chomwe chilipo chingalowe m'malo mwa mabatire a lithiamu-ion pang'ono, koma kafukufuku ndi chitukuko chowonjezereka chikufunika.
Kufotokozera mphamvu yomangirira pamwamba pa chinthu choyatsira magetsi ndikuwunika momwe zinthu zilili pakati pa makina kumafuna kudziwa mtundu wa mgwirizano womwe ulipo pakati pa maatomu awiri, zovuta za kuyanjana kwa mamolekyulu ndi mamolekyulu, komanso kufalikira kwa kuchuluka kwa maelekitironi pamwamba ndi adsorbent. Kuchuluka kwa maelekitironi pa mfundo yofunika kwambiri ya mgwirizano (BCP) pakati pa maatomu olumikizana ndikofunikira kwambiri poyesa mphamvu ya mgwirizano mu kusanthula kwa QTAIM. Kuchuluka kwa maelekitironi pa mphamvu ya magetsi, kuyanjana kwa maelekitironi pa mphamvu ya magetsi kumakhala kokhazikika, ndipo, kawirikawiri, kuchuluka kwa maelekitironi pa mfundo zofunika izi. Komanso, ngati kuchuluka kwa mphamvu ya magetsi (H(r)) ndi kuchuluka kwa mphamvu ya magetsi (∇2ρ(r)) zonse zili zochepa kuposa 0, izi zimasonyeza kukhalapo kwa kuyanjana kwa maelekitironi (onse). Kumbali inayi, pamene ∇2ρ(r) ndi H(r) zili zazikulu kuposa 0.54, zimasonyeza kukhalapo kwa kuyanjana kwa maelekitironi (osatsekedwa) monga ma bond ofooka a hydrogen, mphamvu za van der Waals ndi kuyanjana kwa magetsi. Kusanthula kwa QTAIM kunavumbulutsa mtundu wa kuyanjana kosagwirizana ndi covalent m'mapangidwe omwe aphunziridwa monga momwe zasonyezedwera mu Zithunzi 7 ndi 8. Kutengera kusanthulako, mamolekyu a chitsanzo omwe akuyimira 3PVA − 2Na Alg ndi Term 1 Na Alg − 3PVA –Mid 1 Na Alg adawonetsa kukhazikika kwakukulu kuposa mamolekyu omwe amalumikizana ndi mayunitsi osiyanasiyana a glycine. Izi zili choncho chifukwa kuyanjana kosagwirizana ndi covalent komwe kumapezeka kwambiri mu kapangidwe ka alginate monga kuyanjana kwa electrostatic ndi ma hydrogen bond kumathandiza alginate kukhazikika kwa ma composites. Kuphatikiza apo, zotsatira zathu zikuwonetsa kufunika kwa kuyanjana kosagwirizana ndi covalent pakati pa mamolekyu a chitsanzo cha 3PVA − 2Na Alg ndi Term 1 Na Alg − 3PVA –Mid 1 Na Alg ndi glycine, zomwe zikusonyeza kuti glycine imagwira ntchito yofunika kwambiri pakusintha chilengedwe chonse chamagetsi cha ma composites.
Kusanthula kwa QTAIM kwa molekyulu ya chitsanzo 3PVA − 2NaAlg yolumikizana ndi (a) 0 Gly, (b) 1 Gly, (c) 2 Gly, (d) 3 Gly, (e) 4 Gly, ndi (f) 5Gly.