Mechanical and chemical degradations of high-capacity anodes, resulting from lithiationinduced stress accumulation, volume expansion and pulverization, and unstable solidelectrolyte interface formation, represent major mechanisms of capacity fading, limiting the lifetime of electrodes for lithium-ion batteries. Here we report that the mechanical degradation on cycling can be deliberately controlled to finely tune mesoporous structure of the metal oxide sphere and optimize stable solid-electrolyte interface by high-rate lithiationinduced reactivation. The reactivated Co 3 O 4 hollow sphere exhibits a reversible capacity above its theoretical value (924 mAh g À 1 at 1.12 C), enhanced rate performance and a cycling stability without capacity fading after 7,000 cycles at a high rate of 5.62 C. In contrast to the conventional approach of mitigating mechanical degradation and capacity fading of anodes using nanostructured materials, high-rate lithiation-induced reactivation offers a new perspective in designing high-performance electrodes for long-lived lithium-ion batteries.
Large-area freestanding graphene papers (GPs) are fabricated by electrospray deposition integrated with a continuous roll-to-roll process. Upon mechanical compaction and thermal annealing, GPs can achieve a thermal conductivity of as high as 1238.3-1434 W m(-1) K(-1) . The super-thermally conductive GPs display an outstanding heat-spread ability and are more efficient in removing hot spots than Cu and Al foils.
Flexible graphene paper (GP) pillared by carbon black (CB) nanoparticles using a simple vacuum filtration method is developed as a high-performance electrode material for supercapacitors. Through the introduction of CB nanoparticles as spacers, the self-restacking of graphene sheets during the filtration process is mitigated to a great extent. The pillared GP-based supercapacitors exhibit excellent electrochemical performances and cyclic stabilities compared with GP without the addition of CB nanoparticles. At a scan rate of 10 mV s(-1) , the specific capacitance of the pillared GP is 138 F g(-1) and 83.2 F g(-1) with negligible 3.85% and 4.35% capacitance degradation after 2000 cycles in aqueous and organic electrolytes, respectively. At an extremely fast scan rate of 500 mV s (-1) , the specific capacitance can reach 80 F g(-1) in aqueous electrolyte. No binder is needed for assembling the supercapacitor cells and the pillared GP itself may serve as a current collector due to its intrinsic high electrical conductivity. The pillared GP has great potential in the development of promising flexible and ultralight-weight supercapacitors for electrochemical energy storage.
A nano-scaled coating of titanium oxide (TiO 2 ) on graphene (G) has been achieved via a novel atomic layer deposition (ALD) method. As a potential supercapacitor material, the TiO 2 -G composites exhibited a capacity of 75 F/g and 84 F/g at a scan rate of 10 mV/s for composites grown using 50 and 100 ALD cycles, respectively. The nearly identical Nyquist plots of the TiO 2 -G composites compared with those of pure graphene demonstrated that the composites possess excellent conductivity for charge transfer and open structures for ion diffusion. In addition, even with 3-4 times additional mass loading (maximum 3.22 mg/cm 2 ), the composites exhibit no obvious degradation with respect to the electrochemical performance. This ALD approach presents a promising route to synthesize advanced graphene-based nanocomposites for supercapacitor applications.
Paired electrosynthesis is a promising technology with the potential to generate value-added products at both electrodes in a cost-effective manner. Herein, 3D vanadium nitride (VN) and Pd/VN hollow nanospheres are successfully fabricated and coupled to carry out simultaneous electrocatalytic oxidation (ECO) and electrocatalytic hydrogenation (ECH) of 5-hydroxymethylfurfural (HMF) into 2, 5-furandicarboxylic acid (FDCA) and 2,5-bishydroxymethyl-tetrahydrofuran (DHMTHF), respectively. VN shows excellent ECO performance with high HMF conversion (≥98%), FDCA selectivity (≥96%), and faradaic efficiency (≥84%) after a stability test, and Pd/VN achieves high ECH selectivity for DHMTHF at ≥88% and an HMF conversion of ≥90%, with a faradaic efficiency of ≥86%. VN and Pd/VN incorporated into a membrane electrode assembly in a paired electrolysis system shows potential for large-scale biomass conversion and upgrading. Theoretical calculations reveal that the higher performance of VN for the production of ECO can be attributed to its lower d-band center level relative to the Fermi level compared to that of V 2 O 5 , which favors HMF chemisorption and activation. This study paves the way for developing paired electrosynthesis technologies with the potential for biomass utilization and energy conversion.
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