Strain-Stabilized Metastable Face-Centered Tetragonal Gold Overlayer for Efficient CO₂ Electroreduction

作     者：Yu, Dan Gao, Lei Sun, Tulai Guo, Jingchun Yuan, Yuliang Zhang, Jiawei Li, Mengfan Li, Xingxing Liu, Maochang Ma, Chao Liu, Qinghua Pan, Anlian Yang, Jinlong Huang, Hongwen 

作者机构：Hunan Univ Coll Mat Sci & Engn Adv Catalyt Engn Res Ctr Minist Educ Changsha 410082 Hunan Peoples R China Zhejiang Univ Technol State Key Lab Breeding Base Green Chem Synth Tech Ctr Electron Microscopy Hangzhou 310014 Zhejiang Peoples R China Zhejiang Univ Technol Coll Chem Engn Hangzhou 310014 Zhejiang Peoples R China Univ Sci & Technol China Dept Chem Phys Hefei Natl Lab Phys Sci Microscale Natl Synchrotron Radiat Lab Hefei 230026 Anhui Peoples R China Xi An Jiao Tong Univ Int Res Ctr Renewable Energy State Key Lab Multiphase Flow Power Engn Xian 710049 Shanxi Peoples R China 

出 版 物：《NANO LETTERS》 (纳米快报)

年 卷 期：2021年第21卷第2期

页      面：1003-1010页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学] 

基　　金：NSFC [U2032149, 21905089, U1932212] Hunan Provincial Natural Science Foundation of China [2020JJ2001, 2020JJ3001] Fundamental Research Funds for the Central Universities Youth Innovation Promotion Association CAS 

主　　题：face-centered tetragonal gold metastable phase interface strain CO2 electroreduction 

摘      要：Synthesis of the unconventional phase of noble metal nanocrystals may create new opportunities in exploring intriguing physicochemical properties but remains challenging. In the research field of thin film growth, the interface strain offers a general driving force to stabilize the metastable phase of epitaxial film. Herein we extend this concept to the field of noble metal nanocrystals and report the solution synthesis of metastable face-centered tetragonal Au that has not been discovered before. The successful synthesis relies on the formation of intermetallic AuCu3@Au core-shell structure, where the interface strain stabilizes the metastable fct Au overlayer. Compared with the face-centered cubic Au counterpart, the metastable fct Au shows greatly improved catalytic activity toward CO2 reduction to CO. The density functional theory calculations and spectroscopic studies reveal that the metastable fct Au upshifts the d-band center, which lowers the energy barrier of key intermediate COOH* formation and thus facilitates the reaction kinetics.