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Ka lebaka la mohloli o mongata oa sodium, libeteri tsa sodium-ion (NIBs) li emela tharollo e 'ngoe e tšepisang bakeng sa polokelo ea matla a electrochemical. Hona joale, tšitiso e kholo nts'etsopele ea theknoloji ea NIB ke khaello ea thepa ea electrode e ka bolokang/tlosang li-ion tsa sodium ka nako e telele. Ka hona, sepheo sa thuto ena ke ho batlisisa ka khopolo-taba phello ea tlatsetso ea glycerol holim'a metsoako ea polyvinyl alcohol (PVA) le sodium alginate (NaAlg) joalo ka thepa ea electrode ea NIB. Thuto ena e shebane le litlhaloso tsa elektroniki, mocheso, le palo ea sebopeho-mosebetsi (QSAR) tsa li-electrolyte tsa polymer tse thehiloeng ho metsoako ea PVA, sodium alginate, le glycerol. Thepa ena e batlisisoa ho sebelisoa mekhoa ea semi-empirical le density functional theory (DFT). Kaha tlhahlobo ea sebopeho e senotse lintlha tsa likamano lipakeng tsa PVA/alginate le glycerol, matla a lekhalo la sehlopha (Eg) a batlisisitsoe. Liphetho li bontša hore ho eketsoa ha glycerol ho fella ka ho fokotseha ha boleng ba Eg ho 0.2814 eV. Sebaka sa matla a motlakase a limolek'hule (MESP) se bontša kabo ea libaka tse ruileng ka lielektrone le tse futsanehileng ka lielektrone le litefiso tsa limolek'hule tsamaisong eohle ea electrolyte. Litekanyetso tsa mocheso tse ithutiloeng li kenyelletsa enthalpy (H), entropy (ΔS), bokhoni ba mocheso (Cp), matla a mahala a Gibbs (G) le mocheso oa sebopeho. Ho phaella moo, litlhaloso tse 'maloa tsa kamano ea sebopeho-mosebetsi (QSAR) tse kang motsotso o felletseng oa dipole (TDM), matla a felletseng (E), bokhoni ba ionization (IP), Log P le polarizability li ile tsa hlahlojoa thutong ena. Liphetho li bontšitse hore H, ΔS, Cp, G le TDM li eketsehile ka mocheso o ntseng o eketseha le litaba tsa glycerol. Ho sa le joalo, mocheso oa sebopeho, IP le E o ile oa fokotseha, e leng se ileng sa ntlafatsa reactivity le polarizability. Ho phaella moo, ka ho eketsa glycerol, motlakase oa sele o ile oa eketseha ho ea ho 2.488 V. DFT le PM6 lipalo tse thehiloeng ho li-electrolyte tse thehiloeng ho PVA/Na Alg glycerol tse theko e tlaase li bontša hore li ka nkela libeteri tsa lithium-ion sebaka ka karolo e itseng ka lebaka la mesebetsi ea tsona e mengata, empa ho hlokahala lintlafatso le lipatlisiso tse ling.
Leha libeteri tsa lithium-ion (LIBs) li sebelisoa haholo, ts'ebeliso ea tsona e tobane le mefokolo e mengata ka lebaka la bophelo ba tsona bo bokhutšoanyane ba potoloho, litšenyehelo tse phahameng le matšoenyeho a polokeho. Libeteri tsa sodium-ion (SIBs) li ka fetoha mokhoa o mong o sebetsang ho feta li-LIB ka lebaka la ho fumaneha ha tsona ka bongata, litšenyehelo tse tlase, le ho se be chefo ha karolo ea sodium. Libeteri tsa sodium-ion (SIBs) li ntse li fetoha sistimi ea bohlokoa ea polokelo ea matla bakeng sa lisebelisoa tsa electrochemical1. Libeteri tsa sodium-ion li itšetleha haholo ka li-electrolyte ho nolofatsa ho tsamaisoa ha li-ion le ho hlahisa motlakase oa motlakase2,3. Li-electrolyte tse metsi li entsoe haholo ka letsoai la tšepe le li-solvents tsa organic. Ts'ebeliso e sebetsang e hloka ho nahanoa ka hloko ka polokeho ea li-electrolyte tse metsi, haholo-holo ha betri e le tlas'a khatello ea mocheso kapa ea motlakase4.
Libetri tsa sodium-ion (SIBs) li lebelletsoe ho nkela libetri tsa lithium-ion sebaka haufinyane ka lebaka la mehloli ea tsona e mengata ea leoatle, ho se be chefo, le litšenyehelo tse tlase tsa thepa. Ho kopanngoa ha li-nanomaterials ho potlakisitse nts'etsopele ea polokelo ea data, lisebelisoa tsa elektroniki le tsa optical. Lingoliloeng tse ngata li bontšitse ts'ebeliso ea li-nanostructures tse fapaneng (mohlala, li-oxide tsa tšepe, graphene, li-nanotubes, le li-fullerene) libetri tsa sodium-ion. Lipatlisiso li shebane le nts'etsopele ea thepa ea anode, ho kenyeletsoa le li-polymer, bakeng sa libetri tsa sodium-ion ka lebaka la ho tenyetseha ha tsona le botsoalle ba tikoloho. Thahasello ea lipatlisiso lefapheng la libetri tsa polymer tse ka tjhajwang hape ntle le pelaelo e tla eketseha. Lisebelisoa tse ncha tsa polymer electrode tse nang le meaho le thepa e ikhethang li ka 'na tsa bula tsela bakeng sa mahlale a polokelo ea matla a mosa tikolohong. Le hoja lisebelisoa tse fapaneng tsa polymer electrode li 'nile tsa hlahlojoa bakeng sa tšebeliso libetri tsa sodium-ion, tšimo ena e ntse e le mehatong ea eona ea pele ea nts'etsopele. Bakeng sa libetri tsa sodium-ion, lisebelisoa tse ling tsa polymer tse nang le litlhophiso tse fapaneng tsa sebopeho li hloka ho hlahlojoa. Ho latela tsebo ea rona ea hona joale ea mokhoa oa ho boloka li-ion tsa sodium ka har'a thepa ea electrode ea polymer, ho ka nahanoa hore lihlopha tsa carbonyl, li-radical tse lokolohileng, le li-heteroatom tsamaisong e kopantsoeng li ka sebetsa e le libaka tse sebetsang tsa ho sebelisana le li-ion tsa sodium. Ka hona, ho bohlokoa ho nts'etsapele li-polymer tse ncha tse nang le bongata bo phahameng ba libaka tsena tse sebetsang. Gel polymer electrolyte (GPE) ke theknoloji e 'ngoe e ntlafatsang ts'epo ea betri, conductivity ea li-ion, ho se lutle, ho tenyetseha ho hoholo, le ts'ebetso e ntle12.
Li-matrices tsa polymer li kenyelletsa thepa e kang PVA le polyethylene oxide (PEO)13. Polymer e kenang ka gel (GPE) e thibela electrolyte e metsi ka har'a matrix ea polymer, e fokotsang kotsi ea ho lutla ha e bapisoa le li-aparthor tsa khoebo14. PVA ke polymer ea maiketsetso e bolang. E na le tumello e phahameng, ha e theko e tlase ebile ha e na chefo. Thepa ena e tsebahala ka thepa ea eona ea ho etsa filimi, botsitso ba lik'hemik'hale le ho khomarela. E boetse e na le lihlopha tse sebetsang (OH) le bongata bo phahameng ba bokhoni ba ho hokahanya15,16,17. Ho kopanya polymer, ho eketsa plasticizer, ho eketsa metsoako le mekhoa ea polymerization ea in situ e sebelisitsoe ho ntlafatsa conductivity ea li-electrolyte tsa polymer tse thehiloeng ho PVA ho fokotsa kristale ea matrix le ho eketsa ho tenyetseha ha ketane18,19,20.
Ho kopanya ke mokhoa oa bohlokoa oa ho nts'etsapele thepa ea polymeric bakeng sa lits'ebetso tsa indasteri. Metswako ea polymer hangata e sebelisetsoa ho: (1) ntlafatsa litšobotsi tsa ts'ebetso ea li-polymer tsa tlhaho lits'ebetsong tsa indasteri; (2) ntlafatsa litšobotsi tsa lik'hemik'hale, tsa 'mele le tsa mechini tsa thepa e ka bolang; le (3) ho ikamahanya le tlhoko e fetohang ka potlako ea lisebelisoa tse ncha indastering ea ho paka lijo. Ho fapana le copolymerization, ho kopanya polymer ke ts'ebetso e theko e tlase e sebelisang lits'ebetso tse bonolo tsa 'mele ho fapana le lits'ebetso tse rarahaneng tsa lik'hemik'hale ho fihlela litšobotsi tse lakatsehang21. Ho theha li-homopolymer, li-polymer tse fapaneng li ka sebelisana ka matla a dipole-dipole, libofo tsa hydrogen, kapa li-complexes tsa charge-transfer22,23. Metswako e entsoeng ka li-polymer tsa tlhaho le tsa maiketsetso e ka kopanya biocompatibility e ntle le litšobotsi tse ntle tsa mechini, e leng se etsang thepa e phahameng ka litšenyehelo tse tlase tsa tlhahiso24,25. Ka hona, ho bile le thahasello e kholo ho theheng thepa ea polymeric e amanang le biorelevant ka ho kopanya li-polymer tsa maiketsetso le tsa tlhaho. PVA e ka kopanngoa le sodium alginate (NaAlg), cellulose, chitosan le starch26.
Sodium alginate ke polysaccharide ea tlhaho ea polymer le anionic e nkiloeng ho algae e sootho ea leoatle. Sodium alginate e na le β-(1-4)-linked D-mannuronic acid (M) le α-(1-4)-linked L-guluronic acid (G) e hlophisitsoeng ka mefuta ea homopolymeric (poly-M le poly-G) le heteropolymeric blocks (MG kapa GM)27. Karolelano ea dikahare le kamano ea li-block tsa M le G li na le phello e kholo thepeng ea lik'hemik'hale le ea 'mele ea alginate28,29. Sodium alginate e sebelisoa haholo le ho ithutoa ka lebaka la ho bola ha eona, ho lumellana ha eona le lintho tse phelang, litšenyehelo tse tlase, thepa e ntle ea ho etsa filimi, le ho se chefo. Leha ho le joalo, palo e kholo ea lihlopha tsa free hydroxyl (OH) le carboxylate (COO) tse ketane ea alginate e etsa hore alginate e be le hydrophilic haholo. Leha ho le joalo, alginate e na le thepa e fokolang ea mechini ka lebaka la ho robeha le ho tiea ha eona. Ka hona, alginate e ka kopanngoa le thepa e meng ea maiketsetso ho ntlafatsa kutloisiso ea metsi le thepa ea mechini30,31.
Pele ho ralwa thepa e ncha ea electrode, lipalo tsa DFT hangata li sebelisoa ho lekola monyetla oa tlhahiso ea thepa e ncha. Ho phaella moo, bo-rasaense ba sebelisa mohlala oa limolek'hule ho netefatsa le ho bolela esale pele liphetho tsa liteko, ho boloka nako, ho fokotsa litšila tsa lik'hemik'hale, le ho bolela esale pele boitšoaro ba tšebelisano-'moho32. Mohlala oa limolek'hule e se e le lekala le matla le la bohlokoa la saense masimong a mangata, ho kenyeletsoa saense ea thepa, lisebelisoa tsa nanomaterials, k'hemistri ea k'homphieutha, le ho sibolloa ha lithethefatsi33,34. Ka ho sebelisa mananeo a mohlala, bo-rasaense ba ka fumana data ea limolek'hule ka kotloloho, ho kenyeletsoa matla (mocheso oa sebopeho, bokhoni ba ionization, matla a ts'ebetso, jj.) le geometry (likhutlo tsa bond, bolelele ba bond, le likhutlo tsa torsion)35. Ho phaella moo, thepa ea elektroniki (chaja, matla a HOMO le LUMO band gap, electron affinity), thepa ea spectral (mekhoa ea ho thothomela le matla a ikhethang joalo ka li-spectra tsa FTIR), le thepa ea bongata (bophahamo, ho hasana, viscosity, modulus, jj.)36 li ka baloa.
LiNiPO4 e bonts'a melemo e ka bang teng ea ho qothisana lehlokoa le lisebelisoa tsa electrode tse ntle tsa betri ea lithium-ion ka lebaka la boima ba eona bo phahameng ba matla (voltage e sebetsang ea hoo e ka bang 5.1 V). Ho sebelisa ka botlalo molemo oa LiNiPO4 sebakeng se nang le motlakase o phahameng, motlakase o sebetsang o hloka ho theoloa hobane electrolyte e ntlafalitsoeng hona joale e ka lula e tsitsitse feela maemong a tlase ho 4.8 V. Zhang le ba bang ba batlisisitse doping ea litšepe tsohle tsa phetoho tsa 3d, 4d, le 5d sebakeng sa Ni sa LiNiPO4, ba khethile mekhoa ea doping e nang le ts'ebetso e ntle ea electrochemical, 'me ba fetola voltage e sebetsang ea LiNiPO4 ha ba ntse ba boloka botsitso bo lekanyelitsoeng ba ts'ebetso ea eona ea electrochemical. Li-voltage tse tlase ka ho fetisisa tsa ts'ebetso tseo ba li fumaneng e ne e le 4.21, 3.76, le 3.5037 bakeng sa Ti, Nb, le Ta-doped LiNiPO4, ka ho latellana.
Ka hona, sepheo sa phuputso ena ke ho batlisisa ka khopolo-taba phello ea glycerol e le plasticizer holim'a thepa ea elektroniki, litlhaloso tsa QSAR le thepa ea mocheso ea sistimi ea PVA/NaAlg ho sebelisoa lipalo tsa mechini ea quantum bakeng sa ts'ebeliso ea eona libetering tsa ion-ion tse ka nchafatsoang. Likamano tsa limolek'hule pakeng tsa mohlala oa PVA/NaAlg le glycerol li hlahlobiloe ho sebelisoa khopolo-taba ea Bader ea quantum atom of molecules (QTAIM).
Mohlala oa molek'hule o emelang tšebelisano ea PVA le NaAlg ebe o na le glycerol o ntlafalitsoe ho sebelisoa DFT. Mohlala o baliloe ho sebelisoa software ea Gaussian 0938 Lefapheng la Spectroscopy, Setsi sa Lipatlisiso sa Naha, Cairo, Egepeta. Mehlala e ntlafalitsoe ho sebelisoa DFT boemong ba B3LYP/6-311G(d, p)39,40,41,42. Ho netefatsa tšebelisano lipakeng tsa mehlala e ithutiloeng, lithuto tsa maqhubu tse entsoeng boemong bo tšoanang ba khopolo-taba li bontša botsitso ba geometry e ntlafalitsoeng. Ho ba sieo ha maqhubu a fosahetseng har'a maqhubu 'ohle a hlahlobiloeng ho totobatsa sebopeho se hakantsoeng minima ea 'nete e ntle holim'a bokaholimo ba matla a ka bang teng. Liparamente tsa 'mele tse kang TDM, matla a HOMO/LUMO band gap le MESP li baliloe boemong bo tšoanang ba khopolo-taba ea quantum mechanical. Ho phaella moo, diparamitha tse ding tsa mocheso tse kang mocheso wa ho qetela wa sebopeho, matla a mahala, entropy, enthalpy le bokgoni ba mocheso di badilwe ho sebediswa diforomo tse fanweng ho Tafole ya 1. Dikai tse ithutwang di ile tsa fuwa tlhahlobo ya khopolo ya quantum ya diathomo ka hara dimolekhule (QTAIM) e le ho hlwaya dikamano tse etsahalang hodima dibopeho tse ithutwang. Dipalo tsena di entswe ho sebediswa taelo ya "output=wfn" khoutung ya software ya Gaussian 09 mme tsa bontshwa ka setshwantsho ho sebediswa khoutu ya software ya Avogadro43.
Moo E e leng matla a ka hare, P ke kgatello, V ke bophahamo ba modumo, Q ke phapanyetsano ya mocheso pakeng tsa sistimi le tikoloho ya yona, T ke mocheso, ΔH ke phetoho ya enthalpy, ΔG ke phetoho ya matla a mahala, ΔS ke phetoho ya entropy, a le b ke diparamithara tsa ho thothomela, q ke tjhaja ya athomo, mme C ke bongata ba dielektrone tsa athomo44,45. Qetellong, dibopeho tse tshwanang di ile tsa ntlafatswa mme diparamithara tsa QSAR di ile tsa balwa boemong ba PM6 ho sebediswa khoutu ya software ya SCIGRESS46 Lefapheng la Spectroscopy la Setsi sa Naha sa Diphuputso se Cairo, Egepeta.
Mosebetsing oa rona o fetileng47, re hlahlobile mohlala o ka bang teng ka ho fetisisa o hlalosang tšebelisano-'moho ea li-unit tse tharo tsa PVA le li-unit tse peli tsa NaAlg, 'me glycerol e sebetsa e le plasticizer. Joalokaha ho boletsoe kaholimo, ho na le menyetla e 'meli ea tšebelisano-'moho ea PVA le NaAlg. Mefuta e 'meli, e khethiloeng e le 3PVA-2Na Alg (e thehiloeng ho nomoro ea carbon 10) le Term 1Na Alg-3PVA-Mid 1Na Alg, e na le boleng bo fokolang ba sekheo sa matla48 ha e bapisoa le meaho e meng e nahanoang. Ka hona, phello ea tlatsetso ea Gly mohlaleng o ka bang teng ka ho fetisisa oa polymer ea motsoako oa PVA/Na Alg e hlahlobiloe ho sebelisoa meaho e 'meli ea morao-rao: 3PVA-(C10)2Na Alg (e bitsoang 3PVA-2Na Alg bakeng sa bonolo) le Term 1 Na Alg − 3PVA-Mid 1 Na Alg. Ho ea ka lingoliloeng, PVA, NaAlg le glycerol li ka theha feela litlamo tse fokolang tsa haedrojene pakeng tsa lihlopha tse sebetsang tsa hydroxyl. Kaha trimer ea PVA le NaAlg le glycerol dimer li na le lihlopha tse 'maloa tsa OH, ho kopana ho ka bonoa ka e 'ngoe ea lihlopha tsa OH. Setšoantšo sa 1 se bontša tšebelisano pakeng tsa molek'hule ea glycerol ea mohlala le molek'hule ea mohlala ea 3PVA-2Na Alg, 'me Setšoantšo sa 2 se bontša mohlala o hahiloeng oa tšebelisano pakeng tsa molek'hule ea mohlala Term 1Na Alg-3PVA-Mid 1Na Alg le mahloriso a fapaneng a glycerol.
Meaho e ntlafaditsweng: (a) Gly le 3PVA − 2Na Alg di sebelisana le (b) 1 Gly, (c) 2 Gly, (d) 3 Gly, (e) 4 Gly, le (f) 5 Gly.
Dibopeho tse ntlafaditsweng tsa Term 1Na Alg- 3PVA –Mid 1Na Alg e sebelisanang le (a) 1 Gly, (b) 2 Gly, (c) 3 Gly, (d) 4 Gly, (e) 5 Gly, le (f) 6 Gly.
Matla a lekhalo la sehlopha sa dielektrone ke parameter ya bohlokwa eo o lokelang ho e nahana ha o ithuta ka karabelo ya thepa efe kapa efe ya dielektrode. Hobane e hlalosa boitshwaro ba dielektrone ha thepa e fetoha ka ntle. Ka hona, ho a hlokahala ho hakanya matla a lekhalo la sehlopha sa dielektrone a HOMO/LUMO bakeng sa dibopeho tsohle tse ithutwang. Tafole ya 2 e bontsha diphetoho matla a HOMO/LUMO a 3PVA-(C10)2Na Alg le Term 1Na Alg − 3PVA- Mid 1Na Alg ka lebaka la ho eketswa ha glycerol. Ho ya ka ref47, boleng ba Eg ba 3PVA-(C10)2Na Alg ke 0.2908 eV, ha boleng ba Eg ba sebopeho bo bontsha kgonahalo ya tshebedisano ya bobedi (ke hore, Term 1Na Alg − 3PVA- Mid 1Na Alg) ke 0.5706 eV.
Leha ho le jwalo, ho ile ha fumanwa hore ho eketsoa ha glycerol ho bakile phetoho e nyane boleng ba Eg ba 3PVA-(C10)2Na Alg. Ha 3PVA-(C10)2NaAlg e sebelisana le diyuniti tsa glycerol tsa 1, 2, 3, 4 le 5, boleng ba yona ba Eg e bile 0.302, 0.299, 0.308, 0.289 le 0.281 eV, ka ho latellana. Leha ho le jwalo, ho na le temohisiso ya bohlokwa ya hore kamora ho eketsa diyuniti tse 3 tsa glycerol, boleng ba Eg bo ile ba ba bonyenyane ho feta ba 3PVA-(C10)2Na Alg. Mohlala o emelang tshebedisano ya 3PVA-(C10)2Na Alg ka diyuniti tse hlano tsa glycerol ke mohlala o ka bang teng wa tshebedisano. Sena se bolela hore ha palo ya diyuniti tsa glycerol e ntse e eketseha, monyetla wa tshebedisano le wona o a eketseha.
Ho sa le jwalo, bakeng sa monyetla wa bobedi wa tshebedisano, matla a HOMO/LUMO a dimolek'hule tsa mohlala tse emelang 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 le Term 1Na Alg − 3PVA –Mid 1Na Alg- 6Gly e ba 1.343, 1.34 7, 0.976, 0.607, 0.348 le 0.496 eV, ka ho latellana. Tafole ya 2 e bontsha matla a HOMO/LUMO a balwang a lekhalo la sehlopha bakeng sa dibopeho tsohle. Ho feta moo, boits'oaro bo tšoanang ba menyetla ea tšebelisano-'moho ea sehlopha sa pele bo phetoa mona.
Khopolo-taba ea sehlopha fisiks ea boemo bo tiileng e bolela hore ha lekhalo la sehlopha sa thepa ea electrode le fokotseha, ho khanna ha motlakase ka motlakase ha thepa hoa eketseha. Ho sebelisa doping ke mokhoa o tloaelehileng oa ho fokotsa lekhalo la sehlopha sa thepa ea cathode ea sodium-ion. Jiang le ba bang ba sebelisitse Cu doping ho ntlafatsa ho khanna ha motlakase ka motlakase ha thepa ea β-NaMnO2 e nang le mekhahlelo. Ba sebelisa lipalo tsa DFT, ba fumane hore doping e fokotsa lekhalo la sehlopha sa thepa ho tloha ho 0.7 eV ho ea ho 0.3 eV. Sena se bontša hore Cu doping e ntlafatsa ho khanna ha motlakase ka motlakase ha thepa ea β-NaMnO2.
MESP e hlalosoa e le matla a tšebelisano pakeng tsa kabo ea tjhaja ea limolek'hule le tjhaja e le 'ngoe e ntle. MESP e nkoa e le sesebelisoa se sebetsang sa ho utloisisa le ho toloka litšobotsi tsa lik'hemik'hale le reactivity. MESP e ka sebelisoa ho utloisisa mekhoa ea likamano lipakeng tsa thepa ea polymeric. MESP e hlalosa kabo ea tjhaja ka har'a motsoako o ithutoang. Ho phaella moo, MESP e fana ka tlhahisoleseling mabapi le libaka tse sebetsang thepang e ithutoang32. Setšoantšo sa 3 se bontša lipolane tsa MESP tsa 3PVA-(C10) 2Na Alg, 3PVA-(C10) 2Na Alg − 1Gly, 3PVA-(C10) 2Na Alg − 2Gly, 3PVA-(C10) 2Na Alg − 3Gly, 3PVA-(C10) 2Na Alg − 4Gly, le 3PVA-(C10) 2Na Alg − 5Gly e boletsoeng esale pele boemong ba khopolo-taba ea B3LYP/6-311G(d, p).
Meetso ea MESP e baloang ka B3LYP/6-311 g(d, p) bakeng sa (a) Gly le 3PVA − 2Na Alg e sebelisanang le (b) 1 Gly, (c) 2 Gly, (d) 3 Gly, (e) 4 Gly, le (f) 5 Gly.
Ho sa le jwalo, Setshwantsho sa 4 se bontsha diphetho tse badilweng tsa MESP bakeng sa Term 1Na Alg-3PVA – Bohareng ba 1Na Alg, Term 1Na Alg-3PVA – Bohareng ba 1Na Alg-1Gly, Term 1Na Alg-3PVA – Bohareng ba 1Na Alg − 2Gly, Term 1Na Alg-3PVA – Bohareng ba 1Na Alg − 3gly, Term 1Na Alg-3PVA – Bohareng ba 1Na Alg − 4Gly, Term 1Na Alg-3PVA – Bohareng ba 1Na Alg-5gly le Term 1Na Alg-3PVA – Bohareng ba 1Na Alg − 6Gly, ka ho latellana. MESP e badilweng e emetswe e le boitshwaro ba contour. Mela ya contour e emetswe ke mebala e fapaneng. Mmala o mong le o mong o emela boleng bo fapaneng ba electronegativity. Mmala o mofubedu o bontsha dibaka tse nang le electronegative haholo kapa tse arabelang. Ho sa le jwalo, mmala o mosehla o emela dibaka tse sa nke lehlakore 49, 50, 51 sebopehong. Liphetho tsa MESP li bontšitse hore reactivity ea 3PVA-(C10)2Na Alg e eketsehile ka keketseho ea 'mala o mofubelu ho potoloha mehlala e ithutiloeng. Ho sa le joalo, matla a 'mala o mofubelu 'mapeng oa MESP oa molek'hule ea mohlala oa Term 1Na Alg-3PVA - Mid 1Na Alg a fokotseha ka lebaka la tšebelisano le litaba tse fapaneng tsa glycerol. Phetoho kabong ea 'mala o mofubelu ho potoloha sebopeho se reriloeng e bonts'a reactivity, ha keketseho ea matla e tiisa keketseho ea electronegativity ea molek'hule ea mohlala oa 3PVA-(C10)2Na Alg ka lebaka la keketseho ea litaba tsa glycerol.
B3LYP/6-311 g(d, p) e baliloeng MESP Nako ea 1Na Alg-3PVA-Mid 1Na Alg e sebelisanang le (a) 1 Gly, (b) 2 Gly, (c) 3 Gly, (d) 4 Gly, (e) 5 Gly, le (f) 6 Gly.
Meaho eohle e reriloeng e na le liparamente tsa eona tsa mocheso tse kang enthalpy, entropy, bokhoni ba mocheso, matla a mahala le mocheso oa sebopeho tse baloang mochesong o fapaneng ho tloha ho 200 K ho isa ho 500 K. Ho hlalosa boitšoaro ba litsamaiso tsa 'mele, ntle le ho ithuta boitšoaro ba tsona ba elektroniki, ho boetse hoa hlokahala ho ithuta boitšoaro ba tsona ba mocheso e le mosebetsi oa mocheso ka lebaka la tšebelisano ea tsona, e ka baloang ho sebelisoa li-equation tse fanoeng ho Tafole ea 1. Thuto ea liparamente tsena tsa mocheso e nkoa e le sesupo sa bohlokoa sa karabelo le botsitso ba litsamaiso tse joalo tsa 'mele mochesong o fapaneng.
Ha e le enthalpy ea PVA trimer, e qala ka ho arabela le NaAlg dimer, ebe e feta sehlopheng sa OH se khomaretsoeng athomong ea carbon #10, 'me qetellong e na le glycerol. Enthalpy ke tekanyo ea matla tsamaisong ea thermodynamic. Enthalpy e lekana le mocheso oohle tsamaisong, o lekanang le matla a ka hare a tsamaiso hammoho le sehlahisoa sa bophahamo le khatello ea eona. Ka mantsoe a mang, enthalpy e bontša hore na mocheso le mosebetsi o eketsoa kapa o tlosoa hakae nthong e itseng52.
Setšoantšo sa 5 se bonts'a liphetoho tsa enthalpy nakong ea karabelo ea 3PVA-(C10)2Na Alg ka mahloriso a fapaneng a glycerol. Likhutsufatso A0, A1, A2, A3, A4, le A5 li emela limolek'hule tsa mohlala 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, le 3PVA-(C10)2Na Alg − 5Gly, ka ho latellana. Setšoantšo sa 5a se bonts'a hore enthalpy e eketseha ka mocheso o ntseng o eketseha le litaba tsa glycerol. Enthalpy ea sebopeho se emelang 3PVA-(C10)2NaAlg − 5Gly (ke hore, A5) ho 200 K ke 27.966 cal/mol, ha enthalpy ea sebopeho se emelang 3PVA-2NaAlg ho 200 K e le 13.490 cal/mol. Qetellong, kaha enthalpy e ntle, karabelo ena ke ea endothermic.
Entropy e hlalosoa e le tekanyo ea matla a sa fumaneheng tsamaisong e koetsoeng ea thermodynamic 'me hangata e nkoa e le tekanyo ea pherekano ea sistimi. Setšoantšo sa 5b se bontša phetoho ho entropy ea 3PVA-(C10)2NaAlg ka mocheso le kamoo e sebelisanang le li-unit tse fapaneng tsa glycerol. Grafo e bontša hore entropy e fetoha ka tatellano ha mocheso o ntse o eketseha ho tloha ho 200 K ho ea ho 500 K. Setšoantšo sa 5b se bontša ka ho hlaka hore entropy ea mohlala oa 3PVA-(C10)2Na Alg e atisa ho ba 200 cal/K/mol ho 200 K hobane mohlala oa 3PVA-(C10)2Na Alg o bontša pherekano e fokolang ea lattice. Ha mocheso o ntse o eketseha, mohlala oa 3PVA-(C10)2Na Alg o fetoha pherekano 'me o hlalosa keketseho ea entropy ka mocheso o ntseng o eketseha. Ho feta moo, ho totobetse hore sebopeho sa 3PVA-C10 2Na Alg-5 Gly se na le boleng bo phahameng ka ho fetisisa ba entropy.
Boitšoaro bo tšoanang bo bonoa ho Setšoantšo sa 5c, se bontšang phetoho ea bokhoni ba mocheso ka mocheso. Bokhoni ba mocheso ke bongata ba mocheso bo hlokahalang ho fetola mocheso oa bongata bo itseng ba ntho ka 1 °C47. Setšoantšo sa 5c se bontša liphetoho tsa bokhoni ba mocheso ba molek'hule ea mohlala oa 3PVA-(C10)2NaAlg ka lebaka la likamano le li-unit tsa glycerol tsa 1, 2, 3, 4, le 5. Setšoantšo se bontša hore bokhoni ba mocheso ba mohlala oa 3PVA-(C10)2NaAlg bo eketseha ka tatellano ka mocheso. Keketseho e bonoang ea bokhoni ba mocheso ka mocheso o ntseng o eketseha e bakoa ke ho thothomela ha mocheso oa phonon. Ho phaella moo, ho na le bopaki ba hore ho eketsa bongata ba glycerol ho lebisa keketsehong ea bokhoni ba mocheso ba mohlala oa 3PVA-(C10)2NaAlg. Ho feta moo, sebopeho se bontša hore 3PVA-(C10)2NaAlg−5Gly e na le boleng bo phahameng ka ho fetisisa ba bokhoni ba mocheso ha bo bapisoa le mehaho e meng.
Diparamitha tse ding tse kang matla a mahala le mocheso wa ho qetela wa sebopeho di badilwe bakeng sa dibopeho tse ithutwang mme di bontshitswe ho Setshwantsho sa 5d le e, ka ho latellana. Mocheso wa ho qetela wa sebopeho ke mocheso o lokollwang kapa o monngwang nakong ya ho thehwa ha ntho e hlwekileng ho tswa dikarolong tsa yona tse ka tlasa kgatello e sa kgaotseng. Matla a mahala a ka hlaloswa e le thepa e tshwanang le matla, ke hore, boleng ba wona bo itshetlehile ka bongata ba ntho boemong bo bong le bo bong ba thermodynamic. Matla a mahala le mocheso wa sebopeho sa 3PVA-(C10)2NaAlg−5Gly e ne e le tse tlase ka ho fetisisa mme e ne e le -1318.338 le -1628.154 kcal/mol, ka ho latellana. Ka lehlakoreng le leng, sebopeho se emelang 3PVA-(C10)2NaAlg se na le matla a mahala le boleng ba mocheso ba sebopeho ba -690.340 le -830.673 kcal/mol, ka ho latellana, ha se bapiswa le dibopeho tse ding. Jwalo ka ha ho bontshitswe ho Setshwantsho sa 5, thepa e fapaneng ya mocheso e fetoha ka lebaka la tshebedisano le glycerol. Matla a mahala a Gibbs a na le negative, e leng se bontshang hore sebopeho se sisintsweng se tsitsitse.
PM6 e badile diparamithara tsa mocheso tsa 3PVA- (C10) 2Na Alg (mohlala A0), 3PVA- (C10) 2Na Alg − 1 Gly (mohlala A1), 3PVA- (C10) 2Na Alg − 2 Gly (mohlala A2), 3PVA- (C10) 2Na Alg − 3 Gly (mohlala A3), 3PVA- (C10) 2Na Alg − 4 Gly (mohlala A4), le 3PVA- (C10) 2Na Alg − 5 Gly (mohlala A5), moo (a) e leng enthalpy, (b) entropy, (c) bokgoni ba mocheso, (d) matla a mahala, le (e) mocheso wa sebopeho.
Ka lehlakoreng le leng, mokhoa oa bobeli oa tšebelisano pakeng tsa PVA trimer le dimeric NaAlg o etsahala lihlopheng tsa terminal le bohareng ba OH sebopehong sa PVA trimer. Joalo ka sehlopheng sa pele, liparamente tsa mocheso li baliloe ho sebelisoa boemo bo tšoanang ba khopolo-taba. Setšoantšo sa 6a-e se bontša mefuta e fapaneng ea enthalpy, entropy, bokhoni ba mocheso, matla a mahala le, qetellong, mocheso oa ho thehoa. Setšoantšo sa 6a-c se bontša hore enthalpy, entropy le bokhoni ba mocheso ba Term 1 NaAlg-3PVA-Mid 1 NaAlg li bontša boitšoaro bo tšoanang le ba sehlopha sa pele ha li sebelisana le li-unit tsa glycerol tsa 1, 2, 3, 4, 5 le 6. Ho feta moo, boleng ba tsona bo eketseha butle-butle ka mocheso o ntseng o eketseha. Ho phaella moo, mohlaleng o reriloeng oa Term 1 Na Alg − 3PVA-Mid 1 Na Alg, boleng ba enthalpy, entropy le bokhoni ba mocheso bo eketsehile ka keketseho ea litaba tsa glycerol. Likhutsufatso B0, B1, B2, B3, B4, B5 le B6 li emela meaho e latelang ka ho latellana: Temana ea 1 Na Alg − 3PVA- Bohareng ba 1 Na Alg, Temana ea 1 Na Alg- 3PVA- Bohareng ba 1 Na Alg − 1 Gly, Temana ea 1 Na Alg- 3PVA- Bohareng ba 1 Na Alg − 2gly, Temana ea 1 Na Alg- 3PVA- Bohareng ba 1 Na Alg − 3gly, Temana ea 1 Na Alg- 3PVA- Bohareng ba 1 Na Alg − 4 Gly, Temana ea 1 Na Alg- 3PVA- Bohareng ba 1 Na Alg − 5 Gly le Temana ea 1 Na Alg- 3PVA- Bohareng ba 1 Na Alg − 6 Gly. Jwalo ka ha ho bontshitswe ho Setshwantsho sa 6a–c, ho totobetse hore boleng ba enthalpy, entropy le bokgoni ba mocheso bo a eketseha ha palo ya diyuniti tsa glycerol e eketseha ho tloha ho 1 ho isa ho 6.
PM6 e badile diparamithara tsa mocheso tsa Term 1 Na Alg-3PVA- Mid 1 Na Alg (mohlala B0), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 1 Gly (mohlala B1), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 2 Gly (mohlala B2), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 3 Gly (mohlala B3), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 4 Gly (mohlala B4), Term 1 Na Alg-3PVA- Mid 1 Na Alg – 5 Gly (mohlala B5), le Term 1 Na Alg-3PVA- Mid 1 Na Alg – 6 Gly (mohlala B6), ho kenyeletsoa (a) enthalpy, (b) entropy, (c) bokgoni ba mocheso, (d) matla a mahala, le (e) mocheso wa sebopeho.
Ho phaella moo, sebopeho se emelang Term 1 Na Alg-3PVA- Mid 1 Na Alg-6 Gly se na le boleng bo hodimo ba enthalpy, entropy le bokgoni ba mocheso ha di bapiswa le dibopeho tse ding. Har'a tsona, boleng ba tsona bo eketsehile ho tloha ho 16.703 cal/mol, 257.990 cal/mol/K le 131.323 kcal/mol ho Term 1 Na Alg − 3PVA- Mid 1 Na Alg ho isa ho 33.223 cal/mol, 420.038 cal/mol/K le 275.923 kcal/mol ho Term 1 Na Alg − 3PVA- Mid 1 Na Alg − 6 Gly, ka ho latellana.
Leha ho le jwalo, Ditshwantsho tsa 6d le e di bontsha ho itshetleha ha mocheso wa matla a lokolohileng le mocheso wa ho qetela wa sebopeho (HF). HF e ka hlaloswa e le phetoho ya enthalpy e hlahang ha mole e le nngwe ya ntho e etswa ho tswa ho dielemente tsa yona tlasa maemo a tlhaho le a tloaelehileng. Ho totobetse ho tswa ho setshwantsho hore matla a lokolohileng le mocheso wa ho qetela wa sebopeho sa dibopeho tsohle tse ithutwang di bontsha ho itshetleha ka mola ho mocheso, ke hore, di eketseha butle-butle le ka mola ha mocheso o ntse o eketseha. Ho phaella moo, setshwantsho se boetse se tiisitse hore sebopeho se emelang Term 1 Na Alg − 3PVA- Mid 1 Na Alg − 6 Gly se na le matla a lokolohileng a tlase ka ho fetisisa le HF e tlase ka ho fetisisa. Diparamitha ka bobedi di theohile ho tloha ho -758.337 ho ya ho -899.741 K cal/mol ho term 1 Na Alg − 3PVA- Mid 1 Na Alg − 6 Gly ho ya ho -1,476.591 le -1,828.523 K cal/mol. Ho totobala ho tsoa liphellong hore HF ​​ea fokotseha ha li-unit tsa glycerol li eketseha. Sena se bolela hore ka lebaka la keketseho ea lihlopha tse sebetsang, reactivity le eona ea eketseha 'me ka hona ho hlokahala matla a fokolang ho etsa karabelo. Sena se tiisa hore PVA/NaAlg e entsoeng ka polasetiki e ka sebelisoa libetering ka lebaka la reactivity ea eona e phahameng.
Ka kakaretso, litlamorao tsa mocheso li arotsoe ka mefuta e 'meli: litlamorao tsa mocheso o tlase le litlamorao tsa mocheso o phahameng. Litlamorao tsa mocheso o tlase li utluoa haholo-holo linaheng tse libakeng tse phahameng, joalo ka Greenland, Canada le Russia. Mariha, mocheso oa moea o kantle libakeng tsena o ka tlase ho likhato tse lefela tsa Celsius. Nako ea bophelo le ts'ebetso ea libeteri tsa lithium-ion li ka angoa ke mocheso o tlase, haholo-holo tse sebelisoang likoloing tsa motlakase tse kopantsoeng tsa plug-in, likoloi tsa motlakase tse hloekileng, le likoloi tsa motlakase tse kopantsoeng. Ho tsamaea sepakapakeng ke tikoloho e 'ngoe e batang e hlokang libeteri tsa lithium-ion. Mohlala, mocheso ho Mars o ka theohela ho likhato tse -120 tsa Celsius, e leng se bakang tšitiso e kholo ts'ebelisong ea libeteri tsa lithium-ion sepakapakeng. Lithempereichara tse tlase tsa ts'ebetso li ka lebisa ho fokotseha ha sekhahla sa phetisetso ea tjhaja le ts'ebetso ea lik'hemik'hale ea libeteri tsa lithium-ion, e leng se fellang ka ho fokotseha ha sekhahla sa ho hasana ha li-ion tsa lithium ka har'a elektrode le conductivity ea ionic ho electrolyte. Ho senyeha hona ho fella ka ho fokotseha ha bokhoni ba matla le matla, 'me ka linako tse ling esita le ho fokotseha ha ts'ebetso53.
Phello ea mocheso o phahameng e etsahala libakeng tse fapaneng tsa ts'ebeliso, ho kenyeletsoa le libaka tsa mocheso o phahameng le o tlase, ha phello ea mocheso o tlase e lekanyelitsoe haholo-holo libakeng tsa ts'ebeliso ea mocheso o tlase. Phello ea mocheso o tlase e khethoa haholo-holo ke mocheso o potolohileng, ha phello ea mocheso o phahameng hangata e amahanngoa ka nepo le mocheso o phahameng ka har'a betri ea lithium-ion nakong ea ts'ebetso.
Libetri tsa Lithium-ion li hlahisa mocheso tlas'a maemo a phahameng a hona joale (ho kenyeletsoa ho tjhaja ka potlako le ho ntsha tjhaja ka potlako), e leng se etsang hore mocheso oa kahare o phahame. Ho pepesehela mocheso o phahameng ho ka boela ha baka ho senyeha ha ts'ebetso ea betri, ho kenyeletsoa tahlehelo ea bokhoni le matla. Ka tloaelo, tahlehelo ea lithium le ho tsosolosoa ha thepa e sebetsang mochesong o phahameng ho lebisa tahlehelong ea bokhoni, 'me tahlehelo ea matla e bakoa ke keketseho ea khanyetso ea kahare. Haeba mocheso o tsoa taolong, ho hlaha ho baleha ha mocheso, e leng se ka lebisang ho chesoeng ka tšohanyetso kapa esita le ho phatloha.
Lipalo tsa QSAR ke mokhoa oa ho etsa mohlala oa lipalo kapa oa lipalo o sebelisoang ho khetholla likamano lipakeng tsa ts'ebetso ea baeloji le thepa ea sebopeho sa metsoako. Limolek'hule tsohle tse entsoeng li ntlafalitsoe 'me thepa e meng ea QSAR e baliloe boemong ba PM6. Tafole ea 3 e thathamisa tse ling tsa litlhaloso tsa QSAR tse baliloeng. Mehlala ea litlhaloso tse joalo ke tjhaja, TDM, matla ohle (E), bokhoni ba ionization (IP), Log P, le polarizability (sheba Tafole ea 1 bakeng sa liforomo tsa ho fumana IP le Log P).
Liphetho tsa lipalo li bontša hore tefiso eohle ea meaho eohle e ithutiloeng ke lefela kaha e boemong ba mobu. Bakeng sa monyetla oa pele oa tšebelisano, TDM ea glycerol e ne e le 2.788 Debye le 6.840 Debye bakeng sa 3PVA-(C10) 2Na Alg, ha boleng ba TDM bo ile ba eketsoa ho 17.990 Debye, 8.848 Debye, 5.874 Debye, 7.568 Debye le 12.779 Debye ha 3PVA-(C10) 2Na Alg e sebelisana le li-unit tsa glycerol tse 1, 2, 3, 4 le 5, ka ho latellana. Ha boleng ba TDM bo le holimo, ho na le ho phahama ha ts'ebetso ea eona le tikoloho.
Matla ohle (E) le ona a badilwe, mme boleng ba E ba glycerol le 3PVA-(C10)2 NaAlg bo fumanwe e le -141.833 eV le -200092.503 eV, ka ho latellana. Ho sa le jwalo, dibopeho tse emelang 3PVA-(C10)2 NaAlg di sebelisana le diyuniti tsa glycerol tse 1, 2, 3, 4 le 5; E e ba -996.837, -1108.440, -1238.740, -1372.075 le -1548.031 eV, ka ho latellana. Ho eketsa dikahare tsa glycerol ho lebisa phokotsong ya matla ohle mme ka hona ho eketsa reactivity. Ho itshetlehile ka palo yohle ya matla, ho fihlelletswe qeto ya hore molek'hule ya mohlala, e leng 3PVA-2Na Alg-5 Gly, e arabela ho feta dimolek'hule tse ding tsa mohlala. Ketsahalo ena e amana le sebopeho sa tsona. 3PVA-(C10)2NaAlg e na le lihlopha tse peli feela tsa -COONa, ha meaho e meng e na le lihlopha tse peli tsa -COONa empa e na le lihlopha tse 'maloa tsa OH, ho bolelang hore karabelo ea tsona tikolohong e ea eketseha.
Ho phaella moo, matla a ionization (IE) a dibopeho tsohle a a nahanwa thutong ena. Matla a ionization ke parameter ya bohlokwa bakeng sa ho lekanya reactivity ya mohlala o ithutwang. Matla a hlokahalang ho tsamaisa elektrone ho tloha ntlheng e le nngwe ya molek'hule ho ya ho infinity a bitswa matla a ionization. A emela tekanyo ya ionization (ke hore reactivity) ya molek'hule. Ha matla a ionization a le hodimo, reactivity e ba tlase. Diphetho tsa IE tsa 3PVA-(C10)2NaAlg tse sebedisanang le diyuniti tsa glycerol tsa 1, 2, 3, 4 le 5 e ne e le -9.256, -9.393, -9.393, -9.248 le -9.323 eV, ka ho latellana, ha di-IE tsa glycerol le 3PVA-(C10)2NaAlg e ne e le -5.157 le -9.341 eV, ka ho latellana. Kaha ho eketsoa ha glycerol ho bakile phokotseho ya boleng ba IP, reactivity ya dimolek'hule e ile ya eketseha, e leng se eketsang ho sebetsa ha molek'hule ya mohlala wa PVA/NaAlg/glycerol disebedisweng tsa electrochemical.
Tlhaloso ea bohlano ho Tafole ea 3 ke Log P, e leng logarithm ea coefficient ea karohano 'me e sebelisoa ho hlalosa hore na sebopeho se ithutoang se na le moea o phaphametseng kapa o phaphametseng. Boleng ba Log P bo fosahetseng bo bontša molek'hule o phaphametseng, ho bolelang hore o qhalana habonolo ka metsing 'me o qhalana hampe ka har'a metsoako ea lintho tse phelang. Boleng bo botle bo bontša mokhoa o fapaneng.
Ho latela liphetho tse fumanoeng, ho ka fihleloa qeto ea hore meaho eohle e phela metsing, kaha boleng ba eona ba Log P (3PVA-(C10)2Na Alg − 1Gly, 3PVA-(C10)2Na Alg − 2Gly, 3PVA-(C10)2Na Alg − 3Gly, 3PVA-(C10)2Na Alg − 4Gly le 3PVA-(C10)2Na Alg − 5Gly) ke -3.537, -5.261, -6.342, -7.423 le -8.504, ka ho latellana, ha boleng ba Log P ba glycerol e le -1.081 feela le 3PVA-(C10)2Na Alg e le -3.100 feela. Sena se bolela hore thepa ea sebopeho se ithutoang e tla fetoha ha limolek'hule tsa metsi li kenyelletsoa sebopehong sa sona.
Qetellong, polarizability ea meaho eohle le eona e baloa boemong ba PM6 ho sebelisoa mokhoa oa semi-empirical. Ho ile ha hlokomeloa pele hore polarizability ea thepa e ngata e itšetlehile ka mabaka a fapaneng. Ntlha ea bohlokoa ka ho fetisisa ke bophahamo ba sebopeho se ithutoang. Bakeng sa meaho eohle e kenyeletsang mofuta oa pele oa tšebelisano lipakeng tsa 3PVA le 2NaAlg (tšebelisano e etsahala ka nomoro ea athomo ea carbon 10), polarizability e ntlafala ka ho eketsoa ha glycerol. Polarizability e eketseha ho tloha ho 29.690 Å ho ea ho 35.076, 40.665, 45.177, 50.239 le 54.638 Å ka lebaka la tšebelisano le li-unit tsa glycerol tsa 1, 2, 3, 4 le 5. Kahoo, ho fumanoe hore molek'hule ea mohlala e nang le polarizability e phahameng ka ho fetisisa ke 3PVA-(C10)2NaAlg−5Gly, ha molek'hule ea mohlala e nang le polarizability e tlase ka ho fetisisa ke 3PVA-(C10)2NaAlg, e leng 29.690 Å.
Tlhahlobo ea litlhaloso tsa QSAR e senotse hore sebopeho se emelang 3PVA-(C10)2NaAlg − 5Gly ke sona se arabelang ka ho fetisisa bakeng sa tšebelisano ea pele e reriloeng.
Bakeng sa mokhoa oa bobeli oa tšebelisano-'moho pakeng tsa PVA trimer le NaAlg dimer, liphetho li bontša hore litefiso tsa tsona li tšoana le tse hlahisitsoeng karolong e fetileng bakeng sa tšebelisano-'moho ea pele. Meaho eohle ha e na tjhaja ea elektroniki ea lefela, ho bolelang hore kaofela ha eona e boemong ba fatše.
Jwalo ka ha ho bontshitswe ho Tafole ya 4, boleng ba TDM (bo balwang boemong ba PM6) ba Term 1 Na Alg − 3PVA-Mid 1 Na Alg bo eketsehile ho tloha ho 11.581 Debye ho ya ho 15.756, 19.720, 21.756, 22.732, 15.507, le 15.756 ha Term 1 Na Alg − 3PVA-Mid 1 Na Alg e arabela ka diyuniti tse 1, 2, 3, 4, 5, le 6 tsa glycerol. Leha ho le jwalo, matla ohle a fokotseha ha palo ya diyuniti tsa glycerol e eketseha, mme ha Term 1 Na Alg − 3PVA- Mid 1 Na Alg e sebelisana le palo e itseng ya diyuniti tsa glycerol (1 ho isa ho 6), matla ohle ke − 996.985, − 1129.013, − 1267.211, − 1321.775, − 1418.964, le − 1637.432 eV, ka ho latellana.
Bakeng sa monyetla oa bobeli oa tšebelisano, IP, Log P le polarizability le tsona li baloa boemong ba khopolo-taba ea PM6. Ka hona, ba nahanne ka litlhaloso tse tharo tse matla ka ho fetisisa tsa reactivity ea limolek'hule. Bakeng sa meaho e emelang End 1 Na Alg-3PVA-Mid 1 Na Alg e sebelisanang le li-unit tsa glycerol tsa 1, 2, 3, 4, 5 le 6, IP e eketseha ho tloha ho −9.385 eV ho ea ho −8.946, −8.848, −8.430, −9.537, −7.997 le −8.900 eV. Leha ho le joalo, boleng ba Log P bo baliloeng bo ne bo le tlase ka lebaka la ho kenngoa ha plasticization ea End 1 Na Alg-3PVA-Mid 1 Na Alg ka glycerol. Ha dikahare tsa glycerol di ntse di eketseha ho tloha ho 1 ho isa ho 6, boleng ba yona bo fetoha -5.334, -6.415, -7.496, -9.096, -9.861 le -10.53 ho ena le -3.643. Qetellong, data ya polarizability e bontshitse hore ho eketsa dikahare tsa glycerol ho bakile keketseho ya polarizability ya Term 1 Na Alg-3PVA- Mid 1 Na Alg. Polarizability ya molek'hule ya mohlala Term 1 Na Alg-3PVA- Mid 1 Na Alg e eketsehile ho tloha ho 31.703 Å ho isa ho 63.198 Å kamora ho sebelisana le diyuniti tse 6 tsa glycerol. Ho bohlokwa ho hlokomela hore ho eketsa palo ya diyuniti tsa glycerol ka monyetla wa bobedi wa ho sebelisana ho etswa ho netefatsa hore ho sa tsotellehe palo e kgolo ya diathomo le sebopeho se rarahaneng, tshebetso e ntse e ntlafala ka keketseho ya dikahare tsa glycerol. Kahoo, ho ka thoe mohlala o fumanehang oa PVA/Na Alg/glycerin o ka nkela libeteri tsa lithium-ion sebaka ka karolo e itseng, empa ho hlokahala lipatlisiso le nts'etsopele e eketsehileng.
Ho hlalosa bokgoni ba ho tlama ba bokaholimo ho adsorbate le ho lekola dikamano tse ikgethang pakeng tsa ditsamaiso ho hloka tsebo ya mofuta wa tlamo e teng pakeng tsa diathomo tse pedi, ho rarahana ha dikamano tsa dimolekhule le tsa ka hare ho dimolekhule, le kabo ya bongata ba dieleketerone ba bokaholimo le adsorbent. Bongata ba dieleketerone ntlheng ya bohlokwa ya tlamo (BCP) pakeng tsa diathomo tse sebedisanang bo bohlokwa bakeng sa ho lekola matla a tlamo tlhahlobong ya QTAIM. Ha bongata ba tjhaja ya dieleketerone bo phahame, kamano ya covalent e tsitsitse haholoanyane mme, ka kakaretso, bongata ba dieleketerone bo phahame dintlheng tsena tsa bohlokwa. Ho feta moo, haeba bongata ba matla a dieleketerone ka bobedi (H(r)) le bongata ba tjhaja ya Laplace (∇2ρ(r)) di le ka tlase ho 0, sena se bontsha boteng ba dikamano tsa covalent (kakaretso). Ka lehlakoreng le leng, ha ∇2ρ(r) le H(r) di le kgolo ho feta 0.54, ho bontsha boteng ba dikamano tse seng tsa covalent (khetla e kwetsweng) tse kang dikamano tse fokolang tsa hydrogen, matla a van der Waals le dikamano tsa electrostatic. Tlhahlobo ea QTAIM e senotse mofuta oa likamano tse seng tsa covalent meahong e ithutiloeng joalo ka ha ho bontšitsoe ho Setšoantšo sa 7 le sa 8. Ho latela tlhahlobo, limolek'hule tsa mohlala tse emelang 3PVA − 2Na Alg le Term 1 Na Alg − 3PVA –Mid 1 Na Alg li bontšitse botsitso bo phahameng ho feta limolek'hule tse sebelisanang le li-unit tse fapaneng tsa glycine. Sena se bakoa ke hore likamano tse 'maloa tse seng tsa covalent tse atileng haholo sebopehong sa alginate joalo ka likamano tsa electrostatic le liboto tsa hydrogen li nolofalletsa alginate ho tsitsisa metsoako. Ho feta moo, liphetho tsa rona li bontša bohlokoa ba likamano tse seng tsa covalent pakeng tsa limolek'hule tsa mohlala tsa 3PVA − 2Na Alg le Term 1 Na Alg − 3PVA –Mid 1 Na Alg le glycine, e leng se bontšang hore glycine e bapala karolo ea bohlokoa ho fetoleng tikoloho ea elektroniki ea metsoako.
Tlhahlobo ea QTAIM ea molek'hule ea mohlala ea 3PVA − 2NaAlg e sebelisanang le (a) 0 Gly, (b) 1 Gly, (c) 2 Gly, (d) 3 Gly, (e) 4 Gly, le (f) 5Gly.