Faculty Publications
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Item In situ vanadophosphomolybdate impregnated into conducting polypyrrole for supercapacitor(Elsevier Ltd, 2020) Anandan Vannathan, A.A.; Maity, S.; Kella, T.; Shee, D.; Das, P.P.; Mal, S.S.The fast modernization and advancement in lifestyle increase the consumption of power daily due to all innovative technologies, e.g., hybrid vehicles, solar cells, smart power grid, communication devices, artificial hearts, etc. Conducting organic polymer-based energy storage devices had attracted much attention due to the conductive nature for a long time. However, its application has been restricted because of swelling and shrinking capability during the charge and discharge cycle. The combination of redox-active inorganic metal oxides, such as polyoxometalates (multi-metal oxide cluster) with conduction polymers, could enhance the material's stability due to its fast multi-electron redox property. Here, we report the two polypyrroles combined vanadophosphomolybdates, namely PPy-H4[PVMo11O40] and PPy-H5[PV2Mo10O40] nanohybrid electrode materials. The PPy-H5[PV2Mo10O40] electrode material behaves as pseudocapacitance and can deliver an excellent capacitance of 561.1 F/g in 0.1 M H2SO4 electrolyte solution at a 0.2 A/g current density, indicating capacitive composite material. The electrochemical impedance spectroscopy (EIS) reveals that PPy-H5[PV2Mo10O40] is more capacitive than PPy-H4[PVMo11O40] and PPy with equivalent series resistance (ESR) of 5.74 ?. The cell capacitance of PPy-H5[PV2Mo10O40] and PPy-H4[PVMo11O40] are found to be 5.38 and 9.15 mF, stipulating in small SC cell application. Likewise, the PPy-H5[PV2Mo10O40] nanohybrid electrode shows better responsive behavior with a relaxation time of 0.16 ms. Furthermore, the PPy-H5[PV2Mo10O40] electrode exhibits outstanding cycle stability, retaining ~95% of its capacitance after 4500 cycles as compare to PPy-H4[PVMo11O40] (~91%) electrode. © 2020Item One-Pot Synthesis of Polyoxometalate Decorated Polyindole for Energy Storage Supercapacitors(American Chemical Society, 2021) Anandan Vannathan, A.A.; Kella, T.; Shee, D.; Mal, S.S.The demand for energy storage supercapacitor devices has increased interest in completing all innovative technologies and renewable energy requirements. Here, we report a simple method of two polyoxomolybdate (H4[PVMo11O40] and H5[PV2Mo10O40]) doped polyindole (PIn) composites for electrochemical supercapacitors. The interactions between polyoxomolybdates and PIn were measured by Fourier transform infrared spectroscopy (FTIR), and powder XRD, and stability was measured by thermogravimetry. The field emission scanning microscopy (FESEM) was employed to investigate the morphology of the materials. The electrochemical measurements show that the PIn/PV2Mo10 electrode exhibits a higher capacitance of 198.09 F/g with an energy density of 10.19 Wh/kg and a power density of 198.54 W/kg at 0.2 A/g current density than the PIn/PVMo11 electrode. Both electrodes show a pseudocapacitance behavior due to the doping of redox-active polyoxomolybdates on the PIn surface and enhance the electrochemical properties. The electrodes' capacitive nature was measured by electrochemical impedance spectroscopy (EIS), which shows that the PIn/PVMo11 electrode has a resistive nature within the electrode-electrode interface. Moreover, the PIn/PV2Mo10 electrode offers remarkable cycle stability, retaining ?84% of its capacitance after 10,000 cycles (?83% for the PIn/PVMo11 electrode). The higher specific capacitance, faster charge/discharge rates, and higher cycle stability make them promising electrodes in supercapacitors. ©Item Activated carbon- supported Vanado-nickelate (IV) based hybrid materials for energy application(Elsevier Ltd, 2021) Maity, S.; BM, N.; Kella, T.; Shee, D.; Das, P.P.; Mal, S.S.The rapid development of supercapacitor (SC) technology leads to increased demand for nanofabrication of novel and effective electroactive hybrid materials for next-generation energy storage devices. Herein, nickel tetradecavanadate, K2H5[NiV14O40](NiV14), is doped into porous activated carbon (AC), for the first time, in different wt.% in order to investigate the homogeneous loading of the inorganic metal-oxide component on the AC matrix. The resulting complex, AC-NiV14, is found to have possessed an enhanced electrochemical characteristic (for both symmetric and asymmetric SC cell), which operates at a significantly higher potential of 1.2 V. The combination of the double-layer capacitance (EDLC) and the redox-active polyoxometalate cluster leads to an intrinsic increase in specific capacitance (capacity) (from 45.3 Fg?1 (54.4 Cg?1) for AC to 316 Fg?1 (379.2 Cg?1) for 15 wt.% AC-NiV14 at a current density of 1 Ag?1). It was also observed that there is an increase of 20% in the operating voltage compared to conventional AC supercapacitors with acidic aqueous electrolytes. Firstly, symmetric supercapacitor's electrochemical performances of various wt.% of NiV14 composition were studied in acidic aqueous electrolyte (0.5 M H2SO4) solution. We observed that the 15 wt.% of AC-NiV14 hybrid electrode showed remarkable specific energy value (~63.2 Wh kg?1) compared with pristine AC and NiV14 electrodes, separately. Besides, the asymmetric layout (AC//AC-NiV14) increased the potential window up to 1.5 V and enhanced the specific energy and power values (90.1 Whkg?1 and 2400 Wkg?1, respectively), with 98% coulombic efficiency. Meanwhile, the AC-NiV14//NiV14 asymmetric cell possesses a specific capacitance (capacity) of 375 Fg?1 (450 Cg?1) with a maximum power of 3140 Wkg?1 at the high current density of 2 Ag?1. © 2021 Elsevier LtdItem Organic cation linkers polyoxomolybdate-polypyrrole nanocomposite-based supercapacitors(Springer Science and Business Media Deutschland GmbH, 2021) Muhammed Anees, P.K.; Anandan Vannathan, A.; Kella, T.; Shee, D.; Mal, S.A few new hybrid electrode materials have been synthesized and immobilized for the next-generation energy storage device. The hybrid electrodes PVMo11-TBA, PVMo11-BTA, PVMo11-TBP, PVMo11-TBA-PPy, PVMo11-BTA-PPy, and PVMo11-TBP-PPy were well characterized by NMR, XRD, FTIR, FESEM, BET, and tested for electrochemical performance. Among these hybrid electrode materials, the PVMo11-TBA-PPy electrode shows a high specific capacitance of 144.37 F/g at a 1A/g current density and incredible power and energy density of 1100.16 W/kg and 15.28 Wh/kg, respectively. The high electrode’s capacitance was due to the synergistic effect between the PPy and TBA-PVMo11 and high ionic diffusion compared with other synthesized electrodes. It also exhibited high cycle stability of 72.78% after 4500 cycles at 1 M H2SO4 electrolyte. The EIS offers a lower ESR value of 0.72 ohms for the PVMo11-TBA-PPy than PVMo11-TBA, indicating the rapid charge/discharge rate. On the other hand, the PVMo11-BTA-PPy and PVMo11-TBP-PPy electrodes showed lower capacitance values of 26.98 and 19.53. F/g at 0.4 and 1 A/g current density, respectively. Lowering the capacitance could be the prevention of the interaction of organic cations with the counter polyanion. © 2021, The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.Item Electrochemical performance of activated carbon-supported vanadomolybdates electrodes for energy conversion(Elsevier Ltd, 2021) Maity, S.; Anandan Vannathan, A.; Kella, T.; Shee, D.; Das, P.P.; Mal, S.Reinforcing polyoxomolybdates (POMs) into the activated carbon (AC) template engenders a nanohybrid electrode material for high-performance supercapacitor applications. Herein, a first-time novel integration of two polyoxometalates ([PVMo11O40]4-, [PV2Mo10O40]5-) with AC has been demonstrated, and their structural and electrochemical performances were analyzed. AC-VMo11 composite displayed an enhanced capacitance of 450 Fg-1 with an improved energy density of 59.7 Whkg-1. Furthermore, the symmetric supercapacitor cell for AC-VMo11 and AC-V2Mo10 showed high cell capacitances of 38.8 and 20.01 mF, respectively, alongside 99.99% capacitance retention of over 5000 cycles. In addition, the influence of ionic liquid as an electrolyte on AC-V2Mo10 based supercapacitor cell was investigated in tetrabutylammonium bromide (TBAB) electrolyte solution. © 2021 Elsevier Ltd and Techna Group S.r.l.Item Selective dehydration of 1-butanol to butenes over silica supported heteropolyacid catalysts: Mechanistic aspect(Elsevier B.V., 2021) Kella, T.; Vennathan, A.A.; Dutta, S.; Mal, S.; Shee, D.Butenes are considered as important olefinic building block to produce fuels/fuel additives and commodity chemicals. In the present investigation, selective dehydration of 1-butanol to butenes was studied in a continuous-flow fixed-bed reactor using various silica-supported heteropolyacid (HPA) catalysts such as phosphotungstic acid (PTA), silicotungstic acid (STA), phosphomolybdic acid (PMA), and silicomolybdic acid (SMA) as the solid acid catalysts. The physicochemical properties of these HPA were determined by BET, powder XRD, FTIR, NH3-TPD, and Py-FTIR. The acid strength and Brønsted/Lewis (B/L) acid ratio were increased with higher loading of HPA on silica. The nature of HPA (addenda and hetero atom) and loading of HPA are important factors for the dehydration of 1-butanol and selectivity towards butenes. PTA and STA showed superior catalytic activity than PMA and SMA. The reaction temperature and WHSV also strongly affected the butanol conversion and selectivity of butenes. The selectivity of di-n?butyl ether decreases with the rising temperature from 523 K to 623 K. The isomerization of 1-butene leading to the formation of other butene isomers depends on the HPA loading, temperature, and WHSV. The presence of molybdenum addendum atom in PMA and SMA promotes dehydrogenation and hydrogenation, leading to the formation of various light hydrocarbons. The 20PTA/SiO2 catalyst afforded 99.8% selectivity towards butenes at quantitative conversion of 1-butanol, whereas the 20STA/SiO2 catalyst gave nearly 97.0% conversion of 1-butanol and 99.9% butenes selectivity at 673 K, 37.4 h?1 of WHSV. © 2021Item Imidazolium cation linkers of polyoxomolybdate-polypyrrole nanocomposite electrode-based energy storage supercapacitors(Elsevier Ltd, 2022) Muhammed Anees, P.K.; Anandan Vannathan, A.A.; Abhijith, M.B.; Kella, T.; Shee, D.; Mal, S.S.The electrochemical properties of a new hybrid electrode, liquid-polyoxometalate-polypyrrole (BMIM-PVMo11-PPy) have been studied. The H4[PVMo11O40] (PVMo11) was combined with 1-Butyl-3-methyl-imidazolium (BMIM) ionic liquid and then doped on the polypyrrole (PPy) surface. In order to investigate the interaction between the BMIM, PVMo11, and PPy compound was characterized using various analytical techniques, such as Infrared spectroscopy, thermal stability analysis, powder X-ray diffraction, multinuclear NMR (1H and 13C), FESEM, EDX, and surface adsorption studies. The electrochemical performance of the BMIM-PVMo11-PPy composite material has been tested in an aqueous 0.25 M H2SO4 electrolytic solution. The BMIM-PVMo11-PPy composite exhibits the highest specific capacitance of 527.39 F g−1 at a current density of 1 A g−1, along with remarkable specific energy and power of 51.07 Wh kg−1 and 1078.96 W kg−1, respectively. The BMIM-PVMo11-PPy composite was observed to light up red and blue color LED bulbs for 66 and 16 s, respectively, with 84 mg of sample coated on carbon cloth, suggesting an incredible specific power of that material. © 2021 Elsevier B.V.Item Investigations of redox-active polyoxomolybdate embedded polyaniline-based electrode material for energy application(Springer Science and Business Media Deutschland GmbH, 2022) Anandan Vannathan, A.A.; Kella, T.; Shee, D.; Mal, S.S.Higher capacitance supercapacitors have received considerable attention, including their massive power density, high stability, and long cycle life. On the other hand, polymers have been known for their energy storage device application because of the pseudocapacitance behavior resulting from the extended conjugation over the polymer backbone. Here, we report a simple chemical bath deposition method for the synthesis of two polyoxometalates (H4[PVMo11O40] and H5[PV2Mo10O40]) impregnated polyaniline (PAni) composite (PVMo11@PAni and PV2Mo10@PAni) for electrochemical supercapacitors. Various analytical methods characterized the electrode materials, e.g., Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), powder X-ray diffraction (PXRD) method, and the morphological features of those electrodes were acquired by field emission scanning microscopy (FESEM). The exceptionally high average capacitance of 1371 F g−1 was obtained for the composite PVMo11@PAni electrode at a 3 A g−1 current density and 1 V potential window with an energy density of 137.5 W h kg−1. The PVMo11@PAni composite electrode showed almost 4.3 times the higher energy density than pure PAni and 2.3 times higher than PV2Mo10@PAni. In contrast, PV2Mo10@PAni composite showed 1.9 times more energy density than pure PAni composite electrode. Interestingly, high average capacitance, charge–discharge rates, and high energy density with high-level power delivery make them promising electrode candidates for supercapacitors. © 2021, The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.Item High-performance electrochemical supercapacitors based on polyoxometalate integrated into polyaniline and activated carbon nanohybrid(Springer Science and Business Media Deutschland GmbH, 2023) Anandan Vannathan, A.A.; Kella, T.; Shee, D.; Mal, S.S.Polyaniline (PANI) and carbonaceous materials and metallic compounds have played a significant role in energy storage and conversion devices. PANI has demonstrated tremendous potential in the supercapacitor industry due to its high specific capacitance, high flexibility, and economical price. The CPs damage the hierarchical structure during the charging and discharging process and start swelling. Thus, incorporating polyoxometalates (POMs) into the conducting polymer matrix increases the stability of the electrode material. Here, we have demonstrated a comparative study of two newly synthesized composite materials consisting of K5H2[PV4W8O40] ·11H2O, (PV4W8) POM incorporated into two different supports, such as pseudocapacitive polyaniline (PANI) and EDLC activated carbon (AC) matrix. It was observed that the PANI-PV4W8 composite exhibited excellent capacitance nature at 0.5 M H2SO4 electrolyte solution than AC-PV4W8. The PANI-PV4W8 composite demonstrated the specific capacitance of 584 F g−1 at 0.8 A g−1. The composite also exhibited energy and power density of 81Wh kg−1 and 1598 W kg−1, respectively. Besides, the composite shows 93.13% capacity retention after 4500 cycles by cyclic voltammetry measurement at a 500 mV s−1 scan rate. Furthermore, the AC-PV4W8 showed a specific capacitance of 62 F g−1 at the current density of 0.6 A g−1. Interestingly, The PANI-PV4W8 composite could glow up the red and yellow LED bulb for more than a minute, suggesting a promising electrode material for practical supercapacitor purposes. © 2023, The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.