Crystal engineering--the planning and construction of crystalline supramolecular architectures from modular building blocks--permits the rational design of functional molecular materials that exhibit technologically useful behaviour such as conductivity and superconductivity, ferromagnetism and nonlinear optical properties. Because the presence of two cooperative properties in the same crystal lattice might result in new physical phenomena and novel applications, a particularly attractive goal is the design of molecular materials with two properties that are difficult or impossible to combine in a conventional inorganic solid with a continuous lattice. A promising strategy for creating this type of 'bi-functionality' targets hybrid organic/inorganic crystals comprising two functional sub-lattices exhibiting distinct properties. In this way, the organic pi-electron donor bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) and its derivatives, which form the basis of most known molecular conductors and superconductors, have been combined with molecular magnetic anions, yielding predominantly materials with conventional semiconducting or conducting properties, but also systems that are both superconducting and paramagnetic. But interesting bulk magnetic properties fail to develop, owing to the discrete nature of the inorganic anions. Another strategy for achieving cooperative magnetism involves insertion of functional bulky cations into a polymeric magnetic anion, such as the bimetallic oxalato complex [MnIICrIII(C2O4)3]-, but only insoluble powders have been obtained in most cases. Here we report the synthesis of single crystals formed by infinite sheets of this magnetic coordination polymer interleaved with layers of conducting BEDT-TTF cations, and show that this molecule-based compound displays ferromagnetism and metallic conductivity.

Industrially profitable water splitting is one of the great challenges in the development of a viable and sustainable hydrogen economy. Alkaline electrolysers using Earth-abundant catalysts remain the most economically viable route to electrolytic hydrogen, but improved efficiency is desirable. Recently, electron spin polarization was described as a potential way to improve water-splitting catalysis. Here, we report the significant enhancement of alkaline water electrolysis when a moderate magnetic field (≤450 mT) is applied to the anode. Current density increments above 100% (over 100 mA cm −2) were found for highly magnetic electrocatalysts, such as the mixed oxide NiZnFe 4 O x. Magnetic enhancement works even for decorated Ni-foam electrodes with very high current densities, improving their intrinsic activity by about 40% to reach over 1 A cm −2 at low overpotentials. Thanks to its simplicity, our discovery opens opportunities for implementing magnetic enhancement in water splitting.

The lack of an efficient, robust, and inexpensive water oxidation catalyst (WOC) is arguably the biggest challenge for the technological development of artificial photosynthesis devices. Here we report the catalytic activity found in a cobalt hexacyanoferrate (CoHCF) Prussian blue-type coordination polymer. This material is competitive with state-of-the-art metal oxides and exhibits an unparalleled long-term stability at neutral pH and ambient conditions, maintaining constant catalytic rates for weeks. In addition to its remarkable catalytic activity, CoHCF adds the typical properties of molecule-based materials: transparency to visible light, porosity, flexibility, processability, and low density. Such features make CoHCF a promising WOC candidate for advancement in solar fuels production.