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Multilayer Strategy for Photoelectrochemical Hydrogen Generation: New Electrode Architecture that Alleviates Multiple Bottlenecks.

ABSTRACT: Years of research have demonstrated that the use of multiple components is essential to the development of a commercial photoelectrode to address specific bottlenecks, such as low charge separation and injection efficiency, low carrier diffusion length and lifetime, and poor durability. A facile strategy for the synthesis of multilayered photoanodes from atomic-layer-deposited ultrathin films has enabled a new type of electrode architecture with a total multilayer thickness of 15-17 nm. We illustrate the advantages of this electrode architecture by using nanolayers to address different bottlenecks, thus producing a multilayer photoelectrode with improved interface kinetics and shorter electron transport path, as determined by interface analyses. The photocurrent density was twice that of the bare structure and reached a maximum of 33.3 ± 2.1 mA cm^-2 at 1.23 V_RHE. An integrated overall water-splitting cell consisting of an electrocatalytic NiS cathode and Bi₂S₃/NiS/NiFeO/TiO₂ photoanode was used for precious-metal-free seawater splitting at a cell voltage of 1.23 V without degradation. The results and root analyses suggest that the distinctive advantages of the electrode architecture, which are superior to those of bulk bottom-up core-shell and hierarchical architectures, originate from the high density of active sites and nanometer-scale layer thickness, which enhance the suitability for interface-oriented energy conversion processes.

SUBMITTER: Seenivasan S

PROVIDER: S-EPMC8956779 | biostudies-literature | 2022 Mar

REPOSITORIES: biostudies-literature

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Multilayer Strategy for Photoelectrochemical Hydrogen Generation: New Electrode Architecture that Alleviates Multiple Bottlenecks.

Seenivasan Selvaraj S Moon Hee H Kim Do-Heyoung DH

Nano-micro letters 20220325 1

Years of research have demonstrated that the use of multiple components is essential to the development of a commercial photoelectrode to address specific bottlenecks, such as low charge separation and injection efficiency, low carrier diffusion length and lifetime, and poor durability. A facile strategy for the synthesis of multilayered photoanodes from atomic-layer-deposited ultrathin films has enabled a new type of electrode architecture with a total multilayer thickness of 15-17 nm. We illus ...[more]

PMID: 35334000

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Project description:One of the emerging and environmentally friendly technologies is the photoelectrochemical generation of green hydrogen; however, the cheap cost of production and the need for customizing photoelectrode properties are thought to be the main obstacles to the widespread adoption of this technology. The primary players in hydrogen production by photoelectrochemical (PEC) water splitting, which is becoming more common on a worldwide basis, are solar renewable energy and widely available metal oxide based PEC electrodes. This study attempts to prepare nanoparticulate and nanorod-arrayed films to better understand how nanomorphology can impact structural, optical, and PEC hydrogen production efficiency, as well as electrode stability. Chemical bath deposition (CBD) and spray pyrolysis are used to create ZnO nanostructured photoelectrodes. Various characterization methods are used to investigate morphologies, structures, elemental analysis, and optical characteristics. The crystallite size of the wurtzite hexagonal nanorod arrayed film was 100.8 nm for the (002) orientation, while the crystallite size of nanoparticulate ZnO was 42.1 nm for the favored (101) orientation. The lowest dislocation values for (101) nanoparticulate orientation and (002) nanorod orientation are 5.6 × 10-4 and 1.0 × 10-4 dislocation/nm2, respectively. By changing the surface morphology from nanoparticulate to hexagonal nanorod arrangement, the band gap is decreased to 2.99 eV. Under white and monochromatic light irradiation, the PEC generation of H2 is investigated using the proposed photoelectrodes. The solar-to-hydrogen conversion rate of ZnO nanorod-arrayed electrodes was 3.72% and 3.12%, respectively, under 390 and 405 nm monochromatic light, which is higher than previously reported values for other ZnO nanostructures. The output H2 generation rates for white light and 390 nm monochromatic illuminations were 28.43 and 26.11 mmol.h-1cm-2, respectively. The nanorod-arrayed photoelectrode retains 96.6% of its original photocurrent after 10 reusability cycles, compared to 87.4% for the nanoparticulate ZnO photoelectrode. The computation of conversion efficiencies, H2 output rates, Tafel slope, and corrosion current, as well as the application of low-cost design methods for the photoelectrodes, show how the nanorod-arrayed morphology offers low-cost, high-quality PEC performance and durability.

Dataset Information

Multilayer Strategy for Photoelectrochemical Hydrogen Generation: New Electrode Architecture that Alleviates Multiple Bottlenecks.

Publications

Multilayer Strategy for Photoelectrochemical Hydrogen Generation: New Electrode Architecture that Alleviates Multiple Bottlenecks.

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