Highly active and low-cost electrocatalysts for water oxidation are required due to the demands on sustainable solar fuels; however, developing highly efficient catalysts to meet industrial requirements remains a challenge. Herein, we report a monolayer of nickel–vanadium-layered double hydroxide that shows a current density of 27 mA cm−2 (57 mA cm−2 after ohmic-drop correction) at an overpotential of 350 mV for water oxidation. Such performance is comparable to those of the best-performing nickel–iron-layered double hydroxides for water oxidation in alkaline media. Mechanistic studies indicate that the nickel–vanadium-layered double hydroxides can provide high intrinsic catalytic activity, mainly due to enhanced conductivity, facile electron transfer and abundant active sites. This work may expand the scope of cost-effective electrocatalysts for water splitting.

Light driven water splitting was achieved by a tandem dye-sensitized photoelectrochemical cell with two photoactive electrodes. The photoanode is constituted by an organic dye L0 as photosensitizer and a molecular complex Ru1 as water oxidation catalyst on meso-porous TiO2, while the photocathode is constructed with an organic dye P1 as photoabsorber and a molecular complex Co1 as hydrogen generation catalyst on nanostructured NiO. By combining the photocathode and the photoanode, this tandem DS-PEC cell can split water by visible light under neutral pH conditions without applying any bias.

As one of the most remarkable oxygen evolution reaction (OER) electrocatalysts, metal chalcogenides have been intensively reported during the past few decades because of their high OER activities. It has been reported that electron-chemical conversion of metal chalcogenides into oxides/hydroxides would take place after the OER. However, the transition mechanism of such unstable structures, as well as the real active sites and catalytic activity during the OER for these electrocatalysts, has not been understood yet; therefore a direct observation for the electrocatalytic water oxidation process, especially at nano or even angstrom scale, is urgently needed. In this research, by employing advanced Cs-corrected transmission electron microscopy (TEM), a step by step oxidational evolution of amorphous electrocatalyst CoS x into crystallized CoOOH in the OER has been in situ captured: irreversible conversion of CoS x to crystallized CoOOH is initiated on the surface of the electrocatalysts with a morphology change via Co(OH) 2 intermediate during the OER measurement, where CoOOH is confirmed as the real active species. Besides, this transition process has also been confirmed by multiple applications of X-ray photoelectron spectroscopy (XPS), in situ Fourier-transform infrared spectroscopy (FTIR), and other ex situ technologies. Moreover, on the basis of this discovery, a high-efficiency electrocatalyst of a nitrogen-doped graphene foam (NGF) coated by CoS x has been explored through a thorough structure transformation of CoOOH. We believe this in situ and in-depth observation of structural evolution in the OER measurement can provide insights into the fundamental understanding of the mechanism for the OER catalysts, thus enabling the more rational design of low-cost and high-efficient electrocatalysts for water splitting.

We investigated a range of different mesoporous NiO electrodes prepared by different research groups and private firms in Europe to determine the parameters which influence good quality photoelectrochemical devices. This benchmarking study aims to solve some of the discrepancies in the literature regarding the performance of p-DSCs due to differences in the quality of the device fabrication. The information obtained will lay the foundation for future photocatalytic systems based on sensitized NiO so that new dyes and catalysts can be tested with a standardized material. The textural and electrochemical properties of the semiconducting material are key to the performance of photocathodes. We found that both commercial and non-commercial NiO gave promising solar cell and water-splitting devices. The NiO samples which had the two highest solar cell efficiency (0.145% and 0.089%) also gave the best overall theoretical H2 conversion.

Photoelectrochemical (PEC) cells using molecular catalysts to split water into hydrogen and oxygen have been investigated intensively during the past years. However, the high-cost of Pt counter electrodes and instability of molecular PEC cells hinder the practical applications. We describe in this article a Pt-free tandem molecular PEC cell, for the first time, employing molecular ruthenium- and cobalt-catalysts with strong dipicolinic acid anchoring groups on the respective photoanode and photocathode for total water splitting. The Pt-free tandem molecular PEC cell showed an effective and steady photocurrent density of ca. 25 μA cm(-2) for water splitting driven by visible light without external bias. This study indicates that tandem molecular PEC cells can provide great potential to the Pt-free devices for light driven total water splitting.