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Hydrogen is a promising future sustainable fuel candidate with boundless opportunities. Research into photoelectrochemical (PEC) water splitting based on a lead halide perovskite (LHP) has progressed significantly with the aim of more efficient solar hydrogen production. Herein, we unite a well-known photo-absorbing LHP with cost-effective water-splitting catalysts, and we introduce two types of monolithic LHP-based PEC devices that act as a photocathode and a photoanode for the hydrogen evolution reaction and oxygen evolution reaction, leading to efficient unbiased overall water splitting.Through the integration of these two monolithic LHP-based photoelectrodes, an unbiased solar-to-hydrogen conversion efficiency of 10.64% and a photocurrent density of 8.65 mA cm −2 are achieved.perovskite, photoelectrochemical cell, photoelectrode, unassisted | INTRODUCTIONPhotoelectrochemical (PEC) water splitting, 1 a promising artificial photosynthesis method, is a potential alternative technique for generating renewable fuel. Conventional PEC devices with metal oxides can generate renewable energy sources, such as hydrogen, from water splitting, which can alleviate CO 2 emissions from fossil fuels. However, most readily employed metal oxide-based PEC devices exhibit poor photocurrent density under 1 sun conditions and Carbon Energy.

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Facile synthesis of hierarchically porous metal–organic frameworks (MOFs) with adjustable porosity and high crystallinity attracts great attention yet remains challenging. Herein, a micromolar amount of dye‐based modulator (Rhodamine B (RhB)) is employed to easily and controllably tailor the pore size of a Ti‐based metal–organic framework (MIL‐125‐NH2). The RhB used in this method is easily removed by washing or photodegradation, avoiding secondary posttreatment. It is demonstrated that the carboxyl functional group and the steric effects of RhB are indispensable for enlarging the pore size of the MIL‐125‐NH2. The resulting hierarchically porous MIL‐125‐NH2 (RH‐MIL‐125‐NH2) exhibits optimized adsorption and photocatalytic activity because the newly formed mesopore with defects concurrently facilitates mass transport of guest molecules (toluene) and photogenerated charge separation. This work offers a meaningful basis for the construction of hierarchically porous MOFs and demonstrates the superiority of the hierarchical pore structure for adsorption and heterogeneous catalysis.

Aqueous photoelectrochemical (PEC) cells have long been considered a promising technology to convert solar energy into hydrogen. However, the solar‐to‐H2 (STH) efficiency and cost‐effectiveness of PEC water splitting are significantly limited by sluggish oxygen evolution reaction (OER) kinetics and the low economic value of the produced O2, hindering the practical commercialization of PEC cells. Recently, organic upgrading PEC reactions, especially for alternative OERs, have received tremendous attention, which improves not only the STH efficiency but also the economic effectiveness of the overall reaction. In this review, PEC reaction fundamentals and reactant‐product cost analysis of organic upgrading reactions are briefly reviewed, recent advances made in organic upgrading reactions, which are categorized by their reactant substrates, such as methanol, ethanol, glycol, glycerol, and complex hydrocarbons, are then summarized and discussed. Finally, the current status, further outlooks, and challenges toward industrial applications are discussed.