Titanium Anode Conductivity Thiab Catalytic Mechanism Taw Qhia

1. Conductive mechanism ntawm hlau oxide electrode

Hluav taws xob conductivity yog qhov kev ua tau zoo tshaj plaws uas cov electrode yuav tsum muaj. Raws li cov qauv atomic tau piav qhia los ntawm Goodenough, Ti⁴⁺thiab O^2-txheej electron orbitals yog hybridized los ua δ bonds thiab π bonds. Lub valence electrons txaus los sau cov kab hluav taws xob tsawg ntawm δ thiab π, thaum lub zog siab band tseem khoob. Raws li kev xav ntawm cov khoom siv, cov qauv molecular no tsis yooj yim rau kev siv hluav taws xob. Ua kom Ti02 conductive. Nws yog ib qho tsim nyog rau embed cov ntsiab lus nrog ib los yog ntau tshaj valence electrons nyob rau hauv Ti02, cov electrons yuav nyob rau hauv conduction band los yog ua tus cab kuj ntawm lotus.

Ru0₂yog ib qho kev hloov pauv hlau oxide nrog cov qauv rutile. Lub sab nrauv electron configuration ntawm Ru yog 4d⁷5s¹. Tom qab plaub lub tshuab hluav taws xob tau muab rau ob lub pa oxygen, cov pa atoms ua tiav cov 8-electron txheej, thiab muaj 4 qhov seem dawb electrons koom nrog kev sib txuas lus. Doping Ru in TiO₂, kev daws teeb meem ntawm cov txheej txheem tuaj yeem qhia tau tias: Ru_δTi_(n-δ)O_2ne_4δ (1.13)

Hauv cov qauv, δ sawv cev rau tus naj npawb ntawm atoms ntawm Ti hloov los ntawm Ru, thiab n yog tus naj npawb ntawm atoms ntawm Ti hauv Ti 0₂. Ntxiv rau tag nrho pawg hauv Ru0₂-Ti0₂cov tshuaj, muaj ib tug electron-muaj zog band (e_4δ). Piv nrog rau cov electrons nyob rau hauv tag nrho cov qhab, cov electrons nyob rau hauv no lub zog band yog tsawg khi thiab yuav zoo siab rau lub conduction band nrog tsuas yog {{0}}}.2ev zog, thiaj li hais tias txwv tsis pub band dav ntawm Ti0.₂yog sib npaug ntawm cov insulator. 3. Tsis tas li ntawd, Ru0₂yog cov hlau tsis muaj oxygen, uas ua rau muaj cov khoom siv hluav taws xob ntau ntxiv. Tsis tas li ntawd, nyob rau hauv ntau yam txheej txheem ntawm oxide txheej txheej txheem, ib feem ntawm cov pa atoms yog hloov los ntawm chlorine atoms, uas ua rau kom tus xov tooj ntawm unshared electrons. Yog li ntawd, TiO₂yog embedded nrog Ru0₂los yog Ru0₂yog embedded nrog TiO₂, thiab qhov sib tov no ua rau cov electrode conductive.

Doping 1% mol ntawm Ta thiab Nb hauv TiO₂(ob qho tib si tsuas yog ib qho hluav taws xob ntau dua Ti), qhov kev coj ua uas tau nce los ntawm 4160 zaug thiab 5500 zaug, feem. Hauv Ru0₂-Ti0₂n-hom semiconductor, tus pub ruthenium muaj 4 dawb electrons, uas yog ntau tshaj li cov dawb electrons uas Ta thiab Nb muaj peev xwm muab tau, yog li cov conductivity ntawm cov khoom tov yog zoo heev.

2. Catalytic mechanism ntawm hlau oxide electrode

Ru0₂, Ib0₂, PbO, thiab lwm yam. npaj los ntawm thermal decomposition yog non-stoichiometric defect qauv tebchaw. Siv cov thermal decomposition ntawm RuCl₃ntawm 300 degree -500 degree ua piv txwv, RuO_xCl_yH_zyog tau. Txij li thaum cov pa tsis xws luag yog tsim nyob rau hauv lub siv lead ua lattice, Ru³⁺yuav tsum muaj. Thaum muaj qhov zoo voltage yog siv rau electrode, thawj Ru³⁺zoo siab los hloov cov electrons mus rau titanium matrix, tsim Ru⁴⁺nrog rau qhov muaj zog tshaj qhov chaw them nqi. Cov kab lus tuaj yeem sau ua:

Ru³⁺→ Ru⁴⁺ + e^- (1.14)

Ru⁴⁺+ Cl^- → Ru₄+ Cl_{kev tshaj tawm}+ e^- (1.15)

Lub sijhawm no, Ru⁴⁺yog lub chaw ua haujlwm nyob rau saum npoo ntawm cov khoom siv hluav taws xob semiconductor thiab yog qhov muaj txiaj ntsig zoo uas tuaj yeem txais cov khoom siv hluav taws xob. Raws li kev ua haujlwm electrostatic, Ru⁴⁺yuav nyiam Cl^-ntawm oxide/solution interface, ua rau Cl^-kom tso tawm rau nws, thiab cov electrons raug thauj mus rau titanium matrix los ntawm Ru⁴⁺, cov qauv tshuaj tiv thaiv yog:

Ru⁴⁺+ Cl^-→ Ru⁴⁺Cl_{kev tshaj tawm}+ e^- (1.16)

Lub sijhawm no, Ru⁴⁺Cl_{kev tshaj tawm}ua ke nrog Cl^-ntawm lub interface los tsim Cl₂, thiab Ru⁴⁺tau txais electrons thiab hloov mus rau Ru³⁺. Cov qauv tshuaj tiv thaiv yog:

Ru⁴⁺Cl_{kev tshaj tawm}+ Cl^- → Ru³⁺+C1₂ (1.17)

Vim Ru⁴⁺, Ru³⁺hloov los ntawm 4d⁴rau 4d⁵, thiab tsim ntawm C1₂kuj txo lub zog ntawm lub cev, cov tshuaj tiv thaiv yog ib qho yooj yim mus ua, yog li formula (1.14) yog tus nqi tswj cov kauj ruam.

Raws li cov txheej txheem catalytic ntawm Ru02, cov kws tshawb fawb ntseeg tias PdO tsim los ntawm thermal decomposition ntawm PdCl₂yog ib qho tsis-stoichiometric oxygen-deficient compound, thiab muaj Pd⁺nyob rau hauv lub siv lead ua lattice, thiab cov tshuaj chlorine evolution mechanism ntawm nws zoo ib yam li cov Ru³⁺, yog li cov ntsiab lus ntawm titanium-based noble hlau oxide Lub catalytic mechanism ntawm electrode yog:

Mn⁺ → M⁽ⁿ⁺¹⁾⁺ + e^- (1.18)

M⁽ⁿ⁺¹⁾⁺+ Cl^- → M(n+1)+Clads + e^- (1.19)

M⁽ⁿ⁺¹⁾⁺Cl_{kev tshaj tawm}+ Cl^- → Mn⁺+ Cl₂ (1.20)

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