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1.
Small ; : e2406113, 2024 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-39279593

RESUMEN

Fabrication of cost-effective and robust metal-based electrocatalysts for hydrogen evolution reactions (HER) across the entire pH range has garnered significant attention in harvesting renewable energy. Herein, the fabrication of 3D high-surface Ni Foam-Graphene-Carbon Nanotubes (NGC) decorated with phosphorous-inserted tin selenide (SnSe-P) showcases unprecedented HER activity with minimal overpotentials across all pH ranges (52 mV in acidic, 93 mV in basic, and 198 mV in neutral conditions@10 mA cm-2) and stability at 1 A cm-2 for 72 h. The as-designed catalyst shows a low overpotential of 122 mV@10 mA cm-2 in alkaline seawater, achieved through controlled electronic distribution on Sn site after incorporation of P in NGC-SnSe-P. A stable cell voltage of 1.56 V@10 mA cm⁻2 is achieved for prolonged time in 1 m KOH toward overall water electrolysis. Experimental and theoretical investigation reveals that the insertion of P in layered SnSe enables s orbitals of H* and p orbitals of Sn to interact, favoring the adsorption of the H* intermediate. A renewable approach is adopted by using silicon solar cells (η = 10.66%) to power up the electrolyzer, yielding a solar-to-hydrogen (STH) conversion efficiency of 7.70% in 1 m KOH and 5.65% in alkaline seawater, aiming toward green hydrogen production.

2.
ACS Appl Mater Interfaces ; 16(20): 26899-26914, 2024 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-38741334

RESUMEN

The extreme sensitivity of 2D-layered materials to environmental adsorbates, which is typically seen as a challenge, is harnessed in this study to fine-tune the material properties. This work investigates the impact of environmental adsorbates on electrical properties by studying metal-semiconductor-metal (MSM) devices fabricated on CVD-synthesized SnSe flakes. The freshly prepared devices exhibit positive photoconductivity (PPC), whereas they gradually develop negative photoconductivity (NPC) after being exposed to an ambient environment for ∼1 day. While the photodetectors based on positive photoconductivity exhibit a responsivity and detectivity of 6.1 A/W and 5.06 × 108 Jones, the same for the negative photoconductivity-based photodetector reaches up to 36.3 A/W and 1.49 × 109 Jones, respectively. In addition, the noise-equivalent power of the NPC photodetector decreases by 300 times as compared to the PPC device, which implies a prominent detection capability of the NPC device against weak photo signals. To substantiate the hypothesis that negative photoconductivity stems from the photodesorption of water and oxygen molecules on the dangling bonds of SnSe flakes, the flakes are etched along the most active planes (010) with a focused laser beam in an inert environment, which enhances responsivity by 43%, supporting negative photoconductivity linked to photodesorption. Furthermore, the humidity-dependent dark current variation of the NPC photodetectors is used to design a humidity sensor for human respiration monitoring with faster response and recovery times of 0.72 and 0.68 s, respectively. These findings open up the possibility of tuning the photoelectrical response of layered materials in a facile manner to develop future sensors and optoelectronic multifunctional devices.

3.
Small ; 20(14): e2306756, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38126960

RESUMEN

For an uninterrupted self-powered network, the requirement of miniaturized energy storage device is of utmost importance. This study explores the potential utilization of phosphorus-doped nickel oxide (P-NiO) to design highly efficient durable micro-supercapacitors. The introduction of P as a dopant serves to enhance the electrical conductivity of bare NiO, leading to 11-fold augmentation in volumetric capacitance to 841.92 Fcm-3 followed by significant enhancement of energy and power density from 6.71 to 42.096 mWhcm-3 and 0.47 to 1.046 Wcm-3, respectively. Theoretical calculations used to determine the adsorption energy of OH- ions, revealing higher in case of bare NiO (1.52 eV) as compared to phosphorus-doped NiO (0.64 eV) leading to high electrochemical energy storage performance. The as-designed micro-supercapacitor (MSC) device demonstrates a facile integration with the photovoltaic system for renewable energy storage and smooth transfer to external loads for enlightening the blue LED for ≈1 min. The choice of P-NiO/Ni not only contributes to cost reduction but also ensures minimal lattice mismatch at the interface facilitating high durability up to 15 K cycles along with capacitive retention of ≈100% and coulombic efficiency of 93%. Thus, the heterostructure unveils the possibilities of exploring miniaturized energy storage devices for portable electronics.

4.
Small ; 19(50): e2304399, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37626463

RESUMEN

Water splitting via an uninterrupted electrochemical process through hybrid energy storage devices generating continuous hydrogen is cost-effective and green approach to address the looming energy and environmental crisis toward constant supply of hydrogen fuel in fuel cell driven automobile sector. The high surface area metal-organic framework (MOF) driven bimetallic phosphides (ZnP2 @CoP) on top of CNT-carbon cloth matrix is utilized as positive and negative electrodes in energy storage devices and overall water splitting. The as-prepared positive electrode exhibits excellent specific capacitances/capacity of 1600 F g-1 /800 C g-1 @ 1A g-1 and the corresponding hybrid device reveals an energy density of 83.03 Wh kg-1 at power density of 749.9 W kg-1 . Simultaneously, the electrocatalytic performance of heterostructure shows overpotentials of 90 mV@HER and 204 mV@OER at current density of 10 and 20 mA cm-2 , respectively in alkaline electrocatalyzer. Undoubtedly, it shows overall water splitting with low cell voltage of 1.53 V@10 mA cm-2 having faradic and solar-to-hydrogen conversion efficiency of 98.81% and 9.94%, respectively. In addition, the real phase demonstration of the overall water-splitting is performed where the electrocatalyzer is connected with a series of hybrid supercapacitor devices powered up by the 6 V standard silicon solar panel to produce uninterrupted green H2 .

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