N‐doped carbon nanomaterials have rapidly grown as the most important metal‐free catalysts in a wide range of chemical and electrochemical reactions. This current report summarizes the latest advances in N‐doped carbon electrocatalysts prepared by N mono‐doping and co‐doping with other heteroatoms. The structure–performance relationship of these materials is subsequently rationalized and perspectives on developing more efficient and sustainable electrocatalysts from carbon nanomaterials are also suggested.

Polymer electrolyte membrane fuel cells (PEFCs) are an efficient and clean alternative power source, but the high cost impedes widespread commercialization. The fuel cell membrane, e.g. Nafion, contributes significantly to this cost, and therefore novel alternatives are required. Temperature is also an important factor; high temperature operation leads to faster reaction kinetics, lower electrocatalyst loading, and improved water management, thereby further reducing cost. However, higher temperature puts greater demands on the membrane. Conductivity is related strongly to humidification and therefore this generally decreases above 100°C. Nanocellulose membranes for fuel cells, in which the proton conductivity increases up to 120°C, are here reported for the first time. The hydrogen barrier properties are far superior to conventional ionomer membranes. Fuel cells with nanocellulose membranes are successfully operated at 80°C. Additionally, these membranes are environmentally friendly and biodegradable.

Single-crystal metals have distinctive properties owing to the absence of grain boundaries and strong anisotropy. Commercial single-crystal metals are usually synthesized by bulk crystal growth or by deposition of thin films onto substrates, and they are expensive and small. We prepared extremely large single-crystal metal foils by “contact-free annealing” from commercial polycrystalline foils. The colossal grain growth (up to 32 square centimeters) is achieved by minimizing contact stresses, resulting in a preferred in-plane and out-of-plane crystal orientation, and is driven by surface energy minimization during the rotation of the crystal lattice followed by “consumption” of neighboring grains. Industrial-scale production of single-crystal metal foils is possible as a result of this discovery.

Folded graphene in which two layers are stacked with a twist angle between them has been predicted to exhibit unique electronic, thermal, and magnetic properties. We report the folding of a single crystal monolayer graphene film grown on a Cu(111) substrate by using a tailored substrate having a hydrophobic region and a hydrophilic region. Controlled film delamination from the hydrophilic region was used to prepare macroscopic folded graphene with good uniformity on the millimeter scale. This process was used to create many folded sheets each with a defined twist angle between the two sheets. By identifying the original lattice orientation of the monolayer graphene on Cu foil, or establishing the relation between the fold angle and twist angle, this folding technique allows for the preparation of twisted bilayer graphene films with defined stacking orientations and may also be extended to create folded structures of other two-dimensional nanomaterials.

Abstract