Kua wehea te karāpiti ki te karāpiti horihori me te karāpiti tūturu, ko te nui o te karāpiti tūturu kua whakamātauhia o te ao he tata ki te 2 piriona tana.
Ka whiwhihia te karāpeti horihori mā te wetewete me te whakamahana i ngā rauemi kei roto he waro i raro i te pēhanga noa. E hiahiatia ana he pāmahana me te pūngao teitei hei kaha akiaki mō tēnei panonitanga, ā, ka hurihia te hanganga koretake hei hanganga tioata karāpeti kua whakaritea.
Ko te whakakāwhata i te tikanga whānui ko te whakarerekētanga o ngā ngota waro mā te maimoatanga wera nui i runga ake i te 2000 ℃. Heoi, ko ētahi rauemi waro i te pāmahana teitei i runga ake i te 3000 ℃, i mōhiotia tēnei momo rauemi waro ko te "waro mārō". Mō ngā rauemi waro ngāwari ki te whakakāwhata, ko te tikanga whakakāwhata tuku iho ko te tikanga pāmahana teitei me te pēhanga teitei, te whakakāwhata catalytic, te tikanga whakatakoto kohu matū, me ētahi atu.
He huarahi whai hua te whakakāwhata hei whakamahi i ngā rauemi waro me te uara nui. Whai muri i te rangahau whānui me te hōhonu a ngā tohunga, kua tino pakari inaianei. Heoi, kei te whakawhāitihia te whakamahinga o te whakakāwhata tuku iho i roto i te ahumahi e ētahi āhuatanga kino, nō reira he mea e kore e taea te karo te tūhura i ngā tikanga whakakāwhata hou.
Neke atu i te rautau 19 te whanaketanga o te tikanga hiko tote rewa, ā, kei te haere tonu te auahatanga me te whanaketanga o ōna ariā taketake me ngā tikanga hou. Ināianei kāore e herea noa ki te umanga whakarewa tuku iho. I te tīmatanga o te rautau 21, kua riro te whakarewa i roto i te pūnaha tote rewa hei whakarite whakaiti hiko waikura totoka o ngā konganuku huānga hei arotahi ki te kaha ake.
Nō nā tata nei, kua tino arohia te huarahi hou mō te whakarite i ngā rauemi karāpeti mā te whakamahi i te hiko tote rewa.
Mā te pōraitanga katote me te whakanoho hiko, ka hurihia ngā momo rauemi mata waro e rua hei rauemi nano-karāpiti me te uara tāpiri nui. Ki te whakatauritea ki te hangarau whakakārāpiti tuku iho, he pai ngā painga o te tikanga whakakārāpiti hou, arā, he iti ake te pāmahana whakakārāpiti me te āhua ka taea te whakahaere.
Ka arotakehia e tēnei pepa te ahunga whakamua o te whakakāwhata mā te tikanga hikohiko, ka whakaurua tēnei hangarau hou, ka tātarihia ōna painga me ōna ngoikoretanga, me te matapae i tōna whanaketanga ā muri ake nei.
Tuatahi, te tikanga whakapolarisasi katote hiko tote rewa
1.1 ngā rauemi mata
I tēnei wā, ko te rauemi mata matua o te graphite horihori ko te ngira Coke me te pitch Coke o te taumata graphitization teitei, arā, mā te toenga hinu me te tāra waro hei rauemi mata hei whakaputa rauemi waro kounga teitei, he iti te porosity, he iti te whanariki, he iti te ihirangi pungarehu me ngā painga o te graphitization, i muri i tōna whakaritenga ki te graphite he ātete pai ki te pānga, he kaha miihini teitei, he iti te ātete.
Heoi, nā te iti o ngā rahui hinu me te piki me te heke o ngā utu hinu kua aukati i tōna whanaketanga, nō reira kua noho ko te rapu rauemi mata hou hei raruraru nui hei whakatau.
He iti noa ngā herenga o ngā tikanga whakakāwhata tuku iho, ā, he rerekē ngā rauemi mata e whakamahia ana e ngā tikanga whakakāwhata rerekē. Mō te waro kāore i te whakakāwhata, he uaua ki ngā tikanga tuku iho te whakakāwhata, engari ko te tātai hikohiko o te whakakāwhata tote rewa ka pakaru i ngā herenga o ngā rauemi mata, ā, he pai mō te nuinga o ngā rauemi waro tuku iho.
Ko ngā rauemi waro tuku iho ko te waro pango, te waro whakahohe, te waro, me ētahi atu, ā, ko te waro te mea tino whai hua. Ko te waro te matū o te waituhi waro, ā, ka hangaia hei hua karāpeti i te pāmahana teitei i muri i te maimoatanga o mua.
Nō nā tata nei, e whakaarohia ana e tēnei pepa he tikanga hikohiko hou, pērā i a Peng, mā te hikohiko tote rewa, kāore pea e taea te whakakāwhata i te pango waro ki roto i te tioata teitei o te karāhe. Ko te hikohiko o ngā tauira karāhe kei roto ngā maramara nanometer karāhe āhua rau, he nui te horahanga mata motuhake, ā, i te wā e whakamahia ana mō te pākahiko lithium, he pai ake te mahi hikohiko o te karāhe i te karāhe taiao.
I whakauruhia e Zhu me ētahi atu te waro kounga iti kua tukatukahia ki roto i te pūnaha tote rewa CaCl2 mō te hikohiko i te 950 ℃, ā, i angitu te huri i te waro kounga iti ki te karāpeti he teitei te tioata, i whakaatu i te tere pai me te roa o te huringa i te wā i whakamahia ai hei anode mō te pākahiko lithium ion.
E whakaatu ana te whakamātautau he mea taea te huri i ngā momo rauemi waro tuku iho ki te karāpeti mā te whakamahi i te hiko tote rewa, e huaki ana i tētahi ara hou mō te karāpeti hangai ā muri ake nei.
1.2 te tikanga o
Ko te tikanga hiko tote whakarewa e whakamahi ana i te rauemi waro hei katote, ā, ka hurihia hei karāpeti me te tioata teitei mā te whakapūtanga katote. I tēnei wā, e kōrero ana ngā tuhinga o nāianei mō te tango i te hāora me te whakarite anō i ngā ngota waro i tawhiti i roto i te tukanga hurihanga pea o te whakapūtanga katote.
Ka ārai te noho o te hāora i roto i ngā rauemi waro i te whakakāwhata ki tētahi taumata. I roto i te tukanga whakakāwhata tuku iho, ka āta tangohia te hāora ina teitei ake te pāmahana i te 1600K. Heoi, he tino watea te tango waikura mā te whakakōrori katote.
I roto i ngā whakamātautau, i whakatakoto tuatahi a Peng i te tikanga pūmanawa pōraruraru cathodic electrolysis tote rewa, arā, ko te graphitization te wāhi tuatahi hei tīmatanga, arā, ko te whakanoho i te microsphere waro totoka/atanga electrolyte. Tuatahi, ka hangaia he microsphere waro huri noa i te anga graphite taketake, he rite te diameter, kātahi ka horapa ngā ngota waro waro koretake ki te papa graphite o waho, kia tino graphitized.
Ka haere tahi te tukanga whakakāwhata me te tango i te hāora, ā, kua whakaūtia anō hoki tēnei e ngā whakamātautau.
I whakamātauhia hoki tēnei tirohanga e Jin me ētahi atu mā roto i ngā whakamātautau. I muri i te whakawarotanga o te hukahuka, i mahia te whakakāwhata (17% te nui o te hāora). I muri i te whakakāwhata, i hangaia e ngā porowhita waro totoka taketake (Pikitia 1a me te 1c) he anga porowhita i titoa mai i ngā nanopepa kāwhata (Pikitia 1b me te 1d).
Mā te hikohiko o ngā muka waro (16% hāora), ka taea te huri i ngā muka waro hei ngongo karāpeti i muri i te whakakārāpeti kia rite ki te tikanga hurihanga kua whakaarohia i roto i ngā tuhinga.
E whakaponohia ana, ko te nekehanga tawhiti kei raro i te pōrotanga cathodic o ngā ngota waro, me tukatuka te karāhe tioata teitei ki te waro amorphous kia whakarerekētia, me tukatuka te karāhe hangai i ngā hanganga nano ahurei o ngā raupua, engari kāore i te mārama te āhua motuhake o te pānga ki te hanganga nanometer karāhe, pērā i te hāora mai i te anga waro i muri i te tauhohenga karāhe, me ētahi atu.
I tēnei wā, kei te tīmatanga tonu te rangahau mō te tikanga, ā, me haere tonu ngā rangahau.
1.3 Te āhua o te graphite hangai
Ka whakamahia te SEM hei tirotiro i te āhua o te mata moroiti o te karāpeti, ka whakamahia te TEM hei tirotiro i te āhua o te hanganga iti iho i te 0.2 μm, ko te XRD me te inenga Raman ngā huarahi e whakamahia whānuitia ana hei whakaahua i te hanganga moroiti o te karāpeti, ka whakamahia te XRD hei whakaahua i ngā mōhiohio tioata o te karāpeti, ā, ka whakamahia te inenga Raman hei whakaahua i ngā hapa me te taumata o te raupapa o te karāpeti.
He maha ngā pūwero i roto i te karāpiti i hangaia mā te whakapūwero katote o te hiko tote rewa. Mō ngā rauemi mata rerekē, pērā i te hiko waro pango, ka whiwhihia he hanganga nano pūwero rite ki te rau. Ka whakahaerehia te tātari XRD me te tātaritanga Raman ki te waro pango i muri i te hiko.
I te 827 ℃, i muri i te tukatuka ki te ngaohiko 2.6V mō te 1 hāora, he rite tonu te ahua Raman o te pango waro ki te ahua o te karāpeti arumoni. I muri i te tukatuka i te pango waro ki ngā pāmahana rerekē, ka inehia te tihi āhua karāpeti koi (002). Ko te tihi diffraction (002) e tohu ana i te taumata o te whakatakotoranga o te paparanga waro kakara i roto i te karāpeti.
Ka koi ake te paparanga waro, ka nui ake te whakatakotoranga.
I whakamahia e Zhu te waro parakore kua purea hei katote i roto i te whakamātautau, ā, i hurihia te hanganga moroiti o te hua kua whakakāwhatia mai i te hanganga kirikiri ki te hanganga kāwhata nui, ā, i kitea anō hoki te paparanga kāwhata piri i raro i te karu hiko tuku tere teitei.
I roto i ngā hihi Raman, me te panonitanga o ngā āhuatanga whakamātautau, i rerekē anō hoki te uara ID/Ig. I te wā i 950 ℃ te pāmahana hikohiko, 6 hāora te roa o te wā hikohiko, ā, 2.6V te ngaohiko hikohiko, 0.3 te uara ID/Ig iti rawa, ā, he iti rawa te tihi D i te tihi G. I taua wā anō, ko te putanga mai o te tihi 2D he tohu anō hoki i te hanganga o te hanganga karāhe tino pai.
Ko te tihi whakarara koi (002) i roto i te ahua XRD e whakaū ana hoki i te angitu o te huringa o te waro ngoikore ki te karāpeti he teitei te tioata.
I roto i te tukanga whakakāwhata, ka whai wāhi nui te pikinga o te pāmahana me te ngaohiko, engari ka whakaitihia te hua o te kāwhata e te ngaohiko teitei rawa, ā, ka arahi te pāmahana teitei rawa, te roa rawa rānei o te wā whakakāwhata ki te moumou rauemi, nō reira mō ngā rauemi waro rerekē, he mea tino nui kia tūhuratia ngā āhuatanga hiko tino tika, koinei hoki te arotahi me te uauatanga.
He tino pai ngā āhuatanga hikohiko o tēnei hanganga nano, he rite ki te rau, he kirikiri. Nā te nui o ngā pūwero ka taea te whakauru/te tango wawe i ngā katote, ka puta he rauemi katote kounga teitei mō ngā pākahiko, me ērā atu. Nō reira, ko te tikanga hikohiko whakakāwhata he tikanga tino kaha ki te whakakāwhata.
Tikanga whakanoho hiko tote rewa
2.1 Te whakatakoto hiko o te hauhā waro
Hei te hau kati kōtuhi tino nui, he rauemi whakahou kore-paitini, kore-kino, iti te utu, ā, ngāwari te tiki. Heoi, ko te waro i roto i te CO2 kei te āhua waikura teitei rawa, nō reira he tino pumau te CO2 i te pāmahana, ā, he uaua ki te whakamahi anō.
Ko ngā rangahau tuatahi mō te whakanoho hiko CO2 ka taea te whai i ngā tau 1960. I angitu a Ingram me ētahi atu ki te whakarite i te waro ki runga i te hiko koura i roto i te pūnaha tote rewa o Li2CO3-Na2CO3-K2CO3.
I tohu a Van me ētahi atu he rerekē ngā hanganga o ngā paura waro i whiwhihia mai i ngā pūmanawa whakaiti rerekē, tae atu ki te karāpeti, te waro amorphous me ngā muka nano waro.
Mā te tote rewa hei hopu i te CO2 me te tikanga whakarite angitu o te rauemi waro, whai muri i te wā roa o te rangahau a ngā tohunga kua arotahi ki te tikanga hanganga whakatakotoranga waro me te pānga o ngā āhuatanga hiko ki te hua whakamutunga, tae atu ki te pāmahana hiko, te ngaohiko hiko me te hanganga o te tote me ngā hiko rewa, me ētahi atu, kua whakatakotohia he turanga pakari e te whakarite i ngā rauemi karāhe mahi teitei mō te whakanoho hiko o te CO2.
Mā te whakarerekē i te irahiko me te whakamahi i te pūnaha tote rewa e ahu mai ana i te CaCl2 me te pai ake o te hopu CO2, i angitu a Hu me ētahi atu ki te whakarite i te graphene me te tohu whakarawhiotanga teitei ake me ngā nanotube waro me ētahi atu hanganga nanographite mā te ako i ngā āhuatanga hikohiko pēnei i te pāmahana hikohiko, te hanganga irahiko me te hanganga tote rewa.
Ki te whakaritea ki te pūnaha warowaihā, he iti te utu me te ngāwari ki te tiki i te CaCl2, he nui te kawe hiko, he ngāwari ki te rewa ki te wai, ā, he nui ake te wairewatanga o ngā katote hāora, e whakarato ana i ngā tikanga ariā mō te hurihanga o te CO2 ki ngā hua karāpeti he nui te uara tāpiri.
2.2 Tikanga Whakawhiti
Ko te whakarite i ngā rauemi waro nui-tāpiri mā te whakanoho hiko o te CO2 mai i te tote rewa ko te nuinga o te wā ko te hopu CO2 me te whakaiti ā-kore. Ka oti te hopu o te CO2 mā te O2- kore utu i roto i te tote rewa, e whakaaturia ana i te Whārite (1):
CO2+O2-→CO3 2- (1)
I tēnei wā, e toru ngā tikanga tauhohenga whakaiti ā-kore kua whakaarohia: te tauhohenga kotahi-taahiraa, te tauhohenga rua-taahiraa me te tikanga tauhohenga whakaiti whakarewa.
I tuatahitia te whakaaro o te tikanga tauhohenga kotahi-taahiraa e Ingram, e whakaaturia ana i te Whārite (2):
CO3 2-+ 4E – →C+3O2- (2)
I whakatakotoria te tikanga tauhohenga e rua-taahiraa e Borucka et al., e whakaaturia ana i te Whārite (3-4):
CO3 2-+ 2E – →CO2 2-+O2- (3)
CO2 2-+ 2E – →C+2O2- (4)
Nā Deanhardt me ētahi atu i whakaaro ko te tikanga o te tauhohenga whakaiti whakarewa i whakatakoto. I whakapono rātou ka whakaitihia ngā katote whakarewa ki te whakarewa i te tuatahi i roto i te katote, kātahi ka whakaitihia te whakarewa ki ngā katote warowaihā, e whakaaturia ana i te Whārite (5~6):
M- + E – →M (5)
4 m + M2CO3 – > C + 3 m2o (6)
I tēnei wā, e whakaaetia whānuitia ana te tikanga tauhohenga kotahi-taahiraa i roto i ngā tuhinga o nāianei.
I ako a Yin me ētahi atu i te pūnaha kāponāte Li-Na-K me te nikara hei katote, te hauhā tine hei anote, me te waea hiriwa hei hiko tohutoro, ā, i whiwhi i te ahua whakamātautau voltammetry huringa i te Pikitia 2 (tere matawai o te 100 mV/s) i te katote nikara, ā, i kitea kotahi noa te tihi whakaiti (i te -2.0V) i roto i te matawai kino.
Nō reira, ka taea te whakatau kotahi anake te tauhohenga i puta i te wā o te whakaiti i te warowaihā.
I whiwhi a Gao me ētahi atu i te cyclic voltammetry ōrite i roto i te pūnaha warowaihā ōrite.
I whakamahia e Ge me ētahi atu te anode inert me te cathode tungsten hei hopu i te CO2 i roto i te pūnaha LiCl-Li2CO3, ā, i whiwhi i ngā whakaahua rite tonu, ā, ko te tihi whakaiti o te whakatakotoranga waro anake i puta i roto i te matawai kino.
I roto i te pūnaha tote rewa o te konganuku kawakore, ka puta ngā konganuku kawakore me te CO i te wā e whakatakotoria ana te waro e te katote. Heoi, nā te mea he iti ake ngā āhuatanga pāmahana o te tauhohenga whakatakoto waro i te pāmahana iti iho, ko te whakahekenga o te warokawa ki te waro anake ka kitea i roto i te whakamātautau.
2.3 Te hopunga o te CO2 e te tote rewa hei whakarite i ngā hua karāpeti
Ka taea te whakarite i ngā rauemi nano graphite tāpiri-uara nui pērā i te graphene me ngā nanotube waro mā te whakanoho hiko o te CO2 mai i te tote rewa mā te whakahaere i ngā āhuatanga whakamātautau. I whakamahia e Hu me ētahi atu te maitai kore waikura hei katote i roto i te pūnaha tote rewa CaCl2-NaCl-CaO, ā, i whakamātauria mō te 4 hāora i raro i te āhuatanga o te ngaohiko pumau 2.6V i ngā pāmahana rerekē.
Nā te whakakorikori o te rino me te pānga pahū o te CO i waenga i ngā paparanga karāpiti, i kitea te karāpīne i runga i te mata o te katote. Kei te whakaatuhia te tukanga whakarite o te karāpīne i te Pikitia 3.
Te pikitia
I muri mai, i tāpirihia te Li2SO4 i runga i te pūnaha tote rewa o CaCl2-NaClCaO, ā, ko te pāmahana hikohiko he 625 ℃. I muri i te 4h o te hikohiko, i te wā kotahi i kitea ai te graphene me ngā nanotubes waro i roto i te whakatakotoranga cathodic o te waro, i kitea e te rangahau he pānga pai a Li+ me SO4 2- ki te graphitization.
Ka whakauruhia angitutia hoki te whanariki ki roto i te tinana waro, ā, ka taea te whiwhi i ngā rau karāpeti tino angiangi me te waro miro mā te whakahaere i ngā āhuatanga hikohiko.
He mea nui ngā rauemi pēnei i te pāmahana hiko o te teitei me te iti mō te hanganga o te graphene, he māmā ake te whakaputa CO i te waro ina neke atu i te 800 ℃ te pāmahana, ā, kāore he whakatakotoranga waro ina neke atu i te 950 ℃, nō reira he mea tino nui te whakahaere i te pāmahana hei whakaputa i te graphene me ngā nanotube waro, me te whakahoki mai i te hiahia ki te tauhohenga whakatakotoranga waro CO hei whakarite kia pumau te graphene i roto i te cathode.
Mā ēnei mahi ka whakaratohia he tikanga hou mō te whakarite i ngā hua nano-graphite mā te CO2, he mea tino nui mō te otinga o ngā hau kati kōtuhi me te whakarite i te graphene.
3. Whakarāpopototanga me te Tirohanga
Nā te tere o te whanaketanga o te umanga pūngao hou, kāore i taea e te karāpeti māori te whakatutuki i te hiahia o nāianei, ā, he pai ake ngā āhuatanga ā-tinana me te matū o te karāpeti horihori i te karāpeti māori, nō reira he whāinga roa te whakakārāpeti iti te utu, he pai te mahi, ā, he pai hoki mō te taiao.
Ko te tikanga hiko-matū i roto i ngā rauemi mata totoka me te hau mā te tikanga o te pōraitanga cathodic me te whakatakotoranga hiko-matū i angitu te tango i ngā rauemi karāpeti me te uara tāpiri teitei, ki te whakaritea ki te tikanga tuku iho o te karāpeti, he nui ake te whai huatanga o te tikanga hiko-matū, he iti ake te whakapaunga pūngao, he tiaki taiao matomato, he iti noa te whakawhāititanga e ngā rauemi whiriwhiri i te wā kotahi, kia rite ki ngā āhuatanga hiko-matū rerekē ka taea te whakarite i ngā momo hanganga karāpeti rerekē.
He huarahi whai hua tēnei hei huri i ngā momo waro kore-āhua me ngā hau kati kōtuhi katoa hei rauemi karāhe nano-hanganga whai hua, ā, he pai hoki te tūmanako mō te tono.
I tēnei wā, kei te tīmatanga tonu tēnei hangarau. He iti noa ngā rangahau mō te whakakāwhata mā te tikanga hikohiko, ā, he maha tonu ngā tukanga kāore anō kia mōhiotia. Nō reira, me tīmata mai i ngā rauemi mata, me te whakahaere i tētahi rangahau whānui me te pūnaha mō ngā momo waro kore-āhua, ā, i te wā kotahi ka tūhuratia te pāmahana me ngā hihiri o te hurihanga kāwhata ki tētahi taumata hohonu ake.
He nui te hiranga o ēnei mō te whanaketanga o te umanga karāpeti ā muri ake nei.
Wā tuku: Mei-10-2021