Tuning Crystal Phase of Palladium–Selenium Nanowires for Enhanced Ethylene Glycol Electrocatalytic Oxidation

作者：Liping Wang, Wei Yan, Qingping Yu, Liangbin Liu, Cheng‐Wei Kao, Yucheng Huang, Ting‐Shan Chan, Zhiwei Hu, Haixin Lin, Dazhi Shen, Xiaoqing Huang, Yunhua Li · 发表于：Small · 年份：2024 · DOI：10.1002/smll.202403448 · 被引用次数：19 · 研究领域：Electrocatalysts for Energy Conversion、Catalytic Processes in Materials Science、Advanced battery technologies research

Abstract Alcohol electrooxidation is pivotal for a sustainable energy economy. However, designing efficient electrocatalysts for this process is still a formidable challenge. Herein, palladium–selenium nanowires featuring distinct crystal phases: monoclinic Pd 7 Se 2 and tetragonal Pd 4.5 Se for ethylene glycol electrooxidation reaction (EGOR) are synthesized. Notably, the supported monoclinic Pd 7 Se 2 nanowires ( m ‐Pd 7 Se 2 NWs/C) exhibit superior EGOR activity, achieving a mass activity (MA) and specific activity (SA) of 10.4 A mg Pd −1 (18.7 mA cm −2 ), which are 8.0 (6.7) and 10.4 (8.2) times versus the tetragonal Pd 4.5 Se and commercial Pd/C and surpass those reported in the literature. Furthermore, m ‐Pd 7 Se 2 NWs/C displays robust catalytic activity for other alcohol electrooxidation. Comprehensive characterization and density functional theory (DFT) calculations reveal that the enhanced electrocatalytic performance is attributed to the increased formation of Pd 0 on the high‐index facets of the m ‐Pd 7 Se 2 NWs, which lowers the energy barriers for the C─C bond dissociation in CHOHCHOH* and the CO* oxidation to CO 2 *. This study provides palladium‐based alloy electrocatalysts exhibiting the highest mass activity reported to date for the electrooxidation of ethylene glycol, achieved through the crystalline phase engineering strategy.