Developing efficient electrocatalysts for alkaline water electrolysis is central to substantial progress of alkaline hydrogen production. Herein, a Ni5P4 electrocatalyst incorporating single‐atom Ru (Ni5P4‐Ru) is synthesized through the filling of Ru3+ species into the metal vacancies of nickel hydroxides and subsequent phosphorization treatment. Electron paramagnetic resonance spectroscopy, X‐ray‐based measurements, and electron microscopy observations confirm the strong interaction between the nickel‐vacancy defect and Ru cation, resulting in more than 3.83 wt% single‐atom Ru incorporation in the obtained Ni5P4‐Ru. The Ni5P4‐Ru as an alkaline hydrogen evolution reaction catalyst achieves low onset potential of 17 mV and an overpotential of 54 mV at a current density of 10 mA cm‐2 together with a small Tafel slope of 52.0 mV decade‐1 and long‐term stability. Further spectroscopy analyses combined with density functional theory calculations reveal that the doped Ru sites can cause localized structure polarization, which brings the low energy barrier for water dissociation on Ru site and the optimized hydrogen adsorption free energy on the interstitial site, well rationalizing the experimental reactivity.
The ambiguous mechanism of electrocatalysts for oxygen evolution reaction (OER) greatly hinders their industrial applications towards renewable and clean energy conversion. Here, we elaborately prepared cobalt sulfide catalyst to give...
Isolated dual transition metal atoms (Ni and Fe) were uniformly embedded into graphitic carbon nitrideviaa metal–Nxbond, resulting in highly efficient catalytic activity due to the electronic structure reconfiguration.
Aqueous zinc (Zn) ion energy devices have demonstrated remarkable significance as a substitute of their lithium counterparts. Developing cheap and nontoxic electrode active materials is crucial for maximizing the storage of Zn ions. As a new star of 2D materials, MXenes can pose unique layered structure and abundant surface chemistry, largely benefiting the surface storage of ions. Herein, carbon nanotube (CNT) delaminated V2C MXene (DV2C@CNT) has been demonstrated, as a promising electrode for high‐performance Zn‐ion supercapacitor. The as‐prepared DV2C@CNT electrodes display favorable electrochemical activity with reversible proton (H+) and Zn ion (Zn2+) co‐insertion/extraction process in ZnSO4 solutions. Due to the superior conductive network formed by CNT, the delaminated MXene exhibit a high specific capacity of 190.2 F g−1 at 0.5 A g−1 with excellent rate performance and durability. More interestingly, the characterizations clearly reveal that zinc hydroxide sulfate hydrate nanoflakes can immediately precipitate onto the electrode even at the initial assembly process, which can be ascribed to the spontaneous formation of the electrostatic field in the primary battery. The operando X‐ray absorption spectroscopic measurements further confirm the dynamic hydrate precipitation during charging/discharging cycles, offering a better understanding of energy storage mechanism in Zn‐ion devices with MXene electrodes.
Hydrogen production from electrochemical water splitting is very promising but still challenging. In article number 1906972, Li Song and co‐workers develop nickel phosphide nanocatalysts incorporated with single‐atomic noble metal for highly efficient alkaline water electrolysis. The doped metallic sites can cause localized structure polarization, largely promoting the hydrogen evolution from phosphide catalysts.
Molybdenum disulfide (MoS 2 ) has attracted much attention as a promising alternative to Pt-based catalysts for highly efficient hydrogen generation. However, it suffers sluggish kinetics for driving the hydrogen evolution reaction (HER) process because of inert basal planes, especially in alkaline solution. Here, we show a combination of heteroatom doping and phase transformation strategies to engineer the inplane structure of MoS 2 , that trigger their catalytic activities. Systematic characterizations are performed with advanced aberration-corrected microscopy and X-ray techniques, indicating that an as-designed MoS 2 catalyst has a distorted zigzagchain superlattice in metallic phase, while its in-plane structure was engineered via the incorporation of cobalt and oxygen species. The optimal Co, O dual-doped metallic phase molybdenum disulfide (1T-MoS 2 ) electrocatalyst shows a significantly enhanced HER activity with a low overpotential of 113 mV at 10 mA cm −2 and corresponding small Tafel slope of 50 mV dec −1 , accompanied by the robust stability in alkaline media. The calculated turnover frequency is higher than 6.65 H 2 s −1 at an overpotential of 200 mV. More indepth insights from the first-principle calculations illustrate that the water dissociation as a rate-determining step was largely accelerated by the in-plane Co−O−Mo species and fast electron transfer of the catalyst. Benefiting from ingenious design and fine identifications, this work provides a fundamental understanding of the relationships among heteroatom doping, phase transformation, and performance for MoS 2 -based catalysts.
Buffer reactions can forwardly boycott the changes induced by external causes. Here, we demonstrate a significant buffer role of tiny Mn in a self-optimized cathode for aqueous Zn-ion battery. Our...
Ammonia borane (AB) is regarded as a highly promising candidate for chemical hydrogen-storage materials. Developing low-cost yet efficient catalysts for the dehydrogenation of AB is central to achieving hydrogen conversion. Here a heterostructure of Ni/Ni 2 P nanoparticles deposited on a defective carbon framework for the hydrolysis of AB is developed by elaborately controlling phosphorization conditions. The electronic structure and interfacial interaction of the ternary components are probed by synchrotron-based X-ray absorption fine structure and further simulated via density functional theory. By adjusting the content of Ni and Ni 2 P in the hetrostructure, the optimized hybrid exhibits catalytic performance of H 2 generation from the hydrolysis of AB under ambient conditions with a turnover frequency of 68.3 mol (H 2 ) mol −1 (Cat) min −1 and an activation energy (E a ) of 44.99 kJ mol −1 , implying its high potential as an efficient supplement for noble-metal-based catalysts in hydrogen energy applications.
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