Electrocatalytic reduction of nitrogen (N2) at ambient conditions is an alternative strategy to produce ammonia (NH3) to complement the commonly applied Haber–Bosch process. However, the achievement of high Faradaic efficiencies and high NH3 yield is still challenging. Here, Au single sites stabilized on N‐doped porous and highly oxidizing (“noble”) carbon catalysts showing excellent performance in N2 electroreduction are reported. At a potential of −0.2 V versus reversible hydrogen electrode, a stable NH3 yield of 2.32 µg h−1 cm−2 is produced at a Faradaic efficiency of 12.3%. Besides, there is no notable fluctuation of Faradaic efficiency and NH3 yield in six‐cycle test, which indicates good stability. This work opens up new insights to improve N2 fixation performance by introducing catalytically active single sites into noble carbon materials for N2 electroreduction.
Rational design and construction of a multifunctional electrocatalyst featuring with high efficiency and low cost is fundamentally important to realize new energy technologies. Herein, a trifunctional electrocatalyst composed of FePx nanoparticles and Fe–N–C moiety supported on the N‐, P‐codoped carbon (NPC) is masterly synthesized by a facile one‐pot pyrolysis of the mixture of tannic acid, ferrous chloride, and sodium hydrogen phosphate. The synergy of each component in the FePx/Fe–N–C/NPC catalyst renders high catalytic activities and excellent durability toward both oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The electrocatalytic performance and practicability of the robust FePx/Fe–N–C/NPC catalyst are further investigated under the practical operation conditions. Particularly, the overall water splitting cell assembled by the FePx/Fe–N–C/NPC catalyst only requires a voltage of 1.58 V to output the benchmark current density of 10 mA cm−2, which is superior to that of IrO2–Pt/C‐based cell. Moreover, the FePx/Fe–N–C/NPC‐based zinc–air batteries deliver high round‐trip efficiency and remarkable cycling stability, much better than that of Pt/C–IrO2 pair‐based batteries. This work offers a new strategy to design and synthesize highly effective multifunctional electrocatalysts using cheaper tannic acid derived carbon as support applied in electrochemical energy devices.
Electrochemical conversion of CO into fuels using electricity generated from renewable sources helps to create an artificial carbon cycle. However, the low efficiency and poor stability hinder the practical use of most conventional electrocatalysts. In this work, a 2D hierarchical Pd/SnO structure, ultrathin Pd nanosheets partially capped by SnO nanoparticles, is designed to enable multi-electron transfer for selective electroreduction of CO into CH OH. Such a structure design not only enhances the adsorption of CO on SnO , but also weakens the binding strength of CO on Pd due to the as-built Pd-O-Sn interfaces, which is demonstrated to be critical to improve the electrocatalytic selectivity and stability of Pd catalysts. This work provides a new strategy to improve electrochemical performance of metal-based catalysts by creating metal oxide interfaces for selective electroreduction of CO .
Rational designing of the composition and structure of electrode material is of great significance for achieving highly efficient energy storage and conversion in electrochemical energy devices. Herein, MoS2/NiS yolk–shell microspheres are successfully synthesized via a facile ionic liquid‐assisted one‐step hydrothermal method. With the favorable interface effect and hollow structure, the electrodes assembled with MoS2/NiS hybrid microspheres present remarkably enhanced electrochemical performance for both overall water splitting and asymmetric supercapacitors. In particular, to deliver a current density of 10 mA cm−2, the MoS2/NiS‐based electrolysis cell for overall water splitting only needs an output voltage of 1.64 V in the alkaline medium, lower than that of Pt/C–IrO2‐based electrolysis cells (1.70 V). As an electrode for supercapacitors, the MoS2/NiS hybrid microspheres exhibit a specific capacitance of 1493 F g−1 at current density of 0.2 A g−1, and remain 1165 F g−1 even at a large current density of 2 A g−1, implying outstanding charge storage capacity and excellent rate performance. The MoS2/NiS‐ and active carbon‐based asymmetric supercapacitor manifests a maximum energy density of 31 Wh kg−1 at a power density of 155.7 W kg−1, and remarkable cycling stability with a capacitance retention of approximately 100% after 10 000 cycles.
The targeted thermal condensation of a hexaazatriphenylene-based precursor leads to porous and oxidation-resistant ("noble") carbons. Simple condensation of the pre-aligned molecular precursor produces nitrogen-rich carbons with C N-type stoichiometry. Despite the absence of any porogen and metal species involved in the synthesis, the specific surface areas of the molecular carbons reach up to 1000 m g due to the significant microporosity of the materials. The content and type of nitrogen species is controllable by the carbonization temperature whilst porosity remains largely unaffected at the same time. The resulting noble carbons are distinguished by a highly polarizable micropore structure and have thus high adsorption affinity towards molecules such as H O and CO . This molecular precursor approach opens new possibilities for the synthesis of porous noble carbons under molecular control, providing access to the special physical properties of the C N structure and extending the known spectrum of classical porous carbons.
3D PdCu alloy nanosheets exhibit enhanced electrocatalytic activity toward hydrogen evolution reaction and ethanol oxidation reaction in alkaline media. Simultaneous hydrogen and acetate production via a solar-powered cell for ethanol reforming has been fabricated using the nanosheets as bifunctional electrocatalysts. The device is promising for the production of both hydrogen and value-added chemicals using renewable energy.
Ru nanoparticles have been demonstrated to be highly active electrocatalysts for the hydrogen evolution reaction (HER). At present, most of Ru nanoparticles-based HER electrocatalysts with high activity are supported by heteroatom-doped carbon substrates. Few metal oxides with large band gap (more than 5 eV) as the substrates of Ru nanoparticles are employed for the HER. By using large band gap metal oxides substrates, we can distinguish the contribution of Ru nanoparticles from the substrates. Here, a highly efficient Ru/HfO2 composite is developed by tuning numbers of Ru-O-Hf bonds and oxygen vacancies, resulting in a 20-fold enhancement in mass activity over commercial Pt/C in an alkaline medium. Density functional theory (DFT) calculations reveal that strong metal-support interaction via Ru-O-Hf bonds and the oxygen vacancies in the supported Ru samples synergistically lower the energy barrier for water dissociation to improve catalytic activities.
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