Electrocatalytic Hydrogen Evolution Research Articles

Cobalt-doping mediated low-valence Rh centers in rhodium sulfide superconductor for improved electrocatalytic hydrogen evolution

Cobalt-doping mediated low-valence Rh centers in rhodium sulfide superconductor for improved electrocatalytic hydrogen evolution

Molybdenum-tailored perovskite oxides for efficient electrocatalytic hydrogen evolution via B-site engineering in alkaline media

Molybdenum-tailored perovskite oxides for efficient electrocatalytic hydrogen evolution via B-site engineering in alkaline media

Unsymmetrical Bis(thiosemicarbazone) Ligands and Their Nickel(II) Complexes: Synthesis, Characterization and Photocatalytic Activity

The widespread use of organic dyes in industrial processes has led to a considerable release of these compounds into water systems, making the removal of organic contaminants from freshwater a pressing challenge. Photocatalysis, particularly through coordination compounds, presents a promising solution to this problem. In this study, we report the synthesis and characterization of three novel dissymmetric bis(thiosemicarbazone) ligands and their corresponding nickel(II) complexes, which have been extensively analyzed using various techniques. We evaluated the photocatalytic degradation of methyl orange by these nickel complexes, with results demonstrating that they exhibit superior efficiency compared to previously reported nickel-based complexes. Theoretical calculations reveal a correlation between the HOMO–LUMO energy gap and the energies of the involved orbitals. Additionally, with the growing demand for sustainable fuels that do not contribute to greenhouse gas emissions, molecular hydrogen stands out as a promising candidate. Given the potential of bis(thiosemicarbazone) complexes for electrocatalytic hydrogen evolution, we performed preliminary experiments to assess the ability of these nickel complexes to function as photocatalysts for water splitting. The results show that the three nickel complexes successfully generate hydrogen under the tested conditions, although further optimization is necessary to improve hydrogen production efficiency.

Design a functional graphene with decoration of dual transition metal dopants for hydrogen evolution electrocatalysis.

Since hydrogen is a promising alternative to fossil fuels due to its high energy density and environmental friendliness, water electrolysis for hydrogen production has received widespread attentions wherein the development of active and stable catalytic materials is a key research direction. This article designs a dual transition metal doped functional graphene for hydrogen evolution reaction via density functional theory calculations. Among varied combinations, 16 candidates are screened out that are expected to be stable as reflected by the criterion of formation energy Ef < 0 and active due to its free energy of hydrogen adsorption ∆GH within the window of ±0.3 eV. Considering its feasibility in structural modification and electronic adjustment due to the strong dd orbital couplings, the homogeneous dual-atom moiety delivers improved performance toward hydrogen evolution in comparison with the single-atom counterpart. Owing to the good resistance of electrochemical dissolution, the work figures out the potential combinations of Cu2C3N3, Rh2C6, Rh2C3N3 and Rh2N6 endowed with the ∆GH values of -0.03, 0.12, -0.21, and 0.06 eV, respectively, being comparable to the benchmark Pt materials. Therefore, this study provides a new direction for the experimental synthesis of highly active carbon-based electrocatalysts and highlights the well-tuning ability posed by dual-atom interaction.

Platinum/(Carbon-Nanotube) Electrocatalyst Boosts Hydrogen Evolution Reaction in Acidic, Neutral and Alkaline Solutions.

Widely used catalysts for electrocatalytic hydrogen (H2) evolution reaction (HER) have high platinum (Pt) contents and show low efficiencies in neutral and alkaline solutions. Herein, a carbon nanotube (CNT) supported Pt catalyst (Pt/CNT45) with 1 wt.% Pt is fabricated. For HER, the mass activity of Pt/CNT45 in acidic (18.76 A mgPt -1), neutral (3.92 A mgPt -1), and alkaline (3.88 A mgPt -1) solutions is respectively much higher than those on commercial Pt/C catalyst with 20 wt.% Pt (acidic: 0.31 A mgPt -1, neutral: 0.03 A mgPt -1, alkaline: 0.07 A mgPt -1). Thus, Pt/CNT45 enhances HER not only in acidic solutions but also in neutral and alkaline solutions. Ptδ+ at Pt-CNT interface on Pt/CNT45 promotes water (H2O) dissociation and hydroxyl (OH) desorption from Pt/CNT45, thus enhancing HER. This work opens a new way for enhancing HER in a wider pH range by catalyst with low Pt content, and helpful for commercialization.

Size-Controllable High-Entropy Alloys Toward Stable Hydrogen Production at Industrial-Scale Current Densities.

Efficient and stable electrocatalytic hydrogen evolution reaction (HER) at high current densities is highly desirable for industrial-scale hydrogen production, which is yet challenging, because of the electrocatalyst with short lifespans during the acidic HER process. Here, a controllable preparation technique is successfully developed to synthesize PdPtRuRhAu high-entropy alloys (HEAs) of various sizes, within the 3.14nm particles (HEA-3.14) demonstrating exceptional catalytic performance and stable hydrogen production at current densities of -500 and -1000 mA·cm-2 with negligible activity loss over 100h. Theoretical calculations indicate that the bridge adsorption site of Pd-Au serves as an ideal location for HER, with HEA-3.14 possessing the highest proportion of such sites, reaching 18.97%. To further analyze the thermodynamic stability of HEAs, an element-encoding machine learning model is developed from over 300000 preprocessed dataset of HEAs that achieving an impressively low RMSE of 58.6°C and a high R2 value of 0.98. By integrating thermodynamic modeling with machine learning methods, the melting point of the PdPtRuRhAu HEAs at 3.14nm (366°C) is predicted, which aligns well with the results obtained from differential scanning calorimetry tests. This work offers new insights and approaches for designing HEAs that reliably produce hydrogen at high current densities.

Valence State Hydrogen Channel Enhances Sustained and Controllable Electrocatalytic Hydrogen Evolution in Diabetic Skin Wound Healing

Valence State Hydrogen Channel Enhances Sustained and Controllable Electrocatalytic Hydrogen Evolution in Diabetic Skin Wound Healing

Valence State Hydrogen Channel Enhances Sustained and Controllable Electrocatalytic Hydrogen Evolution in Diabetic Skin Wound Healing.

Diabetes significantly increases the risk of serious health issues, including prolonged skin inflammation and delayed wound healing, owing to inferior glucose control and suppression of the immune system. Although traditional hydrogen (H2) therapy is slightly effective, its ability to tailor the release of H2 on the skin is limited. Accordingly, this study proposed a novel strategy for electrocatalytic H2 release under neutral conditions to promote wound healing in diabetic mice and rabbit. Herein, a defect-engineered cobalt phosphide (CoP) catalyst was designed by introducing a neutral single-metal electrocatalytic Hydrogen valence state channel into CoP. By effectively regulating the formation and transfer of *H active species during the CoP catalytic process, a considerable enhancement in neutral electrocatalytic H2 evolution performance was achieved (-78.0 mV@-10.0 mA cm-2). Based on this superior catalytic performance, we developed a flexible electrode (namely, CoP/flexible gold electrode made by screen printing (FGSP) by combining a convenient electrolysis platform with continuous electrolyte supply and FGSP, enabling customized H2 release and accelerating wound healing in diabetic mice and rabbits. Notably, the designed flexible electrode features adjustable dimensions, interchangeable substrates, and material adaptability, meeting the diverse needs of clinical and basic research and demonstrating significant potential for applications in clinical medicine.

Testing mixed metal bimetallic, and monometallic, cryptates for electrocatalytic hydrogen evolution.

Appropriately designed catalysts help to minimise the energy required to convert the energy-poor feedstock H2O into energy-rich molecular H2. Herein, two families of pyridazine-based cryptates, mononuclear [MIILi](BF4)2 and mixed metal dinuclear [MIICuILi](BF4)3 (M = Fe, Co, Cu or Zn; Li is the Schiff base cryptand made by 2 : 3 condensation of tris(2-aminoethyl)amine and 3,6-diformylpyridazine), are investigated as potential electrocatalysts for the hydrogen evolution reaction (HER) in MeCN with acetic acid as the proton source. The synthesis and structures of a new mixed metal cryptate, [ZnIICuILi](BF4)3, and the tetrafluoroborate analogue of the previously reported perchlorate salt of the mono-zinc cryptate, [ZnIILi](BF4)2·0.5H2O, are reported. Electrocatalytic HER testing showed that a deposit forms on the glassy carbon working electrode during electrolysis and it is the active species responsible for the very modest activity observed. The deposits formed by the heterobinuclear cryptates had higher activities (2.0 < TON2h < 3.5) than the deposits formed by the mononuclear cryptates (TON2h < 0.75). But unfortunately the control, using CuI(MeCN)4BF4, had a similar TON2h (2.3) to those seen for the heterobinculear cryptates, which indicates that it is the deposit formed by the CuI cation present in the heterobinuclear cryptates that is likely responsible for the observed, very modest, HER activity.

Covalent Grafting of Graphene Quantum Dots onto Stepped TiO2-Mediated Electronic Modulation for Electrocatalytic Hydrogen Evolution.

The interaction between electrocatalytic active centers and their support is essential to the electrocatalytic performance, which could regulate the electronic structure of the metal centers but requires precise design. Herein, we report on covalent grafting of graphene quantum dots (GQDs) on stepped TiO2 as a support to anchoring cobalt phosphide nanoparticles (CoP/GQD/S-TiO2) for electrocatalytic hydrogen evolution reaction (HER). The covalent ester bonds between GQDs and TiO2 endow enlarged anchoring sites to achieve highly dispersed electroactive CoP nanoparticles but, more importantly, provide an efficient electron-transfer pathway from TiO2 to GQDs which could regulate the electronic structure of CoP. Therefore, such CoP/GQD/S-TiO2 exhibits a superior electrocatalytic HER performance compared with CoP/S-TiO2, exhibiting a mass activity which is 6.3 times that of the CoP/S-TiO2 counterpart and long-term stability over 100 h electrolysis. Mechanistic studies reveal that sufficient electron transfer occurs from TiO2 to the π-conjunction in GQDs via the Ti-C-P pathway and further injects into grafted Co centers, inducing the formation of electron-rich Co centers to enrich and stabilize the hydrated alkaline cations (AC+) for facilitated alkaline HER kinetics. Our study provides a new idea for electronic structure engineering of catalysts via covalent bonding toward boosted electrocatalysis.

Laser Synthesis of Platinum Single-Atom Catalysts for Hydrogen Evolution Reaction.

Platinum (Pt)-based heterogeneous catalysts show excellent performance for the electrocatalytic hydrogen evolution reaction (HER); however, the high cost and earth paucity of Pt means that efforts are being directed to reducing Pt usage, whilst maximizing catalytic efficiency. In this work, a two-step laser annealing process was employed to synthesize Pt single-atom catalysts (SACs) on a MOF-derived carbon substrate. The laser irradiation of a metal-organic framework (MOF) film (ZIF67@ZIF8 composite) by rapid scanning of a ns pulsed infrared (IR; 1064 nm) laser across the freeze-dried MOF resulted in a metal-loaded graphitized film. This was followed by loading this film with chloroplatinic acid (H2PtCl6), followed by further irradiation with an ultraviolet (UV; 355 nm) laser, resulting in pyrolysis of H2PtCl6 to form the SAC, along with a further reduction of the MOF to form a Pt-decorated laser-induced annealed MOF (Pt-LIA-ZIF8@ZIF67). The Pt-LIA-ZIF8@ZIF67 catalyst with a Pt loading of 0.86 wt. % exhibited exceptionally high activity for the HER in acidic conditions. The atomically dispersed Pt on the carbon substrate exhibited a small overpotential of 68.8 mV at 10 mA cm-2 for the hydrogen evolution reaction with a mass activity 20.52 times that of a commercial Pt/C catalyst at an overpotential of 50 mV vs. RHE. Finally, we note that the synthesis method is simple, fast, and versatile, and potentially scalable for the mass production of SACs for electrocatalytic applications.

Growth behavior and electronic regulation of Pt on various Mo-based supports for hydrogen evolution electrocatalysis

Growth behavior and electronic regulation of Pt on various Mo-based supports for hydrogen evolution electrocatalysis

Design and architecture of ZnIn2S4 and ZnIn2S4-based hybrid materials for photocatalytic, electrocatalytic and photoelectrochemical hydrogen evolution

Photocatalytic innovations are routinely employed in the production of hydrogen, remediation of environmental damage, lowering CO2 emissions, and numerous additional critical disciplines because of their sustainability, ease of being implemented,...

CoPc-based donor-acceptor covalent organic frameworks with charge transfer for efficient electrocatalytic oxygen reduction reaction and hydrogen evolution reaction

CoPc-based donor-acceptor covalent organic frameworks with charge transfer for efficient electrocatalytic oxygen reduction reaction and hydrogen evolution reaction

Self-supported electrocatalysts for electrocatalytic hydrogen evolution reaction

Self-supported electrocatalysts for electrocatalytic hydrogen evolution reaction

Size-dependent electrocatalytic hydrogen evolution activity of arrays of edge-like defects in MoS2 crystals patterned by focused ion beam

Introducing surface defects on molybdenum disulfide (MoS2) crystals is important to enhance the electrocatalytic activity toward the hydrogen evolution reaction (HER).

Enhancing electrocatalytic hydrogen evolution via engineering unsaturated electronic structures in MoS2.

The search for efficient, earth-abundant electrocatalysts for the hydrogen evolution reaction (HER) has identified unsaturated molybdenum disulfide (MoS2) as a leading candidate. This review synthesises recent advancements in the engineering of MoS2 to enhance its electrocatalytic properties. It focuses on strategies for designing an unsaturated electronic structure on metal catalytic centers and their role in boosting the efficiency of the hydrogen evolution reaction (HER). It also considers how to optimize the electronic structures of unsaturated MoS2 for enhanced catalytic performance. This review commences with an examination of the fundamental crystal structure of MoS2; it elucidates the classical unsaturated electron configurations and the intrinsic factors that contribute to such electronic structures. Furthermore, it introduces popular strategies for constructing unsaturated electronic structures at the atomic level, such as nanostructure engineering, surface chemical modification and interlayer coupling engineering. It also discusses the challenges and future research directions in the study of MoS2 electronic structures, with the aim of broadening their application in sustainable hydrogen production.

In situ grown Ru-doped Ni(OH)2 nanosheets on nickel foam for stable electrocatalytic hydrogen evolution reaction

Ru/Ni(OH)2–NF was grown in situ on the backbone of nickel foam using a simple one-pot hydrothermal method as an excellent electrocatalyst for HER.

Theoretical screening of multifunctional single-atom catalysts supported by VS2 monolayer for the electrocatalytic hydrogen evolution, oxygen evolution and oxygen reduction reactions

Theoretical screening of multifunctional single-atom catalysts supported by VS2 monolayer for the electrocatalytic hydrogen evolution, oxygen evolution and oxygen reduction reactions

The Electrocatalytic Hydrogen Evolution Performance of Manganese Carbonate in an Acidic Medium

AbstractHydrogen, a sustainable alternative to fossil fuels, can be efficiently produced by electrochemical water splitting, which involves hydrogen evolution reaction (HER) at the cathode and oxygen evolution reaction (OER) at the anode. Both HER and OER require electrocatalysts. The large scale implementation of this technology depends heavily on the development of highly active, stable, and cost‐effective electrocatalysts. In view of this, several electrocatalysts have been explored. Herein, the electrocatalytic hydrogen evolution performance of MnCO3 synthesized by hydrothermal method is reported. While MnCO3 is chosen as the electrocatalyst owing to cost‐effect and abundant precursors, environmental friendliness, and good electrochemical activity, the hydrothermal method is chosen for its simplicity, efficiency, and scalability. The micron size MnCO3 synthesized hydrothermally exhibits η10 of 143 mV, a Tafel slope of 72 mV dec−1 and retains its performance over 3000 cycles and 14 h of continuous operation in 0.5 M H2SO4, demonstrating its utility in sustainable hydrogen production.