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Graphitic carbon nitrides and their composites with various morphologies and bandgaps engineered for the hydrogen evolution reaction under visible light are reviewed.

Nanostructured porous carbon materials have diverse applications including sorbents, catalyst supports for fuel cells, electrode materials for capacitors, and hydrogen storage systems. When these materials have hierarchical porosity, interconnected pores of different dimensions, their potential application is increased. Hierarchical nanostructured carbons (HNCs) that contain 3D-interconnected macroporous/mesoporous and mesoporous/microporous structures have enhanced properties compared with single-sized porous carbon materials, because they have improved mass transport through the macropores/mesopores and enhanced selectivity and increased specific surface area on the level of fine pore systems through mesopores/micropores. The HNCs with macro/mesoporosity are of particular interest because chemists can tailor specific applications through controllable synthesis of HNCs with designed nanostructures. An efficient and commonly used technique for creating HNCs is "nanocasting", a technique that first involves the creation of a sacrificial silica template with hierarchical porous nanostructure and then the impregnation of the silica template with an appropriate carbon source. This is followed by carbonization of the filled carbon precursor, and subsequent removal of the silica template. The resulting HNC is an inverse replica of its parent hierarchical nanostructured silica (HNS). Through such nanocasting, scientists can create different HNC frameworks with tailored pore structures and narrow pore size distribution. Generally, HNSs with specific structure and 3D-interconnected porosity are needed to fabricate HNCs using the nanocasting strategy. However, how can we fabricate a HNS framework with tailored structure and hierarchical porosity of meso-macropores? This Account reports on our recent work in the development of novel HNCs and their interesting applications. We have explored a series of strategies to address the challenges in synthesis of HNSs and HNCs. Through careful control of experimental parameters, we found we could readily create new HNSs and HNCs with tailored structure and hierarchical porosity. In this Account, we describe the applications of the HNCs in low-temperature fuel cells, in Li ion batteries, in quantum-dot-sensitized solar cells (QDSSCs) and as hydrogen storage materials. Fuel cell and QDSSC polarization performance data reveal that both the ordered HNC and spherical HNC with uniform macro- and mesoporosity demonstrate superior catalyst support effect and considerably enhanced photovoltaic performance due to their incredible structural characteristics. For hydrogen and lithium storage applications, primary experimental results show that spherical HNCs with uniform macroporous core/mesoporous shell and ordered HNC are highly beneficial in terms of a high hydrogen (or Li) uptake, good rate capability and excellent cycling retainability. These data suggest that the innovative HNCs with tailored nanostructure may find promising applications in the rapid and efficient storage of hydrogen (or Li).

This review focuses on polyhedron-engineered Pt-based nanocrystals as highly active ORR catalysts for PEMFCs.