Molten Salts‐Driven Discovery of a Polar Mixed‐Anion 3D Framework at the Nanoscale: Zn4Si2O7Cl2, Charge Transport and Photoelectrocatalytic Water Splitting

Author:

Kumar Ram1ORCID,Song Yang1ORCID,Ghoridi Anissa1ORCID,Boullay Philippe2ORCID,Rousse Gwenaelle3ORCID,Gervais Christel1ORCID,Coelho Diogo Cristina4,Kabbour Houria5ORCID,Sassoye Capucine1ORCID,Beaunier Patricia6,Castaing Victor7ORCID,Viana Bruno7ORCID,Luisa Ruiz Gonzalez Maria89ORCID,Calbet José Gonzalez89ORCID,Laberty‐Robert Christel1ORCID,Portehault David1ORCID

Affiliation:

1. Sorbonne Université CNRS Collège de France Laboratoire de Chimie de la Matière Condensée de Paris (CMCP) 4 place Jussieu 75005 Paris France

2. Normandie Université ENSICAEN UNICAEN CNRS CRISMAT 14000 Caen France

3. PSL Research University Sorbonne Université Collège de France Chimie du Solide et de l'Energie UMR 8260 Collège de France 11 place Marcelin Berthelot 75007 Paris France

4. Sorbonne Université CNRS Institut des Matériaux de Paris-Centre IMPC 75005 Paris France

5. Univ. Lille CNRS ENSCL Centrale Lille Univ. Artois UMR 8181-UCCS-Unité de Catalyse et de Chimie du Solide 59000 Lille France

6. Sorbonne Université CNRS Laboratoire de Réactivité de Surface (LRS) 4 place Jussieu 75005 Paris France

7. PSL Research University Chimie ParisTech CNRS Institut de Recherche de Chimie de Paris 11 rue Pierre et Marie Curie 75005 Paris France

8. Departamento de Química Inorgánica Facultad de Químicas Universidad Complutense 28040 Madrid Spain

9. Centro Nacional de Microscopía Electrónica Universidad Complutense 28040 Madrid Spain

Abstract

AbstractMixed‐anion compounds widen the chemical space of attainable materials compared to single anionic compounds, but the exploration of their structural diversity is limited by common synthetic paths. Especially, oxychlorides rely mainly on layered structures, which suffer from low stability during photo(electro)catalytic processes. Herein we report a strategy to design a new polar 3D tetrahedral framework with composition Zn4Si2O7Cl2. We use a molten salt medium to enable low temperature crystallization of nanowires of this new compound, by relying on tetrahedral building units present in the melt to build the connectivity of the oxychloride. These units are combined with silicon‐based connectors from a non‐oxidic Zintl phase to enable precise tuning of the oxygen content. This structure brings high chemical and thermal stability, as well as strongly anisotropic hole mobility along the polar axis. These features, associated with the ability to adjust the transport properties by doping, enable to tune water splitting properties for photoelectrocatalytic H2 evolution and water oxidation. This work then paves the way to a new family of mixed‐anion solids

Funder

Collège de France

H2020 European Research Council

Conseil Régional, Île-de-France

Publisher

Wiley

Subject

General Medicine

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