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Perovskites have been firmly established as one of the most promising materials for third-generation solar cells. There remain several great and lingering challenges to be addressed regarding device efficiency and stability. The photovoltaic efficiency of perovskite solar cells (PSCs) depends drastically on the charge-carrier dynamics. This complex process includes charge-carrier generation, extraction, transport and collection, each of which needs to be modulated in a favorable manner to achieve high performance. Two-dimensional materials (TDMs) including graphene and its derivatives, transition metal dichalcogenides ( e.g. , MoS 2 , WS 2 ), black phosphorus (BP), metal nanosheets and two-dimensional (2D) perovskite active layers have attracted much attention for application in perovskite solar cells due to their high carrier mobility and tunable work function properties which greatly impact the charge carrier dynamics of PSCs. To date, significant advances have been achieved in the field of TDM-based PSCs. In this review, the recent progress in the development and application of TDMs ( i.e. , graphene, graphdiyne, transition metal dichalcogenides, BP, and others) as electrodes, hole transporting layers, electron transporting layers and buffer layers in PSCs is detailed. 2D perovskites as active absorber materials in PSCs are also summarized. The effect of TDMs and 2D perovskites on the charge carrier dynamics of PSCs is discussed to provide a comprehensive understanding of their optoelectronic processes. The challenges facing the PSC devices are emphasized with corresponding solutions to these problems provided with the overall goal of improving the efficiency and stability of photovoltaic devices. 

Abstract Although tremendous efforts have been devoted to understanding the origin of boosted charge storage on heteroatom‐doped carbons, none of the present studies has shown a whole landscape. Herein, by both experimental evidence and theoretical simulation, it is demonstrated that heteroatom doping not only results in a broadened operating voltage, but also successfully promotes the specific capacitance in aqueous supercapacitors. In particular, the electrolyte cations adsorbed on heteroatom‐doped carbon can effectively inhibit hydrogen evolution reaction, a key step of water decomposition during the charging process, which broadens the voltage window of aqueous electrolytes even beyond the thermodynamic limit of water (1.23 V). Furthermore, the reduced adsorption energy of heteroatom‐doped carbon consequently leads to more stored cations on the heteroatom‐doped carbon surface, thus yielding a boosted charge storage performance. 

Abstract Ever‐developing energy storage technologies demand the pursuit of advanced materials with multiple functionalities. Recent studies revealed that multiple heteroatom‐doped carbon has been wildly used for bi‐functional or even tri‐functional energy storage and conversion. However, few efforts have been made to uncover the origin of multi‐functionalities. Herein, a nitrogen, phosphorus, and sulfur tri‐doped carbon is designed in this work with large porosity, rich heteroatoms doping and high mass density, exhibiting excellent bifunctionalities on supercapacitors and oxygen reduction reaction. Importantly, the density functional theory calculations demonstrate the relevant co‐doping and tri‐doping generate more active sites on neighboring carbon atoms than single doping, and the same type of active sites may enhance bifunctionalities simultaneously. The present investigations provide a promising guidance on the design of multi‐functional materials for future energy storage and conversion applications.