Photocatalytic reduction of CO2 into valuable fuels is one of the potential strategies to solve the carbon cycle and energy crisis.Graphitic carbon nitride(g-C3N4),as a typical two-dimensional(2D)semicon-ductor with a bandgap of～2.7 eV,has attracted wide attention in photocatalytic CO2 reduction.How-ever,the performance of g-C3N4 is greatly limited by the rapid recombination of photogenerated charge carriers and weak CO2 activation capacity.Construction of van der Waals heterostructure with the max-imum interface contact area can improve the transfer/seperation efficiency of interface charge carriers.Ultrathin metal antimony(Sb)nanosheet(antimonene)with high carrier mobility and 2D layered struc-ture,is a good candidate material to construct 2D/2D Sb/g-C3N4 van der Waals heterostructure.In this work,the density functional theory(DFT)calculations indicated that antimonene has higher carrier mo-bility than g-C3N4 nanosheets.Obvious charge transfer and in-plane structure distortion will occur at the interface of Sb/g-C3N4,which endow stronger CO2 activation ability on di-coordinated N active site.The ultrathin g-C3N4 and antimonene nanosheets were prepared by ultrasonic exfoliation method,and Sb/g-C3N4 van der Waals heterostructures were constructed by self-assembly process.The photolumi-nescence(PL)and time-resolved photoluminescence(TRPL)indicated that the Sb/g-C3N4 van der Waals heterostructures have a better photogenerated charge separation efficiency than pure g-C3N4 nanosheets.In-situ FTIR spectroscopy demonstrated a stronger ability of CO2 activation to*COOH on Sb/g-C3N4 van der Waals heterostructure.As a result,the Sb/g-C3N4 van der Waals heterostructures showed a higher CO yield with 2.03 umol g-1 h-1,which is 3.2 times that of pure g-C3N4.This work provides a reference for activating CO2 and promoting CO2 reduction by van der Waals heterostructure.

Jinfeng Zhang;Junwei Fu;Kai Dai

Key Laboratory of Green and Precise Synthetic Chemistry and Applications,Ministry of Education,Huaibei Normal University,Huaibei 235000,China;School of Physics and Electronics,Central South University,Changsha 410083,China

材料科学技术（英文版）

[1]Jinfeng Zhang;Junwei Fu;Kai Dai-.Graphitic carbon nitride/antimonene van der Waals heterostructure with enhanced photocatalytic CO2 reduction activity)[J].材料科学技术（英文版）,2022(21):192-198

antimonene,seperation

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