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Lattice and Surface Engineering of Ruthenium Nanostructures for Enhanced Hydrogen Oxidation Catalysis
Authors:Yuanting Dong  Qintao Sun  Changhong Zhan  Juntao Zhang  Hao Yang  Tao Cheng  Yong Xu  Zhiwei Hu  Chih-Wen Pao  Hongbo Geng  Xiaoqing Huang
Affiliation:1. State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 China;2. Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123 China;3. Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology, Guangzhou, 510006 China;4. Max Planck Institute for Chemical Physics of Solids, Nothnitzer Strasse 40, 01187 Dresden, Germany;5. National Synchrotron Radiation Research Center, 101 Hsin-Ann Road, Hsinchu, 30076 Taiwan;6. School of Materials Engineering, Changshu Institute of Technology, Changshu, 215500 China
Abstract:Ru has recently been considered as a promising alternative of Pt toward hydrogen oxidation reaction (HOR) due to its lower price and similar hydrogen binding energy (HBE) in comparison to Pt. Nevertheless, the catalytic performance of Ru toward HOR is far from the satisfaction of practical application. Herein, it is demonstrated that the modification of Ru multi-layered nanosheet (MLNS) with Ni can significantly promote the HOR performance. In particular, the HOR performance is strongly related to the Ni location on the surface or in the lattice of Ru MLNS. Experimental and theoretical investigations suggest that Ni in the lattice of Ru MLNS (lattice engineering) optimizes the HBE, while Ni species on the surface (surface engineering) decrease the free energy of water formation, as a result of the significantly enhanced HOR performance. The optimal catalyst, where Ni is located both on the surface and in the lattice, displays superior alkaline HOR performance to commercial Pt/C and Ru/C. The present study not only systematically reveals the significance of Ni modification on Ru toward HOR, but also promotes the fundamental researches on catalyst design for fuel cell reactions and beyond.
Keywords:hydrogen oxidation reactions  lattice engineering  Ni modifications  Ru  surface engineering
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