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Self-Activation of Inorganic-Organic Hybrids Derived through Continuous Synthesis of Polyoxomolybdate and para-Phenylenediamine Enables Very High Lithium-Ion Storage Capacity

  • Inorganic-organic hybrid materials with redox-active components were prepared by an aqueous precipitation reaction of ammonium heptamolybdate (AHM) with para-phenylenediamine (PPD). A scalable and low-energy continuous wet chemical synthesis process, known as the microjet process, was used to prepare particles with large surface area in the submicrometer range with high purity and reproducibility on a large scale. Two different crystalline hybrid products were formed depending on the ratio of molybdate to organic ligand and pH. A ratio of para-phenylenediamine to ammonium heptamolybdate from 1 : 1 to 5 : 1 resulted in the compound [C6H10N2]2[Mo8O26] ⋅ 6 H2O, while higher PPD ratios from 9 : 1 to 30 : 1 yielded a composition of [C6H9N2]4[NH4]2[Mo7O24] ⋅ 3 H2O. The electrochemical behavior of the two products was tested in a battery cell environment. Only the second of the two hybrid materials showed an exceptionally high capacity of 1084 mAh g−1 at 100 mA g−1 after 150 cycles. The maximum capacity was reached after an induction phase, which can be explained by a combination of a conversion reaction with lithium to Li2MoO4 and an additional in situ polymerization of PPD. The final hybrid material is a promising material for lithium-ion battery (LIB) applications.

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Document Type:Article
Author:Mana Abdirahman MohamedORCiD, Stefanie ArnoldORCiD, Oliver JankaORCiD, Antje QuadeORCiD, Volker PresserORCiD, Guido KickelbickORCiD
Parent Title (English):ChemSusChem
First Page:e202202213
Year of first Publication:2023
Release Date:2023/04/11
Tag:continuous synthesis; electrodes; inorganic-organic hybrid materials; lithium-ion batteries; polyoxometalates
Impact:09.140 (2021)
Funding Information:German Science Foundation. Grant Numbers 256/349-1, 256/506-1
DDC classes:500 Naturwissenschaften und Mathematik / 540 Chemie
Open Access:Open Access
Signature:INM 2023/027
Licence (German):License LogoCreative Commons - CC BY-NC-ND - Namensnennung - Nicht kommerziell - Keine Bearbeitungen 4.0 International