Search Results (8)

In this study, a sulfur-doped cobalt–iron catalyst (CoFeS/NF) was synthesized on a nickel foam (NF) substrate via a facile one-step electrodeposition method, and its performance in urea electrolysis for hydrogen production was systematically investigated. Sulfur doping induced significant morphology optimization, forming a highly dispersed nanosheet structure, which enhanced the specific surface area increase by 1.9 times compared with the undoped sample, exposing abundant active sites. Meanwhile, the introduction of sulfur facilitated electron redistribution at the surface modulated the valence states of nickel and cobalt, promoted the formation of high-valence Ni³⁺/Co³⁺, optimized the adsorption energy of the reaction intermediates, and reduced the charge transfer resistance. Electrochemical evaluations revealed that CoFeS/NF achieves a current density of 10 mA cm⁻² at a remarkably low potential of 1.18 V for the urea oxidation reaction (UOR), outperforming both the undoped catalyst (1.24 V) and commercial RuO₂ (1.35 V). In addition, the catalyst also exhibited excellent catalytic activity and long-term stability in the total urea decomposition process, which was attributed to the amorphous structure and the synergistic enhancement of corrosion resistance by sulfur doping. This study provides a new idea for the application of sulfur doping strategy in the design of multifunctional electrocatalysts, which promotes the coupled development of urea wastewater treatment and efficient hydrogen production technology. Full article

Accessible and superior electrocatalysts to overcome the sluggish oxygen evolution reaction (OER) are pivotal for sustainable and low-cost hydrogen production through electrocatalytic water splitting. The iron and nickel oxohydroxide complexes are regarded as the most promising OER electrocatalyst attributed to their inexpensive costs, easy preparation, and robust stability. In particular, the Fe-doped NiOOH is widely deemed to be superior constituents for OER in an alkaline environment. However, the facile construction of robust Fe-doped NiOOH electrocatalysts is still a great challenge. Herein, we report the facile construction of Fe-doped NiOOH on Ni(OH)₂ hierarchical nanosheet arrays grown on nickel foam (FeNi@NiA) as efficient OER electrocatalysts through a facile in-situ electrochemical activation of FeNi-based Prussian blue analogues (PBA) derived from Ni(OH)₂. The resultant FeNi@NiA heterostructure shows high intrinsic activity for OER due to the modulation of the overall electronic energy state and the electrical conductivity. Importantly, the electrochemical measurement revealed that FeNi@NiA exhibits a low overpotential of 240 mV at 10 mA/cm² with a small Tafel slope of 62 mV dec⁻¹ in 1.0 M KOH, outperforming the commercial RuO₂ electrocatalysts for OER. Full article

In this work, we synthesize hierarchical In₂S₃/NiFe-layered double hydroxide (In₂S₃/NiFe-LDH) nanoarrays on an F-doped SnO₂ glass substrate via a two-step method, which the In₂S₃ electrode film was firstly prepared using chemical bath deposition on F-doped SnO₂ glass substrate, and then the layered NiFe-LDH was deposited on In₂S₃ electrode film by hydrothermal synthesis. The two-component photoanode In₂S₃/NiFe-LDH exhibits significantly enhanced photoelectrochemical properties compared with the In₂S₃ single-component; due to that, the NiFe-LDH nanosheets depositing on the surface of In₂S₃ nanocrystal can reduce the accumulation of photogenic holes, facilitate the separation of photogenerated charge carriers, and enhance the light response and absorption. After being decorated with the NiFe-LDH nanosheets, the In₂S₃/NiFe-LDH photoanode displays a lower onset potential of 0.06 V and an enhanced photocurrent density as high as 0.30 mA·cm⁻² at the potential of 1.0 V (vs. RHE). Furthermore, it also displays a 90% degradation rate of xylose oxidizing into xylose acid in 3 h under UV light. This work provides a promising approach for designing new heterojunctions applied to biomass degradation. Full article

Oxygen evolution reaction is a momentous part of electrochemical energy storage and conversion devices such as rechargeable metal–air batteries. It is particularly urgent to develop low-cost and efficient electrocatalysts for oxygen evolution reactions. As a potential substitute for noble metal electrocatalysts, transition metal selenides still prove challenging in improving the activity of oxygen evolution reaction and research into reaction intermediates. In this study, a simple one-step solvothermal method was used to prepare a polymetallic compound carbon matrix composite (Co₉Se₈/Ni₃Se₄/Fe₃O₄@C) with a multilayered nanosheets structure. It exhibited good OER activity in an alkaline electrolyte solution, with an overpotential of 268 mV at 10 mA/cm². In addition, this catalyst also showed excellent performance in the 24 h stability test. The composite presents a multi-layer sheet structure, which effectively improves the contact between the active site and the electrolyte. The selenide formed by Ni and Co has a synergistic effect, and Fe₃O₄ and Co₉Se₈ form a heterojunction structure which can effectively improve the reaction activity by initiating the electronic coupling effect through the interface modification. In addition, carbon quantum dots have rich heteroatoms and electron transferability, which improves the electrochemical properties of the composites. This work provides a new strategy for the preparation of highly efficient OER electrocatalysts utilizing the multi-metal synergistic effect. Full article

Carbon dioxide (CO₂) adsorption on decorated graphene (GR) sheets with transition metals (TMs) including iron, nickel and zinc was investigated for removing this hazardous gas from the environment. TM-doped GR results in higher activity toward gas detecting than pristine graphene nanosheets. TM embedding restrains hydrogen evolution on the C sites, leaving more available sites for a CO₂ decrease. The Langmuir adsorption model with ONIOM using CAM-B3LYP functional and LANL2DZ and 6-31+G (d,p) basis sets due to Gaussian 16 revision C.01 program on the complexes of CO₂→(Fe, Ni, Zn) embedded on the GR was accomplished. The changes of charge density illustrated a more considerable charge transfer for Zn-embedded GR. The thermodynamic results from IR spectroscopy indicated that $\Delta {\mathrm{G}}_{\mathrm{ads},\mathrm{CO}2\to \mathrm{Zn}@\mathrm{C}-\mathrm{GR}}^{\mathrm{o}}$ has the notable gap of Gibbs free energy adsorption with a dipole moment which defines the alterations between the Gibbs free energy of the initial compounds ($\Delta {\mathrm{G}}_{\mathrm{CO}2 }^{\mathrm{o}}$ and $\Delta {\mathrm{G}}_{\mathrm{Zn}@\mathrm{C}-\mathrm{GR}}^{\mathrm{o}}$) and product compound ($\Delta {\mathrm{G}}_{\mathrm{CO}2\to \mathrm{Zn}@\mathrm{C}-\mathrm{GR}}^{\mathrm{o}}$) through polarizability. Frontier molecular orbital and band energy gaps accompanying some chemical reactivity parameters represented the behavior of molecular electrical transport of the (Fe, Ni, Zn) embedding of GR for the adsorption of CO₂ gas molecules. Our results have provided a favorable understanding of the interaction between TM-embedded graphene nanosheets and CO₂. Full article

In this research, the ability of transition metals (TM)-doped graphene nanosheets to adsorb the toxic gas CO has been investigated. The Langmuir adsorption model was used, with a three-layered ONIOM, using the CAM-B3LYP functional accompanying the LANL2DZ and 6-31+G (d,p) basis sets, and using the Gaussian 16 revision C.01 program, on the complexes of CO adsorbed on (Fe, Ni, Zn)-doped graphene nanosheets. The order of the changes of charge density for the Langmuir adsorption of CO on Fe-doped, Ni-doped, and Zn-doped graphene nanosheets has been investigated. This shows the greatest change of charge density for the Ni-doped graphene nanosheet. However, based on NMR spectroscopy, sharp peaks around the Ni-doped area on the surface of the graphene nanosheet have been observed. In addition, the Ni-doped graphene nanosheet has a large effect on the bond orbitals of C-Ni in the adsorption of CO, having the maximum occupancy. The values of $\Delta G_{ads}^o$, calculated through IR, showed that $\Delta G_{ads,\mathrm{CO}\to \mathrm{Fe}-\mathrm{doped} \mathrm{GR}}^o$ has the highest value, because of a charge density transfer from the oxygen atom in carbon monoxide to the Fe-doped graphene nanosheet. The frontier molecular orbitals, HOMO and LUMO, and the band energy gap accompanying some chemical reactivity parameters, have revealed the attributes of the molecular electrical transport of (Fe, Ni, Zn)-doped graphene nanosheets for the adsorption of CO. As a result, since a CO molecule interacts simultaneously with a Fe, Ni, or Zn atom and the C-C nanosheet, at first it might be separated, as in this state a CO atom constructs a physical bond with the Fe, Ni, or Zn atom, and then the other could be adsorbed chemically on the C-C nanosheet surface. Finally, our results have shown that a considerable amount of charge transfer occurs between CO molecules and TM-doped graphene nanosheets after adsorption, which suggests that TM-doped graphene is more sensitive and selective to the adsorption of CO than a pristine graphene surface. Full article

Iron-based nanomaterials (NMs) are increasingly used to promote extracellular electron transfer (EET) for energy production in bioelectrochemical systems (BESs). However, the composition and roles of planktonic bacteria in the solution regulated by iron-based NMs have rarely been taken into account. Herein, the changes of the microbial community in the solution by S-doped NiFe₂O₄ anodes have been demonstrated and used for constructing electroactive consortia on normal carbon cloth anodes, which could achieve the same level of electricity generation as NMs-mediated biofilm, as indicated by the significantly high voltage response (0.64 V) and power density (3.5 W m⁻²), whereas with different microbial diversity and connections. Network analysis showed that the introduction of iron-based NMs made Geobacter positively interact with f_Rhodocyclaceae, improving the competitiveness of the consortium (Geobacter and f_Rhodocyclaceae). Additionally, planktonic bacteria regulated by S-doped anode alone cannot hinder the stimulation of Geobacter by electricity and acetate, while the assistance of lining biofilm enhanced the cooperation of sulfur-oxidizing bacteria (SOB) and fermentative bacteria (FB), thus promoting the electroactivity of microbial consortia. This study reveals the effect of S-doped NiFe₂O₄ NMs on the network of microbial communities in MFCs and highlights the importance of globality of microbial community, which provides a feasible solution for the safer and more economical environmental applications of NMs. Full article

Mixed nickel-iron (Ni-Fe) compounds have recently emerged as promising non-precious electrocatalysts for alkaline water splitting. The understanding of the charge-transfer mechanism involved in the multi-step Faradic reaction, however, is still limited for the overall electrochemical process. In this paper, electrochemical impedance spectroscopy (EIS) measurements of Fe incorporated Ni oxide nanosheets were used to study the reaction kinetics for both hydrogen (HER) and oxygen (OER) evolution reactions in alkaline media. Our results showed that Fe incorporation improves the catalytic property of NiO nanosheets because of the lower reaction resistance and faster intermediate transformations. Detailed EIS modeling enables a separation of the surface coverage relaxation from the charge transfer resistance, with an inductive behavior observed in the low-frequency range for HER, holding important information on the dominating reaction mechanism. For OER, the good agreement between the EIS experimental results and a model with an inductance loop indicated that similar inductive behavior would be determining the EIS response at very low frequencies. The physical significance of the elementary steps gives insight into the governing reaction mechanisms involved in the electron and hole charge transfer, as well as the inherent properties of catalysts and their surface coverage relaxation. Full article