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Tailoring the photoelectrochemistry of catalytic metal-insulator-semiconductor (MIS) photoanodes by a dissolution method.

ABSTRACT: Apart from being key structures of modern microelectronics, metal-insulator-semiconductor (MIS) junctions are highly promising electrodes for artificial leaves, i.e. photoelectrochemical cells that can convert sunlight into energy-rich fuels. Here, we demonstrate that homogeneous Si/SiO_x/Ni MIS junctions, employed as photoanodes, can be functionalized with a redox-active species and simultaneously converted into high-photovoltage inhomogeneous MIS junctions by electrochemical dissolution. We also report on the considerable enhancement of performance towards urea oxidation, induced by this process. Finally, we demonstrate that both phenomena can be employed synergistically to design highly-efficient Si-based photoanodes. These findings open doors for the manufacturing of artificial leaves that can generate H₂ under solar illumination using contaminated water.

SUBMITTER: Loget G

PROVIDER: S-EPMC6684633 | biostudies-literature | 2019 Aug

REPOSITORIES: biostudies-literature

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Tailoring the photoelectrochemistry of catalytic metal-insulator-semiconductor (MIS) photoanodes by a dissolution method.

Loget G G Mériadec C C Dorcet V V Fabre B B Vacher A A Fryars S S Ababou-Girard S S

Nature communications 20190806 1

Apart from being key structures of modern microelectronics, metal-insulator-semiconductor (MIS) junctions are highly promising electrodes for artificial leaves, i.e. photoelectrochemical cells that can convert sunlight into energy-rich fuels. Here, we demonstrate that homogeneous Si/SiO<sub>x</sub>/Ni MIS junctions, employed as photoanodes, can be functionalized with a redox-active species and simultaneously converted into high-photovoltage inhomogeneous MIS junctions by electrochemical dissolut ...[more]

PMID: 31387994

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Project description:We analyze the ferroelectric domain-wall induced negative capacitance (NC) effect in Metal-FE-Insulator-Metal (MFIM) and Metal-FE-Insulator-Semiconductor (MFIS) stacks through phase-field simulations by self-consistently solving time-dependent Ginzburg Landau equation, Poisson's equation and semiconductor charge equations. Considering Hf0.5Zr0.5O2 as the ferroelectric material, we study 180° ferroelectric domain formation in MFIM and MFIS stacks and their polarization switching characteristics. Our analysis signifies that the applied voltage-induced polarization switching via soft domain-wall displacement exhibits non-hysteretic characteristics. In addition, the change in domain-wall energy, due to domain-wall displacement, exhibits a long-range interaction and thus, leads to a non-homogeneous effective local negative permittivity in the ferroelectric. Such effects yield an average negative effective permittivity that further provides an enhanced charge response in the MFIM stack, compared to Metal-Insulator-Metal. Furthermore, we show that the domain-wall induced negative effective permittivity is not an intrinsic property of the ferroelectric material and therefore, is dependent on its thickness, the gradient energy coefficient and the in-plane permittivity of the underlying insulator. Similar to the MFIM stack, MFIS stack also exhibits an enhanced charge/capacitance response compared to Metal-Oxide-Semiconductor (MOS) capacitor. Simultaneously, the multi-domain state of the ferroelectric induces non-homogeneous potential in the underlying insulator and semiconductor layer. At low applied voltages, such non-homogeneity leads to the co-existence of electrons and holes in an undoped semiconductor. In addition, we show that with the ferroelectric layer being in the 180° multi-domain state, the minimum potential at the ferroelectric-dielectric interface and hence, the minimum surface potential in the semiconductor, does not exceed the applied voltage (in-spite of the local differential amplification and charge enhancement).

Dataset Information

Tailoring the photoelectrochemistry of catalytic metal-insulator-semiconductor (MIS) photoanodes by a dissolution method.

Publications

Tailoring the photoelectrochemistry of catalytic metal-insulator-semiconductor (MIS) photoanodes by a dissolution method.

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