RESUMEN
The electrocatalytic nitrogen reduction reaction (NRR) is a crucial process in addressing energy shortages and environmental concerns by synthesizing the NH3. However, the difficulty of N2 activation and fewer NRR active sites limit the application of NRR. Therefore, the NRR performance can be improved by rapid electron transport paths to participate in multi-electron reactions and N2 activation. Doping with transition metal element is a viable strategy to provide electrons and electronic channels in the NRR. This study focuses on the synthesis of Fe2(MoO4)3 (FeMo) and x%La-doped FeMo (x = 3, 5, 7, and 10) using the hydrothermal method. La-doping creates electron transport channels Fe2+-O2--Fe3+ and oxygen vacancies, achieving an equal molar ratio of Fe2+/Fe3+. This strategy enables the super-exchange in Fe2+-O2--Fe3+, and then enhances electron transport speed for a rapid hydrogenation reaction. Therefore, the synergistic effect of Fe2+/Fe3+ cycling and oxygen vacancies improves the NRR performance. Notably, 5%La-FeMo demonstrates the superior NRR performance (NH3 yield rate: 29.6 µg h-1 mgcat-1, Faradaic efficiency: 5.8%) at -0.8 V (vs. RHE). This work analyzes the influence of the catalyst electronic environment on the NRR performance based on the effect on different valence states of ions on electron transport.
RESUMEN
The achievement of the outstanding theoretical capacitance of nickel sulfide (NiS2 ) is challenging due to its low conductivity, slow electrochemical kinetics, and poor structural stability. In this study, we utilize polyaniline (PANI) as a linker to anchor the NiS2 with a hollow bowl-like structure, uniformly dispersed at the surface of graphene oxide (GO)(NiS2 @15PG). The presence of PANI provides growth sites, resulting in a uniform and dense arrangement of NiS2 . This morphological modulation of NiS2 increases the contact area between the active material to electrolyte. Additionally, PANI effectively connects NiS2 with the conductive network of GO, which advances the electrical conductivity and ion diffusion properties. As a result, the Rct (charge transfer resistance) and Zw (Warburg impedance) of NiS2 @15PG decrease by 82.61 % and 66.76 % respectively. This unique structure confers NiS2 @15PG with high specific capacitance (536.13â C g-1 at 1â A g-1 ) and excellent multiplicative property of 60.93 % at 20â A g-1 . The assembled NiS2 @15PG//YP-50 supercapacitors (HSC) demonstrates an energy density (13.09â Wh kg-1 ) at a high-power density (16â kW kg-1 ). The capacity retention after 10,000 cycles at 5â A g-1 is 86.59 %, indicating its significant potential for practical applications.
RESUMEN
Construction of S-scheme heterojunction is an efficient strategy to enhance photocatalytic efficiency. Besides the retained redox ability, the wide work function gap and intimate interface contact are essential for efficient degradation. Nontoxic magnesium oxide (MgO) with two dimensional (2D) structures and high work function is a potential material for S-scheme photocatalysts. Herein, MgO was used to in-situ grown on graphitic carbon nitride (g-C3N4) for constructing the strongly connected MgO/g-C3N4 S-scheme photocatalyst with tight Mg-N bonds. Meanwhile, the presence of Mg-N bonds induces the formation of oxygen vacancy in MgO, which enhances the Fenton-like degradation. Furthermore, the Mg-N bond promotes the charge migration between MgO and g-C3N4. Consisting of the enhanced Fenton-like process and photocatalysis, the MgO/g-C3N4 shows a higher photo-Fenton degradation activity (80.01%) for degradation of organic pollutants (Rhodamine B, 100 mg L-1) in water, than g-C3N4 (28.46%) and MgO (55.64%). Therefore, the interfacial chemical bonds in heterojunction photocatalysts provide an efficient strategy for further enhancing the photocatalysis of S-scheme photocatalysts.