Solar energy-assisted water oxidative hydrogen peroxide (H2O2) production on an anode combined with H2 production on a cathode increases the value of solar water splitting, but the challenge of the dominant oxidative product, O2, needs to be overcome. Here, we report a SnO2–x overlayer coated BiVO4 photoanode, which demonstrates the great ability to near-completely suppress O2 evolution for photoelectrochemical (PEC) H2O oxidative H2O2 evolution. Based on the surface hole accumulation measured by surface photovoltage, downward quasi-hole Fermi energy at the photoanode/electrolyte interface and thermodynamic Gibbs free energy between 2-electron and 4-electron competitive reactions, we are able to consider the photoinduced holes of BiVO4 that migrate to the SnO2–x overlayer kinetically favor H2O2 evolution with great selectivity by reduced band bending. The formation of H2O2 may be mediated by the formation of hydroxyl radicals (OH·), from 1-electron water oxidation reactions, as evidenced by spin-trapping electron paramagnetic resonance (EPR) studies conducted herein. In addition to the H2O oxidative H2O2 evolution from PEC water splitting, the SnO2–x /BiVO4 photoanode can also inhibit H2O2 decomposition into O2 under either electrocatalysis or photocatalysis conditions for continuous H2O2 accumulation. Overall, the SnO2–x /BiVO4 photoanode achieves a Faraday efficiency (FE) of over 86% for H2O2 generation in a wide potential region (0.6–2.1 V vs reversible hydrogen electrode (RHE)) and an H2O2 evolution rate averaging 0.825 μmol/min/cm2 at 1.23 V vs RHE under AM 1.5 illumination, corresponding to a solar to H2O2 efficiency of ∼5.6%; this performance surpasses almost all previous solar energy-assisted H2O2 evolution performances. Because of the simultaneous production of H2O2 and H2 by solar water splitting in the PEC cells, our results highlight a potentially greener and more cost-effective approach for “solar-to-fuel” conversion.

Order/disorder interfacial engineering realizes highly efficient co-catalyst free hydrogen generation.

Using whole-cell recordings from presynaptic terminals and postsynaptic principal neurons in the mouse medial nucleus of the trapezoid body (MNTB), we have characterized properties of the calyx of Held synapse during the first three postnatal weeks. We observed that evoked excitatory postsynaptic currents (EPSCs) mediated by NMDA receptors (NMDAR) increased until postnatal day 11/12 (P11/12) after which they declined to very low or undetectable levels at P16. Meanwhile, EPSCs mediated by AMPA receptors (AMPAR) showed an approximate three-fold increase in amplitude. These changes were paralleled by NMDAR and AMPAR currents evoked by exogenous NMDA and kainate to MNTB neurons except that whole-cell kainate currents remained constant after P7/8 while AMPAR-EPSCs continued to increase. We found that the decay time constant t for NMDAR-EPSCs and AMPAR-EPSCs declined by about 30 % and 70 %, respectively. Analyses of NMDAR-EPSCs with subunit-specific pharmacological agents including ifenprodil, N,N,N‚,N‚-tetrakis(2-pyridylmethyl)-ethylenediamine (TPEN), zinc and Mg 2+ revealed subtle developmental changes in subunit composition. As maturation progressed, this synapse displayed a reduction in the number of presynaptic spike failures and the extent of synaptic depression in response to trains of stimuli (50-300 Hz) while the recovery rate from depression accelerated. These results demonstrate profound changes in the size and kinetics of postsynaptic glutamate receptors and in the spike-firing capability of presynaptic terminals at the calyx of Held-MNTB synapse during early development. We suggest that these concurrent presynaptic and postsynaptic adaptations represent important steps for synapse consolidation and refinement and ultimately for the development of fast high-fidelity transmission at this synapse. synaptic properties of the mouse calyx of Held-MNTB synapse within the first three postnatal weeks. We found that synaptic NMDARs were present only transiently within the first 2 weeks, and exhibited a unique developmental profile. Although synaptic AMPARs exhibited a nearly linear growth in density over the same period, the total population of functional AMPARs (i.e. whole-cell kainate currents) reached a maximum by the end of the first postnatal week. We suggest that these changes, along with concurrent alterations in kinetic properties of EPSCs and in synaptic depression and recovery, contribute significantly to the development of high-fidelity synaptic transmission at this synapse. Part of this study had been previously published in abstract form (Joshi & Wang, 2000). METHODS Slice preparationMice were housed in the facility certified by the Canadian Council of Animal Care and used for this study according to a protocol approved by the Hospital for Sick Children Animal Care Committee. Brainstem slices were prepared from P3-P18 mice (CD1/C57 black) as previously described (Forsythe & BarnesDavis, 1993). Mice were decapitated with a small guillotine and brains were rapidly dissected and immersed in ice-cold artif...