Kukura translucent graphite firimu paNi uye ayo maviri-nzira polymer-yemahara kufambisa

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Nanoscale graphite films (NGFs) akasimba nanomaterials anogona kugadzirwa necatalytic chemical vapor deposition, asi mibvunzo inoramba iri pamusoro pekureruka kwekutamisa uye kuti morphology yepasi inokanganisa sei kushandiswa kwavo mumidziyo yechizvarwa chinotevera. Pano tinoshuma kukura kwe NGF kumativi ose maviri e polycrystalline nickel foil (nzvimbo 55 cm2, ukobvu hunenge 100 nm) uye kushandura kwayo kusina polymer (kumberi neshure, nzvimbo inosvika 6 cm2). Nekuda kweiyo morphology yecatalyst foil, iwo maviri kabhoni mafirimu anosiyana muhunhu hwavo uye humwe hunhu (sekushata kwepamusoro). Isu tinoratidza kuti NGFs ine rougher backside yakanyatsokodzera kuti NO2 ionekwe, nepo yakapfava uye yakawanda conductive NGFs kudivi remberi (2000 S/cm, sheet resistance - 50 ohms/m2) inogona kuita conductors. chiteshi kana electrode yesolar cell (sezvo inotumira 62% yechiedza chinooneka). Pakazere, iyo yakatsanangurwa kukura uye maitiro ekufambisa anogona kubatsira kuona NGF seimwe kabhoni zvinhu zvetekinoroji yekushandisa uko graphene uye micron-makobvu graphite mafirimu asina kukodzera.
Graphite chinhu chinoshandiswa zvakanyanya mumaindasitiri. Zvinonyanya kukosha, graphite ine zvimiro zveyakaderera mashoma density uye yakakwirira-mu-ndege inopisa uye magetsi conductivity, uye yakagadzikana zvakanyanya munzvimbo dzakaoma dzekupisa nemakemikari1,2. Flake graphite inonyanya kuzivikanwa yekutanga zvinyorwa zvegraphene research3. Kana yakagadziriswa kuita mafirimu matete, inogona kushandiswa mumhando dzakasiyana siyana dzekushandisa, kusanganisira kupisa sinks yemidziyo yemagetsi yakadai sema smartphones4,5,6,7, sechinhu chinoshanda mumasensa8,9,10 uye chekudzivirira kwemagetsi kupindira11. 12 uye mafirimu e-lithography mune yakanyanyisa ultraviolet13,14, kuitisa nzira mumasero ezuva15,16. Kune ese maapplication aya, zvingave zvakakosha kana nzvimbo huru dzemagraphite films (NGFs) dzine ukobvu hunodzorwa mu nanoscale <100 nm dzingagadzirwa nyore uye kutakurwa.
Mafirimu egraphite anogadzirwa nenzira dzakasiyana. Mune imwe nguva, kupinza uye kuwedzera kunoteverwa neexfoliation kwakashandiswa kugadzira graphene flakes10,11,17. Maflakes anofanirwa kugadziridzwa zvakare kuita mafirimu ehukobvu hunodiwa, uye kazhinji zvinotora mazuva akati wandei kugadzira mapepa akakora emagraphite. Imwe nzira ndeyekutanga negraphtable yakasimba precursors. Muindasitiri, mapepa emapolymer anoiswa carbonized (pa1000-1500 ° C) obva aitwa graphitized (pa2800-3200 ° C) kuti aumbe akanyatsorongeka akaturikidzana zvinhu. Kunyangwe mhando yemafirimu aya yakakwira, mashandisirwo esimba akakosha1,18,19 uye ukobvu hudiki hunogumira kune mashoma microns1,18,19,20.
Catalytic chemical vapor deposition (CVD) inzira inozivikanwa yekugadzira graphene uye ultrathin graphite films (<10 nm) ine high structural quality uye inonzwisisika cost21,22,23,24,25,26,27. Zvisinei, zvichienzaniswa nekukura kwemagraphene uye ultrathin graphite films28, kukura-nzvimbo yakakura uye / kana kushandiswa kweNGF kushandisa CVD kunotonyanya kuongororwa11,13,29,30,31,32,33.
CVD-yakakura graphene uye graphite mafirimu anowanzoda kuendeswa kune anoshanda substrates34. Aya mafirimu akaonda ekufambisa anosanganisira nzira mbiri huru35: (1) non-etch transfer36,37 uye (2) etch-based wet chemical transfer (substrate inotsigirwa)14,34,38. Imwe neimwe nzira ine zvimwe zvakanakira nezvayakaipira uye inofanirwa kusarudzwa zvichienderana neyakagadzirirwa kushandiswa, sekutsanangurwa kumwe kwe35,39. Kune mafirimu egraphene/graphite akakurira pacatalytic substrates, kutamiswa kuburikidza neakanyorova kemikari maitiro (ayo polymethyl methacrylate (PMMA) ndiyo inonyanya kushandiswa tsigiro layer) inoramba iri sarudzo yekutanga13,30,34,38,40,41,42. Iwe et al. Zvakataurwa kuti hapana polymer yakashandiswa kuchinjisa NGF (sample size inosvika 4 cm2) 25,43, asi hapana ruzivo rwakapihwa maererano nekugadzikana kwemuenzaniso uye / kana kubata panguva yekufambisa; Wet chemistry process uchishandisa mapolymers ane akati wandei nhanho, kusanganisira mashandisirwo uye kunotevera kubviswa kwechibairo chepolymer layer30,38,40,41,42. Iyi nzira ine zvipingamupinyi: semuenzaniso, masara epolymer anogona kushandura zvinhu zvemufirimu wakakura38. Kuwedzera kugadzirisa kunogona kubvisa yasara polymer, asi aya ekuwedzera matanho anowedzera mutengo uye nguva yekugadzirwa kwemafirimu38,40. Munguva yekukura kweCVD, girafu ye graphene inoiswa kwete chete kudivi repamberi recatalyst foil (divi rinotarisana nemhepo inoyerera), asiwo kumashure kwayo. Nekudaro, iyo yekupedzisira inoonekwa seyakaraswa uye inogona kukurumidza kubviswa ne soft plasma38,41. Kudzokorodza firimu iri kunogona kubatsira kuwedzera goho, kunyangwe riri remhando yakaderera pane yekabhoni firimu.
Pano, isu tinoshuma gadziriro yewafer-scale bifacial kukura kweNGF ine yakakwirira dhizaini mhando papolycrystalline nickel foil neCVD. Yakaongororwa kuti kushata kwepamberi uye kumashure kweiyo foil kunobata sei morphology uye chimiro cheNGF. Isu tinoratidza zvakare inodhura-inoshanda uye ine hushamwari hwepolymer-yemahara kuchinjisa kweNGF kubva kumativi ese ari nickel foil kuenda kune akawanda-anoshanda substrates uye tinoratidza kuti emberi uye kumashure mafirimu akakodzera sei kune akasiyana maapplication.
Zvikamu zvinotevera zvinokurukura makubvu emufirimu akasiyana-siyana zvichienderana nehuwandu hwemagrafu akaturikidzana: (i) single layer graphene (SLG, 1 layer), (ii) few layer graphene (FLG, < 10 layers), (iii) multilayer graphene ( MLG, 10-30 layers) uye (iv) NGF (~300 layers). Iyo yekupedzisira ndiyo yakajairika ukobvu inoratidzirwa sechikamu chenzvimbo (inenge 97% nzvimbo pa100 µm2)30. Ndosaka firimu rose richingonzi NGF.
Polycrystalline nickel foils inoshandiswa kugadzira graphene uye graphite mafirimu ane akasiyana maumbirwo semhedzisiro yekugadzira kwavo uye kunotevera kugadzirisa. Isu munguva pfupi yapfuura takashuma chidzidzo chekugadzirisa maitiro ekukura kweNGF30. Isu tinoratidza kuti maparamita ekuita senge annealing nguva uye kamuri yekumanikidza panguva yekukura nhanho inoita basa rakakosha mukuwana NGFs yeunifomu ukobvu. Pano, takaenderera mberi nekuongorora kukura kweNGF pane yakasvibiswa pamberi (FS) uye isina kusvibiswa kumashure (BS) nzvimbo dze nickel foil (Fig. 1a). Mhando mitatu yemasampuli FS uye BS akaongororwa, akanyorwa muTebhu 1. Pamusoro pekutarisa kwekuona, yunifomu yekukura kweNGF kumativi ose maviri e nickel foil (NiAG) inogona kuonekwa nekushanduka kwemavara ehuwandu hweNi substrate kubva kune chimiro chesimbi sirivha. grey kune matte grey ruvara (Fig. 1a); microscopic zviyero zvakasimbiswa (Fig. 1b, c). Yakajairika Raman spectrum yeFS-NGF inocherechedzwa munzvimbo inopenya uye inotaridzwa nemiseve tsvuku, yebhuruu uye orenji muFigure 1b inoratidzwa muMufananidzo 1c. Chimiro cheRaman peaks yegraphite G (1683 cm−1) uye 2D (2696 cm-1) inosimbisa kukura kwecrystalline yakanyanya NGF (Fig. 1c, Tafura SI1). Mumufirimu wese, huwandu hweRaman spectra ine intensity ratio (I2D / IG) ~ 0.3 yakaonekwa, nepo Raman spectra ine I2D / IG = 0.8 isingawanzo cherechedzwa. Kusavapo kwepamusoro pepamusoro (D = 1350 cm-1) mufirimu yose inoratidza hupamhi hwepamusoro hwekukura kweNGF. Migumisiro yakafanana yeRaman yakawanikwa paBS-NGF sampuli (Mufananidzo SI1 a uye b, Tafura SI1).
Kuenzanisa kweNiAG FS- uye BS-NGF: (a) Mufananidzo weiyo yakajairwa NGF (NiAG) sampuli inoratidza NGF kukura pawafer scale (55 cm2) uye inoguma BS- uye FS-Ni foil samples, (b) FS-NGF Mifananidzo/ Ni yakawanikwa nemaikorosikopu yemaziso, (c) yakajairika Raman spectra yakanyorwa panzvimbo dzakasiyana mupanera b, (d, f) SEM mifananidzo pahukuru hwakasiyana paFS-NGF/Ni, (e, g) SEM mifananidzo pahukuru hwakasiyana. Sets BS -NGF/Ni. Museve webhuruu unoratidza dunhu reFLG, museve weorenji unoratidza dunhu reMLG (padyo nenharaunda yeFLG), museve mutsvuku unoratidza dunhu reNGF, uye museve wemagenta unoratidza kupetwa.
Sezvo kukura kunoenderana nehupamhi hwekutanga substrate, saizi yekristaro, kutaridzika, uye miganhu yezviyo, kuwana zvine musoro kutonga kweNGF ukobvu munzvimbo dzakakura kunoramba kuri dambudziko20,34,44. Chidzidzo ichi chakashandisa zvinyorwa zvatakambotsikisa30. Iyi nzira inoburitsa dunhu rakajeka re0.1 kusvika 3% pa100 µm230. Muzvikamu zvinotevera, tinopa mibairo yemhando mbiri dzematunhu. High magnification SEM mifananidzo inoratidza kuvapo kwenzvimbo dzakasiyana-siyana dzakajeka kumativi ose (Fig. 1f, g), zvichiratidza kuvapo kweFLG neMLG nharaunda30,45. Izvi zvakasimbiswawo neRaman kuparadzira (Fig. 1c) uye TEM migumisiro (yakakurukurwa gare gare muchikamu "FS-NGF: chimiro uye zvinhu"). Matunhu eFLG neMLG akacherechedzwa paFS- uye BS-NGF/Ni masampuli (kumberi nekumashure NGF akakurira paNi) anogona kunge akakurira pahombe dzeNi(111) tsanga dzakaumbwa panguva yepre-annealing22,30,45. Kupeta kwakaonekwa kumativi ose (Fig. 1b, yakanyorwa nemiseve yepepuru). Aya mapeta anowanzo kuwanikwa muCVD-yakakura graphene uye graphite mafirimu nekuda kwekusiyana kukuru muhuwandu hwekuwedzera kwekupisa pakati pegraphite uye nickel substrate30,38.
Mufananidzo weAFM wakasimbisa kuti FS-NGF sampu yakanga yakanyatsonaka kupfuura BS-NGF sampuli (Mufananidzo SI1) (Mufananidzo SI2). Midzi inoreva square (RMS) roughness values ​​​​yeFS-NGF/Ni (Fig. SI2c) uye BS-NGF/Ni (Fig. SI2d) i82 uye 200 nm, zvichiteerana (yakayerwa pamusoro penzvimbo ye20 × 20 μm2). Iyo yakakwirira roughness inogona kunzwisiswa zvichienderana nekuongororwa kwepamusoro kwe nickel (NiAR) foil mumamiriro ekugamuchirwa (Mufananidzo SI3). SEM mifananidzo yeFS uye BS-NiAR inoratidzwa muFigures SI3a-d, ichiratidza akasiyana epamusoro morphologies: yakakwenenzverwa FS-Ni foil ine nano- uye micron-saizi spherical particles, nepo isina kupepereswa BS-Ni foil inoratidza manera ekugadzira. sezvimedu zvine simba guru. uye kuderera. Yakaderera uye yakakwira resolution mifananidzo ye annealed nickel foil (NiA) inoratidzwa muMufananidzo SI3e–h. Munhamba idzi, tinogona kuona kuvepo kwezvimedu zvenickel zvakati wandei pamativi ese enickel foil (Fig. SI3e–h). Mbeu hombe dzinogona kunge dziine Ni(111) yakatarisana, sezvakambotaurwa30,46. Pane misiyano yakakura mune nickel foil morphology pakati peFS-NiA neBS-NiA. Iyo yakakwirira roughness yeBS-NGF / Ni inokonzerwa nepamusoro-soro yeBS-NiAR, iyo yepamusoro inoramba ichinyanya kuoma kunyange mushure mekuvhara (Mufananidzo SI3). Iyi mhando yemaitiro epamusoro pamberi pekukura inobvumira kushata kwegraphene uye graphite mafirimu kuti adzorwe. Izvo zvinofanirwa kucherechedzwa kuti iyo yekutanga substrate yakagadziridzwa zviyo panguva yekukura kwegraphene, iyo yakadzikira zvishoma saizi yezviyo uye yakawedzera kushata kwepamusoro kweiyo substrate kana ichienzaniswa neyakavharwa foil uye catalyst film22.
Kunyatsogadzirisa iyo substrate pamusoro roughness, annealing nguva (saizi yezviyo)30,47 uye kuburitsa control43 kuchabatsira kudzikisa yedunhu NGF ukobvu kufanana kune µm2 uye/kana kunyange nm2 chiyero (kureva, ukobvu kusiyanisa kwemananomita mashoma). Kudzora kushata kwepamusoro kweiyo substrate, nzira dzakadai se electrolytic polishing yeinoguma nickel foil inogona kutariswa48. Iyo pretreated nickel foil inogona kubva yavharwa pane yakaderera tembiricha (<900 °C) 46 uye nguva (<5 min) kudzivirira kuumbwa kwehombe Ni(111) tsanga (iyo inobatsira FLG kukura).
SLG neFLG graphene haikwanisi kumira pamusoro pekudengenyeka kweasidhi nemvura, inoda mashizha ekutsigira emagetsi panguva yekunyorova kwemakemikari ekufambisa maitiro22,34,38. Mukupesana nekunyorova kwemakemikari ekufambisa kwepolymer-inotsigirwa single-layer graphene38, takaona kuti mativi ese eiyo-yakura NGF anogona kutamiswa pasina kutsigirwa kwepolymer, sezvakaratidzwa muFigure 2a (ona Mufananidzo SI4a kuti uwane rumwe ruzivo). Kutamiswa kweNGF kune yakapihwa substrate kunotanga nekunyorova etching yepasi pasi Ni30.49 firimu. Iwo akakura NGF/Ni/NGF samples akaiswa husiku humwe mu15 mL ye70% HNO3 yakadirwa ne600 mL ye deionized (DI) mvura. Mushure mokunge Ni foil yakanyungudutswa zvachose, FS-NGF inoramba yakadzikama uye inoyangarara pamusoro pemvura, sezvinongoita NGF / Ni / NGF sampuli, apo BS-NGF inonyudzwa mumvura (Fig. 2a, b). Iyo yakasarudzika NGF yakabva yatamiswa kubva kune imwe beaker yaive nemvura yakachena yakasvibiswa kuenda kune imwe beaker uye iyo yakasarudzika NGF yakashambidzwa zvakakwana, ichidzokorora kane kusvika katanhatu kuburikidza neconcave girazi ndiro. Pakupedzisira, FS-NGF uye BS-NGF yakaiswa pane yaidiwa substrate (Fig. 2c).
Polymer-isina wet chemical transfer process ye NGF inokura pa nickel foil: (a) process flow diagram (ona Mufananidzo SI4 kuti uwane rumwe ruzivo), (b) Digital foto yeakaparadzaniswa NGF mushure meNi etching (2 samples), (c) Muenzaniso FS - uye BS-NGF kuendeswa kuSiO2 / Si substrate, (d) FS-NGF kuendeswa kune opaque polymer substrate, (e) BS-NGF kubva kumuenzaniso wakafanana nepaneti d (yakakamurwa kuita zvikamu zviviri), inoendeswa kune goridhe rakaputirwa bepa reC. uye Nafion (flexible transparent substrate, mipendero yakanyorwa nemakona matsvuku).
Ziva kuti SLG kutapurirana kunoitwa uchishandisa nzira dzakanyorova dzekufambisa makemikari zvinoda nguva yakazara ye20-24 maawa 38. Iine iyo polymer-yemahara yekufambisa nzira inoratidzwa pano (Mufananidzo SI4a), iyo yakazara NGF yekuchinjisa nguva yekufambisa yakaderedzwa zvakanyanya (anenge maawa gumi nemashanu). Maitiro acho anosanganisira: (Chikamu 1) Gadzirira etching mhinduro uye isa sampuli mairi (~ maminitsi gumi), wozomirira husiku hwese kuti Ni etching (~ 7200 maminetsi), (Danho 2) Shamba nemvura yakasvibiswa (Nhanho - 3) . chengetedza mumvura yakasvibiswa kana kuendesa kune chinangwa substrate (20 min). Mvura yakavharirwa pakati pe NGF uye yakawanda matrix inobviswa ne capillary action (uchishandisa blotting paper) 38, ipapo madonhwe emvura akasara anobviswa nekuoma kwechisikigo (anenge 30 min), uye pakupedzisira sampu inoomeswa kwemaminitsi gumi. min muovheni yekutsvaira (10–1 mbar) pa50–90 °C (60 min) 38.
Graphite inozivikanwa nekumira kuvapo kwemvura nemhepo pakudziya kwakanyanya (≥ 200 °C)50,51,52. Takaedza sampuli tichishandisa Raman spectroscopy, SEM, uye XRD mushure mekuchengetedza mumvura yakasvibiswa patembiricha yekamuri uye mumabhodhoro akavharwa chero kupi zvako kubva pamazuva mashoma kusvika kune rimwe gore (Mufananidzo SI4). Hapana kuderedzwa kunoonekwa. Mufananidzo 2c inoratidza yakasununguka-yakamira FS-NGF uye BS-NGF mumvura yakasvibiswa. Takavatora paSiO2 (300 nm) / Si substrate, sezvakaratidzwa pakutanga kweMufananidzo 2c. Pamusoro pezvo, sezvakaratidzwa muMufananidzo 2d, e, NGF inoenderera inogona kuendeswa kune akasiyana ma substrates semapolymers (Thermabright polyamide kubva kuNexolve neNafion) uye negoridhe-yakavharwa kabhoni pepa. Iyo inoyangarara FS-NGF yakaiswa nyore pane yakanangwa substrate (Fig. 2c, d). Zvisinei, masampuli eBS-NGF akakura kudarika 3 cm2 akanga akaoma kubata paakanyudzwa zvachose mumvura. Kazhinji, pavanotanga kukunguruka mumvura, nekuda kwekubata kusina hanya dzimwe nguva vanoputsa muzvikamu zviviri kana zvitatu (Fig. 2e). Pakazara, isu takakwanisa kuwana polymer-yemahara kuchinjirwa kwePS- uye BS-NGF (inoenderera mberi seamless kufambisa pasina NGF/Ni/NGF kukura pa6 cm2) yemasampuli anosvika 6 uye 3 cm2 munzvimbo, zvichiteerana. Chero zvimedu zvakasara zvakakura kana zvidiki zvinogona (kuonekwa zviri nyore mune etching mhinduro kana deionized mvura) pane inodiwa substrate (~ 1 mm2, Figure SI4b, ona sampuli inotamisirwa kune mhangura grid se "FS-NGF: Mamiriro uye Zvivakwa (yakurukurwa) pasi pe “Structure and Properties”) kana chitoro chekushandisa mune ramangwana (Figure SI4). Zvichienderana nechiyero ichi, tinofungidzira kuti NGF inogona kudzoserwa mugoho rinosvika 98-99% (mushure mekukura kwekutamisa).
Kutamisa samples pasina polymer kwakaongororwa zvakadzama. Surface morphological maitiro akawanikwa paFS- uye BS-NGF / SiO2 / Si (Fig. 2c) achishandisa optical microscopy (OM) uye SEM mifananidzo (Fig. SI5 uye Fig. 3) yakaratidza kuti sampuli idzi dzakatamiswa pasina microscopy. Kukuvadzwa kwechimiro kunoonekwa sekutsemuka, maburi, kana nzvimbo dzakavhurwa. Kupeta pakukura kweNGF (Fig. 3b, d, yakaratidzirwa nemiseve yepepuru) yakaramba yakasimba mushure mekutamiswa. Ose ari maviri FS- uye BS-NGFs anoumbwa ne FLG matunhu (nzvimbo dzakapenya dzinoratidzwa nebhuruu miseve muFigure 3). Sezvineiwo, kusiyana neashoma matunhu akakuvadzwa anowanzo onekwa panguva yepolymer kutamiswa kwema ultrathin graphite mafirimu, akati wandei ma micron-saizi FLG neMLG matunhu anobatana neNGF (akamisikidzwa nemiseve yebhuruu muFigure 3d) akatamiswa pasina kutsemuka kana kuputsika (Mufananidzo 3d) . 3). . Mechanical kutendeseka kwakasimbiswa zvakare uchishandisa TEM neSEM mifananidzo yeNGF inotamisirwa palace-carbon copper grids, sezvakazokurukurwa gare gare ("FS-NGF: Mamiriro uye Zvivakwa"). Iyo yakatamiswa BS-NGF/SiO2/Si yakaoma kupfuura FS-NGF/SiO2/Si ine rms kukosha kwe140 nm uye 17 nm, zvichiteerana, sezvakaratidzwa muFigure SI6a uye b (20 × 20 μm2). Iyo RMS kukosha kweNGF inotamirwa kuSiO2 / Si substrate (RMS <2 nm) yakanyanya kuderera (inenge 3 nguva) kupfuura iyo yeNGF yakakura paNi (Figure SI2), zvichiratidza kuti iyo yakawedzera roughness inogona kuenderana neNi surface. Mukuwedzera, mifananidzo yeAFM yakaitwa pamicheto yeFS- uye BS-NGF / SiO2 / Si samples yakaratidza NGF yakakura ye100 uye 80 nm, maererano (Fig. SI7). Ukobvu hudiki hweBS-NGF hunogona kunge huri mhedzisiro yekusave kuratidzwa zvakananga kune precursor gasi.
Yakatamiswa NGF (NiAG) isina polymer paSiO2/Si wafer (ona Mufananidzo 2c): (a,b) SEM mifananidzo yekutamiswa FS-NGF: yakaderera uye yakakwirira magnification (inoenderana neorenji sikweya mupaneru). Nzvimbo dzakafanana) - a). (c, d) SEM mifananidzo yekutamiswa BS-NGF: yakaderera uye yakakwirira magnification (inoenderana neyakajairwa nzvimbo inoratidzwa neorenji sikweya mupaneru c). (e, f) AFM mifananidzo yekutamiswa FS- uye BS-NGFs. Museve webhuruu unomiririra FLG dunhu - kupenya kusiyanisa, cyan museve - dema MLG musiyano, museve mutsvuku - mutema musiyano unomiririra dunhu reNGF, museve wemagenta unomiririra kupeta.
Mushonga wemakemikari wekukura uye kuendeswa FS- uye BS-NGFs yakaongororwa ne X-ray photoelectron spectroscopy (XPS) (Fig. 4). Peak isina simba yakaonekwa mune yakayerwa spectra (Fig. 4a, b), inoenderana neNi substrate (850 eV) yeFS- uye BS-NGFs yakakura (NiAG). Iko hakuna mapeaks muyero yakayerwa yekutamiswa FS- uye BS-NGF / SiO2 / Si (Fig. 4c; zvakafanana mhedzisiro yeBS-NGF/SiO2/Si haina kuratidzwa), zvichiratidza kuti hapana yakasara Ni kusvibiswa mushure mekutamiswa. . Mifananidzo 4d-f inoratidza iyo yakakwirira-resolution spectra yeC 1 s, O 1 s uye Si 2p simba mazinga eFS-NGF/SiO2/Si. Simba rinosunga reC 1 s yegraphite i284.4 eV53.54. Iyo mutsara chimiro chepamusoro chegraphite chinowanzoonekwa seasymmetrical, sezvakaratidzwa mumufananidzo 4d54. Iyo yepamusoro-resolution core-level C 1 s spectrum (Fig. 4d) yakasimbisawo kuendeswa kwakachena (kureva, hapana masara epolymer), iyo inopindirana nezvidzidzo zvekare38. Iwo mutsara weiyo C 1 s spectra yeiyo ichangokura sampuli (NiAG) uye mushure mekutamiswa ndeye 0.55 uye 0.62 eV, zvichiteerana. Aya makosi akakwira kupfuura ayo eSLG (0.49 eV yeSLG pane SiO2 substrate)38. Nekudaro, izvi zvakakosha zvidiki pane zvakambotaurwa mutsara weiyo yakanyanya kutarisisa pyrolytic graphene samples (~ 0.75 eV) 53,54,55, zvichiratidza kusavapo kweakakanganisika kabhoni nzvimbo mune yazvino zvinhu. Iyo C 1 s uye O 1 s yepasi level spectra zvakare haina mapendekete, kubvisa kudiwa kwepamusoro-resolution peak deconvolution54. Pane π → π* satellite peak yakatenderedza 291.1 eV, iyo inowanzoonekwa muma graphite samples. I103 eV uye 532.5 eV zviratidzo muSi 2p uye O 1 s core level spectra (ona Fig. 4e, f) inonzi inonzi SiO2 56 substrate, maererano. XPS inzira inobata kumeso, saka masaini anoenderana neNi uye SiO2 akaonekwa pamberi uye mushure mekutamisa NGF, zvichiteerana, anofungidzirwa kuti anobva mudunhu reFLG. Migumisiro yakafanana yakacherechedzwa kune yakatamiswa BS-NGF samples (isina kuratidzwa).
NiAG XPS mhedzisiro: (ac) Ongororo inotaridzika yeakasiyana elemental atomic maumbirwo eakakura FS-NGF/Ni, BS-NGF/Ni uye akatamiswa FS-NGF/SiO2/Si, zvichiteerana. (d-f) High-resolution spectra yemazinga epakati C 1 s, O 1s uye Si 2p yeFS-NGF / SiO2 / Si muenzaniso.
Hunhu hwese hwemakristasi eNGF akatamiswa akaongororwa uchishandisa X-ray diffraction (XRD). Yakajairika XRD maitiro (Fig. SI8) yekutamiswa FS- uye BS-NGF / SiO2 / Si inoratidza kuvapo kwepamusoro peaks (0 0 0 2) uye (0 0 0 4) pa26.6 ° uye 54.7 °, yakafanana negraphite. . Izvi zvinosimbisa hupamhi hwekristani hwepamusoro hweNGF uye hunofananidzwa nechepakati chepakati che d = 0.335 nm, iyo inochengetwa mushure mekutamisa danho. Kusimba kweiyo diffraction peak (0 0 0 2) inenge 30 nguva iyo ye diffraction peak (0 0 0 4), zvichiratidza kuti NGF crystal ndege yakanyatsoenderana nemuenzaniso wepamusoro.
Zvinoenderana nemhedzisiro yeSEM, Raman spectroscopy, XPS uye XRD, mhando yeBS-NGF/Ni yakawanikwa yakafanana neyeFS-NGF/Ni, kunyangwe rms roughness yayo yaive yakakwira zvishoma (Figure SI2, SI5) uye SI7).
MaSLG ane polymer tsigiro akaturikidzana kusvika 200 nm gobvu anogona kuyangarara pamusoro pemvura. Iyi setup inowanzo shandiswa mupolymer-inobatsira wet makemikari ekufambisa maitiro22,38. Graphene uye graphite zviri hydrophobic (wet angle 80–90°) 57. Iyo inogona kuita simba pamusoro pegraphene neFLG yakanzi yakati sandarara, iine simba rakaderera (~ 1 kJ/mol) rekufamba kwemvura kumberi kwepamusoro58. Zvisinei, kuverengera kupindirana kwemasimba emvura ane graphene uye mitsara mitatu yegraphene inenge - 13 uye - 15 kJ / mol, 58 maererano, zvichiratidza kuti kuwirirana kwemvura ne NGF (inenge 300 layers) yakaderera kana ichienzaniswa negraphene. Ichi chinogona kunge chiri chimwe chezvikonzero nei yakasununguka NGF ichiramba yakati sandara pamusoro pemvura, nepo yakasununguka graphene (iyo inoyangarara mumvura) inokwidibira kumusoro nekuputsika. Kana NGF ichinyudzwa zvachose mumvura (mibairo yakafanana kune rough uye flat NGF), mipendero yayo inobhenda (Mufananidzo SI4). Panyaya yekunyudzwa kwakakwana, zvinotarisirwa kuti NGF-mvura yekudyidzana simba inenge yakapetwa kaviri (ichienzaniswa neinoyangarara NGF) uye kuti mipendero ye NGF peta kuchengetedza yakakwirira yekuona angle (hydrophobicity). Isu tinotenda kuti marongero anogona kugadzirwa kuti adzivise kupeta kwemipendero yeakamisikidzwa NGFs. Imwe nzira ndeye kushandisa zvakasanganiswa zvinonyungudutsa kugadzirisa kunyorova kwefirimu regraphite59.
Kuendeswa kweSLG kune akasiyana marudzi e substrates kuburikidza nemvura yakanyorovesa makemikari ekufambisa maitiro kwakambotaurwa. Zvinowanzogamuchirwa kuti mauto asina simba evan der Waals aripo pakati pegraphene/graphite mafirimu uye substrates (ngave yakasimba substrates seSiO2/Si38,41,46,60, SiC38, Au42, Si pillars22 uye lacy carbon films30, 34 kana flexible substrates. zvakadai se polyimide 37). Pano tinofungidzira kuti kudyidzana kwemhando imwe chete ndiko kunotonga. Hatina kucherechedza chero kukuvadzwa kana kupenengura kweNGF kune chero ipi zvayo substrates inoratidzwa pano panguva yekubata kwemuchina (panguva yekuratidzwa pasi pevacuum uye / kana mamiriro emuchadenga kana panguva yekuchengetedza) (semuenzaniso, Mufananidzo 2, SI7 uye SI9). Mukuwedzera, isu hatina kutarisa peak yeSiC mu XPS C 1 s spectrum yezinga repakati re NGF / SiO2 / Si sampuli (Fig. 4). Izvi zvinoratidza kuti hapana chisungo chemakemikari pakati pe NGF uye chinangwa che substrate.
Muchikamu chakapfuura, "Polymer-free transfer of FS- neBS-NGF," takaratidza kuti NGF inogona kukura uye kuendesa kumativi ose e nickel foil. Aya maFS-NGF neBS-NGF haana kufanana maererano nekushata kwepamusoro, izvo zvakaita kuti tiongorore maapplication akakodzera emhando yega yega.
Tichifunga nezvekujeka uye kutsetseka kwepamusoro kweFS-NGF, takadzidza chimiro chayo chenzvimbo, maziso uye magetsi emagetsi mune zvakadzama. Chimiro uye chimiro cheFS-NGF pasina polymer transfer yaionekwa nekutapurirana electron microscopy (TEM) imaging uye yakasarudzwa nzvimbo electron diffraction (SAED) pattern analysis. Migumisiro inoenderana inoratidzwa mumufananidzo 5. Low magnification planar TEM imaging yakaratidza kuvapo kweNGF neFLG nzvimbo dzine maitiro akasiyana-siyana erekitironi, kureva nzvimbo dzakasvibirira uye dzakajeka, zvichienderana (Fig. 5a). Iyo firimu yakazara inoratidza yakanaka mechani kutendeseka uye kugadzikana pakati penzvimbo dzakasiyana dzeNGF neFLG, ine yakanaka kupindirana uye isina kukuvadzwa kana kubvarura, iyo yakasimbiswa zvakare neSEM (Mufananidzo 3) uye yakakwirira magnification TEM zvidzidzo (Mufananidzo 5c-e). Kunyanya, muFig. Figure 5d inoratidza chimiro chebhiriji pachikamu chayo chikuru (chinzvimbo chakaratidzwa nemuseve une mavara madema muMufananidzo 5d), iyo inoratidzirwa nechimiro chetatu uye ine graphene layer nehupamhi hunenge 51. Iyo yakagadzirwa ine interplanar spacing ye 0.33 ± 0.01 nm inowedzerwazve kune akati wandei akaturikidzana egraphene munzvimbo yakamanikana (magumo emuseve wakasimba mutema muMufananidzo 5 d).
Planar TEM mufananidzo wepolymer-isina NiAG sampuli pane kabhoni lacy copper grid: (a, b) Yakaderera magnification TEM mifananidzo inosanganisira NGF neFLG matunhu, (ce) Yakakwirira magnification mifananidzo yematunhu akasiyana-siyana mupaneru-a uye mapaneru-b ari miseve ine mavara ane mavara akafanana. Miseve yakasvibira mumapanera a uye c inoratidza nzvimbo dzakatenderedzwa dzekukuvara panguva yekumisikidzwa kwedanda. (f-i) Mune mapaneru kusvika ku c, SAED mapatani munzvimbo dzakasiyana anoratidzwa nebhuruu, cyan, orenji, uye dzvuku madenderedzwa zvichiteerana.
Chimiro cheribhoni muMufananidzo 5c chinoratidza (chakaiswa museve mutsvuku) kutarisisa kwakatwasuka kwendege dzemagraphite lattice, izvo zvingave zvichikonzerwa nekuumbwa kwenanofolds pamwe chete nefirimu (inoiswa muFigure 5c) nekuda kwekunyanya kusingabhadharwe kushushikana kweshear30,61,62 . Pasi pepamusoro-resolution TEM, aya nanofolds 30 anoratidza yakasiyana crystallographic orientation pane imwe nzvimbo yeNGF; ndege dzepasi dzegirafu regirafu dzakatariswa dzinenge dzakadzika, pane kuti dzakatwasuka senge imwe firimu (inoiswa muFigure 5c). Saizvozvo, iyo FLG dunhu rinomboratidza mutsara uye nhete mabhendi-akange akapeta (akamisikidzwa nemiseve yebhuruu), ayo anoonekwa pakudzika uye nepakati kukura muFigure 5b, 5e, zvichiteerana. Iyo inset muFigure 5e inosimbisa kuvepo kwemaviri- uye matatu-layer graphene layers muFLG sector (interplanar kureba 0.33 ± 0.01 nm), iri muchibvumirano chakanaka nemhedzisiro yedu yapfuura30. Pamusoro pezvo, akarekodhwa SEM mifananidzo yepolymer-isina NGF inotamirwa pamhangura grid ane lacy kabhoni mafirimu (mushure mekuita epamusoro-kutarisa TEM zviyero) inoratidzwa muMufananidzo SI9. Iyo yakamiswa zvakanaka FLG dunhu (yakanyorwa nemuseve webhuruu) uye dunhu rakaputsika muMufananidzo SI9f. Museve webhuruu (pamucheto wekuchinjirwa NGF) unounzwa nemaune kuratidza kuti dunhu reFLG rinogona kuramba maitiro ekutamisa pasina polymer. Muchidimbu, mifananidzo iyi inosimbisa kuti yakamiswa zvishoma NGF (kusanganisira iyo FLG dunhu) inochengetedza hunhu hwemagetsi kunyangwe mushure mekubata kwakasimba uye kuratidzwa kune yakakwira vacuum panguva yeTEM uye SEM zviyero (Mufananidzo SI9).
Nekuda kwekunaka kwakadzikama kweNGF (ona Mufananidzo 5a), hazvina kuoma kutungamira maflakes pamwe ne [0001] domain axis kuti uongorore iyo SAED chimiro. Zvichienderana nehupamhi hwepanzvimbo yefirimu uye nzvimbo yaro, nzvimbo dzakawanda dzekufarira (12 points) dzakaonekwa nokuda kwezvidzidzo zve electron diffraction. MuMifananidzo 5a–c, ina dzematunhu akajairwa aya anoratidzwa uye akaiswa mavara madenderedzwa (bhuruu, cyan, orenji, uye tsvuku). Mifananidzo 2 uye 3 yeSAED mode. Mifananidzo 5f uye g yakawanikwa kubva munharaunda yeFLG inoratidzwa muMifananidzo 5 uye 5. Sezvinoratidzwa muMifananidzo 5b uye c, maererano. Vane hexagonal chimiro chakafanana neyakamonyoroka graphene63. Kunyanya, Mufananidzo 5f unoratidza maitiro matatu akaiswa kumusoro ane kutaridzika kwakafanana kwe [0001] zone axis, inotenderedzwa ne10 ° uye 20 °, sezvinoratidzwa neangular mismatch yezviviri zvitatu zve (10-10) zvinoratidzira. Saizvozvowo, Mufananidzo 5g unoratidza maviri makuru akaiswa hexagonal mapatani akatenderedzwa ne20°. Mapoka maviri kana matatu emapateni ane hexagonal mudunhu reFLG anogona kusimuka kubva kune matatu ari-mundege kana kunze-ye-ndege graphene layers 33 yakatenderedzwa yakabatana kune imwe neimwe. Kusiyana neizvi, maerekitironi diffraction mapatani muMufananidzo 5h, i (inoenderana nenharaunda yeNGF inoratidzwa muMufananidzo 5a) inoratidza imwe [0001] pateni ine huwandu hwepamusoro hwekusiyanisa simba, hunoenderana nehukuru hwezvinhu. Iyi mienzaniso yeSAED inoenderana neyakakura girafu chimiro uye kutarisisa kwepakati pane FLG, sezvakatsanangurwa kubva kune index 64. Hunhu hwekristaro zvinhu zveNGF zvakaratidza kugarisana kwemaviri kana matatu superimposed graphite (kana graphene) crystallites. Chinonyanya kukosha munharaunda yeFLG ndechekuti makristallite ane imwe dhigirii ye-mu-ndege kana kunze-kwe-ndege misorientation. Graphite particles/ layers ane in-plane rotation angles of 17°, 22° and 25° akambotaurwa kuNGF akakurira pamafirimu eNi 64. Kutenderera kwekona ukoshi hwakacherechedzwa muchidzidzo ichi hunoenderana nemakona ekutenderera kwakambocherechedzwa (±1°) yeakamonyoroka BLG63 graphene.
Iwo magetsi emagetsi eNGF/SiO2/Si akayerwa pa300 K pamusoro penzvimbo ye10×3 mm2. Iko kukosha kweiyo electron carrier concentration, kufamba uye conductivity ndeye 1.6 × 1020 cm-3, 220 cm2 V-1 C-1 uye 2000 S-cm-1, zvichiteerana. Mafambiro uye maitiro ekufambisa kweNGF yedu akafanana neyechisikigo graphite2 uye yakakwirira pane inotengeswa inowanikwa yakanyanya kutariswa pyrolytic graphite (yakagadzirwa pa3000 ° C) 29. Iwo akacherechedzwa erekitironi mutakuri wehuwandu hwemaodha maviri ehukuru akakwira kupfuura ayo achangobva kushumwa (7.25 × 10 cm-3) yemicron-yakakora graphite mafirimu akagadzirirwa nepamusoro-tembiricha (3200 ° C) polyimide mapepa 20 .
Isu takaitawo UV-inooneka transmittance zviyero paFS-NGF yakaendeswa kune quartz substrates (Mufananidzo 6). Mhedzisiro inobuda inoratidza kutenderera kunoramba kuripo kwe62% muhuwandu hwe350-800 nm, zvichiratidza kuti NGF inopenya kuchiedza chinooneka. Muchokwadi, zita rekuti "KAUST" rinogona kuonekwa mumufananidzo wedhijitari wemuenzaniso muMufananidzo 6b. Kunyange zvazvo nanocrystalline chimiro che NGF chakasiyana neiyo SLG, nhamba yezvikamu zvinogona kuenzaniswa nekushandisa mutemo we 2.3% kurasikirwa kwekutapurirana pane imwe nhanho65. Maererano nehukama uhwu, nhamba yegraphene layers ine 38% kutapukirwa kurasikirwa ndeye 21. Iyo yakakura NGF inonyanya kuumbwa ne300 graphene layers, kureva anenge 100 nm gobvu (Fig. 1, SI5 uye SI7). Naizvozvo, isu tinofungidzira kuti yakacherechedzwa optical transparency inoenderana FLG neMLG matunhu, sezvo ari kugoverwa mufirimu rose (Fig. 1, 3, 5 uye 6c). Pamusoro peiyo iri pamusoro pezvimiro data, conductivity uye pachena zvakare inosimbisa yakakwira crystalline mhando yeakatamiswa NGF.
(a) UV-inooneka transmittance kuyerwa, (b) yakajairika NGF kutamiswa pane quartz uchishandisa mumiriri sampuli. (c) Schematic yeNGF (bhokisi rakasviba) rine matunhu akagoverwa akaenzana eFLG neMLG akamisikidzwa segrey zvimiro zvisina kurongeka mumuenzaniso wese (ona Mufananidzo 1) (inenge 0.1-3% nzvimbo pa100 μm2). Iwo maumbirwo asina kurongeka uye saizi yawo mudhayagiramu ndeyekuenzanisira chete uye haienderane nenzvimbo chaidzo.
Translucent NGF inokura neCVD yakamboendeswa kunzvimbo isina silicon uye yakashandiswa mumasero ezuva15,16. Izvo zvinoguma simba rekushandura simba (PCE) ndeye 1.5%. Aya ma NGF anoita mabasa akawanda akadai seanoshanda makomisheni akaturikidzana, nzira dzekufambisa dzekuchaja, uye maelectrodes akajeka15,16. Zvisinei, firimu regirafu harina kufanana. Kuwedzera optimization kunodiwa nekunyatso kudzora kupikisa pepa uye optical transmittance yegraphite electrode, sezvo zvinhu zviviri izvi zvinoita basa rakakosha pakuona kukosha kwePCE ye solar cell15,16. Kazhinji, mafirimu egraphene ane 97.7% akajeka kune chiedza chinooneka, asi ane mashizha ekupikisa 200-3000 ohms / sq.16. Kuramba kwepamusoro kwemafirimu egraphene kunogona kuderedzwa nekuwedzera nhamba yezvikamu (zvakawanda kuendeswa kwegraphene layers) uye doping neHNO3 (~ 30 Ohm/sq.)66. Nekudaro, maitiro aya anotora nguva yakareba uye akasiyana ekutamisa akaturikidzana haagare achichengeta yakanaka kuonana. Rutivi rwedu rwemberi NGF ine zvivakwa zvakaita se conductivity 2000 S/cm, bhaisikopo pepa rekudzivirira 50 ohm/sq. uye 62% pachena, zvichiita kuti ive imwe nzira inoshandiswa kune conductive channels kana counter electrodes mumasero ezuva15,16.
Kunyange zvazvo chimiro nemakemikari epamusoro eBS-NGF akafanana neFS-NGF, kushata kwayo kwakasiyana ("Kukura kweFS- uye BS-NGF"). Pakutanga, takashandisa Ultra-yakaonda firimu graphite22 segasi sensor. Naizvozvo, takaedza kugona kwekushandisa BS-NGF yemabasa ekunzwa gasi (Mufananidzo SI10). Kutanga, mm2-yakakura zvikamu zveBS-NGF zvakaendeswa kune interdigitating electrode sensor chip (Mufananidzo SI10a-c). Zvinyorwa zvekugadzira zve chip zvakambotaurwa; nzvimbo yayo inoshanda inonzwisisika i9 mm267. Mumifananidzo yeSEM ​​(Mufananidzo SI10b uye c), iyo electrode yegoridhe iri pasi inoonekwa zvakajeka kuburikidza neNGF. Zvekare, zvinogona kuoneka kuti yunifomu chip coverage yakawanikwa kune ese masampuli. Gasi sensor zviyero zvemagasi akasiyana-siyana akanyorwa (Fig. SI10d) (Fig. SI11) uye mhedzisiro yekupindura mhinduro inoratidzwa muFig. SI10g. Pamwe nemamwe magasi anopindira anosanganisira SO2 (200 ppm), H2 (2%), CH4 (200 ppm), CO2 (2%), H2S (200 ppm) uye NH3 (200 ppm). Chimwe chikonzero chinogona kunge chiri NO2. electrophilic chimiro chegasi22,68. Kana yakashambadzirwa pamusoro pegraphene, inoderedza kutorwa kwemaerekitironi ikozvino nehurongwa. Kuenzanisa kweiyo nguva yekupindura data yeBS-NGF sensor ine yakambodhindwa ma sensors inoratidzwa muTafura SI2. Iyo nzira yekugadzirisa zvakare NGF sensors uchishandisa UV plasma, O3 plasma kana thermal (50-150 ° C) kurapwa kwemasamples akafumurwa ari kuenderera mberi, zvinoteedzerwa nekuitwa kweakamisikidzwa masisitimu69.
Munguva yeCVD maitiro, kukura kwegraphene kunoitika pamativi ese eiyo catalyst substrate41. Nekudaro, BS-graphene inowanzoburitswa panguva yekufambisa maitiro41. Muchidzidzo ichi, tinoratidza kuti kukura kwepamusoro kweNGF uye kufambisa kwepolymer-isina NGF kunogona kuwanikwa pamativi ese erutsigiro rwecatalyst. BS-NGF yakaonda (~ 80 nm) kupfuura FS-NGF (~ 100 nm), uye kusiyana uku kunotsanangurwa nechokwadi chokuti BS-Ni haisi kuratidzwa zvakananga kune inotangira gasi inoyerera. Isu takaona zvakare kuti kushata kweNiAR substrate kunokanganisa kushata kweNGF. Izvi zvinoratidza kuti yakakura planar FS-NGF inogona kushandiswa sechinhu chinotangira chegraphene (ne exfoliation method70) kana senzira inofambisa mumasero ezuva15,16. Kusiyana neizvi, BS-NGF ichashandiswa pakuona gasi (Fig. SI9) uye zvichida kune simba rekuchengetedza magetsi71,72 apo kuoma kwayo kwepamusoro kuchave kunobatsira.
Tichifunga nezvezviri pamusoro, zvinobatsira kubatanidza basa razvino nemafirimu egraphite akadhindwa akakura neCVD uye kushandisa nickel foil. Sezvinoonekwa muTable 2, madzvinyiriro akakwirira atakashandisa akapfupisa nguva yekuita (danho rekukura) kunyangwe pakudziya kwakadzikira (muchikamu che850-1300 ° C). Takawanawo kukura kwakakura kudarika nguva dzose, zvichiratidza mukana wekuwedzera. Pane zvimwe zvinhu zvinofanirwa kutariswa, zvimwe zvacho zvatakaisa mutafura.
Kaviri-mativi emhando yepamusoro NGF yakarimwa panickel foil necatalytic CVD. Nekubvisa echinyakare mapolymer substrates (seaya anoshandiswa muCVD graphene), tinowana yakachena uye isina hurema-isina kunyorova kutamiswa kweNGF (yakakura kumashure uye kumberi mativi enickel foil) kune akasiyana maitiro-akakosha substrates. Zvinonyanya kukosha, NGF inosanganisira FLG neMLG matunhu (kazhinji 0.1% kusvika 3% pa100 µm2) ayo akanyatsobatanidzwa mufirimu gobvu. Planar TEM inoratidza kuti matunhu aya anoumbwa nematakwe maviri kusvika matatu matatu egraphite/graphene particles (makristasi kana akaturikidzana, zvichiteerana), mamwe ayo ane kutenderera kusawirirana kwe10-20 °. Matunhu eFLG neMLG ane basa rekubuda pachena kweFS-NGF kuchiedza chinooneka. Kana ari mapepa emashure, anogona kutakurwa akaenzana nemashizha epamberi uye, sezvakaratidzwa, anogona kuva nechinangwa chekushanda (somuenzaniso, nokuda kwekuona gasi). Zvidzidzo izvi zvinobatsira kwazvo kudzikisa marara uye mitengo mumaindasitiri eCVD maitiro.
Kazhinji, avhareji ukobvu hweCVD NGF iri pakati pe (yakaderera- uye yakawanda-layer) graphene uye maindasitiri (micrometer) graphite mapepa. Huwandu hwezvivakwa zvavo zvinonakidza, zvakasanganiswa nenzira yakapusa yatakagadzira yekugadzira uye kutakura kwavo, inoita kuti mafirimu aya anyanyokodzera zvikumbiro zvinoda mhinduro inoshanda yegraphite, pasina kubhadhariswa kwesimba rinonyanya simba rekugadzira maindasitiri maitiro anoshandiswa parizvino.
Iyo 25-μm-yakakora nickel foil (99.5% kuchena, Goodfellow) yakaiswa mune yekutengesa CVD reactor (Aixtron 4-inch BMPro). Iyo sisitimu yakacheneswa ne argon uye yakasimudzwa kune yakadzika yekumanikidza ye10-3 mbar. Zvadaro nickel foil yakaiswa. muAr / H2 (Mushure mekutanga-annealing yeNi foil ye 5 min, iyo foil yakaratidzwa kumanikidziro e500 mbar pa900 ° C. NGF yakaiswa mukuyerera kweCH4 / H2 (100 cm3 imwe neimwe) ye5 min. Muenzaniso wacho wakabva watonhodzwa kusvika kune tembiricha pazasi 700 ° C uchishandisa Ar flow (4000 cm3) pa40 ° C/min Tsanangudzo pamusoro pekugadzirisa kweiyo NGF kukura inotsanangurwa kumwe kunhu30.
Iyo yepamusoro morphology yemuenzaniso yakaonekwa neSEM vachishandisa Zeiss Merlin microscope (1 kV, 50 pA). Sample pamusoro roughness uye NGF ukobvu akayerwa uchishandisa AFM (Dimension Icon SPM, Bruker). Zviyero zveTEM neSAED zvakaitwa pachishandiswa FEI Titan 80–300 Cubed maikorosikopu yakashongedzerwa nepfuti inopenya yakakwira (300 kV), FEI Wien mhando monochromator uye CEOS lens spherical aberration corrector kuti vawane mhinduro dzekupedzisira. kugadziriswa kwenzvimbo 0.09 nm. NGF samples dzakaendeswa kune kabhoni lacy yakavharwa mhangura grids yeflat TEM imaging uye SAED chimiro chekuongorora. Nokudaro, mazhinji emuenzaniso flocs anomiswa mu pores ye membrane inotsigira. Yakatamiswa NGF samples yakaongororwa neXRD. X-ray diffraction mapatani akawanikwa pachishandiswa poda diffractometer (Brucker, D2 phase shifter neCu Kα source, 1.5418 Å uye LYNXEYE detector) vachishandisa Cu radiation source ine danda dhayamita ye3 mm.
Zviyero zvakati wandei zveRaman point zvakarekodhwa vachishandisa inosanganisa confocal microscope (Alpha 300 RA, WITeC). A 532 nm laser ine yakaderera excitation simba (25%) yakashandiswa kudzivirira thermally induced mhedzisiro. X-ray photoelectron spectroscopy (XPS) yakaitwa paKratos Axis Ultra spectrometer pamusoro peimwe nzvimbo ye300 × 700 μm2 uchishandisa monochromatic Al Kα mwaranzi (hν = 1486.6 eV) pasimba re150 W. Resolution spectra yakawanikwa pa. kutapurirana masimba e160 eV uye 20 eV, zvichiteerana. NGF samples dzakatamirwa paSiO2 dzakachekwa kuita zvidimbu (3 × 10 mm2 imwe neimwe) vachishandisa PLS6MW (1.06 μm) ytterbium fiber laser pa 30 W. Copper wire contacts (50 μm gobvu) akagadzirwa achishandisa sirivheri paste pasi pe optical microscope. Kutakurwa kwemagetsi uye Horo maitiro ekuedza akaitwa paaya masampuli pa300 K uye magineti mutsauko we ± 9 Tesla mune yemuviri zvimiro zvekuyera system (PPMS EverCool-II, Quantum Dhizaini, USA). Yakatapurirwa UV-vis spectra yakarekodhwa ichishandisa Lambda 950 UV-vis spectrophotometer mu350-800 nm NGF renji yakaendeswa kune quartz substrates uye quartz referensi samples.
Iyo kemikari inopikisa sensor (interdigitated electrode chip) yakasungirirwa kune tsika yakadhindwa redunhu bhodhi 73 uye kushorwa kwacho kwakatorwa kwenguva pfupi. Iyo yakadhindwa yedunhu bhodhi iyo iyo mudziyo uripo inobatanidzwa kune yekusangana matinji uye yakaiswa mukati meiyo gasi inonzwa chamber 74. Kupikiswa kuyerwa kwakatorwa pamhepo ye1 V nekuenderera mberi scan kubva pakucheneswa kusvika kune gasi kuratidzwa uyezve kuchenesa zvakare. Imba yacho yakatanga kucheneswa nekuchenesa ne nitrogen pa 200 cm3 kweawa imwe kuti ive nechokwadi chekubviswa kwevamwe vaongorori varipo mukamuri, kusanganisira unyoro. Vaongorori vega vega vakabva vasunungurwa zvishoma nezvishoma mukamuri panguva imwechete yekuyerera kwe200 cm3 nekuvhara N2 cylinder.
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