Carrier recombination involved in polymeric photocatalysts includes undissociated exciton decay and charge recombination, which are the major hindrance limiting their photocatalytic activities. Realizing highly efficient charge generation and separation simultaneously in one polymeric system is therefore a fundamental strategy for the potential success of solar-to-hydrogen conversion but remains a great challenge. Here, we develop a large π-delocalized direct Z-scheme polymeric heterostructure (g-C₃N₄/P1Cl-T) that synergistically integrates a two-dimensional (2D) donor–acceptor conjugated polymer (P1Cl-T) with g-C₃N₄. We demonstrate that the intermolecular π–π stacking successfully rebuilds the extended π-network over the whole polymeric heterojunction, thus facilitating full-visible-light absorption, exciton dissociation and charge transport. The combination of spectroscopic analysis and theoretical calculations reveals that both resonance energy transfer and Z-scheme charge transfer occur upon light illumination. With the intense synergy among the large π-delocalization, π–π stacking interactions and internal electric field, the g-C₃N₄/P1Cl-T photocatalyst shows an unprecedentedly high hydrogen evolution rate of ∼111.8 mmol h⁻¹ g⁻¹ with apparent quantum yields (AQYs) of 46.75% at 475 nm and 1.77% at 700 nm, which is about 48-fold higher than that of pristine g-C₃N₄ and tops those for all the previously reported polymer-based photocatalysts.

As a “hot” member of two-dimensional (2D) materials, black phosphorus (BP) has received growing interest in a variety of fields in physics, chemistry, materials, and biomedicine since 2014. Owing to the exclusive 2D layered structure, some fantastic properties such as tunable band structure, high charge mobility, and in-plane anisotropy provide BP with great potential for application in electronic/optoelectronic devices, energy source conversion and storage, etc. However, with in-depth investigations, the performance deficiencies of BP-based devices are exposed, originating from the poor chemical stability of BP. To address the above issues, a variety of BP/carbon hybrid composites have been constructed as an emerging type of multifunctional materials by the integration of the unique properties of carbon materials with the merits of BP into a single hybrid heterostructure, showing improved performance for applications. In this review, the enhanced stability of BP is presented based on the fundamental chemistry of BP degradation, which originates from the formation of P–C/P–O–C bonds or van der Waals interactions in BP/carbon hybrid composites. Recent research studies focusing on the utilization of BP/carbon hybrid composites for electrochemical energy storage, photocatalytic hydrogen production and optoelectronic devices are summarized, in which approaches toward the assembly of BP/carbon hybrid composites are introduced. Finally, the extant challenges and potential applications of BP/carbon hybrid materials are also proposed.

A low-cost spiro[3.3]heptane-2,6-dispirofluorene (SDF) based hole transporting material termed SDF-OMeTAD has been designed and synthesized via a two-step reaction, representing a considerable simplification with respect to that of the well-known spiro-OMeTAD. The SDF-OMeTAD was exploited in lead halide planar perovskite solar cells using low-temperature solution-processed SnO₂ as the electron transporting layer, delivering a competitive power conversion efficiency of 13.01% with an open-circuit voltage of 1.10 V under 100 mW cm⁻² AM 1.5G solar illumination. The facile synthesis approach of SDF-OMeTAD from commercially available starting materials will facilitate SDF-based molecules to be further exploited in thin film organic–inorganic perovskite solar cells and can be optimized to further enhance power conversion efficiency.