Photocatalytic hydrogen evolution based on the use of carbon nitride (CN) catalyst offers a sustainable route to convert solar energy into hydrogen energy; however, its activity is severely restricted by the sluggish transfer of photogenerated charges. Herein, we report a novel approach involving boron (B) doping-induced π-electron delocalization in CN for efficient hydrogen (H2) evolution. The as-prepared B-doped CN (BCN) catalyst presented an 8.6-fold enhancement in the H2-evolution rate (7924.0 μmol h−1 g−1) under visible-light irradiation compared with pristine CN, which corresponded to an apparent quantum yield (AQY) of 14.5% at 405 nm. Experimental analysis and density functional theory (DFT) calculations demonstrated that B doping induced π-electron delocalization in conjugated CN rings to generate a new intermediate state within the band gap to provide a new transfer path for visible-light utilization, thus achieving the high separation and transfer of photoinduced carriers. This work provides a new approach to adjust the electronic structure of CN-like conjugated polymer semiconductors for efficient catalytic energy conversion.
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In recent years, research concerning layered double hydroxides (LDHs) topological transformation materials in the field of photocatalysis and electrocatalysis, such as hydrogen production, and chemical transformation of C1 species, has been widely reported. Research shows that not only the dispersion of active site can be improved, but also phase composition, specific crystal plane and interface structure can be regulated by selecting different calcination temperature, atmosphere and other topological transformation conditions. This kind of materials thus exhibits superior performance in catalytic conversion and utilization of various energy sources. In this review, we will introduce the process and mechanism of LDHs topological transformation, and then review the research progress of LDHs topological transformation materials in energy catalysis from the aspects of photocatalysis and electrocatalysis.
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