Hydrogen peroxide (H2O2) has received increasing attention because it is not only a mild and environmentally friendly oxidant for organic synthesis and environmental remediation but also a promising new liquid fuel. The production of H2O2 by photocatalysis is a sustainable process, since it uses water and oxygen as the source materials and solar light as the energy. Encouraging processes have been developed in the last decade for the photocatalytic production of H2O2. In this Review we summarize research progress in the development of processes for the photocatalytic production of H2O2. After a brief introduction emphasizing the superiorities of the photocatalytic generation of H2O2, the basic principles of establishing an efficient photocatalytic system for generating H2O2 are discussed, highlighting the advanced photocatalysts used. This Review is concluded by a brief summary and outlook for future advances in this emerging research field.

The synthesis of hydrogen peroxide (H2O2) from H2O and O2 by metal-free photocatalysts (e.g., graphitic carbon nitride, C3N4) is a potentially promising approach to generate H2O2. However, the photocatalytic H2O2 generation activity of the pristine C3N4 in pure H2O is poor due to unpropitious rapid charge recombination and unfavorable selectivity. Herein, we report a facile method to boost the photocatalytic H2O2 production by grafting cationic polyethylenimine (PEI) molecules onto C3N4. Experimental results and density functional theory (DFT) calculations demonstrate PEI can tune the local electronic environment of C3N4. The unique intermolecular electronic interaction in PEI/C3N4 not only improves the electron–hole separation but also promotes the two-electron O2 reduction to H2O2 via the sequential two-step single-electron reduction route. With the synergy of improved charge separation and high selectivity of two-electron O2 reduction, PEI/C3N4 exhibits an unexpectedly high H2O2 generation activity of 208.1 μmol g–1 h–1, which is 25-fold higher than that of pristine C3N4. This study establishes a paradigm of tuning the electronic property of C3N4 via functional molecules for boosted photocatalysis activity and selectivity.

Development of novel hybrid photocatalysts with high efficiency and durability for photocatalytic hydrogen generation is highly desired but still remains a grand challenge currently. In the present work, we reported the exploration of ternary hybrid TiO2/CuO/Cu thoroughly mesoporous nanofibers via a foaming-assisted electrospinning technique. It is found that by adjusting the Cu contents in the solutions, the unitary (TiO2), binary (TiO2/CuO, TiO2/Cu), and ternary (TiO2/CuO/Cu) mesoporous products can be obtained, enabling the growth of TiO2/CuO/Cu ternary hybrids in a tailored manner. The photocatalytic behavior of the as-synthesized products as well as P25 was evaluated in terms of their hydrogen evolution efficiency for the photodecomposition water under Xe lamp irradiation. The results showed that the ternary TiO2/CuO/Cu thoroughly mesoporous nanofibers exhibit a robust stability and the most efficient photocatalytic H2 evolution with the highest release rate of ∼851.3 μmol g(-1) h(-1), which was profoundly enhanced for more than 3.5 times with respect to those of the pristine TiO2 counterparts and commercial P25, suggesting their promising applications in clean energy production.

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Recently, preparation of mesoporous fibers has attracted extensive attentions because of their unique and broad applications in photocatalysis, optoelectronics, and biomaterials. However, it remains a great challenge to fabricate thoroughly mesoporous nanofibers with high purity and uniformity. Here, we report a general, simple and cost-effective strategy, namely, foaming-assisted electrospinning, for producing mesoporous nanofibers with high purity and enhanced specific surface areas. As a proof of concept, the as-fabricated mesoporous TiO2 fibers exhibit much higher photocatalytic activity and stability than both the conventional solid counterparts and the commercially available P25. The abundant vapors released from the introduced foaming agents are responsible for the creation of pores with uniform spatial distribution in the spun precursor fibers. The present work represents a critically important step in advancing the electrospinning technique for generating mesoporous fibers in a facile and universal manner.

Limited light harvesting and charge collection are recognized as grand challenges for the exploration of highly efficient TiO2 photoanodes. To overcome these intrinsic shortcomings, we reported the designed photoanode based on TiO2 nanoarrays with both hydrogenation treatment and surface decoration of carbon quantum dots (CQDs) toward efficient photoelectrochemical water splitting. The results revealed that hydrogenation treatment could cause the formation of oxygen vacancies to suppress the recombination of photoinduced carriers. Meanwhile, the decorated CQDs could not only play as the electron reservoirs to trap photoinduced electrons but also remarkably enhance the solar light harvesting due to their upconversion effect. The as-fabricated photoanodes exhibited a large photocurrent density of ∼3.0 mA/cm2 at 1.23 V versus reversible hydrogen electrode under simulated sunlight, which was the highest one among hydrogenated TiO2 photoanodes ever reported and was ∼6 times that of pristine analogues.

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In the present work, we report a ternary WO 3 /BiVO 4 /ZnO photoanode with boosted PEC efficiency and stability toward highly efficient water splitting. The type-II WO 3 /BiVO 4 heterojunction arrays are firstly prepared by hydrothermal growth of WO 3 nanoplate arrays onto the substrates of fluorine-doped tin oxide (FTO)-coated glass, followed by spin-coating of BiVO 4 layers onto the WO 3 nanoplate surfaces. After that, thin ZnO layers are further introduced onto the WO 3 /BiVO 4 heterojunction arrays via atomic layer deposition (ALD), leading to the construction of ternary WO 3 /BiVO 4 /ZnO photoanodes. It is verified that the ZnO thin layer in the WO 3 /BiVO 4 /ZnO photoanode contains abundant oxygen vacancies, which could act as an effective passivation layer to enhance the charge separation and surface water oxidation kinetics of photogenerated carriers. The as-prepared WO 3 /BiVO 4 / ZnO photoanode produces a photocurrent of 2.96 mA cm −2 under simulated sunlight with an incident photon-to-current conversion efficiency (IPCE) of ∼72.8% at 380 nm at a potential of 1.23 V versus RHE without cocatalysts, both of which are comparable to the state-of-the-art WO 3 /BiVO 4 counterparts. Moreover, the photocurrent of the WO 3 /BiVO 4 /ZnO photoanode shows only 9% decay after 6 h, suggesting its high photoelectrochemical (PEC) stability.