Rechargeable aqueous Zn/MnO battery chemistry in a neutral or mildly acidic electrolyte has attracted extensive attention recently because all the components (anode, cathode, and electrolyte) in a Zn/MnO battery are safe, abundant, and sustainable. However, the reaction mechanism of the MnO cathode remains a topic of discussion. Herein, we design a highly reversible aqueous Zn/MnO battery where the binder-free MnO cathode was fabricated by in situ electrodeposition of MnO on carbon fiber paper in mild acidic ZnSO+MnSO electrolyte. Electrochemical and structural analysis identify that the MnO cathode experience a consequent H and Zn insertion/extraction process with high reversibility and cycling stability. To our best knowledge, it is the first report on rechargeable aqueous batteries with a consequent ion-insertion reaction mechanism.
In conventional solid-state photovoltaics, electron-hole pairs are created by light absorption in a semiconductor and separated by the electric field spaning a micrometre-thick depletion region. The maximum voltage these devices can produce is equal to the semiconductor electronic bandgap. Here, we report the discovery of a fundamentally different mechanism for photovoltaic charge separation, which operates over a distance of 1-2 nm and produces voltages that are significantly higher than the bandgap. The separation happens at previously unobserved nanoscale steps of the electrostatic potential that naturally occur at ferroelectric domain walls in the complex oxide BiFeO(3). Electric-field control over domain structure allows the photovoltaic effect to be reversed in polarity or turned off. This new degree of control, and the high voltages produced, may find application in optoelectronic devices.
Carbon-based supercapacitors can provide high electrical power, but they do not have sufficient energy density to directly compete with batteries. We found that a nitrogen-doped ordered mesoporous few-layer carbon has a capacitance of 855 farads per gram in aqueous electrolytes and can be bipolarly charged or discharged at a fast, carbon-like speed. The improvement mostly stems from robust redox reactions at nitrogen-associated defects that transform inert graphene-like layered carbon into an electrochemically active substance without affecting its electric conductivity. These bipolar aqueous-electrolyte electrochemical cells offer power densities and lifetimes similar to those of carbon-based supercapacitors and can store a specific energy of 41 watt-hours per kilogram (19.5 watt-hours per liter).
Rechargeable Li-metal batteries using high-voltage cathodes can deliver the highest possible energy densities among all electrochemistries. However, the notorious reactivity of metallic lithium as well as the catalytic nature of high-voltage cathode materials largely prevents their practical application. Here, we report a non-flammable fluorinated electrolyte that supports the most aggressive and high-voltage cathodes in a Li-metal battery. Our battery shows high cycling stability, as evidenced by the efficiencies for Li-metal plating/stripping (99.2%) for a 5 V cathode LiCoPO (~99.81%) and a Ni-rich LiNiMnCoO cathode (~99.93%). At a loading of 2.0 mAh cm, our full cells retain ~93% of their original capacities after 1,000 cycles. Surface analyses and quantum chemistry calculations show that stabilization of these aggressive chemistries at extreme potentials is due to the formation of a several-nanometre-thick fluorinated interphase.
Black TiO2 attracts enormous attention due to its large solar absorption and induced excellent photocatalytic activity. Herein, a new approach assisted by hydrogen plasma to synthesize unique H‐doped black titania with a core/shell structure (TiO2@TiO2‐xHx) is presented, superior to the high H2‐pressure process (under 20 bar for five days). The black titania possesses the largest solar absorption (≈83%), far more than any other reported black titania (the record (high‐pressure): ≈30%). H doping is favorable to eliminate the recombination centers of light‐induced electrons and holes. High absorption and low recombination ensure the excellent photocatalytic activity for the black titania in the photo‐oxidation of organic molecules in water and the production of hydrogen. The H‐doped amorphous shell is proposed to play the same role as Ag or Pt loading on TiO2 nanocrystals, which induces the localized surface plasma resonance and black coloration. Photocatalytic water splitting and cleaning using TiO2‐xHx is believed to have a bright future for sustainable energy sources and cleaning environment.
Utilizing solar energy for hydrogen generation and water cleaning is a great challenge due to insufficient visible-light power conversion. Here we report a mass production approach to synthesize black titania by aluminium reduction. The obtained sample possesses a unique crystalline core-amorphous shell structure (TiO 2 @TiO 2Àx ). The black titania absorbs $65% of the total solar energy by improving visible and infrared absorption, superior to the recently reported ones ($30%) and pristine TiO 2 ($5%). The unique core-shell structure (TiO 2 @TiO 2Àx ) and high absorption boost the photocatalytic water cleaning and water splitting.The black titania is also an excellent photoelectrochemical electrode exhibiting a high solar-to-hydrogen efficiency (1.7%). A large photothermic effect may enable black titania "capture" solar energy for solar thermal collectors. The Al-reduced amorphous shell is proved to be an excellent candidate to absorb more solar light and receive more efficient photocatalysis.
Narrow electrochemical stability window (1.23 V) of aqueous electrolytes has always been the key obstacle preventing aqueous sodium ion chemistry of practical energy density and cycle life. The sodium ion Water-in-Salt Electrolyte (NaWiSE) eliminates this barrier by offering a 2.5 V window through suppressing hydrogen evolution on anode with the formation of a Na + -conducting solidelectrolyte-interphase (SEI) and reducing the overall electrochemical activity of water on cathode. A full aqueous Na-ion battery constructed on Na 0.66 [Mn 0.66 Ti 0.34 ]O 2 as cathode and NaTi 2 (PO 4 ) 3 as anode exhibits superior performance at both low and high rates, as exemplified by extraordinarily high coulombic efficiency (> 99.2%) at a low rate (0.2 C) for >350 cycles, and excellent cycling stability with negligible capacity losses (0.006 % per cycle) at a high rate (1C) for >1200 cycles. Molecular modeling revealed some key difference between Li-ion and Na-ion WiSE, and identified a more pronounced ion aggregation with frequent contacts between the sodium cation and fluorine of anion in the latter as one main factor responsible for the formation of a dense SEI at lower salt concentration than its Li cousin.
4.0 V aqueous LIBs of both high energy density and high safety are made possible by a new interphase formed from an ''inhomogeneous additive'' approach that effectively stabilizes graphite or lithium-metal anode materials.
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