Sandwich-Polarized Heterojunction: Efficient Charge Separation and Redox Capability Protection for Photocatalytic Overall Water Splitting.

Photocatalytic overall water splitting is a potential strategy to address energy crisis and environmental issues. However, it remains a great challenge to design an efficient photocatalyst, which not only possesses large spatial separation of photogenerated electrons and holes (PEH) to suppress recombination, but also can preserve the redox capability to drive the reaction. Herein, we design a new type of sandwich-polarized heterojunction by inserting a polarized semiconductor into the interlayer of the conventional photocatalyst. The inserted sublayer with out-of-plane polarization can induce a large electrostatic potential difference between the top and bottom photocatalytic sublayers. Then, the band edges of the top and bottom sublayers can be shifted to form the type II band alignment. Also, the valence band maximum and conduction band minimum will be located on different photocatalytic sublayers to facilitate the spatial separation of PEH. Simultaneously, different from the conventional type II heterojunction that reduces the redox capability, the electrostatic potential difference also acts as an auxiliary booster to offset the reduced redox potential of PEH. Taking the C2N/In2Se3/C2N heterojunction as an example, the polarized In2Se3 effectively promotes the interface transfer of PEH in 1-5 ps and extends the lifetime of PEH to ∼186 ns, which is about six times that of bilayer C2N. Simultaneously, the redox power of C2N is well preserved. Our work offers a promising scheme to advance the photocatalytic overall water splitting.

Spin-resolved bunching and noise characteristics in double quantum dots coupled to ferromagnetic electrodes.

We study spin-resolved noise in Coulomb blockaded double quantum dots coupled to ferromagnetic electrodes. The modulation of the interdot coupling and spin polarization in the electrodes gives rise to an intriguing dynamical spin ↑-↑ (↓-↓) blockade mechanism: bunching of up (down) spins due to dynamical blockade of an up (down) spin. In contrast to the conventional dynamical spin ↑-↓ bunching (bunching of up spins associated with a dynamical blockade of a down spin), this new bunching behavior is found to be intimately associated with the spin mutual-correlation, i.e. the noise fluctuation between opposite spin currents. We further demonstrate that the dynamical spin ↑-↑ and ↑-↓ bunching of tunneling events may be coexistent in the regime of weak interdot coupling and low spin polarization.

Photoelectrocatalytic degradation of tetracycline by highly effective TiO2 nanopore arrays electrode.

The widely utilization of pharmaceutical and personal care products (PPCPs) in the pharmaceutical therapies and agricultural husbandry has led to the worldwide pollution in the environment. In this study, the photoelectrocatalytic (PEC) behaviors of typical PPCPs, tetracycline (TC), were performed via a highly effective TiO(2) nanopore arrays (TNPs) electrode, comparing with electrochemical (EC) and photocatalytic (PC) process. A significant photoelectrochemical synergetic effect in TC degradation was observed on the TNPs electrode and the rate constant for the PEC process of TNPs electrode was approximately 6.7 times as high as its PC process. The TC removal rate achieved approximately 80% within 3h PEC reaction by TNPs electrode, which is approximately 25% higher than that obtained for a conventional coated TiO(2) nanofilm electrode fabricated by sol-gel method. The possible mechanism involved in the PEC degradation of TC by TNPs electrode was discussed. Furthermore, the TNPs electrode also shows enhanced photocurrent response compared with that for the coated TiO(2) nanofilm electrode. Such kind of TiO(2) nanopores will have many potential applications in various areas as an outstanding photoelectrochemical material.