The coupling of H 2 O and O 2 by solar energy is regarded as the Holy Grail reaction for a manufacturing route of H 2 O 2 ; however, its efficiency has suffered from low O 2 solubility in aqueous solution and difficult-to-inhibit side reactions. Herein, a liquid−solid−gas triphase system has been designed to directly utilize abundant atmospheric O 2 for H 2 O 2 photosynthesis, the most important of which is the superhydrophobic photocatalyst of amino-containing ligands combined with Pd, loaded on BiVO 4 (Pd/A/BiVO 4 ). This relatively separated catalyst and product system successfully avoids the decomposition of produced H 2 O 2 and contributes to the accumulation of a high-concentration H 2 O 2 solution. The enrichment of O 2 and the kinetics of carriers and reaction intermediates are tunable via the interaction between Pd and amino groups, which promotes the photosynthetic yield of H 2 O 2 to 805.9 μmol g −1 h −1 in pure water under visible illumination. During the reaction, O 2 is not only converted into H 2 O 2 as a reactant but also participates in the construction of Pd-O x sites as a dynamic catalyst. Also, the Pd-O x intermediate is identified as a catalytic and photoelectronic dual center. This research opens up an intriguing avenue for designing the H 2 O 2 photosynthesis system.
A binary component catalyst consists of single atoms (SAs-Pt and Au) anchored on self-doped TiO 2 nanotubes (TNTs), was developed for photocatalytic CO 2 reduction. The defects introduced TNTs substrate was stabilized with atomic Pt and Au via strong metal support interactions (MSI), due to which, the covalent interactions of Pt-O and Au-Ti facilitated an effective transfer of photo-generated electrons from the defective sites to the SAs, and in turn an enhanced separation of electron-hole pairs and charge-carrier transmission. The Pt-Au/R-TNTs with 0.33 wt% of SA metals, exhibited a maximum of 149 times higher photocatalytic performance than unmodi ed R-TNT and a total apparent quantum yield (AQY) of 17.9%, in which the yield of CH 4 and C 2 H 6 reached to 360.0 and 28.8 µmol g − 1 h − 1 , respectively.The metals loading shifted the oxidation path of H 2 O from •OH generation into O 2 evolution, that inhibited the self-oxidization of the photocatalyst.
The selective conversion of dilute NO pollutant into low-toxic product and simultaneous storage of metabolic nitrogen for crop plants remains a great challenge from the perspective of waste management and sustainable chemistry. This study demonstrates that this bottleneck can be well tackled by refining the reactive oxygen species (ROS) on Ni-modified NH 2 -UiO-66(Zr) (Ni@NU) using nickel foam (NF) as a three-dimensional (3D) substrate through a flow photoanode reactor via the gas-phase photoelectrocatalysis. By rationally refining the ROS to * OH, Ni@NU/NF can rapidly eliminate 82 % of NO without releasing remarkable NO 2 under a low bias voltage (0.3 V) and visible light irradiation. The abundant mesoporous pores on Ni@NU/NF are conducive to the diffusion and storage of the formed nitrate, which enables the progressive conversion NO into nitrate with selectivity over 99 % for long-term use. Through calculation, 90 % of NO could be recovered as the nitrate species, indicating that this state-of-the-art strategy can capture, enrich and recycle the pollutant N source from the atmosphere. This study offers a new perspective of NO pollutant treatment and sustainable nitrogen exploitation, which may possess great potential to the development of highly efficient air purification systems for industrial and indoor NO x control.
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