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.
Document Type: | Article |
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Author: | Mana Abdirahman MohamedORCiD, Stefanie ArnoldORCiD, Oliver JankaORCiD, Antje QuadeORCiD, Volker PresserORCiD, Guido KickelbickORCiD |
URN: | urn:nbn:de:bsz:291:415-5739 |
DOI: | https://doi.org/10.1002/cssc.202202213 |
ISSN: | 1864-564X |
Parent Title (English): | ChemSusChem |
Volume: | 16 |
First Page: | e202202213 |
Language: | English |
Year of first Publication: | 2023 |
Release Date: | 2023/04/11 |
Tag: | continuous synthesis; electrodes; inorganic-organic hybrid materials; lithium-ion batteries; polyoxometalates |
Impact: | 07.50 (2023) |
Funding Information: | German Science Foundation. Grant Numbers 256/349-1, 256/506-1 |
Scientific Units: | Energy Materials |
DDC classes: | 500 Naturwissenschaften und Mathematik / 540 Chemie |
Open Access: | Open Access |
Signature: | INM 2023/027 |
Licence (German): | Creative Commons - CC BY-NC-ND - Namensnennung - Nicht kommerziell - Keine Bearbeitungen 4.0 International |