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Ubonisa ikharawusi yezilayidi ezithathu ngaxeshanye.Sebenzisa amaqhosha angaphambili nalandelayo ukutyhutyha izilayidi ezithathu ngexesha, okanye sebenzisa amaqhosha esilayidi ekupheleni ukuya kwizilayidi ezithathu ngexesha.
Kwiminyaka embalwa edlulileyo, kuye kwakho uphuhliso olukhawulezayo lweealloyi zetsimbi elulwelo zokwenziwa kwe-nano-/meso-ubungakanani obuncinci kunye nezakhiwo ezidibeneyo ezinonxibelelwano olukhulu kakhulu lwezixhobo ezahlukeneyo.Nangona kunjalo, le ndlela okwangoku inemida emibini ebalulekileyo.Okokuqala, ivelisa izakhiwo eziqhubekayo kunye ne-topology ephezulu yoluhlu olulinganiselweyo lwe-alloy compositions.Okwesibini, isakhiwo sinobukhulu obukhulu be-binder ngenxa yokwandiswa okukhulu ngexesha lokuhlukana kobushushu obuphezulu.Apha, sibonisa ngokubala kunye nangomfuniselo ukuba le mida inokoyiswa ngokongeza into kwizinyibiliko zesinyithi ezikhuthaza i-topology ekumgangatho ophezulu ngokunciphisa ukuvuza kwezinto ezingenakulinganiswa ngexesha lokudityaniswa.Okulandelayo, sichaza oku kufunyanisiweyo ngokubonisa ukuba ugqithiso lwesambuku sokuhanjiswa kwezinto ezingaxutywanga kulwelo olunyibilikayo lunefuthe elinamandla kwi-evolution yeqhezu eliqinileyo kunye ne-topology yezakhiwo ngexesha lokuqhekeka.Iziphumo zityhila umahluko osisiseko phakathi kwesinyithi solwelo kunye nokususwa kokungcola kwe-electrochemical, kwaye kusekwa indlela entsha yokufumana izakhiwo kwiintsimbi ezingamanzi ezinobungakanani obunikiweyo kunye netopology.
Ugunyaziso luguqukele kubuchwephesha obunamandla nobuguquguqukayo bokwenziwa kwe-nano-/meso-ubungakanani beepores ezivulekileyo kunye nezakhiwo ezihlanganisiweyo ezinomgangatho ophezulu wobuso obuphezulu kwizinto ezahlukeneyo ezisebenzayo kunye nezakhiwo ezifana ne-catalysts1,2, iiseli zamafutha3,4, i-electrolytic capacitors5, I-6, izixhobo ezichasene nomonakalo we-radiation 7, izixhobo zebhetri ezinomthamo ophezulu kunye nozinzo olongeziweyo lomatshini 8, 9 okanye izinto ezidibeneyo ezineempawu ezibalaseleyo zoomatshini. ingxubevange” kwimeko-bume yangaphandle, nto leyo ekhokelela kuhlengahlengiso lwezinto ezinganyibilikiyo zengxubevange ezine-topology engabalulekanga, eyahlukileyo kwi-topology yealloyi yokuqala., Ukubunjwa kwezithako.Nangona i-electrochemical delegation (ECD) eqhelekileyo kusetyenziswa i-electrolytes njengeyona ndawo ifundwayo ukuza kuthi ga ngoku, le ndlela inciphisa iinkqubo zogunyaziso (ezifana ne-Ag-Au okanye i-Ni-Pt) kwezo ziqulathe izinto ezibekekileyo (Au, Pt) kwaye umahluko omkhulu ngokwaneleyo ekunciphiseni amandla okubonelela nge-porosity.Inyathelo elibalulekileyo ekoyiseni lo mda ibe kukufunyanwa kwakhona kwendlela yolwelo lwesinyithi yolwelo13,14 (LMD), esebenzisa ingxubevange yesinyithi solwelo (umz., Cu, Ni, Bi, Mg, njl. njl.) kunye nezinye izinto zokusingqongileyo .(umz. TaTi, NbTi, FeCrNi, SiMg, njl.)6,8,10,11,14,15,16,17,18,19.I-LMD kunye nokususwa kwayo kwe-alloy metal eqinile (SMD) i-variant isebenza kumaqondo aphantsi xa isiseko sesinyithi sinzima20,21 okubangela ukuba kuhlanganiswe izigaba ezimbini okanye ngaphezulu ezidibeneyo emva kokufakwa kweekhemikhali zesigaba esinye.Ezi zigaba ziyakwazi ukuguquka zibe yi-pores evulekileyo.izakhiwo.Iindlela zokuthumela ziye zaphuculwa ngakumbi ngokungeniswa kwamva nje kokuthunyelwa kwesigaba somphunga (VPD), esebenzisa ukungafani koxinzelelo lomoya wezinto eziqinileyo ukwenza izakhiwo ezivulekileyo ze-nanoporous ngokunyuka okukhethiweyo kwento enye22,23.
Kwinqanaba lomgangatho, zonke ezi ndlela zokususa ukungcola zabelana ngeempawu ezimbini ezibalulekileyo zenkqubo yokususwa kokungcola okucwangcisiweyo.Okokuqala, oku kukuchithwa okukhethiweyo kwezinto ezikhankanywe ngasentla (ezifana ne-B kwi-alloy elula i-AXB1-X) kwimeko yangaphandle.Okwesibini, okokuqala kuphawulwe kwizifundo zovavanyo oluphambili kunye nethiyori kwi-ECD24, kukusasazwa kwento enganyibilikiyo A kunye nojongano phakathi kwealloyi kunye nokusingqongileyo ngexesha lokususwa kobumdaka.I-Diffusion iyakwazi ukwenza imimandla ecebileyo ye-atomic ngenkqubo efana nokubola kwe-spinodal kwi-alloys eninzi, nangona inqunyelwe yi-interface.Ngaphandle koku kufana, iindlela ezahlukeneyo zokususa ialloy zinokuvelisa iimorphology ezahlukeneyo ngezizathu ezingacacanga18.Ngelixa i-ECD inokuvelisa ulwakhiwo olunxulumene ne-topologically olulungeleleneyo oluphezulu lwamaqhezu e-athomu (X) yezinto ezinganyibilikiyo (ezifana ne-Au kwi-AgAu) ephantsi njenge-5% 25, ​​izifundo zokubala kunye novavanyo lwe-LMD zibonisa ukuba le ndlela ebonakala ifana ivelisa kuphela izakhiwo ezinxulumene ne-topologically. .Ngokomzekelo, kwi-X enkulu kakhulu, i-bicontinuous structure ehambelanayo malunga ne-20% kwimeko ye-alloys ye-TaTi edibeneyo yi-Cu iyanyibilika (jonga i-Fig. 2 kwi-ref. 18 uthelekiso olusecaleni kunye ne-ECD eyahlukeneyo kunye nefom ye-LMD X. ).Oku kungafani kuchazwa ngokwethiyori yindlela yokukhula edityanisiweyo eyahlukileyo ukusuka kwi-interfacial spinodal decomposition kwaye ifana kakhulu ne-eutectic-coupled growth26.Kwimeko yokususwa kokungcola, ukukhula okudityanisiweyo okudityanisiweyo kuvumela i-A-rich filaments (okanye i-flakes kwi-2D) kunye ne-B-rich rich channel channels ukuba zikhule ngokubambisana ngokusasazwa ngexesha lokususwa kokungcola15.Ukukhula ngababini kukhokelela kulwakhiwo olulungelelanisiweyo lwe-topologically olungadityaniswanga kumbindi we-X kwaye lucinezelwe kwindawo esezantsi ye-X, apho kuphela iziqithi ezingadityaniswanga ezityebileyo kwisigaba se-A ezinokubumba.Kwi-X enkulu, ukukhula okudityanisiweyo kuya kuzinza, kuthanda ukuyilwa kolwakhiwo oludityaniswe ngokugqibeleleyo lwe-3D olugcina imfezeko yolwakhiwo nasemva kokwenziwa kwesigaba esinye.Okubangel 'umdla kukuba, ulwakhiwo lwe-orientation oluveliswe yi-LMD17 okanye i-SMD20 (Fe80Cr20) XNi1-X alloys iye yajongwa ngokomfuniselo kwi-X ukuya kuthi ga kwi-0.5, iphakamisa ukuba ukukhula okudityanisiweyo kuyindlela exhaphakileyo ye-LMD kunye ne-SMD kunokuba i-ECD ibangele i-porous. yiba nesakhiwo solungelelwaniso esikhethwayo.
Ukucacisa isizathu salo mahluko phakathi kwe-ECD kunye ne-NMD morphology, senze ukulinganisa kwintsimi yesigaba kunye nezifundo zovavanyo ze-NMD ye-TaXTi1-X alloys, apho i-kinetics yokuchithwa kwaguqulwa ngokudibanisa izinto ezinyibilikisiweyo kubhedu olumanzi.Sagqiba ekubeni nangona zombini i-ECD kunye ne-LMD zilawulwa ngokuchithwa okukhethiweyo kunye nokusabalalisa kwe-interfacial diffusion, ezi nkqubo zimbini nazo zineentlukwano ezibalulekileyo ezinokukhokelela ekuhlukeni kwe-morphological18.Okokuqala, i-peel kinetics kwi-ECD ilawulwa yi-interface ene-peel ye-front ye-peel ye-V12 eqhubekayo njengomsebenzi we-voltage esetyenzisiweyo.Oku kuyinyani nangona iqhekeza elincinci leengqungquthela ezilahlayo (umzekelo, i-Pt kwi-Ag-Au) yongezwa kwi-alloy yomzali, ebuyisela i-interfacial fluidity, ihlambulule kwaye izinze izinto ezingaxutywanga, kodwa ngaphandle koko igcina i-morphology efanayo 27.Izakhiwo ezidityanisiweyo ze-Topologically zifumaneka kuphela kwi-X ephantsi kwi-V ephantsi, kwaye ukugcinwa kwezinto ezixubileyo ze-25 kukhulu ukugcina iqhezu eliqinileyo lomthamo omkhulu ngokwaneleyo ukukhusela ukuhlukana kwesakhiwo.Oku kuphakamisa ukuba izinga lokuchithwa ngokubhekiselele kwi-interfacial diffusion inokudlala indima ebalulekileyo ekukhethweni kwe-morphological.Ngokwahlukileyo, i-kinetics yokususa i-alloy kwi-LMD i-diffusion controlled15,16 kwaye izinga liyancipha ngokukhawuleza ngexesha \ (V \ sim \ sqrt {{D}_{l}/t}\), apho i-Dl iyinto ephosakeleyo. kwi-coefficient ye-fluid diffusion..
Okwesibini, ngexesha le-ECD, ukunyibilika kwezinto ezingenakulinganiswa kwi-electrolyte kuphantsi kakhulu, ngoko ke banokusasaza kuphela kwi-interface ye-alloy-electrolyte.Ngokwahlukileyo, kwi-LMD, izinto "ezingenakulinganiswa" (A) ze-AXB1-X ze-alloys zangaphambili zihlala zincinci, nangona zilinganiselwe, ukunyibilika.Oku kunyibilika kuncinci kunokuthatyathelwa kuhlalutyo lomzobo wesigaba se-ternary senkqubo ye-CuTaTi ternary eboniswe kuMzobo owoNgezelelweyo 1. Ukunyibilika kunokulinganiswa ngokucwangcisa umgca we-liquidius ngokuchasene nogxininiso lwe-equilibrium ye-Ta kunye ne-Ti kwicala lolwelo lojongano (\( {c}_{{{{{{\rm{Ta))))))}}}} ^{l}\ ) kunye \({c}_{{{{{\rm{Ti}}} }}}} }^ {l}\), ngokulandelelanayo, kwiqondo logunyaziso (Umfanekiso owongezelelweyo 1b) ujongano oluqinileyo-olwelwelo lwendawo ye-thermodynamic equilibrium igcinwa ngexesha lokuxutywa, }}}}}}^{l}\) imalunga rhoqo kwaye ixabiso layo lihambelana no X. Umzobo owongezelelweyo 1b ubonisa ukuba \({c}_{{{{{{\rm{Ta}}}}}}}))}^{l}\) iwela kuluhlu 10 -3 − 10 ^{l}\) zilingana no-15.16.Oku "kuvuza" kwezinto ezingenakulinganiswa kwi-alloy kunokuchaphazela zombini ukubunjwa kwesakhiwo se-interfacial kwi-delamination front, ekuphenduleni kwayo, okunokuthi kube negalelo ekuchithweni kunye nokuqhekeka kwesakhiwo ngenxa yokusabalalisa umthamo.
Ukuze uvavanye ngokwahlukileyo igalelo (i) izinga elincitshisiweyo lokususwa kwe-alloy V kunye (ii) nesantya esincitshisiweyo sokungenwa kwezinto ezingenakulinganiswa kwi-melt, siqhube ngamanyathelo amabini.Okokuqala, ngenxa ye-(V \ sim \ sqrt{{D}_{l}/t}\), ngokufunda i-morphological evolution yesakhiwo se-bundle front, kwakunokwenzeka ukufunda umphumo wokunciphisa i-V ngokwaneleyo.ixesha elikhulu.Ke ngoko, siye saphanda esi siphumo ngokuqhuba ukulinganisa kwebala lesigaba kwixesha elide kunezifundo zangaphambili, ezithe zatyhila ubukho bezakhiwo zolungelelwaniso ezingadityaniswanga ze-topologically ezenziwe kukukhula okudityanisiweyo kwe-X15 ephakathi.Okwesibini, ukwenzela ukuphanda umphumo wezinto ezingenakulinganiswa ekunciphiseni izinga lokuvuza, songeze i-Ti kunye ne-Ag kwi-melt yobhedu ukuze kwandiswe kwaye kuncitshiswe izinga lokuvuza, ngokulandelelana, kwaye sifunde i-morphology ebangele, i-kinetics yokwahlula, kunye nokusabalalisa koxinzelelo nyibilika.abathunywa I-Cu iyanyibilika ngokusebenzisa izibalo kunye nemifuniselo ngaphakathi kwesakhiwo se-alloy.Songeze izongezo zeTi ukusuka kwi-10% ukuya kwi-30% kumajelo eendaba ukususa i-Cu melt.Ukongezwa kwe-Ti kwandisa ugxininiso lwe-Ti kumda woluhlu olunikezelweyo, olunciphisa i-gradient yoxinaniso lwe-Ti ngaphakathi kolu luhlu kunye nokunciphisa izinga lokuchithwa.Ikwanyusa izinga lokuvuza kukaTa ngokunyusa \({c}_{{{({\rm{Ti}}}}}}}}^{l}\), ngoko \({c}_{{{{{{{ {\ rm{Ta}}}}}}} ^ {l}\) (Umzobo owongezelelweyo we-1b). Ukunyibilika kwezinto ezixutyiweyo kwinyibilika, senze imodeli yeCuAgTaTi quaternary system njengenkqubo esebenzayo (CuAg)TaTi ternary system apho ukunyibilika kweTi kunye neTa kuxhomekeke kuxinzelelo lwe-Ag kwiCuAg enyibilikayo (jonga inqaku) 2 kunye neSupplementary. Amakhiwane 2-4).Ukongezwa kwe-Ag akunyusi ukugxininiswa kwe-Ti kumda wesakhiwo esinikezelweyo.Nangona kunjalo, ekubeni ukunyibilika kwe-Ti kwi-Ag kungaphantsi kunoko kweCu, oku kunciphisa \({c}_{{{{{\rm{Ta}}}}}}}}}^{l}\) (Fig eyoNgezelelweyo . 1 ) 4b) kunye nesantya sokuvuza Ta.
Iziphumo zokulinganisa intsimi yesigaba zibonisa ukuba ukukhula okudityanisiweyo kuye kungazinzi ngexesha elide ngokwaneleyo ukukhuthaza ukusekwa kwezakhiwo ezidityaniswe kumgangatho ophezulu kwindawo ebolileyo.Siqinisekisa ngovavanyo esi sigqibo ngokubonisa ukuba umaleko ongaphantsi we-alloy ye-Ta15T85, eyenza kufutshane nomphambili we-delamination kwinqanaba lamva lokudityaniswa, uhlala ubopheleleke ngokomgangatho emva kokukrolwa kwesigaba sobhedu olutyebileyo.Iziphumo zethu zikwacebisa ukuba izinga lokuvuza linempembelelo enzulu kwi-morphological evolution ngenxa yothutho oluninzi lwe-diffussive ye-immiscible elements in liquids melts.Kuboniswa apha ukuba esi siphumo, esingekho kwi-ECD, sichaphazela kakhulu iiprofayili zoxinaniso zezinto ezahlukeneyo kuluhlu olunikezelweyo, iqhekeza lesigaba esiqinileyo, kunye ne-topology yesakhiwo se-LMD.
Kweli candelo, siqala sibonise iziphumo zophando lwethu ngesigaba sokulinganisa intsimi yesiphumo sokongeza i-Ti okanye i-Ag kwi-Cu iyanyibilika okubangelwa yi-morphologies eyahlukeneyo.Kwikhiwane.Umzobo 1 ubonisa iziphumo zemodeli ye-dimensional ye-three-dimensional field ye-TaXTi1-X alloys efunyenwe kwi-Cu70Ti30, Cu70Ag30 kunye ne-copper ecocekileyo enyibilikayo kunye nomxholo ophantsi we-athomu yezinto ezingenakulinganiswa ukusuka kwi-5 ukuya kwi-15%.Imiqolo emibini yokuqala ibonisa ukuba ukongezwa kokubili kwe-Ti kunye ne-Ag kukhuthaza ukubunjwa kwezakhiwo ezidibeneyo ze-topologically xa kuthelekiswa nesakhiwo esingenasiphelo se-Cu ecocekileyo (umqolo wesithathu).Nangona kunjalo, ukongezwa kwe-Ti, njengoko bekulindelekile, kwenyuse ukuvuza kwe-Ta, ngaloo ndlela kuthintelwa ukunyibilika kwee-alloys ezisezantsi ze-X (Ta5Ti95 kunye ne-Ta10Ti90) kwaye kubangele ukunyibilika okukhulu komaleko we-porous okhutshiweyo ngexesha le-Ta15Ti85 delamination.Ngokuchasene noko, ukongezwa kwe-Ag (umqolo wesibini) kunegalelo ekwakhiweni kolwakhiwo olunxulumene ne-topologically yazo zonke iikhomponenti ze-alloy yesiseko kunye nokuchithwa okuncinci koluhlu olunikezelweyo.Ukuqulunqwa kwesakhiwo se-bicontinuous kuboniswe ngokongezwa kwiMifanekiso.I-1b, ebonisa imifanekiso yesakhiwo esinikezelweyo kunye nobunzulu okwandayo be-delamination ukusuka ekhohlo ukuya ekunene kunye nomfanekiso wojongano oluqinileyo-olulwelo kubunzulu obukhulu (umfanekiso osekunene kude).
Ukulinganisa intsimi yesigaba se-3D (128 × 128 × 128 nm3) ebonisa isiphumo esimangalisayo sokongeza i-solute kulwelo olunyibilikayo kwi-morphology yokugqibela yealloyi enikezelweyo.Uphawu olungasentla lubonisa ukubunjwa kwe-alloy yomzali (TaXTi1-X) kunye nophawu oluthe nkqo lubonisa ukunyibilika kwe-Cu-based softening medium.Iindawo ezinezinga eliphezulu le-Ta kwisakhiwo ngaphandle kokungcola ziboniswa nge-brown, kunye ne-solid-liquid interface iboniswe ngeblue.b Ukulinganisa okuthathu kwebala lesigaba se-Ta15Ti85 ye-precursor alloy engagqitywanga kwi-Cu70Ag30 melt (190 × 190 × 190 nm3).Izakhelo ezi-3 zokuqala zibonisa ummandla oqinileyo wesakhiwo esigunyazisiweyo kubunzulu obahlukeneyo bogunyaziso, kwaye isakhelo sokugqibela sibonisa kuphela ujongano oluqinileyo-olwelo kubunzulu obukhulu.Imuvi ehambelana no (b) iboniswa kwiMovie eyoNgezelelweyo 1.
Umphumo wokongezwa kwe-solute waphononongwa ngakumbi nge-2D yesigaba sokulinganisa intsimi, ebonelele ngolwazi olongezelelweyo malunga nokwakheka kwemowudi ye-interfacial kwi-delamination front kunye nokuvumela ukufikelela kubude obuninzi kunye nezikali zexesha kune-3D ukulinganisa ukulinganisa i-delamination kinetics.Kwikhiwane.Umzobo we-2 ubonisa imifanekiso yokulinganisa ukususwa kwe-alloy ye-precursor ye-Ta15Ti85 nge-Cu70Ti30 kunye ne-Cu70Ag30 iyanyibilika.Kuzo zombini ezi meko, ukukhula okudityanisiweyo kokusasazwa akuzinzanga kakhulu.Esikhundleni sokungena ngokuthe nkqo kwi-alloy, iingcebiso zemijelo yamanzi zihamba nge-chaotically ekhohlo kwaye ekunene kwiindlela ezinzima kakhulu ngexesha lenkqubo yokukhula ezinzileyo ekhuthaza izakhiwo ezihambelanayo ezikhuthaza ukusekwa kwezakhiwo ezinxulumene ne-topologically kwisithuba se-3D (Fig. 1).Nangona kunjalo, kukho umahluko obalulekileyo phakathi kwezongezo ze-Ti kunye ne-Ag.I-Cu70Ti30 inyibilika (umzobo 2a), ukungqubana kwemijelo yolwelo emibini kukhokelela ekudityanisweni kojongano oluqinileyo olululwelo, olukhokelela ekukhutshelweni kwezibophelelo eziqinileyo ezithinjwe yimijelo emibini ukusuka kwisakhiwo kwaye, ekugqibeleni, ukunyibilika. .Ngokuchasene noko, i-Cu70Ag30 inyibilika (Umfanekiso 2b), ukuphuculwa kweTa kwi-interface phakathi kwezigaba eziqinileyo kunye nolwelo zithintela ukuhlangana ngenxa yokuncipha kwe-Ta ukuvuza kwi-melting.Ngenxa yoko, ukunyanzeliswa kwebhondi kwi-delamination front kucinezelwe, ngaloo ndlela kukhuthazwa ukubunjwa kwezakhiwo ezidibeneyo.Kuyathakazelisa ukuba i-chaotic oscillatory motion ye-chaotic channel ye-liquid channel yenza isakhiwo esine-dimensional-dimensional kunye neqondo elithile lokulungelelanisa xa i-cutoff icinezelwe (Umfanekiso we-2b).Nangona kunjalo, oku kulungelelaniswa akusiyo isiphumo sokukhula okuzinzileyo kwebhondi.Kwi-3D, ukungena okungazinzanga kudala i-non-coaxial edibeneyo i-bicontinuous structure (Umfanekiso 1b).
Izifinyezo zesigaba se-2D sokulinganisa indawo ye-Cu70Ti30 (a) kunye ne-Cu70Ag30 (b) enyibilikayo yaphinda yanyibilika ukuya kwi-alloyi ye-Ta15Ti85 ebonisa ukukhula okungazinzanga okudityanisiweyo.Imifanekiso ebonisa ubunzulu obahlukeneyo bokushenxiswa kobumdaka obulinganiswa ukusuka kwindawo yokuqala yesiqina esisicaba/ujongano olululwelo.I-insets ibonisa iindlela ezahlukeneyo zokungqubana kweshaneli yolwelo, ekhokelela ekudibaneni kwezibophelelo eziqinileyo kunye nokugcinwa kwe-Cu70Ti30 kunye ne-Cu70Ag30 iyanyibilika, ngokulandelanayo.Ububanzi besizinda se-Cu70Ti30 yi-1024 nm, i-Cu70Ag30 yi-384 nm.Ibhendi enemibala ibonisa i-concentration ye-Ta, kunye nemibala eyahlukeneyo yahlula phakathi kwendawo engamanzi (i-blue blue), i-alloy yesiseko (i-blue blue), kunye nesakhiwo esingaxutywanga (phantse sibomvu).Iimuvi zale milinganiso zibonakaliswe kwiiMovie ezoNgezelelweyo 2 kunye no-3, eziqaqambisa iindlela ezintsonkothileyo ezigqobhoza imijelo yolwelo ngexesha lokukhula okungazinzanga kokusasazwa okudityanisiweyo.
Ezinye iziphumo ze-2D isigaba se-simulation field siboniswe kwi-Fig.3.Igrafu yobunzulu be-delamination ngokuchasene nexesha (ithambeka elilingana no-V) kwifig.I-3a ibonisa ukuba ukongezwa kwe-Ti okanye i-Ag kwi-Cu iyanyibilika kunciphisa i-kinetics yokwahlula, njengoko kulindelwe.Kwikhiwane.I-3b ibonisa ukuba oku kucotha kubangelwe kukuncipha kwethayimdi yoxinaniso ye-Ti kulwelo olungaphakathi koluhlu olunikezelweyo.Ikwabonisa ukuba ukongezwa kwe-Ti(Ag) kwandisa (kwehla) ugxininiso lwe-Ti kwicala elingamanzi lojongano (\({c}_{{{{{{\rm{Ti)))))")) ))) ^ {l \) ), okukhokelela ekuvuzeni kwe-Ta, kulinganiswe ngeqhezu le-Ta elichithwe kwi-nyibilika njengomsebenzi wexesha (umzobo 3c), okwandisa (ukuncipha) kunye nokongezwa kwe-Ti (Ag) ).Umzobo we-3d ubonisa ukuba kuzo zombini i-solutes, i-volume fraction of solids ihleli ngaphezu komda wokwenziwa kwezakhiwo ezinxulumene ne-bicontinuous topologically28,29,30.Ngelixa ukongeza i-Ti ekunyibilikeni kwandisa ukuvuza kwe-Ta, kwandisa nokugcinwa kwe-Ti kwi-binder eqinile ngenxa yokulinganisa kwesigaba, ngaloo ndlela ukwandisa iqhezu levolumu ukugcina ukubambisana kwesakhiwo ngaphandle kokungcola.Ubalo lwethu ngokubanzi luyavumelana nemilinganiselo yovavanyo yeqhezu lomthamo we-delamination front.
Ukulinganisa kwintsimi yesigaba se-alloy ye-Ta15Ti85 ilinganisa iziphumo ezahlukeneyo ze-Ti kunye ne-Ag ezongeziweyo kwi-Cu nyibilika kwi-kinetics yokususa i-alloy elinganiswe kubunzulu bokususwa kwe-alloy njengomsebenzi wexesha (a), iprofayile yoxinaniso lwe-Ti kulwelo Ubunzulu bokususwa kwealloyi ngama-400 nm (ubunzulu obunegative buba banzi bube yinyibilika ngaphandle kwesakhiwo sengxubevange (ingxubevange ngaphambili ngasekhohlo) b Ukuvuza kuthelekiswa nexesha (c) kunye neqhezu eliqinileyo kwisakhiwo esingaxutywanga ngokuchasene nokwakhiwa kwenyibilika (d) Uxinzelelo lwezinto ezongezelelweyo kwi-melt ihlelwe ecaleni kwe-abscissa (d) (i-Ti - umgca oluhlaza, i-Ag - umgca omfusa kunye novavanyo).
Kuba isantya se-delamination sangaphambili sincipha ngokuhamba kwexesha, ukuvela kwe-morphology ngexesha le-delamination kubonisa isiphumo sokunciphisa isantya se-delamination.Kuphononongo lwangaphambili lwesigaba sangaphambili, siye sabona ukukhula okudityanisiweyo okufana ne-eutectic okukhokelela kulwakhiwo olulungelelanisiweyo lwe-topologically olungabotshwanga ngexesha lokususwa kwe-alloy ye-Ta15Ti85 ye-precursor alloy ngobhedu olusulungekileyo olunyibilikayo15.Nangona kunjalo, ixesha elide lokulinganisa intsimi yesigaba esifanayo (jonga i-Movie eyoNgezelelweyo ye-4) ukuba xa isantya sangaphambili sokubola siba sincinci ngokwaneleyo, ukukhula okudityanisiweyo kuya kuzinza.Ukungazinzi kuzibonakalisa kwi-lateral rocking of flakes, okuthintela ukulungelelaniswa kwabo kwaye, ngoko, kukhuthaza ukubunjwa kwezakhiwo ezixhunyiwe kwi-topologically.Utshintsho ukusuka ekukhuleni okuzinzileyo ukuya ekukhuleni okungazinzanga kwenzeka kufutshane ne-xi = 250 nm ngesantya se-4.7 mm/s.Ngokuchasene noko, ubunzulu obuhambelanayo be-delamination xi ye-Cu70Ti30 melt imalunga ne-40 nm ngesantya esifanayo.Ngoko ke, asikwazanga ukuqwalasela utshintsho olunjalo xa sisusa i-alloy kunye ne-Cu70Ti30 melt (jonga i-Movie eyoNgezelelweyo ye-3), kuba ukongeza i-30% ye-Ti ekunyibilikeni kunciphisa kakhulu i-kinetics yokususa i-alloy.Okokugqibela, nangona ukukhula okudityanisiweyo okudityanisiweyo kungazinzanga ngenxa yokucotha kwe-delamination kinetics, umgama λ0 weebhondi eziqinileyo kumphambili we-delamination uthobela ngokungqongqo \({\lambda }_{0}^{2}V=C\) umthetho wokumisa. ukukhula15,31 apho i-C ihleli.
Ukuvavanya uqikelelo lokulinganisa intsimi yesigaba, iimvavanyo zokususa i-alloy zenziwa ngeesampulu ezinkulu kunye namaxesha amade okususa i-alloy.Umzobo 4a ngumzobo weskim obonisa iiparamitha eziphambili zesakhiwo esinikezelweyo.Ubunzulu bubonke be-delamination bulingana ne-xi, umgama ukusuka kumda wokuqala wezigaba eziqinileyo kunye nolwelo ukuya kumphambili we-delamination.I-hL ngumgama ukusuka kujongano lokuqala oluqinileyo-olulwelo ukuya kumda wesakhiwo esinikezelweyo phambi kokukrolwa.I-hL enkulu ibonisa ukuvuza okuqinileyo kwe-Ta.Ukusuka kumfanekiso we-SEM wesampulu enikezelweyo, sinokulinganisa ubungakanani be-hD yesakhiwo esinikezelweyo ngaphambi kokubhala.Nangona kunjalo, ekubeni i-melt iphinda iqinise kwiqondo lokushisa, kunokwenzeka ukugcina isakhiwo esinikezelweyo ngaphandle kweebhondi.Ngoko ke, sigxininise i-melt (isigaba esityebileyo sobhedu) ukuze sifumane isakhiwo senguqu kwaye sisebenzise i-hC ukulinganisa ubukhulu besakhiwo senguqu.
umzobo weSchematic of evolution of morphology ngexesha lokususwa kokungcola kunye nokumiselwa kweeparameters zejometri: ukuvuza kwe-leak thickness Ta hL, ubukhulu be-delaminated structure hD, ubukhulu besakhiwo sokudibanisa i-hC.(b), (c) Ukuqinisekiswa kovavanyo lweziphumo zokulinganisa intsimi yesigaba ngokuthelekisa amacandelo e-SEM anqamlezileyo kunye ne-3D emisiweyo yemopholoji ye-Ta15Ti85 ingxubevange elungiswe ukusuka kwi-Cu(b) esulungekileyo kunye ne-Cu70Ag30 enyibilikayo, inika iibhondi ze-topological kunye neSakhiwo sebhondi efanayo (c), isikali somgca 10µm.
Amacandelo anqamlezayo ezakhiwo ezinikezelweyo eziboniswe kwifig.I-4b,c iqinisekisa iziphumo eziqikelelweyo eziphambili zokongeza i-Ti kunye ne-Ag kwi-Cu iyanyibilika kwi-morphology kunye ne-kinetics ye-alloy enikezelweyo.Kwikhiwane.Umfanekiso we-4b ubonisa ummandla ongezantsi we-SEM cut (ngasekhohlo) ye-alloy ye-Ta15T85 edibeneyo ngokuntywiliselwa kubhedu olusulungekileyo lwe-10 s ukuya kubunzulu be-xi ~ 270 μm.Kwisikali sexesha lokulinga elinokulinganiswa, elinemiyalelo emininzi yobukhulu kunokulinganisa kwintsimi yesigaba, isantya sangaphambili sokuqhawula singaphantsi kakhulu kwesantya somda okhankanywe ngasentla we-4.7 mm/s, apho ukukhula okuzinzile kwebhondi ye-eutectic kuzinza.Ke ngoko, ulwakhiwo olungentla komphambili we-peel kulindeleke ukuba ludityaniswe ngokupheleleyo.Ngaphambi kwe-etching, umaleko omncinci we-alloy yesiseko wachithwa ngokupheleleyo (hL = 20 μm), owawunxulumene nokuvuza kweTa (Itheyibhile 1).Emva kokuchongwa kweekhemikhali zesigaba sobhedu olutyebileyo (ekunene), kuphela umaleko obhityileyo wealloyi enikezelweyo (hC = 42 µm) eseleyo, ebonisa ukuba uninzi lwesakhiwo ebesinikezelwe siphulukene nesidima sesakhiwo ngexesha lokurhweba kwaye aluzange, njengoko bekulindelekile, ludityaniswe ngokwendalo (topologically bonded). Isazobe 1a)., owona mfanekiso usekunene kumqolo wesithathu).Kwikhiwane.I-4c ibonisa icandelo elipheleleyo le-SEM elinqamlezileyo kunye nemifanekiso ye-3D ye-etching ye-alloy ye-Ta15Ti85 esuswe ngokuntywiliselwa kwi-Cu70Ag30 inyibilika i-10 s ukuya kubunzulu obumalunga ne-200 µm.Ekubeni ubunzulu be-peel buqikelelwe ngokwethiyori ukuba bunyuke nge \({x}_{i}(t)=\sqrt{4p{D}_{l}t}\) i-kinetics elawulwa yi-diffusion (bona iNqaku eloNgezelelweyo 4) 15 16, Ngokudityaniswa kwe-30% ye-Ag kwi-Cu iyanyibilika, ukuhla kobunzulu bokuhlukana ukusuka kwi-270 μm ukuya kwi-220 μm kuhambelana nokuncipha kwenombolo yePeclet p nge-1.5.Emva kokufakwa kwemichiza yesigaba esityebileyo se-Cu/Ag (ekunene), sonke isakhiwo esigunyazisiweyo sigcina imfezeko yesakhiwo (hC = 200 µm), ebonisa ukuba sisiseko esiqikelelweyo esidityaniswe nge-bicontinuous structure (Figure 1, right most image) umqolo wesibini kwaye uphelele. umqolo ongezantsi).Yonke imilinganiselo ye-alloy yesiseko enikezelweyo i-Ta15T85 kwiinyibiliki ezahlukeneyo zishwankathelwa kwiThebhile.1. Sikwabonisa iziphumo ze-Ta10Ti90 base alloys ezingafakwanga kwii-melts ezahlukeneyo, ziqinisekisa izigqibo zethu.Imilinganiselo yobunzima bokuvuza kwe-Ta ibonise ukuba isakhiwo esichithwe kwi-Cu70Ag30 melt (hL = 0 μm) incinci kune-Cu ecocekileyo enyibilikayo (hL = 20 μm).Ngokuchasene noko, ukongezwa kwe-Ti ekunyibilikeni kunyibilikisa izakhiwo ezithambileyo ezidibeneyo (hL = 190 μm).Ukuncipha kokuchithwa kwesakhiwo esigunyazisiweyo phakathi kwe-Cu esulungekileyo yokunyibilika (hL = 250 μm) kunye ne-Cu70Ag30 enyibilikayo (hL = 150 μm) ibonakala ngakumbi kwii-alloys ezinikezelweyo ezisekelwe kwi-Ta10Ti90.
Ukuqonda umphumo weenyibiliki ezahlukeneyo, senze uhlalutyo olongezelelweyo lobungakanani beziphumo zovavanyo kwi-Fig. 5 (jonga kwakhona iDatha eyoNgezelelweyo 1).Kwikhiwane.Amanani 5a-b abonisa ukuhanjiswa koxinzelelo olulinganisiweyo lwezinto ezahlukeneyo ecaleni kwendlela yokukhupha kwimifuniselo ye-exfoliation kwi-Cu ecocekileyo yokunyibilika (umzobo 5a) kunye ne-Cu70Ag30 inyibilika (umzobo 5b).Ugxininiso lwezinto ezahlukeneyo zicwangciswe kumgama d ukusuka kumphambili we-delamination ukuya kumphetho womaleko we-delamination kwisibophelelo esiqinileyo kunye nesigaba esasilulwelo (esityetyisiweyo kwiCu okanye kwiCuAg) ngexesha le-delamination.Ngokungafaniyo ne-ECD, apho ukugcinwa kwezinto ezixubileyo kuchongwa ngumlinganiselo wokuhlukana, kwi-LMD, ugxininiso kwi-binder eqinile igqitywe yi-equilibrium ye-thermodynamic yendawo phakathi kwezigaba eziqinileyo kunye ne-liquid kwaye, ngoko ke, iipropati zokuhlalisana kwezinto eziqinileyo kunye. izigaba zolwelo.I-alloy State Diagrams.Ngenxa yokuchithwa kwe-Ti ukusuka kwisiseko se-alloy, i-Ti concentration iyancipha ngokunyuka kwe-d ukusuka kumphambili we-delamination ukuya kumda we-delamination layer.Ngenxa yoko, i-concentration ye-Ta iye yanda ngokunyuka kwe-d kunye ne-bundle, eyayihambelana nokulinganisa intsimi yesigaba (iFig. 5 eyongezelelweyo).I-concentration ye-Ti kwi-Cu70Ag30 melt iwela ngokungekho nzulu ngakumbi kune-Cu esulungekileyo yokunyibilika, ehambelana nesantya esicothayo sokususwa kwe-alloy.Iiprofayili zoxinaniso ezilinganisiweyo kwiFig.I-5b ikwabonisa ukuba umlinganiselo wokuxinana kwe-Ag kunye ne-Cu kulwelo awuguquguquki ncam ecaleni komaleko we-alloy enikezelweyo, ngelixa ukulinganisa intsimi yesigaba lo mlinganiso ucingelwa ukuba uhlala uhleli kukulinganisa ukunyibilika njengoko. i-pseudo-element Cu70Ag30.Ngaphandle kwalo mahluko wobungakanani, imodeli yentsimi yesigaba ibamba isiphumo somgangatho ophezulu wokongeza i-Ag ekucinezeleni ukuvuza kwe-Ta.Imodeli egcweleyo yobungakanani bemithamo yogxininiso yazo zonke izinto ezine kwizibophelelo eziqinileyo kunye nolwelo zifuna imodeli echaneke ngakumbi yamacandelo amane edayagram yesigaba seTaTiCuAg, engaphaya kobubanzi balo msebenzi.
Iiprofayile zoxinaniso ezilinganisiweyo ngokuxhomekeke kumgama d ukusuka kumphambili we-delamination we-Ta15Ti85 ingxubevange kwi (a) Cu esulungekileyo nyibilika kunye (b) Cu70Ag30 nyibilika.Uthelekiso lweqhezu lomthamo olinganisiweyo wezinto eziqinileyo ρ(d) zesakhiwo esigunyazisiweyo (umgca oqinileyo) kunye nengqikelelo yethiyori ehambelana nenxaki ngaphandle kokuvuza uTa (umgca odayiweyo).(1) (c) Phakamisa uqikelelo lweequation.(1) Inxaki ilungisiwe kwi-delamination front.(2) Oko kukuthi, ukuvuza kweTa kuqwalaselwa.Ukulinganisa i-avareji bond ububanzi λw kunye nomgama λs (d).Iibhari zempazamo zibonisa ukutenxa okusemgangathweni.
Kwikhiwane.I-5c ithelekisa iqhezu lomthamo olinganisiweyo wezinto eziqinileyo ρ(d) (umgca oqinileyo) kwisakhiwo esigunyazisiweyo seCu kunye neCu70Ag30 ukusuka kwinyibiliko kunye noqikelelo lwethiyori (umgca odawunisiweyo) ofunyenwe kulondolozo lobunzima kusetyenziswa umlinganiselo weTa olinganiselwe kwisibophelelo esiqinileyo \({{ c }_ {Ta} ^{s}(d)\) (Umfanekiso 5a,b) kwaye ungayihoyi ukuvuza kweTa kunye nokuthuthwa kweTa phakathi kweebhondi ezinobunzulu obuhlukeneyo bokuhlukana.Ukuba uTa uyatshintsha ukusuka kwisiqina ukuya kulwelo, yonke iTa ekwisiseko sealloyi kufuneka iphinde isasazwe kwisibophelelo esiqinileyo.Ngoko ke, kulo naliphi na umaleko wolwakhiwo olukude ngokwendlela yokususwa kwe-alloy, ukugcinwa kobunzima kuthetha ukuba \({c}_{Ta}^{s}(d)){S}_{s}(d) )={c}_ {Ta}^{0}(d){S}_{t}\), apho \({c}_{Ta}^{s}(d)\)\) kunye \({c }_{Ta }^ {0}\) lugxininiso lwe-Ta kwindawo d kwi-binder kunye ne-matrix alloy, ngokulandelelana, kunye ne-Ss (d) kunye ne-St ziindawo ezinqamlezileyo zesibophelelo esinzima kunye nommandla wonke okude, ngokulandelelana.Oku kuqikelela iqhezu lomthamo wezinto eziqinileyo kwindawo ekude.
Oku kungasetyenziswa ngokulula kulwakhiwo lwe-Cu ecocekileyo enikezelweyo kunye neCu70Ag30 iyanyibilika kusetyenziswa i- \({c}_{Ta}^{s}(d)\)" ehambelanayo igophe elihambelana nomgca oluhlaza.Ezi ziqikelelo zibekwe ngaphezulu kuMzobo we-5c obonisa ukuba ukungahoyi ukuvuza kwe-Ta yi-predictor engalunganga yokusasazwa kwamaqhezu evolumu.Ukugcinwa kobunzima obungavuziyo buqikelela ukuhla kwe-monotonic kwiqhezu lomthamo ngokunyuka kwe-d, ebonwa ngokomgangatho kwi-Cu esulungekileyo enyibilikayo, kodwa hayi kwi-Cu70Ag30 enyibilikayo, apho u-ρ(d) unobuncinane.Ukongeza, oku kukhokelela kuqikelelo olubalulekileyo lwamaqhezu omthamo kwindawo yokwahlula zombini ezinyibilikayo.Kweyona milinganiselo incinane d ≈ 10 µm, amaxabiso aqikelelweyo ρ kuzo zombini izinyibiliko angaphezulu kwe-0.5, ngelixa amaxabiso alinganisiweyo ρ e-Cu kunye ne-Cu70Ag30 yokunyibilika aphezulu kancinci kuno-0.3 no-0.4, ngokulandelelanayo.
Ukugxininisa indima ephambili yokuvuza kwe-Ta, emva koko sibonisa ukuba umahluko wobungakanani phakathi komlinganiselo kunye noqikelelo lwamaxabiso ρ kufutshane nomphambili wokubola unokupheliswa ngokucokisa uqikelelo lwethu lwethiyori ukubandakanya oku kuvuza.Ukuza kuthi ga ngoku, masibale inani lilonke le-atom zikaTa eziqukuqelayo ukusuka kwinto eqinileyo ukuya elulwelweni xa ukubola okungaphambili kuhambela kude Δxi = vΔt kwisithuba sexesha Δt Δxi = vΔt, apho \(v={\dot{x) )) _{i }( t )\) - izinga lokuchithwa, ubunzulu kunye nexesha kunokufunyanwa kubudlelwane obaziwayo \({x}_{i}(t)=\sqrt{4p{D}_{l}t} } \) deaeration.Umthetho wasekhaya wogcino lobunzima kumphambili wokwahlula (d ≈ 0) kukuba ΔN = DlglΔtSl/va, apho i-gl isithambiso soxinzelelo lwe-athom ze-Ta kulwelo, i-va ngumthamo we-atom ohambelana noxinzelelo oluchazwa njenge iqhezu leathomu, kunye ne-Sl = St - Ss yindawo enqamlezileyo yomjelo wolwelo kumphambili we-delamination.I-concentration gradient gl ingabalwa ngokucinga ukuba ugxininiso lwe-atom ze-Ta lunexabiso elingaguqukiyo \({c}_{Ta}^{l}\) kujongano kwaye lincinci kakhulu kwinyibilika ngaphandle kwendawo ekhutshiweyo, ethi inika \( {g}_ {l}={c}_{Ta}^{l}/{x}_{i}\) Ngoko, \({{\Delta}}}N=({{\Delta} {x}_{i} {S}_{l}/{v}_{a}){c}_{Ta}^{l}/(2p)\).Xa umphambili usiya kumgama Δxi, iqhezu eliqinileyo lilingana nenani lilonke le-atom zikaTa ezisusiweyo kwisiseko sealloyi, \({{\Delta}}{x}_{i}{S}_{t} { c }_{Ta}^ { 0}/{v}_{a}\), ukuya kwinani lenani le-atom zikaTa ezivuza kulwelo, ΔN, kwaye zibandakanywe kwisibophelelo esiqinileyo\({{\Delta} } {x}_{i}{S}_{s {c}_{Ta}^{s}/{v}_{a}\).Le nxaki, kunye nentelekelelo engentla ye-ΔN kunye nobudlelwane St = Ss + Sl kunye nezigaba kumphambili we-delamination.
Kumda wonyibiliko onguziro we-athom ze-Ta, ocutha ukuqikelelwa kwangaphambili kokungabikho kokuvuza, \(\rho ={c}_{Ta}^{0}/{c}_{Ta}^{s}) \) elulwelo ( \({c }_{Ta}^{l}=0\)).Ukusebenzisa amaxabiso \({c}_{Ta}^{l}\malunga ne-0.03\) ukusuka kwimilinganiselo yovavanyo (engaboniswanga kwiSazobe 5a, b) kunye neenombolo zePeclet p ≈ 0.26 kunye ne-p ≈ 0.17 kunye nokugxilwa kwezinto eziqinileyo \ ( {c}_{Ta}^{s}\ malunga ne-0.3\) kunye \({c}_{Ta}^{s}\ malunga ne-0.25\) ye-Cu kunye ne-Cu70Ag30 iyanyibilika, ngokulandelelana , sifumana ixabiso eliqikelelweyo le ukunyibilika, ρ ≈ 0.38 kunye ρ ≈ 0.39.Olu qikelelo ngokobungakanani luvumelana ngokufanelekileyo nemilinganiselo.Eminye iyantlukwano (eqikelelweyo i-0.38 vs. ilinganiswe nge-0.32 ye-Cu esulungekileyo yokunyibilika kunye ne-0.39 eqikelelweyo ngokuchasene ne-0.43 ye-Cu70Ag30 yokunyibilika) inokucaciswa ngomlinganiselo omkhulu wokungaqiniseki malunga noxinzelelo lwe-Ta oluphantsi kakhulu kulwelo (\( {c}_{Ta }^ {l}\ malunga ne-0.03\)), elindeleke ukuba ibenkulu kancinane kwinyibilika yobhedu olusulungekileyo.
Nangona iimvavanyo zangoku zenziwe kwii-alloys ezisisiseko kunye nezinto ezinyibilikayo, silindele ukuba iziphumo zohlalutyo lwale mifuniselo ziya kunceda ekufumaneni ii-equations.(2) Ukusetyenziswa ngokubanzi kwezinye iinkqubo ze-doping ze-LMD kunye nezinye iindlela ezinxulumene nazo ezifana ne-Solid State Impurity Removal (SSD).Kuze kube ngoku, impembelelo yokuvuza kwezinto ezingenakulinganiswa kwisakhiwo se-LMD ayizange ihoywe ngokupheleleyo.Oku kubangelwa ikakhulu kwinto yokuba esi siphumo asibalulekanga kwi-ECDD, kwaye ukuza kuthi ga ngoku kucingelwa ukuba i-NMD iyafana ne-REC.Nangona kunjalo, umahluko ophambili phakathi kwe-ECD kunye ne-LMD kukuba kwi-LMD ukunyibilika kwezinto ezingaxutywanga kulwelo kwandiswa kakhulu ngenxa yoxinaniso oluphezulu lwezinto ezixubeneyo kwicala lolwelo lojongano (\({c}_{Ti} ^{ l}\)), nto leyo eyandisa ugxininiso lweziqalelo ezingachanekanga (\({c}_{Ta}^{l}\)) kwicala lolwelo lojongano kwaye yehlise iqhezu levolyum elixelwe kwangaphambili yinxaki yemeko eqinileyo. .2 {Ta} ^{l}\ Ngokufanayo, phezulu \({c}_{Ti}^{s}\) ivumela i-Cu ukuba ifakwe kwizibophelelo ezinzima, kwaye ukuxinwa kwe-Cu eqinile kwezi zibophelelo kuyahluka ukusuka malunga ne-10% ngokuthe ngcembe. ukuhla kumaxabiso akunamsebenzi emphethweni womaleko omncinci ogunyazisiweyo (iFig. 6). Ngokwahlukileyo koko, ukususwa kwe-electrochemical ye-Ag kwi-AgAu alloys yi-ECD yi-non-equilibrium reaction enganyusi ukunyibilika kwe-Au kwi. i-electrolyte.Ukongezelela kwi-LMD, sinethemba lokuba iziphumo zethu zisebenza kwiidrive zombuso oqinileyo, apho umda oqinileyo kulindeleke ukuba ugcine ukulingana kwe-thermodynamic yendawo ngexesha lokususwa kwe-alloy.Olu lindelo luxhaswa yinyaniso yokuba utshintsho kwiqhekeza kwezinto eziqinileyo kuluhlu olunikezelweyo lwesakhiwo se-SSD sabonwa, oku kuthetha ukuba, ngexesha logunyaziso kukho ukuchithwa kwe-ligament eqinile, ehambelana nokuvuza kwezinto ezingenakulinganiswa.
Kwaye i-equation.(2) Ukuze uqikelele ukuhla okubalulekileyo kwiqhezu eliqinileyo kwindawo yokususa i-alloy ngaphambili ngenxa yokuvuza kwe-Ta, kuyafuneka ukuba kuthathelwe ingqalelo uThutho lweTa kwindawo yokususa i-alloy ukuze kuqondwe ulwabiwo lwamaqhezu aqinileyo kulo lonke. umaleko wokususwa kwe-alloy, ohambelana nobhedu olusulungekileyo kunye ne-Cu70Ag30 enyibilikayo.I-Cu70Ag30 inyibilika (umgca obomvu kwiSazobe 5c), ρ(d) unobuncinane obumalunga nesiqingatha somaleko ogunyazisiweyo.Ubuncinci bubangelwa kukuba inani elipheleleyo le-Ta equlethwe kwi-binder enzima kufuphi nomda woluhlu olunikezelweyo likhulu kune-alloy yesiseko.Oko kukuthi, ku-d ≈ 230 μm \({S}_{s}(d){c}_{Ta}^{s}(d)\, > \,{S}_{t}{c} _ { Ta} ^ {0}\), okanye ilingane ngokupheleleyo, umlinganiselo ρ(d) = Ss(d)/St ≈ 0.35 mkhulu kakhulu kuneequation iqikelele.(1) Akukho kuvuza\({c}_{Ta}^{0}/{c}_{Ta}^{s}(d))\malunga 0.2\).Oku kuthetha ukuba inxalenye ye-Ta ebalekayo ithuthwa ukusuka kumphambili wokwahlula ukuya kwindawo ekude ukusuka kulo mphambili, isasazwa kulwelo kunye nojongano oluqinileyo-olwelo, apho iphinda ifakwe khona.
Olu hlengahlengiso lunesiphumo esichaseneyo sokuvuza kwe-Ta ukutyebisa izibophelelo ze-Ta hard, kwaye ulwabiwo lwamaqhezu alukhuni lunokuchazwa ngokomgangatho njengebhalansi yokuvuza kwe-Ta kunye nokubekwa kwakhona.Kwi-Cu70Ag30 yokunyibilika, uxinaniso lwe-Ag kulwelo luyanda ngokunyuka kwe-d (umgca onamachaphaza amdaka kwiSazobe. .Oku kugcina isahlulo esiluqilima esikhulu ngokwaneleyo ukunqanda ukuqhekeka ngenxa yokuqhawuka koqhagamshelwano oluqinileyo, nto leyo echaza ukuba kutheni izakhiwo ezinikezelwe kwi-Cu70Ag30 zinyibilika zigcina imfezeko yolwakhiwo emva kokubotshwa.Ngokwahlukileyo koko, ukunyibilika kobhedu olusulungekileyo, ukuvuza kunye nokubekwa ngokutsha kuphantse kwacima enye nenye, nto leyo ekhokelela ekuncipheni okucothayo kwezinto eziqinileyo ngaphantsi komda wokuqhekeka kuninzi lomaleko othunyiweyo, kushiya kuphela umaleko obhityileyo ogcina ingqibelelo yesakhiwo kufutshane nomda woluhlu. umaleko ogunyazisiweyo.(Umfanekiso 4b, iThebhile 1).
Ukuza kuthi ga ngoku, uhlalutyo lwethu lujolise ikakhulu ekuchazeni impembelelo enamandla yokuvuza kwezinto ezixubeneyo kwindawo ekhutshiweyo kwiqhezu eliqinileyo kunye ne-topology yezakhiwo ezinikezelweyo.Ngoku makhe sijike kwisiphumo soku kuvuza ekonakaleni kolwakhiwo lwe-bicontinuum ngaphakathi komgangatho ogunyazisiweyo, odla ngokwenzeka ngexesha le-LMD ngenxa yobushushu obuphezulu.Oku kwahlukile kwi-ECD apho i-coarsening ingekhoyo ngexesha lokususwa kwe-alloy, kodwa inokubangelwa kukuhlanjululwa kumaqondo obushushu aphezulu emva kokususwa kwe-alloy.Ukuza kuthi ga ngoku, ukurhabaxa ngexesha le-LMD kuye kwamodareyithwa phantsi kwengcinga yokuba yenzeka ngenxa yokusasazwa kwezinto ezingagungqiyo ecaleni kojongano olululwelo oluqinileyo, olufana nokudityaniswa komphezulu okuphakathi kwezakhiwo ze-ECD ezifakwe i-nanoporous.Ngoko ke, ubungakanani bombhobho bulungiselelwe kusetyenziswa imithetho esemgangathweni yokwandisa i-capillary.
apho i-tc ilixesha elirhabaxa, elichazwa njengexesha eligqithileyo emva kokudlula komphambili we-delamination kubunzulu xi ngaphakathi komaleko we-delamination (apho i-λ inexabiso lokuqala lika-λ00) kude kube sekupheleni komfuniselo we-delamination, kunye nesalathisi sokukala n = 4 isasaza umphezulu.I-Eq kufuneka isetyenziswe ngononophelo.(3) Tolika imilinganiselo ye-λ kunye nomgama d kwisakhiwo sokugqibela ngaphandle kokungcola ekupheleni kovavanyo.Oku kungenxa yokuba ummandla okufutshane nomda womaleko othunyiweyo uthatha ixesha elide ukwandisa kunommandla okufutshane nomphambili.Oku kunokwenziwa ngeeequations ezongezelelweyo.(3) Unxibelelwano no-tc kunye no-d.Olu nxulumano lunokufumaneka ngokulula ngokuqikelela ubunzulu bokususwa kwe-alloyi njengomsebenzi wexesha, \({x}_{i}(t)=\sqrt{4p{D}_{l}t}\), enika i-tc( d ) = te − tf(d), apho ilixesha lovavanyo lonke, \({t}_{f}(d)={(\sqrt{4p{D}_{l}) {t}_{ e } }-d)}^{2}/(4p{D}_{l})\) lixesha lokuba umphambili we-delamination ufikelele kubunzulu obulingana nobunzulu bokugqibela be-delamination thabatha d.Nxulumanisa olu phawu lwe-tc(d) kwinxaki.(3) Qikelela λ(d) (jonga inqaku elongezelelweyo 5).
Ukuvavanya olu qikelelo, senze imilinganiselo yobubanzi kunye nomgama phakathi kweenyanda kumacandelo apheleleyo anqamlezayo wezakhiwo ezinikezelweyo eziboniswe kwi-Supplementary Figure 9 ye-Cu ecocekileyo kunye ne-Cu70Ag30 iyanyibilika.Ukusuka kumgca wokuskena ngependicular ukuya kwicala le-delamination kwimigama eyahlukeneyo d ukusuka kumphambili we-delamination, sifumene i-avareji yobubanzi λw(d) ye-Ta-rich bundles kunye nomndilili womgama λs(d) phakathi kweenyanda.Le milinganiselo iboniswe kwifig.5d kwaye xa kuthelekiswa noqikelelo lwenxaki.(3) kuMfanekiso owongezelelweyo we-10 wamaxabiso ahlukeneyo n.Uthelekiso lubonisa ukuba isalathiso sokusasazwa komphezulu we-n = 4 sinika uqikelelo olubi.Olu qikelelo aluphuculwanga kakhulu ngokukhetha i-n = 3 ye-bulk diffusion-mediated capillary coarsening, umntu anokulindela ngokungenangqondo ukunika ukulingana okungcono ngenxa yokuvuza kwe-Ta kulwelo.
Lo mahluko wobungakanani phakathi kwethiyori kunye nomfuniselo awumangalisi, kuba u-Eq.(3) ichaza i-capillary coarsening kwiqhezu levolyum engaguqukiyo ρ, ngexa kwi-LMD iqhezu lezinto eziqinileyo ρ aliguquguquki.ρ utshintsha ngokwesithuba phakathi komgangatho osusiweyo ekupheleni kokususwa kwe-alloy, njengoko kubonisiwe kwifig.5c.ρ ikwatshintsha kunye nexesha ngexesha lokususwa kobumdaka kubunzulu obumiselweyo bokususa, ukusuka kwixabiso lomphambili wokususa (ophantse ube ngokuguquguqukayo ngexesha kwaye ngaloo ndlela uzimele geqe kwi-tf kunye no-d) ukuya kwixabiso elilinganisiweyo lika-ρ(d) eliboniswe kwiSazobe. 5c ehambelana nexesha lokugqibela.Ukususela kwikhiwane.3d, kunokuqikelelwa ukuba ukubola kwamaxabiso angaphambili malunga ne-0.4 kunye ne-0.35 ye-AgCu kunye ne-Cu ecocekileyo iyanyibilika, ngokulandelanayo, kuzo zonke iimeko eziphezulu kunexabiso lokugqibela le-ρ ngexesha le.Kubalulekile ukuqaphela ukuba ukuhla ku-ρ kunye nexesha kwi-d esisigxina sisiphumo esithe ngqo sobukho be-concentration gradient ye-miscible element (Ti) kulwelo.Ekubeni i-concentration ye-Ti kwi-liquids iyancipha ngokunyuka kwe-d, i-equilibrium concentration ye-Ti kwizinto eziqinileyo nazo ziyancipha umsebenzi we-d, okhokelela ekuchithekeni kwe-Ti kwizibophelelo eziqinileyo kunye nokuncipha kwiqhekeza eliqinileyo ngokuhamba kwexesha.Utshintsho lwexeshana ku-ρ lukwachatshazelwa kukuvuza kunye nokubekwa ngokutsha kweTa.Ke, ngenxa yeziphumo ezongezelelweyo zokuchithwa kunye nokuphindaphinda, silindele ukuba ukucolwa ngexesha le-LMD kuya kuthi, njengomthetho, kwenzeke kumaqhezu evolumu angatshintshiyo, okuya kukhokelela ekuguqukeni kwesakhiwo ukongeza kwi-capillary coarsening, kodwa nangenxa yokusabalalisa ulwelo kwaye hayi ecaleni komda kuphela ulwelo oluqinileyo.
Iinyaniso zeequation.(3) Ububanzi bebhondi kunye nemilinganiselo yezithuba ze-3 ≤ n ≤ 4 ayinakulinganiswa (i-Supplementary Fig. 10), ebonisa ukuba ukuchithwa kunye nokulungiswa kwakhona kungekhona ngenxa yokunciphisa i-interface kudlala indima ephambili kuvavanyo lwangoku.Kwi-capillary coarsening, i-λw kunye ne-λs kulindeleke ukuba zibe nokuxhomekeka okufanayo ku-d, ngelixa i-Fig. 5d ibonisa ukuba i-λs inyuka ngo-d ngokukhawuleza kakhulu kuno-λw kwi-Cu ne-Cu70Ag30 enyibilikayo.Ngelixa ithiyori ecolekileyo ethathela ingqalelo ukupheliswa kunye nokubekwa ngokutsha kufuneka kuthathelwe ingqalelo ukucacisa le milinganiselo ngokobungakanani, lo mahluko ulindeleke ngokomgangatho, ekubeni ukuchithwa ngokupheleleyo kweebhondi ezincinci kunegalelo ekwandeni komgama phakathi kweebhondi.Ukongeza, i-λs ye-Cu70Ag30 inyibilika ifikelela kwixabiso layo eliphezulu kumda we-alloy ngaphandle kwe-alloy, kodwa into yokuba i-λs yobhedu ecocekileyo iyancibilika iqhubeka nokunyuka kwe-monotonically inokuchazwa ngokunyuka kwe-Ag yoxinaniso kulwelo, apho. d isetyenziselwa ukuchaza ρ(d) kumfanekiso 5c ukuziphatha okungaqhelekanga.Ukwandisa ugxininiso lwe-Ag ngokunyuka kwe-d kucinezela ukuvuza kwe-Ta kunye nokuchithwa kwe-binder, okukhokelela ekunciphiseni kwi-λs emva kokufikelela kwixabiso eliphezulu.
Ekugqibeleni, qaphela ukuba izifundo zekhompyutheni ze-capillary coarsening kwi-fraction ye-volume eqhubekayo zibonisa ukuba xa i-fraction yevolumu iwela ngaphantsi komda omalunga ne-0.329.30, i-fragment fragments ngexesha lokunyuka.Ngokwesiqhelo, lo mgubasi unokuba ngaphantsi kancinane ngenxa yokuba ukuqhekeka kunye nokunciphisa i-genus ehambelanayo kwenzeka kwinqanaba lexesha elithelekisekayo okanye elikhulu kunexesha elipheleleyo lokususa i-alloy kolu vavanyo.Inyaniso yokuba izakhiwo ezinikezelweyo kwi-Cu70Ag30 ziyanyibilika zigcina imfezeko yolwakhiwo nangona u-ρ(d) engaphantsi kancinane ka-0.3 kumndilili woluhlu luka-d ibonisa ukuba uqhekeko, ukuba lukhona, lwenzeka ngokuyinxenye kuphela.Umthamo weqhezu lomthamo wokwahlulwa unokuxhomekeka ekuchithweni nasekubuyiseleni inani.
Olu phononongo lufikelela kwizigqibo ezibini eziphambili.Okokuqala, kwaye ngakumbi, i-topology yezakhiwo ezinikezelweyo eziveliswe yi-LMD inokulawulwa ngokukhetha ukunyibilika.Ngokukhetha ukunyibilika ukunciphisa ukunyibilika kwento engenakulinganiswa A ye-AXB1-X yesiseko se-alloy ekunyibilikeni, nangona kunqunyelwe, kunokwenziwa ulwakhiwo olunikezelwe kakhulu olugcina ubumbano lwalo nakwizigxina eziphantsi zento yomgangatho X kunye nentembeko yesakhiwo. .Ngaphambili kwakusaziwa ukuba oku kwakunokwenzeka kwi-ECD25, kodwa kungekhona kwi-LMD.Isiphelo sesibini, esibaluleke ngakumbi, kungenxa yokuba kwi-LMD ingqibelelo yesakhiwo inokugcinwa ngokuguqula i-delegating medium, enika umdla ngokwayo kwaye inokuchaza ukuqwalaselwa kwe-alloy yethu ye-TaTi kwi-Cu kunye ne-CuAg ecocekileyo inyibilika kwi-. ngokubanzi ukucacisa okubalulekileyo, umahluko obungacingelwayo ngaphambili phakathi kwe-ECD ne-LMD.
Kwi-ECD, ukubambisana kwesakhiwo kugcinwa ngokugcina izinga lokususa ukungcola kwinqanaba eliphantsi le-X, elihlala lihlala lihlala lihamba ixesha elide kumandla okuqhuba, amancinci ngokwaneleyo ukugcina i-miscible element B eyaneleyo kwi-binder eqinile ngexesha lokususwa kokungcola ukugcina. umthamo oqinileyo.iqhezu ρ likhulu ngokwaneleyo ukuthintela uqhekeko25.Kwi-LMD, ireyithi yokususa i-alloy \(d{x}_{i}(t)/dt=\sqrt{p{D}_{l}/t}\) iyancipha ngokuhamba kwexesha ngenxa ye-diffusion limited kinetics.Ngaloo ndlela, kungakhathaliseki ukuba luhlobo luni lokwakheka kwenyibilika echaphazela kuphela inani lePeclet p, izinga le-delamination ngokukhawuleza lifikelela kwixabiso elincinci ngokwaneleyo ukugcina inani elaneleyo le-B kwisibophelelo esiqinileyo, esibonakaliswa ngokuthe ngqo kwinto yokuba ρ kwi-delamination. umphambili uhlala ulingana nexesha.Inyani kwaye ngaphezulu komda wokuqhekeka.Njengoko kubonisiwe ngokulinganisa intsimi yesigaba, isantya se-peel sifikelela ngokukhawuleza kwixabiso elincinci ngokwaneleyo ukuphazamisa ukukhula kwe-eutectic bond, ngaloo ndlela kuququzelela ukubunjwa kwezakhiwo eziboshwe nge-topologically ngenxa ye-lateral rocking motion ye-lamellae.Ke ngoko, owona mahluko ongundoqo ongundoqo phakathi kwe-ECD kunye ne-LMD ulele ekuveleni komphambili we-delamination ngokusebenzisa ubume bangaphakathi bomaleko emva kokwahlulwa kunye no-ρ, endaweni yereyithi ye-delamination.
Kwi-ECD, ρ kunye noqhagamshelo luhlala lungaguquguquki kuyo yonke i-remote layer.Kwi-LMD, ngokuchaseneyo, zombini ziyahluka ngaphakathi komaleko, oboniswe ngokucacileyo kolu phononongo, obonisa ukugxininiswa kweathom kunye nokuhanjiswa kwe-ρ kubo bonke ubunzulu bezakhiwo ezinikezelweyo ezidalwe yi-LMD.Kukho izizathu ezibini zolu tshintsho.Okokuqala, nakumda we-zero wokunyibilika ongu-A, i-concentration gradient B kulwelo, engekhoyo kwi-DZE, yenza i-concentration gradient A kwisibophelelo esiqinileyo, esikukulingana kweekhemikhali nolwelo.Ithambeka A, ngokulandelelanayo, yenza i-gradient ρ ngaphakathi kumaleko ngaphandle kokungcola.Okwesibini, ukuvuza kuka-A kulwelo ngenxa yokunganyibiliki kwe-zero ngakumbi kumodareyitha umahluko wendawo ρ ngaphakathi kolu maleko, kunye nokunyibilika okucuthiweyo kunceda ukugcina u-ρ uphezulu kwaye ufana kakhulu nendawo ukugcina uqhagamshelwano.
Okokugqibela, ukuvela kwesayizi yebhondi kunye noqhagamshelo ngaphakathi koluhlu olunikezelweyo ngexesha le-LMD luntsonkothe ​​ngakumbi kunomphezulu we-capillary coarsening kwi-fraction yevolumu eqhubekayo, njengoko bekucingelwa ngaphambili ngokufaniswa nokudityaniswa kwe-nanoporous ECD izakhiwo.Njengoko kubonisiwe apha, ukurhabaxa kwi-LMD kwenzeka kwiqhezu eliqinileyo eliguqukayo ngokwesithuba kwaye lidla ngokuphenjelelwa lugqithiso losasazo lwe-A kunye no-B kwimeko yolwelo ukusuka kumphambili we-delamination ukuya kumda womaleko odibeneyo.Imithetho yokukala ye-capillary coarsening ekhawulelwe ngokusasazwa komphezulu okanye isambuku ayinakubala utshintsho kububanzi kunye nomgama phakathi kweenyanda ngaphakathi komaleko ogunyazisiweyo, kucingelwa ukuba uthutho luka-A no-B olunxulunyaniswa noxinzelelo lweqondo lolwelo ludlala indima elinganayo okanye efanayo.Okubaluleke ngakumbi kunokunciphisa indawo yojongano.Ukuphuhliswa kwethiyori ethathela ingqalelo ezi mpembelelo zahlukeneyo lithemba elibalulekileyo lekamva.
I-Titanium-tantalum binary alloys yathengwa kwi-Arcast, Inc (Oxford, Maine) isebenzisa i-45 kW Ambrell Ekoheat ES unikezelo lwamandla ombane kunye ne-crucible yobhedu epholileyo yamanzi.Emva kokushisa okuningana, i-alloy nganye ifakwe kwiiyure ze-8 kwiqondo lokushisa ngaphakathi kwe-200 ° C. yendawo yokunyibilika ukufikelela kwi-homogenization kunye nokukhula kweenkozo.Iisampulu ezisikwe kule master ingot zadityaniswa ngamabala kwiingcingo zikaTa kwaye zanqunyanyiswa kwingalo yerobhothi.Iibhafu zetsimbi zalungiswa ngokufudumeza umxube we-40 g Cu (McMaster Carr, 99.99%) kunye ne-Ag (Kurt J. Lesker, 99.95%) okanye amasuntswana e-Ti kumandla aphezulu usebenzisa i-4 kW Ameritherm Easyheat inkqubo yokufudumeza induction de ukupheliswa okupheleleyo.iibhafu.nyibilika ngokupheleleyo.Nciphisa amandla kwaye uvumele ibhafu ivuse kwaye ilungelelanise isiqingatha seyure kwiqondo lokushisa lokuphendula lika-1240 ° C.Emva koko ingalo yerobhothi iyancipha, isampuli ibhaptizwa kwindawo yokuhlambela ixesha elimiselweyo kwaye isuswe ukupholisa.Konke ukufudumeza kwe-alloy billet kunye ne-LMD kuqhutywe kwi-atmospheric ye-argon ephezulu yokucoceka (99.999%).Emva kokususa i-alloy, amacandelo anqamlekileyo eesampuli ahlanjululwe kwaye ahlolwe kusetyenziswa i-microscope ye-optical kunye ne-scan electron microscopy (SEM, JEOL JSM-6700F).Uhlalutyo lwe-Elemental lwenziwa yi-energy dispersive X-ray spectroscopy (EDS) kwi-SEM.I-microstructure ye-microstructure ye-three-dimensional microstructure yeesampulu ezinikezelweyo zabonwa ngokunyibilikisa isigaba esityebileyo sobhedu kwi-35% yesisombululo se-nitric acid (ibakala lohlalutyo, i-Fluka).
Ukulinganisa kwenziwa kusetyenziswa imodeli ephuhliswe ngaphambili yentsimi yesigaba sokuqhawula i-alloy ternary15.Imodeli inxulumene nenguquko yentsimi yesigaba ϕ, eyahlula phakathi kwezigaba eziqinileyo kunye nezamanzi, kwintsimi yoxinaniso ci yezinto ezixutywayo.Amandla asimahla enkqubo abonakaliswa njenge
apho i-f(φ) isithintelo esiphindwe kabini esine-minima kwi-φ = 1 kunye ne-φ = 0 ehambelana nezinto eziqinileyo kunye nolwelo, ngokulandelelana, kunye ne-fc(φ, c1, c2, c3) ligalelo lekhemikhali kwinkululeko yevolumu echaza ukuxinana kwamandla I-alloy yeepropati ze-thermodynamic.Ukulinganisa ukuxutywa kwe-Cu ecocekileyo okanye i-CuTi iyancibilika kwii-alloys ze-TaTi, sisebenzisa ifom ye-fc (φ, c1, c2, c3) kunye neeparamitha njengereferensi.15. Ukususa i-alloys ye-TaTi ene-CuAg iyanyibilika, senze lula inkqubo ye-quaternary (CuAg)TaTi kwi-ternary system esebenzayo kunye ne-parameters eyahlukeneyo ngokuxhomekeke kwi-Ag concentration, njengoko kuchazwe kwiNqaku elongezelelweyo 2. intsimi yoxinaniso ifunyenwe kwifom eyahlukileyo kwifom
Apho \({M}_{ij}={M}_{l}(1-\phi){c}_{i}\khohlo({\delta}_{ij}-{c}_{j} \ ekunene)\) yimatrix yokushukuma kweathom, kwaye Lϕ ilawula ikinetics yoncamathiselo lweathom kujongano oluqinileyo-olwelwe.
Idatha yovavanyo exhasa iziphumo zolu phononongo inokufumaneka kwifayile yedatha eyongezelelweyo.Iiparamitha zokulinganisa zinikwe ngolwazi olongezelelweyo.Zonke iinkcukacha zikwafumaneka kubabhali abachaphazelekayo xa beceliwe.
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