title: Au Sub-Nanoclusters on TiO2toward Highly Efficient and Selective Electrocatalyst for N2Conversion to NH3at Ambient Conditions.
abstract: As the NN bond in N2is one of the strongest bonds in chemistry, the fixation of N2to ammonia is a kinetically complex and energetically challenging reaction and, up to now, its synthesis is still heavily relying on energy and capital intensive Haber-Bosch process (150-350 atm, 350-550 °C), wherein the input of H2and energy are largely derived from fossil fuels and thus result in large amount of CO2emission. In this paper, it is demonstrated that by using Au sub-nanoclusters (≈0.5 nm ) embedded on TiO2(Au loading is 1.542 wt%), the electrocatalytic N2reduction reaction (NRR) is indeed possible at ambient condition. Unexpectedly, NRR with very high and stable production yield (NH3: 21.4 µg h-1mg-1cat., Faradaic efficiency: 8.11%) and good selectivity is achieved at -0.2 V versus RHE, which is much higher than that of the best results for N2fixation under ambient conditions, and even comparable to the yield and activation energy under high temperatures and/or pressures. As isolated precious metal active centers dispersed onto oxide supports provide a well-defined system, the special structure of atomic Au cluster would promote other important reactions besides NRR for water splitting, fuel cells, and other electrochemical devices.
authors.affiliation: Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, Department of Materials Science and Engineering, Jilin University, Changchun, 130022, China.
authors.forename: Miao-Miao
authors.initials: MM
authors.lastname: Shi
authors.affiliation: Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, Department of Materials Science and Engineering, Jilin University, Changchun, 130022, China.|State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China.
authors.forename: Di
authors.initials: D
authors.lastname: Bao
authors.affiliation: Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, Department of Materials Science and Engineering, Jilin University, Changchun, 130022, China.
authors.forename: Ba-Ri
authors.initials: BR
authors.lastname: Wulan
authors.affiliation: Institute of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, 100124, P. R. China.
authors.forename: Yong-He
authors.initials: YH
authors.lastname: Li
authors.affiliation: Institute of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, 100124, P. R. China.
authors.forename: Yue-Fei
authors.initials: YF
authors.lastname: Zhang
authors.affiliation: Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, Department of Materials Science and Engineering, Jilin University, Changchun, 130022, China.
authors.forename: Jun-Min
authors.initials: JM
authors.lastname: Yan
authors.affiliation: Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, Department of Materials Science and Engineering, Jilin University, Changchun, 130022, China.
authors.forename: Qing
authors.initials: Q
authors.lastname: Jiang
keywords: Au sub-nanoclusters; electrocatalyst; electrochemical N2 reduction; nitrogen fixation; size-effect