Flow-Chemistry Based Green Synthesis of Graphene Oxide at Minutes Timescale.

Graphene oxide (GO) is broadly investigated in the electrochemical field. However, for industrial applications, it still suffer from high pollution, low efficiency, poor production quality, and safety concerns associated with traditional synthesis methods. Herein, guided by theoretical analyses, a new oxygen-atom-transfer (OAT) mechanism for periodate oxidizing graphite is revealed, exhibiting controllable reaction activity, strong orbital interaction, and abundant electron transfer. Moreover, a flow chemistry strategy with high mass/heat transfer rates is designed to enhance interlayer diffusion and reaction dynamics between oxidants and graphite, ensuring the efficient synthesis of GO within several minutes. As a result, both low oxygen-content GO with large size, and high oxygen-content GO with adequate active sites can be precisely and safely synthesized. Benefitting from the controllability of oxygen content and lateral size, the as-prepared GO sheets can be facilely assembled into fiber/film electrodes that present high mechanical flexibility, large electrical conductivity, and outstanding electrochemical performance.

Microfluidic Synthesis of Multifunctional Micro-/Nanomaterials from Process Intensification: Structural Engineering to High Electrochemical Energy Storage.

Multifunctional micro-/nanomaterials featuring functional superiority and high value-added physicochemical nature have received immense attention in electrochemical energy storage. Microfluidic synthesis has become an emergent technology for massively producing multifunctional micro-/nanomaterials with tunable microstructure and morphology due to its rapid mass/heat transfer and precise fluid controllability. In this review, the latest progresses and achievements in microfluidic-synthesized multifunctional micro-/nanomaterials are summarized via reaction process intensification, multifunctional micro-/nanostructural engineering and electrochemical energy storage applications. The reaction process intensification mechanisms of various micro-/nanomaterials, including quantum dots (QDs), metal materials, conducting polymers, metallic oxides, polyanionic compounds, metal-organic frameworks (MOFs) and two-dimensional (2D) materials, are discussed. Especially, the multifunctional structural engineering principles of as-fabricated micro-/nanomaterials, such as vertically aligned structure, heterostructure, core-shell structure, and tunable microsphere, are introduced. Subsequently, the electrochemical energy storage application of as-prepared multifunctional micro-/nanomaterials is clarified in supercapacitors, lithium-ion batteries, sodium-ion batteries, all-vanadium redox flow batteries, and dielectric capacitors. Finally, the current problems and future forecasts are illustrated.

Microfluidic Printing of Vertically-Oriented Nanosheets/MOFs Hetero-Interface for Intensive Pseudocapacitive Storage.

Efficient manufacture of electroactive vertically-oriented nanosheets with enhanced electrolyte mass diffusion and strong interfacial redox dynamics is critical for realizing high energy density of miniature supercapacitor (SC), but still challenging. Herein, microfluidic droplet printing is developed to controllably construct vertically-oriented graphene/ZIF-67 hetero-microsphere (VAGS/ZIF-67), where the ZIF-67 is coordinately grown on vertically-oriented graphene framework via Co─O─C bonds. The VAGS/ZIF-67 shows ordered porous channel, high electroactivity and strong interfacial interaction, providing rapid electrolyte diffusion dynamics and high faradaic capacitance in KOH solution (1674 F g-1 , 1004 C g-1 ), which are verified by computational fluid dynamics (CFD) and density functional theory (DFT). Moreover, the VAGS/ZIF-67 based SC exhibits large energy density (100 Wh kg-1 ), excellent durability (10 000 cycles and high/low temperature), and robust power-supply applications in portable electronics.

A Novel Bubble-based Microreactor for Enhanced Mass Transfer Dynamics toward Efficient Electrocatalytic Nitrogen Reduction.

Electrocatalytic nitrogen reduction reaction (eNRR) is a promising method for sustainable ammonia production. Although the majority of studies on the eNRR are devoted to developing efficient electrocatalysts, it is critical to study the influence of mass transfer because of the poor N2 transfer efficiency. Herein, a novel bubble-based microreactor (BBMR) is proposed that efficiently promotes the mass transfer behavior during the eNRR using microfluidic strategies. The BBMR possesses abundant triphasic interfaces and provides spatial confinement and accurate potential control, ensuring rapid mass transfer dynamics and improved eNRR performance, as confirmed by experimental and simulation studies. The ammonia yield of the reaction over Ag nanoparticles can be enhanced to 31.35 µg h-1 mgcat. -1, which is twice that of the H-cell. Excellent improvements are also achieved using Ru/C and Fe/g-CN catalysts, with 5.0 and 8.5 times increase in ammonia yield, respectively. This work further demonstrates the significant effect of mass transfer on the eNRR performance and provides an effective strategy for process enhancement through electrode design.