Differential supercapacitor and Schottky diode behaviours in two new isostructural coordination polymers based on redox active metal ions

Chhatan Das; Subhrajyoti Debnath; Vishwas D. Patel; Dhritiman Gupta; Anjan Banerjee; Partha Mahata

doi:10.1039/d3ce00883e

Differential supercapacitor and Schottky diode behaviours in two new isostructural coordination polymers based on redox active metal ions

Chhatan Das, Subhrajyoti Debnath, Vishwas D. Patel, Dhritiman Gupta, Anjan Banerjee, Partha Mahata

Research output: Contribution to journal › Article › peer-review

Abstract

Two new isostructural 2D coordination polymers, denoted 1(Mn) and 2(Fe), have been synthesized using the layer diffusion method. These polymers, {[Mn(PDA)(4-bpdb)(H₂O)₂]·4-bpdb}_n and {[Fe(PDA)(4-bpdb)(H₂O)₂]·4-bpdb}_n, incorporated 1,4-phenylenediacetate (PDA) and 1,4-bis(4-pyridyl)-2,3-diaza-1,3-butadiene (4-bpdb) ligands. Structural analysis through the single-crystal X-ray study revealed that compound 1(Mn) and compound 2(Fe) exhibited a one-dimensional connectivity along the a-axis between metal ions (Mn(ii)/Fe(ii)) and 1,4-phenylenediacetate ligands and formed a 2D layered structure interconnected with 4-bpdb. These layers are arranged in an AAA… pattern along the b-axis, forming a three-dimensional supramolecular structure. Non-bonded 4-bpdb molecules occupy voids within this arrangement, stabilized by hydrogen bonds and π⋯π interactions. The redox-active metal centers (Mn²⁺/Fe²⁺) present in the coordination polymers hold promise for electrochemical studies. Supercapacitor assessment revealed an intriguing discrepancy: compound 1(Mn) demonstrated nearly 2.5 times greater specific capacitance than compound 2(Fe) in a 1 M H₂SO₄ medium, despite their isostructural nature. However, cyclic stability testing showed a reverse trend, with compound 2(Fe) exhibiting excellent stability, retaining 98% capacity after 5000 cycles compared to 1(Mn)'s 78%. Conductivity measurements indicated that compound 1(Mn) possesses conductivity 10 times superior to that of compound 2(Fe). Notably, both compounds exhibited potential for Schottky diode fabrication. Overall, this study highlights the influence of specific metal ions on distinctive supercapacitor characteristics and conductivity within isostructural coordination polymers.

Original language	English
Pages (from-to)	6343-6353
Number of pages	11
Journal	CrystEngComm
Volume	25
Issue number	45
DOIs	https://doi.org/10.1039/d3ce00883e
State	Published - 21 Oct 2023
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2023 The Royal Society of Chemistry.

Funding

This work was supported by UGC-BSR Research Start-Up-Grant (No. F.30-471/2019(BSR)) [PM] of UGC, Government of India. P. Mahata thanks Jadavpur University for RUSA sponsored project (Ref. No.: R-11/106/19). C. Das thanks CSIR, the Government of India for an SRF fellowship (File No: 09/096(0951)/2018-EMR-I). A. Banerjee thanks the Science and Engineering Research Board (SERB), India (File No: SRG/2019/000296) and the University Grants Commission (UGC), India (No. F.30-509/(BSR)) for research grants. S. Debnath thanks the Council of Scientific and Industrial Research (CSIR), India for JRF (File No: 08/0155(12174)/2021-EMR-I). V. D. Patel thanks VIT for Contingency fund for carrying out the experiments.

Funders	Funder number
Jadavpur University	09/096(0951)/2018-EMR-I, R-11/106/19
Vellore Institute of Technology, Chennai
Council of Scientific and Industrial Research, India	08/0155(12174)/2021-EMR-I
University Grants Commission	F.30-471/2019, F.30-509/(BSR)
Science and Engineering Research Board	SRG/2019/000296

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title = "Differential supercapacitor and Schottky diode behaviours in two new isostructural coordination polymers based on redox active metal ions",

abstract = "Two new isostructural 2D coordination polymers, denoted 1(Mn) and 2(Fe), have been synthesized using the layer diffusion method. These polymers, {[Mn(PDA)(4-bpdb)(H2O)2]·4-bpdb}n and {[Fe(PDA)(4-bpdb)(H2O)2]·4-bpdb}n, incorporated 1,4-phenylenediacetate (PDA) and 1,4-bis(4-pyridyl)-2,3-diaza-1,3-butadiene (4-bpdb) ligands. Structural analysis through the single-crystal X-ray study revealed that compound 1(Mn) and compound 2(Fe) exhibited a one-dimensional connectivity along the a-axis between metal ions (Mn(ii)/Fe(ii)) and 1,4-phenylenediacetate ligands and formed a 2D layered structure interconnected with 4-bpdb. These layers are arranged in an AAA… pattern along the b-axis, forming a three-dimensional supramolecular structure. Non-bonded 4-bpdb molecules occupy voids within this arrangement, stabilized by hydrogen bonds and π⋯π interactions. The redox-active metal centers (Mn2+/Fe2+) present in the coordination polymers hold promise for electrochemical studies. Supercapacitor assessment revealed an intriguing discrepancy: compound 1(Mn) demonstrated nearly 2.5 times greater specific capacitance than compound 2(Fe) in a 1 M H2SO4 medium, despite their isostructural nature. However, cyclic stability testing showed a reverse trend, with compound 2(Fe) exhibiting excellent stability, retaining 98% capacity after 5000 cycles compared to 1(Mn)'s 78%. Conductivity measurements indicated that compound 1(Mn) possesses conductivity 10 times superior to that of compound 2(Fe). Notably, both compounds exhibited potential for Schottky diode fabrication. Overall, this study highlights the influence of specific metal ions on distinctive supercapacitor characteristics and conductivity within isostructural coordination polymers.",

author = "Chhatan Das and Subhrajyoti Debnath and Patel, {Vishwas D.} and Dhritiman Gupta and Anjan Banerjee and Partha Mahata",

note = "Publisher Copyright: {\textcopyright} 2023 The Royal Society of Chemistry.",

year = "2023",

month = oct,

day = "21",

doi = "10.1039/d3ce00883e",

language = "אנגלית",

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T1 - Differential supercapacitor and Schottky diode behaviours in two new isostructural coordination polymers based on redox active metal ions

AU - Das, Chhatan

AU - Debnath, Subhrajyoti

AU - Patel, Vishwas D.

AU - Gupta, Dhritiman

AU - Banerjee, Anjan

AU - Mahata, Partha

PY - 2023/10/21

Y1 - 2023/10/21

N2 - Two new isostructural 2D coordination polymers, denoted 1(Mn) and 2(Fe), have been synthesized using the layer diffusion method. These polymers, {[Mn(PDA)(4-bpdb)(H2O)2]·4-bpdb}n and {[Fe(PDA)(4-bpdb)(H2O)2]·4-bpdb}n, incorporated 1,4-phenylenediacetate (PDA) and 1,4-bis(4-pyridyl)-2,3-diaza-1,3-butadiene (4-bpdb) ligands. Structural analysis through the single-crystal X-ray study revealed that compound 1(Mn) and compound 2(Fe) exhibited a one-dimensional connectivity along the a-axis between metal ions (Mn(ii)/Fe(ii)) and 1,4-phenylenediacetate ligands and formed a 2D layered structure interconnected with 4-bpdb. These layers are arranged in an AAA… pattern along the b-axis, forming a three-dimensional supramolecular structure. Non-bonded 4-bpdb molecules occupy voids within this arrangement, stabilized by hydrogen bonds and π⋯π interactions. The redox-active metal centers (Mn2+/Fe2+) present in the coordination polymers hold promise for electrochemical studies. Supercapacitor assessment revealed an intriguing discrepancy: compound 1(Mn) demonstrated nearly 2.5 times greater specific capacitance than compound 2(Fe) in a 1 M H2SO4 medium, despite their isostructural nature. However, cyclic stability testing showed a reverse trend, with compound 2(Fe) exhibiting excellent stability, retaining 98% capacity after 5000 cycles compared to 1(Mn)'s 78%. Conductivity measurements indicated that compound 1(Mn) possesses conductivity 10 times superior to that of compound 2(Fe). Notably, both compounds exhibited potential for Schottky diode fabrication. Overall, this study highlights the influence of specific metal ions on distinctive supercapacitor characteristics and conductivity within isostructural coordination polymers.

AB - Two new isostructural 2D coordination polymers, denoted 1(Mn) and 2(Fe), have been synthesized using the layer diffusion method. These polymers, {[Mn(PDA)(4-bpdb)(H2O)2]·4-bpdb}n and {[Fe(PDA)(4-bpdb)(H2O)2]·4-bpdb}n, incorporated 1,4-phenylenediacetate (PDA) and 1,4-bis(4-pyridyl)-2,3-diaza-1,3-butadiene (4-bpdb) ligands. Structural analysis through the single-crystal X-ray study revealed that compound 1(Mn) and compound 2(Fe) exhibited a one-dimensional connectivity along the a-axis between metal ions (Mn(ii)/Fe(ii)) and 1,4-phenylenediacetate ligands and formed a 2D layered structure interconnected with 4-bpdb. These layers are arranged in an AAA… pattern along the b-axis, forming a three-dimensional supramolecular structure. Non-bonded 4-bpdb molecules occupy voids within this arrangement, stabilized by hydrogen bonds and π⋯π interactions. The redox-active metal centers (Mn2+/Fe2+) present in the coordination polymers hold promise for electrochemical studies. Supercapacitor assessment revealed an intriguing discrepancy: compound 1(Mn) demonstrated nearly 2.5 times greater specific capacitance than compound 2(Fe) in a 1 M H2SO4 medium, despite their isostructural nature. However, cyclic stability testing showed a reverse trend, with compound 2(Fe) exhibiting excellent stability, retaining 98% capacity after 5000 cycles compared to 1(Mn)'s 78%. Conductivity measurements indicated that compound 1(Mn) possesses conductivity 10 times superior to that of compound 2(Fe). Notably, both compounds exhibited potential for Schottky diode fabrication. Overall, this study highlights the influence of specific metal ions on distinctive supercapacitor characteristics and conductivity within isostructural coordination polymers.

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Differential supercapacitor and Schottky diode behaviours in two new isostructural coordination polymers based on redox active metal ions

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