Artificial ammonia synthesis using solar energy is of great significance as it can help narrow the gap to the zero-net emission target.However,the current photocatalytic activity is generally too low for mass production.Herein,we report a novel bismuth bromide oxide(BiOBr)-Tetracyanoquinodimethane(TCNQ)photocatalyst prepared via a facile self-assembly method.Due to the well-match band structure of TCNQ and BiOBr,the separation and transfer of photogenerated electron-hole pairs were significantly boosted.More importantly,the abundant delocalized π electrons of TCNQ.and the electron-withdrawing property of TNCQ made electrons efficiently accumulated on the catalysts,which can strengthen the adsorption and cleavage of nitrogen molecules.As a result,the photocatalytic activity increased significantly.The highest ammonia yield of the optimized sample reached 2.617 mg/(h gcat),which was 5.6-fold as that of pristine BiOBr and higher than the reported BiOBr-based photocatalysts.The isotope labeled 15N2 was used to confirm that the ammonia is formed form the fixation of N2.Meanwhile,the sample also had good stability.After 4-time usage,the photocatalysts still had about 81.8％as the fresh sample.The results of this work provide a new way for optimizing the electronic structure of photocatalysts to achieve highly efficient photochemical N2 reduction.

Derek Hao;Tianyi Ma;Baohua Jia;Yunxia Wei;Xiaojuan Bai;Wei Wei;Bing-Jie Ni

Centre for Technology in Water and Wastewater(CTWW),School of Civil and Environmental Engineering,University of Technology Sydney(UTS),Sydney NSW 2007,Australia;Centre for Translational Atomaterials,Faculty of Science,Engineering and Technology,Swinburne University of Technology,Hawthorn,VIC 3122,Australia;College of Chemistry and Chemical Engineering,Lanzhou City University,Lanzhou 730070,China;Beijing Engineering Research Center of Sustainable Urban Sewage System Construction and Risk Control,Beijing University of Civil Engineering and Architecture,Beijing 102612,China

材料科学技术（英文版）

[1]Derek Hao;Tianyi Ma;Baohua Jia;Yunxia Wei;Xiaojuan Bai;Wei Wei;Bing-Jie Ni-.Small molecule π-conjugated electron acceptor for highly enhanced photocatalytic nitrogen reduction of BiOBr)[J].材料科学技术（英文版）,2022(14):276-281

Tetracyanoquinodimethane,TNCQ

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