It is of great significance to construct heterojunctions using industrially produced co-catalysts. The direct Z-scheme composite photocatalyst provides an effective separation of photogenerated carriers. Herein, a kind of novel 2D/3D direct Z-scheme NiFe-LDH/Zn 0.5 Cd 0.5 S is prepared. Compared with fresh catalysts, the NiFe-layered double hydroxide (LDH)/Zn 0.5 Cd 0.5 S composite exhibits advantages including excellent visible light response ability and photoelectric performance and improved H 2 evolution rate by 11.6 times. Combining with theoretical calculations, ESR, XPS, and experimental results, the direct Z-scheme mechanism of the photocatalytic reaction is proposed. There is a channel for electron transfer between Zn 0.5 Cd 0.5 S and NiFe-LDH, and the electrons of Zn 0.5 Cd 0.5 S directly combine with the valence band holes of NiFe-LDH. Finally, the electrons remaining on NiFe-LDH can reduce H + to generate H 2 . This process effectively achieves separation of photogenerated carriers and increases photocatalytic H 2 evolution.
The electrochemical CO2 reduction to desired chemical feedstocks is of importance, yet it is still challenging to obtain high production selectivity with low overpotential at a current density surpassing the industry benchmark of 100 mA cm−2. Herein, we constructed a low‐cost Zn single‐atom anchored on curved N‐doped carbon nanofibers (Zn SAs/N−C) by a facile noncovalent self‐assembly approach. At a low overpotential of only 330 mV, the Zn SAs/N−C exhibited simultaneously both a high current density up to 121.5 mA cm−2 and a CO FE of 94.7 %, superior to the previous reports. Experiments and DFT calculations revealed that the Zn atoms in Zn−N4 acted as the active sites, while adjacent pyridine‐N coupled with Zn−N4 could synergistically decrease the free energy barrier for intermediate *COOH formation. Importantly, the curvature of catalyst induced Zn 3d electrons that were bound to the Zn−N bonds to return to Zn atom, thereby leading to an increase in electron density of Zn and accelerating CO2 electroreduction to CO.
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