Developing low-cost electrocatalysts to replace precious Ir-based materials is key for oxygen evolution reaction (OER). Here, we report atomically dispersed nickel coordinated with nitrogen and sulfur species in porous carbon nanosheets as an electrocatalyst exhibiting excellent activity and durability for OER with a low overpotential of 1.51 V at 10 mA cm⁻² and a small Tafel slope of 45 mV dec⁻¹ in alkaline media. Such electrocatalyst represents the best among all reported transition metal- and/or heteroatom-doped carbon electrocatalysts and is even superior to benchmark Ir/C. Theoretical and experimental results demonstrate that the well-dispersed molecular S|NiN_x species act as active sites for catalyzing OER. The atomic structure of S|NiN_x centers in the carbon matrix is clearly disclosed by aberration-corrected scanning transmission electron microscopy and synchrotron radiation X-ray absorption spectroscopy together with computational simulations. An integrated photoanode of nanocarbon on a Fe₂O₃ nanosheet array enables highly active solar-driven oxygen production.

Atomically dispersed Ni–N_x species anchored porous carbon matrix with embedded Ni nanoparticles was synthesized for highly efficient hydrogen evolution in alkaline conditions.

Owing to their earth abundance, high atom utilization, and excellent activity, single iron atoms dispersed on nitrogen‐doped carbons (Fe‐N‐C) have emerged as appealing alternatives to noble‐metal platinum (Pt) for catalyzing the oxygen reduction reaction (ORR). However, the ORR activity of current Fe‐N‐C is seriously limited by the low density and inferior exposure of active Fe‐N_x species. Here, a novel zinc‐mediated template synthesis strategy is demonstrated for constructing densely exposed Fe‐N_x moieties on hierarchically porous carbon (SA‐Fe‐NHPC). During the thermal treatment of 2,6‐diaminopyridine/ZnFe/SiO₂ complex, the zinc prevents the formation of iron carbide nanoparticles and the SiO₂ template promotes the generation of hierarchically pores for substantially improving the accessibility of Fe‐N_x moieties after subsequent leaching. As a result, the SA‐Fe‐NHPC electrocatalysts exhibit an unprecedentedly high ORR activity with a half‐wave potential (E_1/2) of 0.93 V in a 0.1 m KOH aqueous solution, which outperforms those for Pt/C catalyst and state‐of‐the‐art noble metal‐free electrocatalysts. As the air electrode in zinc–air batteries, the SA‐Fe‐NHPC demonstrates a large peak power density of 266.4 mW cm⁻² and superior long‐term stability. Therefore, the developed zinc‐mediated template synthesis strategy for boosting the density and accessibility of Fe‐N_x species paves a new avenue toward high‐performance ORR electrocatalysts.

One of the key challenges in two-dimensional (2D) materials is to go beyond graphene, a prototype 2D polymer (2DP), and to synthesize its organic analogues with structural control at the atomic- or molecular-level. Here we show the successful preparation of porphyrin-containing monolayer and multilayer 2DPs through Schiff-base polycondensation reaction at an air–water and liquid–liquid interface, respectively. Both the monolayer and multilayer 2DPs have crystalline structures as indicated by selected area electron diffraction. The monolayer 2DP has a thickness of∼0.7 nm with a lateral size of 4-inch wafer, and it has a Young’s modulus of 267±30 GPa. Notably, the monolayer 2DP functions as an active semiconducting layer in a thin film transistor, while the multilayer 2DP from cobalt-porphyrin monomer efficiently catalyses hydrogen generation from water. This work presents an advance in the synthesis of novel 2D materials for electronics and energy-related applications.