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kọrọ na electrochemical stratification nke boron na-adịghị eduzi n'ime mkpa-layer boron.A na-enweta mmetụta a pụrụ iche site n'itinye nnukwu boron n'ime nchara ígwè nke na-eme ka ọkụ eletrik na-emepe ohere maka ịmepụta boron na atụmatụ a dị irè.Nnwale a na-eme na electrolytes dị iche iche na-enye ngwá ọrụ dị ike maka ịnweta flakes borene nke akụkụ dị iche iche na ọkpụrụkpụ nke ~ 3-6 nm.A na-ekpughekwa usoro nke ikpochapụ boron nke electrochemical.Ya mere, usoro a na-atụ aro nwere ike ịbụ ngwá ọrụ ọhụrụ maka mmepụta nnukwu ihe nke ọkpụkpụ dị nro ma mee ka mmepe nke nyocha nke metụtara burs na ngwa ha nwere ike ime ngwa ngwa.
Ihe akụkụ abụọ (2D) enwetala mmasị dị ukwuu n'afọ ndị na-adịbeghị anya n'ihi njirimara ha pụrụ iche dị ka ọkụ eletrik ma ọ bụ ebe a ma ama na-arụ ọrụ.Mmepe nke ihe graphene adọtara uche gaa na ihe 2D ndị ọzọ, yabụ a na-enyocha ihe ọhụrụ 2D nke ukwuu.Na mgbakwunye na graphene a ma ama, mgbanwe metal dichalcogenides (TMD) dị ka WS21, MoS22, MoSe3, na WSe4 ka amụkwara nke ọma n'oge na-adịbeghị anya.N'agbanyeghị ihe ndị ahụ e kwuru n'elu, hexagonal boron nitride (hBN), phosphorus ojii na nke a rụpụtara nke ọma boronene na nso nso a.N'ime ha, boron dọtara mmasị dị ukwuu dị ka otu n'ime usoro akụkụ abụọ kacha nta.A na-ekpuchi ya dị ka graphene mana ọ na-egosipụta ihe ndị na-adọrọ mmasị n'ihi anisotropy, polymorphism na nhazi kristal.Nnukwu boron na-egosi dị ka ihe mgbanaka ụlọ na B12 icosahedron, mana ụdị kristal boron dị iche iche na-etolite site na ụzọ dị iche iche ijikọ na njikọ dị na B12.N'ihi ya, ihe mgbochi boron anaghị adịkarị ka graphene ma ọ bụ graphite, nke na-eme ka usoro ịnweta boron sie ike.Na mgbakwunye, ọtụtụ ụdị nke borophene polymorphic (dịka ọmụmaatụ, α, β, α1, pmmm) na-eme ka ọ dịkwuo mgbagwoju anya5.Usoro dị iche iche a na-enweta n'oge njikọ ahụ na-emetụta kpọmkwem ihe onwunwe nke harrows.Ya mere, mmepe nke ụzọ sịntetik nke na-eme ka o kwe omume ịnweta borocenes nke na-eme ka ọ bụrụ nke nwere nnukwu akụkụ akụkụ na obere ọkpụkpụ nke flakes chọrọ ugbu a ọmụmụ miri emi.
Ọtụtụ ụzọ maka synthesizing 2D ihe na-dabere na sonochemical Filiks nke nnukwu ihe na-etinye na ihe mgbaze, na-emekarị ihe organic mgbaze, na sonicated ruo ọtụtụ awa.Ranjan et al.6 kpochapuru nnukwu boron n'ime borophene nke ọma site na iji usoro akọwara n'elu.Ha na-amụ ihe dị iche iche nke organic solvents (methanol, ethanol, isopropanol, acetone, DMF, DMSO) na-egosi na sonication exfoliation bụ ụzọ dị mfe iji nweta nnukwu na mkpa boron flakes.Na mgbakwunye, ha gosipụtara na usoro Hummers gbanwetụrụ nwekwara ike iji wepụ boron.Ndị ọzọ egosipụtala ntọhapụ mmiri mmiri: Lin et al.7 na-eji boron crystalline dị ka isi iyi iji mepụta mpempe akwụkwọ β12 dị ala ma jiri ya mee ihe na batrị lithium-sulfur dabeere na borene, na Li et al.8 gosipụtara mpempe akwụkwọ boronene dị ala..Enwere ike nweta ya site na njikọ sonochemical ma jiri ya mee ihe dị ka electrode supercapacitor.Otú ọ dị, ntinye ihe nrịbama atomic Layer (ALD) bụkwa otu n'ime ụzọ njikọ nke ala dị elu maka boron.Mannix et al.9 echekwabara boron atọm na nkwado ọlaọcha dị ọcha nke atọm.Ụzọ a na-eme ka o kwe omume ịnweta akwụkwọ nke boronene ultra-dị ọcha, agbanyeghị mmepụta nke boronene nke ụlọ nyocha nwere oke oke n'ihi ọnọdụ usoro siri ike (oke oghere).Ya mere, ọ dị oke mkpa ịmepụta atụmatụ ọhụrụ dị mma maka ịmepụta boronene, kọwaa usoro uto / stratification, wee mee nyocha nyocha ziri ezi nke ihe onwunwe ya, dị ka polymorphism, nnyefe ọkụ na ọkụ ọkụ.H. Liu et al.10 tụlere ma kọwakwa usoro nke uto boron na mkpụrụ nke Cu(111).Ọ tụgharịrị na atom boron na-etolite nnukwu ụyọkọ 2D dabere na nkeji triangular, na ike nrụpụta na-ebelata site na nha ụyọkọ na-abawanye, na-atụ aro na ụyọkọ boron 2D na mkpụrụ ọla kọpa nwere ike itolite ruo mgbe ebighị ebi.Ntụle zuru ezu nke akwụkwọ boron akụkụ abụọ nke D. Li et al gosipụtara.11, ebe akọwara mkpụrụ okwu dị iche iche na-atụle ngwa nwere ike.E gosiputara nke ọma na enwere ụfọdụ ndakọrịta n'etiti ngụkọ usoro ọmụmụ na nsonaazụ nnwale.Ya mere, a na-achọ ịgbakọ usoro ọmụmụ iji ghọta nke ọma njirimara na usoro nke uto boron.Otu ụzọ isi nweta ebumnobi a bụ iji teepu ntanye dị mfe wepụ boron, mana nke a ka dị ntakịrị iji nyochaa ihe ndị bụ isi ma gbanwee ngwa ya bara uru12.
Ụzọ na-ekwe nkwa nke engineering peeling nke 2D ihe site na nnukwu ihe bụ electrochemical peeling.N'ebe a, otu n'ime electrodes nwere nnukwu ihe.N'ozuzu, ogige ndị a na-ekpochapụkarị site na usoro electrochemical na-arụ ọrụ nke ukwuu.Ha dị ka osisi ma ọ bụ mbadamba abịakọrọ.Enwere ike ịpụpụ graphite nke ọma n'ụzọ dị otú a n'ihi nnukwu ọkụ eletrik ya.Achi na ndị otu ya14 ewepụla graphite nke ọma site n'ịgbanwe mkpara graphite ka ọ bụrụ graphite etinyere n'ihu akpụkpọ ahụ eji egbochi ire ere nke nnukwu ihe.A na-ekpochapụ laminates ndị ọzọ buru ibu nke ọma n'otu ụzọ ahụ, dịka ọmụmaatụ, iji Janus15 electrochemical delamination.N'otu aka ahụ, phosphorus ojii oyi akwa bụ electrochemically stratified, na acidic electrolyte ion na-agbasa n'ime oghere n'etiti n'ígwé n'ihi voltaji etinyere.N'ụzọ dị mwute, a pụghị itinye otu usoro ahụ naanị na stratification nke boron n'ime borophene n'ihi obere ọkụ eletrik nke nnukwu ihe onwunwe.Ma gịnị na-eme ma ọ bụrụ na a na-etinye ntụ ntụ boron rụrụ arụ na nchara ígwè (nickel-nickel ma ọ bụ ọla kọpa-ọla kọpa) iji mee ihe dị ka electrode?Ọ ga-ekwe omume ịkpali conductivity nke boron, nke nwere ike ekewa n'ihu electrochemically dị ka a layered usoro nke eletriki nduzi?Kedu ihe bụ akụkụ nke boronene obere oyi akwa mepere emepe?
N'ime ọmụmụ ihe a, anyị na-aza ajụjụ ndị a wee gosi na atụmatụ a dị mfe na-enye ụzọ ọhụrụ n'izugbe maka ịmepụta ihe dị mkpa, dị ka egosiri na foto 1.
Lithium chloride (LiCl, 99.0%, CAS: 7447-41-8) na boron ntụ ntụ (B, CAS: 7440-42-8) zụtara na Sigma Aldrich (USA).Sodium sulfate (Na2SO4, ≥ 99.0%, CAS: 7757-82-6) sitere na Chempur (Poland).A na-eji Dimethyl sulfoxide (DMSO, CAS: 67-68-5) sitere na Karpinex (Poland).
Atomic Force microscopy (AFM MultiMode 8 (Bruker)) na-enye ozi gbasara ọkpụrụkpụ na lattice size nke layered ihe.Mkpebi dị elu nnyefe eletrọn microscope (HR-TEM) rụrụ site na iji FEI Tecnai F20 mikroskopu na accelerating voltaji nke 200 kV.A na-eme nyocha nyocha nke absorption spectroscopy (AAS) site na iji Hitachi Zeeman polarized atomic absorption spectrophotometer na nebulizer ọkụ iji chọpụta nbugharị nke ion metal n'ime ngwọta n'oge exfoliation electrochemical.A tụlere ikike zeta nke nnukwu boron wee rụọ ya na Zeta Sizer (ZS Nano ZEN 3600, Malvern) iji chọpụta ike elu nke nnukwu boron.Ọ bụ X-ray photoelectron spectroscopy (XPS) mụrụ ihe mejupụtara kemịkalụ na pasentị atọm ikwu nke elu ihe nlele ahụ.Emere nha ndị ahụ site na iji radieshon Mg Ka (hν = 1253.6 eV) na sistemu PREVAC (Poland) nke ejiri Scienta SES 2002 elektrọn ike nyocha (Sweden) na-arụ ọrụ na ike na-ebufe mgbe niile (Ep = 50 eV).A na-ewepụ ụlọ nyocha ahụ na nrụgide dị n'okpuru 5 × 10-9 mbar.
Dịka, 0.1 g nke boron ntụ ntụ n'efu ka a na-ebu ụzọ pịnye n'ime diski mesh metal (nickel ma ọ bụ ọla kọpa) site na iji igwe nrụnye hydraulic.Disk nwere dayameta nke 15 mm.A na-eji diski akwadoro dị ka electrodes.A na-eji ụdị electrolytes abụọ: (i) 1 M LiCl na DMSO na (ii) 1 M Na2SO4 na mmiri deionized.A na-eji waya platinum mee ihe dị ka electrode inyeaka.E gosipụtara eserese schematic nke ebe a na-arụ ọrụ na eserese 1. N'ihe na-apụ apụ electrochemical, a na-etinye ihe dị ugbu a (1 A, 0.5 A, ma ọ bụ 0.1 A) n'etiti cathode na anode.Ogologo oge nnwale ọ bụla bụ 1 elekere.Mgbe nke ahụ gasịrị, a na-achịkọta ihe ndị dị elu, na-agbatị na 5000 rpm ma saa mmiri ugboro ugboro (ugboro 3-5) na mmiri deionized.
Ụdị dị iche iche, dị ka oge na anya n'etiti electrodes, na-emetụta morphology nke ngwaahịa ikpeazụ nke nkewa electrochemical.N'ebe a, anyị na-enyocha mmetụta nke electrolyte, etinyere ugbu a (1 A, 0.5 A na 0.1 A; voltaji 30 V) na ụdị nke metal okporo (Ni dabere na mmetụta size).A nwalere electrolytes abụọ dị iche iche: (i) 1 M lithium chloride (LiCl) na dimethyl sulfoxide (DMSO) na (ii) 1 M sodium sulfate (Na2SO4) na mmiri deionized (DI).Na nke mbụ, lithium cations (Li+) ga-abanye n'ime boron, nke jikọtara ya na ụgwọ na-adịghị mma na usoro ahụ.N'okwu nke ikpeazụ, anion sulfate (SO42-) ga-abanye n'ime boron nke ọma.
Na mbụ, e gosipụtara omume nke electrolytes dị n'elu na ugbu a nke 1 A. Usoro a were 1 hour na ụdị abụọ nke metal grids (Ni na Cu), n'otu n'otu.Ọgụgụ 2 na-egosi ihe onyonyo atomiki ike microscopy (AFM) nke ihe a ga-esi na ya pụta, na profaịlụ ịdị elu kwekọrọ na-egosi na eserese S1.Tụkwasị na nke ahụ, a na-egosi ịdị elu na akụkụ nke flakes mere na nyocha ọ bụla na Tebụl 1. O doro anya, mgbe ị na-eji Na2SO4 dị ka electrolyte, ọkpụkpụ nke flakes dị ntakịrị karịa mgbe ị na-eji grid ọla kọpa.E jiri ya tụnyere flakes agbapụrụ n'ihu onye na-ebu nickel, ọkpụrụkpụ ya na-ebelata ihe dịka ugboro ise.N'ụzọ na-akpali mmasị, nha nkesa nke akpịrịkpa yiri nha.Otú ọ dị, LiCl / DMSO dị irè na usoro nkwụsị nke na-eji ma metal meshes eme ihe, na-eme ka 5-15 dị iche iche nke borocene, dị ka ihe ndị ọzọ na-eme ka mmiri na-egbuke egbuke, na-eme ka ọtụtụ ọkwa nke borocene7,8 pụta.Ya mere, ọmụmụ ihe ndị ọzọ ga-ekpughe usoro zuru ezu nke ihe nlele nke agbadoro na electrolyte a.
Ihe onyonyo AFM nke mpempe akwụkwọ borocene mgbe delamination electrochemical n'ime A Cu_Li + _1 A, B Cu_SO42−_1 A, C Ni_Li + _1 A, na D Ni_SO42−_1 A.
Emere nyocha site na iji microscopy eletrọnịfefe (TEM).Dịka e gosiri na eserese 3, nnukwu usoro boron bụ crystalline, dịka ihe ngosi TEM nke boron na boron Layered na-egosi, yana Fast Fourier Transform (FFT) kwekọrọ na ụkpụrụ Electron Diffraction (SAED) na-esote.Isi ihe dị iche n'etiti ihe nlele mgbe usoro delamination na-adị mfe ịhụ na ihe oyiyi TEM, ebe d-spaces dị nkọ na ebe dị anya dị mkpụmkpụ (0.35-0.9 nm; Table S2).Ọ bụ ezie na ihe atụ ndị a kpụpụtara na ntupu ọla kọpa dabara n'usoro β-rhombohedral nke boron8, ihe atụ ndị ahụ ejiri nickel chepụta.ntupudakọtara amụma amụma nke parampat lattice: β12 na χ317.Nke a gosipụtara na nhazi nke borocene bụ crystalline, mana ọkpụkpụ na kristal ahụ gbanwere n'elu mgbatị ahụ.Agbanyeghị, ọ na-egosi n'ụzọ doro anya ndabere nke grid eji (Cu ma ọ bụ Ni) na kristal nke borene na-esi na ya pụta.Maka Cu ma ọ bụ Ni, ọ nwere ike ịbụ otu-kristal ma ọ bụ polycrystalline, n'otu n'otu.A hụkwara mgbanwe kristal na usoro mkpochapụ ndị ọzọ18,19.N'ọnọdụ anyị, nzọụkwụ d na nhazi ikpeazụ dabere na ụdị grid ejiri (Ni, Cu).Enwere ike ịhụ ọdịiche dị ịrịba ama na ụkpụrụ SAED, na-atụ aro na usoro anyị na-eduga n'ịmepụta ihe owuwu kristal ndị ọzọ.Na mgbakwunye, eserese elemental (EDX) na onyonyo STEM gosipụtara na ihe 2D a kpụrụ akpụ bụ nke boron (Fig. S5).Otú ọ dị, maka nghọta miri emi nke nhazi ahụ, a na-achọkwu ọmụmụ banyere njirimara nke borophenes artificial.Karịsịa, a ga-aga n'ihu na nyocha nke ọnụ ọnụ borene, n'ihi na ha na-arụ ọrụ dị mkpa na nkwụsi ike nke ihe na arụmọrụ catalytic20,21,22.
onyonyo TEM nke nnukwu boron A, B Cu_Li+_1 A na C Ni_Li+_1 A yana ụkpụrụ SAED kwekọrọ (A', B', C');ngwa ngwa Fourier transform (FFT) ntinye na onyonyo TEM.
A na-eme X-ray photoelectron spectroscopy (XPS) iji chọpụta ogo oxidation nke sample borene.N'oge ikpo ọkụ nke ihe atụ borophene, nha boron-boron mụbara site na 6.97% ruo 28.13% (Table S3).Ka ọ dị ugbu a, mbelata nkekọ boron suboxide (BO) na-apụtakarị n'ihi nkewa nke oxides elu yana ngbanwe nke boron suboxide na B2O3, dịka egosiri B2O3 na-abawanye na nlele.Na fig.S8 na-egosi mgbanwe na oke njikọ nke boron na oxide n'elu ikpo ọkụ.Egosiri ụdịdị dị iche iche na fig.S7.Nyocha gosiri na boronene oxidized n'elu na boron: oxide ratio nke 1: 1 tupu kpo oku na 1.5: 1 mgbe kpo oku.Maka nkọwa zuru ezu nke XPS, lee Ozi Mgbakwụnye.
Emere nnwale ndị ọzọ iji nwalee mmetụta nke ugbu a etinyere n'etiti electrodes n'oge nkewa nke electrochemical.Emere ule ndị a na mmiri nke 0.5 A na 0.1 A na LiCl/DMSO, n'otu n'otu.E gosipụtara nsonaazụ nke ọmụmụ AFM na Fig. 4, a na-egosipụtakwa profaịlụ elu kwekọrọ na fig.S2 na S3.N'iburu n'uche na ọkpụrụkpụ nke monolayer borophene dị ihe dị ka 0.4 nm, 12,23 na nyocha na 0.5 A na ọnụnọ nke grid ọla kọpa, flakes ndị kachasị dị nro kwekọrọ na 5-11 borophene layers na akụkụ akụkụ nke ihe dịka 0.6-2.5 μm.Ke adianade do, na nnwale nanickelgrids, flakes nwere oke oke nkesa (4.82-5.27 nm) nwetara.Na-akpali mmasị, boron flakes nwetara site sonochemical ụzọ nwere yiri flake nha na nso nke 1.32-2.32 nm7 ma ọ bụ 1.8-4.7 nm8.Na mgbakwunye, exfoliation electrochemical nke graphene tụrụ aro nke Achi et al.14 rụpụtara nnukwu flakes (> 30 µm), nke nwere ike jikọta na nha ihe mmalite.Otú ọ dị, flakes graphene dị 2-7 nm.Enwere ike nweta flakes nke nha na ịdị elu karịa site na ibelata etinyere ugbu a site na 1 A ruo 0.1 A. Ya mere, ịchịkwa oke udidi ederede a nke ihe 2D bụ atụmatụ dị mfe.Ekwesiri ighota na nnwale emere na nickel grid nke nwere ugbua nke 0.1 A emeghị nke oma.Nke a bụ n'ihi obere eletriki eletrik nke nickel ma e jiri ya tụnyere ọla kọpa na ike zuru oke achọrọ iji mepụta borophene24.Nyocha TEM nke Cu_Li + _0.5 A, Cu_Li + _0.1 A, Cu_SO42-_1 A, Ni_Li-_0.5 A na Ni_SO42-_1 A ka egosiri na eserese S3 na eserese S4, n'otu n'otu.
Mwepu nke electrochemical na-esote AFM imaging.(A) Cu_Li+_1A, (B) Cu_Li+_0.5A, (C) Cu_Li+_0.1A, (D) Ni_Li+_1A, (E) Ni_Li+_0.5A.
N'ebe a, anyị na-atụ aro a ga-ekwe omume usoro maka stratification nke nnukwu akuakuzinwo n'ime mkpa-oyi akwa drills (Fig. 5).Na mbụ, a na-agbanye nnukwu burs n'ime grid Cu / Ni iji mee ka a na-eduzi ya na electrode, bụ nke tinyechara voltaji n'etiti eriri inyeaka (Pt waya) na electrode na-arụ ọrụ.Nke a na-enye ohere ka ion na-akwaga site na electrolyte wee banye n'ime ihe cathode / anode, dabere na electrolyte eji.Nyocha AAS gosipụtara na ọ dịghị ion a tọhapụrụ na nchara ígwè n'oge usoro a (lee Ozi Mgbakwụnye).gosiri na ọ bụ naanị ions sitere na electrolyte nwere ike ịbanye n'ime usoro boron.A na-akpọkarị boron azụmahịa buru ibu nke a na-eji eme ihe na usoro a dị ka "amorphous boron" n'ihi na ọ na-ekesa nkesa nke isi cell, icosahedral B12, nke na-ekpo ọkụ na 1000 ° C iji mepụta usoro β-rhombohedral nyere iwu (Fig. S6). 25 .Dị ka data ahụ si kwuo, a na-ewebata cations lithium ngwa ngwa n'ime ihe owuwu boron na ọkwa mbụ wee dọkasịa iberibe batrị B12, mechaa mepụta usoro boronene nwere akụkụ abụọ nwere usoro iwu siri ike, dị ka β-rhombohedra, β12 ma ọ bụ χ3. , dabere na etinyere ugbu a na nkentupuihe.Iji kpughee njikọ Li + na nnukwu boron na isi ọrụ ya na usoro delamination, a tụrụ ikike zeta (ZP) ka ọ bụrụ -38 ± 3.5 mV (lee Ozi Mgbakwụnye).Uru ZP na-adịghị mma maka nnukwu boron na-egosi na njikọta nke cations lithium dị mma na-arụ ọrụ nke ọma karịa ion ndị ọzọ ejiri na ọmụmụ a (dịka SO42-).Nke a na-akọwakwa nke ọma ntinye nke Li+ n'ime usoro boron, na-eme ka mwepụ electrochemical dịkwuo mma.
Ya mere, anyị emepụtala usoro ọhụrụ maka ịnweta borons dị ala site na electrochemical stratification nke boron site na iji Cu / Ni grids na Li +/DMSO na SO42-/H2O ngwọta.Ọ dịkwa ka ọ na-enye mmepụta na ọkwa dị iche iche dabere na nke etinyere ugbu a na grid eji.A na-atụkwa aro ma tụlere usoro nke usoro mkpochapụ.Enwere ike ikwubi na boronene dị ala na-achịkwa àgwà nwere ike ịmepụta ngwa ngwa site n'ịhọrọ nchara ígwè dị mma dị ka onye na-ebu boron ma na-emeziwanye ihe eji eme ihe ugbu a, bụ nke a pụrụ iji mee ihe n'ụzọ bụ isi na nyocha ma ọ bụ ngwa bara uru.Nke kachasị mkpa, nke a bụ mbọ mbụ na-aga nke ọma n'ịbapụta electrochemical nke boron.A kwenyere na a na-ejikarị ụzọ a mee ka ihe ndị na-adịghị emepụta ihe na-eme ka ọ bụrụ akụkụ abụọ.Otú ọ dị, a chọrọ nghọta ka mma nke nhazi na ihe onwunwe nke synthesized ala-layer burs, yana nyocha ọzọ.
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Nickel waya ntupu bụ ụdị waya ụlọ ọrụakwamere site na nickel waya.Ihe e ji mara ya bụ ịdịte aka ya, nrụzi eletriki, na iguzogide corrosion na nchara.N'ihi ihe ndị pụrụ iche ya, a na-ejikarị eriri nickel eme ihe na ngwa ndị dị ka nzacha, sieving, na nkewa na ụlọ ọrụ dịka ikuku ikuku, kemịkalụ, na nhazi nri.Ọ dị n'ụdị nha ntupu na dayameta waya iji kwado ihe dị iche iche a chọrọ.