Abstract:Bismuth vanadate (BiVO4) is one of the most effective photoanode materials for photoelectrochemical water splitting, while its reaction rate is greatly limited by the poor separation efficiency of photo-generated charges...
“…The dissociation of surface water (leading to surface hydroxyl) on BiVO 4 increases the complexity of reactions and has a profound impact on the formation of surface polaron and carrier dynamics. For instance, Li et al discovered that surface hydroxylation of the BiVO 4 photoanode improves photogenerated charges separation, resulting in an increase in photocurrent density by 4.75 times . By using ambient pressure resonant photoemission spectroscopy combined with first-principles calculations, Wang et al reported that dissociated water molecules caused hydroxylation of VO 4 tetrahedron on BiVO 4 (010), leading to an enhanced stability of the surface polarons and an alternation of the surface electronic structure .…”
mentioning
confidence: 99%
“…For instance, Li et al discovered that surface hydroxylation of the BiVO 4 photoanode improves photogenerated charges separation, resulting in an increase in photocurrent density by 4.75 times. 27 By using ambient pressure resonant photoemission spectroscopy combined with first-principles calculations, Wang et al reported that dissociated water molecules caused hydroxylation of VO 4 tetrahedron on BiVO 4 (010), leading to an enhanced stability of the surface polarons and an alternation of the surface electronic structure. 28 Surface hydroxylation of metal oxides is commonly observed in the photocatalytic water decomposition process; however, the effect of surface hydroxylation on polaron dynamics is still a mystery and requires a detailed time-domain study of the polaron coupled charge carrier dynamics.…”
Polaron-based electron transport restricts the photoelectrochemical
(PEC) water splitting efficiency of BiVO4. However, the
location and dynamics of polarons are significantly dependent on the
surface hydroxylation. By performing ab initio nonadiabatic molecular
dynamics simulations, we demonstrated that hydroxylation of BiVO4(010) surface greatly alleviates the detrimental effect of
oxygen-vacancy-induced electron polaron (EP). Surface hydroxylation
stabilizes the EP at the surface to facilitate water splitting, makes
the polaron a shallow localized state, and reduces the intensity of
high-frequency V–O bond stretching vibrations. By decreasing
the nonadiabatic coupling and decoherence time, the charge carrier
lifetimes are extended by 1–3 orders of magnitude depending
on the hydroxylation coverage. Our study not only reveals that the
surface hydroxylation mitigated detrimental impacts of polarons in
metal oxides but also provided valuable insights into the benign effect
of intermediate species on the photocatalytic reactivity.
“…The dissociation of surface water (leading to surface hydroxyl) on BiVO 4 increases the complexity of reactions and has a profound impact on the formation of surface polaron and carrier dynamics. For instance, Li et al discovered that surface hydroxylation of the BiVO 4 photoanode improves photogenerated charges separation, resulting in an increase in photocurrent density by 4.75 times . By using ambient pressure resonant photoemission spectroscopy combined with first-principles calculations, Wang et al reported that dissociated water molecules caused hydroxylation of VO 4 tetrahedron on BiVO 4 (010), leading to an enhanced stability of the surface polarons and an alternation of the surface electronic structure .…”
mentioning
confidence: 99%
“…For instance, Li et al discovered that surface hydroxylation of the BiVO 4 photoanode improves photogenerated charges separation, resulting in an increase in photocurrent density by 4.75 times. 27 By using ambient pressure resonant photoemission spectroscopy combined with first-principles calculations, Wang et al reported that dissociated water molecules caused hydroxylation of VO 4 tetrahedron on BiVO 4 (010), leading to an enhanced stability of the surface polarons and an alternation of the surface electronic structure. 28 Surface hydroxylation of metal oxides is commonly observed in the photocatalytic water decomposition process; however, the effect of surface hydroxylation on polaron dynamics is still a mystery and requires a detailed time-domain study of the polaron coupled charge carrier dynamics.…”
Polaron-based electron transport restricts the photoelectrochemical
(PEC) water splitting efficiency of BiVO4. However, the
location and dynamics of polarons are significantly dependent on the
surface hydroxylation. By performing ab initio nonadiabatic molecular
dynamics simulations, we demonstrated that hydroxylation of BiVO4(010) surface greatly alleviates the detrimental effect of
oxygen-vacancy-induced electron polaron (EP). Surface hydroxylation
stabilizes the EP at the surface to facilitate water splitting, makes
the polaron a shallow localized state, and reduces the intensity of
high-frequency V–O bond stretching vibrations. By decreasing
the nonadiabatic coupling and decoherence time, the charge carrier
lifetimes are extended by 1–3 orders of magnitude depending
on the hydroxylation coverage. Our study not only reveals that the
surface hydroxylation mitigated detrimental impacts of polarons in
metal oxides but also provided valuable insights into the benign effect
of intermediate species on the photocatalytic reactivity.
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