Electronic structure engineering of single atomic sites by plasmoninduced hot electrons for highly efficient and selective photocatalysis  

作　　者：Xiaoya Huang Xinyuan Li Akang Chen Hongfei Gu Shouyuan Li Tailei Hou Shuwen Zhu Shuang Yu Yin Song Jiatao Zhang 

机构地区：[1]Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications,MIIT Key Laboratory of Medical Molecule Science and Pharmaceutical Engineering,MOE Key Laboratory of Cluster Science,School of Chemistry and Chemical Engineering,School of Materials Science and Engineering,Beijing Institute of Technology,Beijing 100081,China [2]MIIT Key Laboratory of Complex-field Intelligent Exploration,School of Optics and Photonics,Beijing Institute of Technology,Beijing 100081,China

出　　处：《Nano Research》2024年第8期6960-6967,共8页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.22375020,52272186,and 22105116);Beijing Institute of Technology Research Fund Program for Young Scholars.

摘　　要：Single atom(SA)catalysts have achieved great success on highly selective heterogeneous catalysis due to their abundant and homogeneous active sites.The electronic structures of these active sites,restrained by their localized coordination environments,significantly determine their catalytic performances,which are difficult to manipulate.Here,we investigated the effect of localized surface plasmon resonance(LSPR)on engineering the electronic structures of single atomic sites.Typically,core–shell structures consisted of Au core and transition metal SAs loaded N-doped carbon(CN)shell were constructed,namely Au@M-SA/CN(M=Ni,Fe,and Co).It was demonstrated that plasmon-induced hot electrons originated from Au were directionally injected to the M-SAs under visible light irradiation,which significantly changed their electronic structures and meanwhile facilitated improved overall charge separation efficiency.The as-prepared Au@Ni-SA/CN exhibited highly efficient and selective photocatalytic CO_(2) reduction to CO performance,which is 20.8,17.5,and 6.9 times those of Au nanoparticles,Au@CN,and Ni-SA/CN,respectively.Complementary spectroscopy analysis and theoretical calculations confirmed that the plasmon enhanced Ni-SA/CN sites featured increased charge density for efficient intermediate activation,contributing to the superb photocatalytic performance.The work provides a new insight on plasmon and atomic site engineering for efficient and selective catalysis.

关 键 词：single atom catalysts plasmon enhancement coupling effect PHOTOCATALYSIS CO_(2) reduction 

分 类 号：O64[理学—物理化学]