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Facile Synthesis of MoP-RuP2 with Abundant Interfaces to Boost Hydrogen Evolution Reactions in Alkaline Media.

ABSTRACT: Exploiting efficient electrocatalysts for hydrogen evolution reactions (HERs) is important for boosting the large-scale applications of hydrogen energy. Herein, MoP-RuP₂ encapsulated in N,P-codoped carbon (MoP-RuP₂@NPC) with abundant interfaces were prepared via a facile avenue with the low-toxic melamine phosphate as the phosphorous resource. Moreover, the obtained electrocatalyst possessed a porous nanostructure, had abundant exposed active sites and improved the mass transport during the electrocatalytic process. Due to the above merits, the prepared MoP-RuP₂@NPC delivered a greater electrocatalytic performance for HERs (50 mV@10 mA cm^-2) relative to RuP₂@NPC (120 mV) and MoP@NPC (195 mV) in 1 M KOH. Moreover, an ultralow potential of 1.6 V was required to deliver a current density of 10 mA cm^-2 in the two-electrode configuration for overall water splitting. For practical applications, intermittent solar energy, wind energy and thermal energy were utilized to drive the electrolyzer to generate hydrogen gas. This work provides a novel and facile strategy for designing highly efficient and stable nanomaterials toward hydrogen production.

SUBMITTER: Chen Z

PROVIDER: S-EPMC8466548 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Nitrogen Functionalization of CVD Grown Three-Dimensional Graphene Foam for Hydrogen Evolution Reactions in Alkaline Media.

Project description:Three-dimensional graphene foam (3D-GrFoam) is a highly porous structure and sustained lattice formed by graphene layers with sp2 and sp3 hybridized carbon. In this work, chemical vapor deposition (CVD)-grown 3D-GrFoam was nitrogen-doped and platinum functionalized using hydrothermal treatment with different reducing agents (i.e., urea, hydrazine, ammonia, and dihydrogen hexachloroplatinate (IV) hydrate, respectively). X-ray photoelectron spectroscopy (XPS) survey showed that the most electrochemically active nitrogen-doped sample (GrFoam3N) contained 1.8 at % of N, and it exhibited a 172 mV dec-1 Tafel plot associated with the Volmer-Heyrovsky hydrogen evolution (HER) mechanism in 0.1 M KOH. By the hydrothermal process, 0.2 at % of platinum was anchored to the graphene foam surface, and the resultant sample of GrFoamPt yielded a value of 80 mV dec-1 Tafel associated with the Volmer-Tafel HER mechanism. Furthermore, Raman and infrared spectroscopy analysis, as well as scanning electron microscopy (SEM) were carried out to understand the structure of the samples.

| S-EPMC8433733 | biostudies-literature

Ruthenium atomically dispersed in carbon outperforms platinum toward hydrogen evolution in alkaline media.

Project description:Hydrogen evolution reaction is an important process in electrochemical energy technologies. Herein, ruthenium and nitrogen codoped carbon nanowires are prepared as effective hydrogen evolution catalysts. The catalytic performance is markedly better than that of commercial platinum catalyst, with an overpotential of only -12?mV to reach the current density of 10?mV?cm-2 in 1?M KOH and -47?mV in 0.1?M KOH. Comparisons with control experiments suggest that the remarkable activity is mainly ascribed to individual ruthenium atoms embedded within the carbon matrix, with minimal contributions from ruthenium nanoparticles. Consistent results are obtained in first-principles calculations, where RuCxNy moieties are found to show a much lower hydrogen binding energy than ruthenium nanoparticles, and a lower kinetic barrier for water dissociation than platinum. Among these, RuC2N2 stands out as the most active catalytic center, where both ruthenium and adjacent carbon atoms are the possible active sites.

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Understanding Cation Trends for Hydrogen Evolution on Platinum and Gold Electrodes in Alkaline Media.

Project description:In this work, we study how the cation identity and concentration alter the kinetics of the hydrogen evolution reaction (HER) on platinum and gold electrodes. A previous work suggested an inverted activity trend as a function of alkali metal cation when comparing the performance of platinum and gold catalysts in alkaline media. We show that weakly hydrated cations (K+) favor HER on gold only at low overpotentials (or lower alkalinity), whereas in more alkaline pH (or high overpotentials), a higher activity is observed using electrolytes containing strongly hydrated cations (Li+). We find a similar trend for platinum; however, the inhibition of HER by weakly hydrated cations on platinum is observed already at lower alkalinity and lower cation concentrations, suggesting that platinum interacts more strongly with metal cations than gold. We propose that weakly hydrated cations stabilize the transition state of the water dissociation step more favorably due to their higher near-surface concentration in comparison to a strongly hydrated cation such as Li+. However, at high pH and consequently higher near-surface cation concentrations, the accumulation of these species at the outer Helmholtz plane inhibits HER. This is especially pronounced on platinum, where a change in the rate-determining step is observed at pH 13 when using a Li+- or K+-containing electrolyte.

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Project description:Owing to its low cost, high conductivity, and chemical stability, Molybdenum phosphide (MoP) has great potential for electrochemically catalyzing the hydrogen evolution reaction (HER). Unfortunately, the development of high-activity MoP still remains a grand challenge in alkali-electrolyzers due to its sluggish water reduction kinetics. Here, we demonstrate a novel strategy for regulating the HER kinetics of the MoP nanowire cathode through partially substituting P atoms with Se dopants. In alkaline solutions, the Se-doped MoP (Se-MoP) nanowire cathode exhibits excellent HER performance with a greatly-decreased overpotential of ∼61 mV at 10 mA cm-2 and a Tafel slope of ∼63 mV dec-1, outperforming currently reported MoP-based electrocatalysts. Experimental and theoretical investigations reveal that Se doping not only facilitates the water dissociation on MoP, but also optimize the hydrogen adsorption free energy, eventually speeding up the sluggish alkaline HER kinetics. Therefore, this work paves a new path for designing MoP-based electrocatalyst with high HER performance in alkaline electrolyzers.

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Project description: Not available

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Nitrogen-Doped Oxygenated Molybdenum Phosphide as an Efficient Electrocatalyst for Hydrogen Evolution in Alkaline Media.

Project description:Phosphides of transition metals (TMPs) are a developing class of materials for hydrogen evolution reaction (HER) as an alternative to expensive noble metals to produce clean energy. Herein, the nitrogen-doped molybdenum oxide (MoOx) is developed via a facile and simple hydrothermal method, followed by annealing in the N2 atmosphere and phosphorization to form a nitrogen-doped oxygenated molybdenum phosphide (N-MoP) sphere-shaped structure. The developed N-doped phosphide structure depicts enhanced HER activity by reaching a current density of 10 mA cm-2 at a very low overpotential of only 87 mV, which is much better than annealed nitrogen-doped molybdenum oxide (A-MoOx) 138 mV in alkaline medium. N-MoP is a highly efficient electrocatalyst for HER attributed to a more exposed surface, large electrode/electrolyte interface and appropriate binding energies for reactants. This study extends the opportunity of developing nitrogen-doped TMPs, which can display exceptional properties as compared to their oxides.

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Unraveling and leveraging in situ surface amorphization for enhanced hydrogen evolution reaction in alkaline media.

Project description:Surface amorphization provides electrocatalysts with more active sites and flexibility. However, there is still a lack of experimental observations and mechanistic explanations for the in situ amorphization process and its crucial role. Herein, we propose the concept that by in situ reconstructed amorphous surface, metal phosphorus trichalcogenides could intrinsically offer better catalytic performance for the alkaline hydrogen production. Trace Ru (0.81 wt.%) is doped into NiPS3 nanosheets for alkaline hydrogen production. Using in situ electrochemical transmission electron microscopy technique, we confirmed the amorphization process occurred on the edges of NiPS3 is critical for achieving superior activity. Comprehensive characterizations and theoretical calculations reveal Ru primarily stabilized at edges of NiPS3 through in situ formed amorphous layer containing bridging S22- species, which can effectively reduce the reaction energy barrier. This work emphasizes the critical role of in situ formed active layer and suggests its potential for optimizing catalytic activities of electrocatalysts.

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AuAgCu trimetallic nanoparticles based alloy: an advanced electrocatalyst for hydrogen evolution reaction in alkaline media.

Project description:Hydrogen production via cost-effective electrochemical water splitting is one of the most promising approaches to confront the energy crisis and to obtain clean fuels with high energy density. To address this concern, herein, we developed a simple one-step synthesis method for creating an AuAgCu trimetallic alloy using aspirin as a capping agent. This alloy shows potential for efficient electrocatalyst for hydrogen evolution reaction. The trimetallic nanoparticles based alloy exhibit an equiaxed grain-like morphology and a face-centred cubic phase. In HER experiments using a 1 M KOH electrolyte, the AuAgCu alloy shows nearly negligible overpotential compared to mono- and bimetallic catalysts, and the Tafel slope was 32.7 mV dec-1, which is the lowest ever achieved for alloy-based electrocatalysts and extremely close to a commercially available Pt/C with high stability for 21 days and no decrease in current density in alkaline media. Besides, with excellent HER activity and stability, the trimetallic AuAgCu-modified electrode possessed significant durability for over 1000 cycles in the selected range of potential from 0.5 to 0.8 V at different scan rates from 1 to 100 mV s-1. This simple, cost-effective and environmentally friendly methodology can pave the way for the exploitation of mixed metal alloy-based electrocatalysts not only for water splitting but also for other applications, such as fuel cells, lithium-ion batteries and supercapacitors.

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Efficient Hydrogen and Oxygen Evolution Catalysis Using 3D-Structured Nickel Phosphosulfide Nanosheets in Alkaline Media.

Project description:Water electrolysis offers a zero-carbon route to generate renewable energy conversion systems. Herein, a self-supported nickel phosphosulfide nanosheet (NS) electrocatalyst was fabricated at a low temperature on carbon cloth, which was then subjected to Ar etching to enhance its catalytic activity. Etching resulted in better hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance than other samples, with overpotentials of 103.1 mV (at 10 mA cm-2) and 278.9 mV (at 50 mA cm-2), respectively. The characterization results confirmed that Ar etching created a thin amorphous layer around the NiPS3 NSs, which increased the number of active sites and modulated their electronic structures. These 3D-structured NiPS3 NSs and their subsequent Ar etching process show promise for applications in overall water splitting in alkaline media.

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Electrochemical Surface Restructuring of Phosphorus-Doped Carbon@MoP Electrocatalysts for Hydrogen Evolution.

Project description:The hydrogen evolution reaction (HER) through electrocatalysis is promising for the production of clean hydrogen fuel. However, designing the structure of catalysts, controlling their electronic properties, and manipulating their catalytic sites are a significant challenge in this field. Here, we propose an electrochemical surface restructuring strategy to design synergistically interactive phosphorus-doped carbon@MoP electrocatalysts for the HER. A simple electrochemical cycling method is developed to tune the thickness of the carbon layers that cover on MoP core, which significantly influences HER performance. Experimental investigations and theoretical calculations indicate that the inactive surface carbon layers can be removed through electrochemical cycling, leading to a close bond between the MoP and a few layers of coated graphene. The electrons donated by the MoP core enhance the adhesion and electronegativity of the carbon layers; the negatively charged carbon layers act as an active surface. The electrochemically induced optimization of the surface/interface electronic structures in the electrocatalysts significantly promotes the HER. Using this strategy endows the catalyst with excellent activity in terms of the HER in both acidic and alkaline environments (current density of 10 mA cm-2 at low overpotentials, of 68 mV in 0.5 M H2SO4 and 67 mV in 1.0 M KOH).

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