posted on 2022-01-27, 19:15authored byMinghui Sun, Xiaoguang Wang, Yi Li, Honghui Pan, Muthu Murugananthan, Yidong Han, Jie Wu, Ming Zhang, Yanrong Zhang, Zhenhui Kang
The
coupling of H2O and O2 by solar energy
is regarded as the Holy Grail reaction for a manufacturing route of
H2O2; however, its efficiency has suffered from
low O2 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
O2 for H2O2 photosynthesis, the most
important of which is the superhydrophobic photocatalyst of amino-containing
ligands combined with Pd, loaded on BiVO4 (Pd/A/BiVO4). This relatively separated catalyst and product system successfully
avoids the decomposition of produced H2O2 and
contributes to the accumulation of a high-concentration H2O2 solution. The enrichment of O2 and the kinetics
of carriers and reaction intermediates are tunable via the interaction
between Pd and amino groups, which promotes the photosynthetic yield
of H2O2 to 805.9 μmol g–1 h–1 in pure water under visible illumination.
During the reaction, O2 is not only converted into H2O2 as a reactant but also participates in the construction
of Pd-Ox sites as a dynamic catalyst.
Also, the Pd-Ox intermediate is identified
as a catalytic and photoelectronic dual center. This research opens
up an intriguing avenue for designing the H2O2 photosynthesis system.