As the development of oxygen evolution co-catalysts (OECs) is being actively undertaken, the tailored integration of those OECs with photoanodes is expected to be a plausible avenue for achieving highly efficient solar-assisted water splitting. Here, we demonstrate that a black phosphorene (BP) layer, inserted between the OEC and BiVO 4 can improve the photoelectrochemical performance of pre-optimized OEC/BiVO 4 (OEC: NiOOH, MnO x, and CoOOH) systems by 1.2∼1.6-fold, while the OEC overlayer, in turn, can suppress BP self-oxidation to achieve a high durability. A photocurrent density of 4.48 mA·cm −2 at 1.23 V vs reversible hydrogen electrode (RHE) is achieved by the NiOOH/BP/BiVO 4 photoanode. It is found that the intrinsic p -type BP can boost hole extraction from BiVO 4 and prolong holes trapping lifetime on BiVO 4 surface. This work sheds light on the design of BP-based devices for application in solar to fuel conversion, and also suggests a promising nexus between semiconductor and electrocatalyst.

Due to the greenhouse effect, enormous efforts are done for carbon dioxide reduction. By contrast, more attention should be paid for the methane oxidation and conversion, which can help the effective utilization of methane without emission. However, methane conversion and utilization under ambient conditions remains a challenge. Here, this study designs a Co3O4/ZrO2 nanocomposite for the electrochemical oxidation of methane gas using a carbonate electrolyte at room temperature. Co3O4 activated the highly efficient oxidation of methane under mild electric energy with the help of carbonate as an oxidant, which is delivered by ZrO2. Based on the experimental results, acetaldehyde is the key intermediate product. Subsequent nucleophilic addition and free radical addition reactions accounted for the generation of 2‐propanol and 1‐propanol, respectively. Surprisingly, this work achieves a production efficiency of over 60% in the conversion of methane to produce these long‐term stable products. The as‐proposed regional electrochemical methane oxidation provides a new pathway for the synthesis of higher alcohols with high production efficiencies under ambient conditions.

Millions of families around the world remain vulnerable to water scarcity and have no access to drinking water. Advanced oxidation processes (AOPs) are an effective way towards water purification with qualified reactive oxygen species (ROSs) while are impeded by the high-cost and tedious process in either input of consumable reagent, production of ROSs, and the pre-treatment of supporting electrolyte. Herein, we couple solar light-assisted H2O2 production from water and photo-Fenton-like reactions into a self-cyclable system by using an artificial leaf, achieving an unassisted H2O2 production rate of 0.77 μmol/(min·cm2) under 1 Sun AM 1.5 illumination. Furthermore, a large (70 cm2) artificial leaf was used for an unassisted solar-driven bicarbonate-activated hydrogen peroxide (BAP) system with recycled catalysts for real-time wastewater purification with requirements for only water, oxygen and sunlight. This demonstration highlights the feasibility and scalability of photoelectrochemical technology for decentralized environmental governance applications from laboratory benchtops to industry.

The photoelectrochemical (PEC) water splitting efficiency is profoundly restricted by the limited light harvesting, rapid charge recombination, and sluggish water oxidation kinetics, in which the construction of a photoelectrode requires...

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