Electrochemical conversion of nitrate to ammonia offers an efficient approach to reducing nitrate pollutants and a potential technology for low-temperature and low-pressure ammonia synthesis. However, the process is limited by multiple competing reactions and NO3− adsorption on cathode surfaces. Here, we report a Fe/Cu diatomic catalyst on holey nitrogen-doped graphene which exhibits high catalytic activities and selectivity for ammonia production. The catalyst enables a maximum ammonia Faradaic efficiency of 92.51% (−0.3 V(RHE)) and a high NH3 yield rate of 1.08 mmol h−1 mg−1 (at − 0.5 V(RHE)). Computational and theoretical analysis reveals that a relatively strong interaction between NO3− and Fe/Cu promotes the adsorption and discharge of NO3− anions. Nitrogen-oxygen bonds are also shown to be weakened due to the existence of hetero-atomic dual sites which lowers the overall reaction barriers. The dual-site and hetero-atom strategy in this work provides a flexible design for further catalyst development and expands the electrocatalytic techniques for nitrate reduction and ammonia synthesis.

Carbon-coated SiO 2 /TiO 2 (SiO 2 /TiO 2 @C) nanosheets consisting of TiO 2 nanoparticles uniformly embedded in SiO 2 matrix and a carbon-coating layer are fabricated by using acidified titanosilicate JDF-L1 nanosheets as template and precursor. SiO 2 /TiO 2 @C has unique structural features of sheetlike nanostructure, ultrafine TiO 2 nanoparticles distributed in SiO 2 matrix, and carbon coating, which can expedite ion diffusion and electron transfer and relieve volume expansion efficiently, and thus, the synergetic combination of these advantages significantly enhances its Li storage capability. As anode of lithium-ion batteries (LIBs), SiO 2 /TiO 2 @C nanosheets exhibit a high capacity of 998 mAh g −1 at 100 mA g −1 after 100 cycles. Moreover, an ultrahigh capacity of 410 mAh g −1 retains at 2000 mA g −1 after 400 cycles. A mixed reaction mechanism of capacitance and diffusioncontrolled intercalation is revealed by qualitative and quantitative analysis.

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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Metal-organic frameworks have been widely studied in the separation of C 2 hydrocarbons, which usually preferentially bind unsaturated hydrocarbons with the order of acetylene (C 2 H 2 ) > ethylene (C 2 H 4 ) > ethane (C 2 H 6 ). Herein, we report an ultramicroporous fluorinated metal-organic framework Zn-FBA (H 2 FBA = 4,4'-(hexafluoroisopropylidene)bis(benzoic acid)), shows a reversed adsorption order characteristic for C 2 hydrocarbons, that the uptake for C 2 hydrocarbons of the framework and the binding affinity between the guest molecule and the framework follows the order C 2 H 6 > C 2 H 4 > C 2 H 2 . Density-functional theory calculations confirm that the completely reversed adsorption order behavior is attributed to the close van der Waals interactions and multiple cooperative CÀ H•••F hydrogen bonds between the framework and C 2 H 6 . Moreover, Zn-FBA exhibits a high selectivity of about 2.9 for C 2 H 6 over C 2 H 4 at 298 K and 1 bar. The experimental breakthrough studies show that the high-purity C 2 H 4 can be obtained from C 2 H 6 and C 2 H 4 mixtures in one step.

Heteroatom-doped three-dimensional (3D) carbon fiber networks have attracted immense interest because of their extensive applications in energy-storage devices. However, their practical production and usage remain a great challenge because of the costly and complex synthetic procedures. In this work, flexible B, N, and O heteroatom-doped 3D interconnected carbon microfiber networks (BNOCs) with controllable pore sizes and elemental contents were successfully synthesized via a facile one-step “chemical vapor etching and doping” method using cellulose-made paper, the most abundant and cost-effective biomass, as an original network-frame precursor. Under a rational design, the BNOCs exhibited interconnected microfiber-network structure as expressways for electron transport, spacious accessible surface area for charge accumulation, abundant mesopores and macropores for rapid inner-pore ion diffusion, and lots of functional groups for additional pseudocapacitance. Being applied as binder-free electrodes for supercapacitors, BNOC-based supercapacitors not only revealed a high specific capacitance of 357 F g–1, a high capacitance retention of 150 F g–1 at 200 A g–1, a high energy density of 12.4 W h kg–1, and a maximum power density of 300.6 kW kg–1 with an aqueous electrolyte in two-electrode configuration but also exhibited a high specific capacitance of up to 242.4 F g–1 in an all-solid-state supercapacitor.

Hollow MoS2 nanospheres with enhanced energy storage performance has been synthesized from core–shell ZnS@MoS2 nanostructures.

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