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Soluble Complexes of Cobalt Oxide Fragments Bring the Unique CO2Photoreduction Activity of a Bulk Material into the Flexible Domain of Molecular Science

Publicated to:Journal Of The American Chemical Society. 143 (49): 20769-20778 - 2021-12-15 143(49), DOI: 10.1021/jacs.1c08817

Authors: Zhang, Guanyun; Baranov, Mark; Wang, Fei; Poblet, Josep M; Kozuch, Sebastian; Leffler, Nitai; Shames, Alexander, I; Clemente-Juan, Juan M; Neyman, Alevtina; Weinstock, Ira A

Affiliations

Ben Gurion Univ Negev, Dept Chem, IL-84105 Beer Sheva, Israel - Author
Ben Gurion Univ Negev, Dept Phys, IL-84105 Beer Sheva, Israel - Author
Ben Gurion Univ Negev, Ilse Katz Inst Nanoscale Sci & Technol, IL-84105 Beer Sheva, Israel - Author
Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, Tarragona, 43007, Spain - Author
Department of Chemistry, The Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev, Beer Sheva, 84105, Israel - Author
Department of Physics, Ben-Gurion University of the Negev, Beer Sheva, 84105, Israel - Author
Instituto de Ciencia Molecular (ICMol), Universidad de Valencia, Paterna, 46980, Spain - Author
Univ Rovira & Virgili, Dept Quim Fis & Inorgan, Tarragona 43007, Spain - Author
Univ Valencia, Inst Ciencia Mol ICMol, Paterna 46980, Spain - Author
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Abstract

The deposition of metal oxides is essential to the fabrication of numerous multicomponent solid-state devices and catalysts. However, the reproducible formation of homogeneous metal oxide films or of nanoparticle dispersions at solid interfaces remains an ongoing challenge. Here we report that molecular hexaniobate cluster anion complexes of structurally and electronically distinct fragments of cubic-spinel and monoclinic Co3O4 can serve as tractable yet well-defined functional analogues of bulk cobalt oxide. Notably, the energies of the highest-occupied and lowest-unoccupied molecular orbitals (HOMO and LUMO) of the molecular complexes, 1, closely match the valence- and conduction-band (VB and CB) energies of the parent bulk oxides. Use of 1 as a molecular analogue of the parent oxides is demonstrated by its remarkably simple deployment as a cocatalyst for direct Z-scheme reduction of CO2 by solar light and water. Namely, evaporation of an aqueous solution of 1 on TiO2-coated fluorinated tin oxide windows (TiO2/FTO), immersion in wet acetonitrile, and irradiation by simulated solar light under an atmosphere of CO2 give H2, CO, and CH4 in ratios nearly identical to those obtained using 20 nm spinel-Co3O4 nanocrystals, but 15 times more rapidly on a Co basis and more rapidly overall than other reported systems. Detailed investigation of the photocatalytic properties of 1 on TiO2/FTO includes confirmation of a direct Z-scheme charge-carrier migration pathway by in situ irradiated X-ray photoelectron spectroscopy. More generally, the findings point to a potentially important new role for coordination chemistry that bridges the conceptual divide between molecular and solid-state science. ©

Keywords
catalystco3o4efficientnanocrystalsnanomaterialsphotocatalystsreductionsemiconductorwater oxidationBulk materialsCarbon dioxideCobalt compoundsCoordination reactionsDeposition of metalsEnergyFluorinated tin oxidesInterface statesMagnetic-propertiesMetal nanoparticlesMetal-oxideMetalsMolecular orbitalsMolecular scienceMulticomponentsOxide filmsPhoto reductionPhotocatalytic activitySolid-state devicesSoluble complexesTin oxidesTitanium dioxideX ray photoelectron spectroscopy

Quality index

Bibliometric impact. Analysis of the contribution and dissemination channel

The work has been published in the journal Journal Of The American Chemical Society due to its progression and the good impact it has achieved in recent years, according to the agency WoS (JCR), it has become a reference in its field. In the year of publication of the work, 2021, it was in position 16/179, thus managing to position itself as a Q1 (Primer Cuartil), in the category Chemistry, Multidisciplinary. Notably, the journal is positioned above the 90th percentile.

From a relative perspective, and based on the normalized impact indicator calculated from World Citations provided by WoS (ESI, Clarivate), it yields a value for the citation normalization relative to the expected citation rate of: 2.07. This indicates that, compared to works in the same discipline and in the same year of publication, it ranks as a work cited above average. (source consulted: ESI Nov 14, 2024)

This information is reinforced by other indicators of the same type, which, although dynamic over time and dependent on the set of average global citations at the time of their calculation, consistently position the work at some point among the top 50% most cited in its field:

  • Weighted Average of Normalized Impact by the Scopus agency: 2.74 (source consulted: FECYT Feb 2024)
  • Field Citation Ratio (FCR) from Dimensions: 4.68 (source consulted: Dimensions Apr 2025)

Specifically, and according to different indexing agencies, this work has accumulated citations as of 2025-04-30, the following number of citations:

  • WoS: 28
  • Scopus: 31
  • Europe PMC: 1
  • Google Scholar: 25
Impact and social visibility

From the perspective of influence or social adoption, and based on metrics associated with mentions and interactions provided by agencies specializing in calculating the so-called "Alternative or Social Metrics," we can highlight as of 2025-04-30:

  • The use, from an academic perspective evidenced by the Altmetric agency indicator referring to aggregations made by the personal bibliographic manager Mendeley, gives us a total of: 27.
  • The use of this contribution in bookmarks, code forks, additions to favorite lists for recurrent reading, as well as general views, indicates that someone is using the publication as a basis for their current work. This may be a notable indicator of future more formal and academic citations. This claim is supported by the result of the "Capture" indicator, which yields a total of: 27 (PlumX).

With a more dissemination-oriented intent and targeting more general audiences, we can observe other more global scores such as:

  • The Total Score from Altmetric: 2.
  • The number of mentions on the social network Facebook: 1 (Altmetric).
  • The number of mentions on the social network X (formerly Twitter): 3 (Altmetric).
Leadership analysis of institutional authors

This work has been carried out with international collaboration, specifically with researchers from: Israel.