Highly Selective Electroreduction of Nitrobenzene to Aniline by Co-Doped 1T-MoS2.

The selective electrocatalytic reduction of nitrobenzene (NB) to aniline demands a desirable cathodic catalyst to overcome the challenges of the competing hydrogen evolution reaction (HER), a higher overpotential, and a lower selectivity. Here, we deposit Co-doped 1T MoS2 on Ti mesh by the solvothermal method with different doping percentages of Co as x % Co-MoS2 (where x = 3, 5, 8, 10, and 12%). Because of the lowest overpotential, lower charge-transfer resistance, strong suppression of the competing HER, and higher electrochemical surface area, 8% Co-MoS2 achieves 94% selectivity of aniline with 54% faradaic efficiency. The reduction process follows first-order dynamics with a reaction coefficient of 0.5 h-1. Besides, 8% Co-MoS2 is highly stable and retains 81% selectivity even after 8 cycles. Mechanistic studies showed that the selective and exothermic adsorption of the nitro group at x % Co-MoS2 leads to a higher rate of NB reduction and higher selectivity of aniline. The aniline product is successfully removed from the solution by polymerization at FTO. This study signifies the impact of doping metal atoms in tuning the electronic arrangement of 1T-MoS2 for the facilitation of organic transformations.

Sn Anodes Protected by Intermetallic FeSn2 Layers for Long-lifespan Sodium-ion Batteries with High Initial Coulombic Efficiency of 93.8.

With a theoretical capacity of 847 mAh g-1 , Sn has emerged as promising anode material for sodium-ion batteries (SIBs). However, enormous volume expansion and agglomeration of nano Sn lead to low Coulombic efficiency and poor cycling stability. Herein, an intermetallic FeSn2 layer is designed via thermal reduction of polymer-Fe2 O3 coated hollow SnO2 spheres to construct a yolk-shell structured Sn/FeSn2 @C. The FeSn2 layer can relieve internal stress, avoid the agglomeration of Sn to accelerate the Na+ transport, and enable fast electronic conduction, which endows quick electrochemical dynamics and long-term stability. As a result, the Sn/FeSn2 @C anode exhibits high initial Coulombic efficiency (ICE=93.8 %) and a high reversible capacity of 409 mAh g-1 at 1 A g-1 after 1500 cycles, corresponding to an 80 % capacity retention. In addition, NVP//Sn/FeSn2 @C sodium-ion full cell shows outstanding cycle stability (capacity retaining rate of 89.7 % after 200 cycles at 1 C).

Asymmetric Activation of the Nitro Group over a Ag/Graphene Heterointerface to Boost Highly Selective Electrocatalytic Reduction of Nitrobenzene.

The electrocatalytic reduction of nitrobenzene to aniline normally faces high overpotential and poor selectivity because of its six-electron redox nature. Herein, a Ag nanoparticles/laser-induced-graphene (LIG) heterointerface was fabricated on polyimide films and employed as an electrode material for an efficient nitrobenzene reduction reaction (NBRR) via a one-step laser direct writing technology. The first-principles calculations reveal that Ag/LIG shows the lowest activation barriers for the NBRR, which could be attributed to the optimum adsorption of the H atom realized by the appropriate interaction between Ag/LIG heterointerfaces and nitrobenzene. As a result, the overpotential of the NBRR is reduced by 217 mV after silver loading, and Ag/LIG shows a high aniline selectivity of 93%. Furthermore, an electrochemical reduction of nitrobenzene in tandem with an electrochemical oxidative polymerization of aniline was designed to serve as an alternative method to remove nitrobenzene from the aqueous solution. This strategy highlights the significance of heterointerfaces for efficient electrocatalysts, which may stimulate the development of novel electrocatalysts to boost the electrocatalytic activity.

Enhanced Electrochemical Performance of Aprotic Li-CO2 Batteries with a Ruthenium-Complex-Based Mobile Catalyst.

Li-CO2 batteries are regarded as next-generation high-energy-density electrochemical devices. However, the greatest challenge arises from the formation of the discharge product, Li2 CO3 , which would accumulate and deactivate heterogenous catalysts to cause huge polarization. Herein, Ru(bpy)3 Cl2 was employed as a solution-phase catalyst for Li-CO2 batteries and proved to be the most effective one screened so far. Spectroscopy and electrochemical analyses elucidate that the RuII center could interact with both CO2 and amorphous Li2 C2 O4 intermediate, thus promoting electroreduction process and delaying carbonate transformation. As a result, the charge potential is reduced to 3.86 V and over 60 discharge/charge cycles are achieved with a fixed capacity of 1000 mAh g-1 at a current density of 300 mA g-1 . Our work provides a new avenue to improve the electrochemical performance of Li-CO2 batteries with efficient mobile catalysts.

Self-Supported NaTi2(PO4)3 Nanorod Arrays: Balancing Na+ and Electron Kinetics via Optimized Carbon Coating for High-Power Sodium-Ion Capacitor.

The NaTi2(PO4)3 (NTP) anode materials exhibit high Na+ diffusion dynamics; carbon-based materials can effectively improve its limited electronic conductivity. However, the low Na+ diffusion of NTP/C composite materials from inhomogeneous carbon mixing or uncontrollable carbon coating cannot keep up with fast electron transfer, leading to undesirable electrochemical performances. Herein, a uniform and controllable carbon layer is designed on the self-supported-coated NTP nanorod arrays with binder-free (NTP@C NR) to improve Na+ and electron kinetics simultaneously. As a result, the NTP@C NR electrodes possess initial coulombic efficiency (ICE = 97%), good rate capabilities (89.1 mA h g-1 at 100 C), and stability with ≈78.4% of capacity retention rate at even 30 C over 1200 cycles. The sodium-ion capacitors with NTP@C NR as an anode and commercially activated carbon as a cathode exhibit ∼9180.0 W kg-1 of power density at 10 A g-1 and super high retention of ≈94.5% at 1 A g-1 over 7000 cycles. This work will help balance transport kinetics between the ion and electron for materials applied in storage devices.