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Transition from Core-Shell to Janus Segregation Pattern in AgPd Nanoalloy by Ni Doping for the Formate Oxidation
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-03-06 , DOI: 10.1016/j.apcatb.2020.118861
Qiao Wang , Fuyi Chen , Quan Tang , Longfei Guo , Tesfaye Tadesse Gebremariam , Tao Jin , Huazhen Liu , Bo Kou , Zhen Li , Weiqi Bian

Developing the nanoalloys with well-designed chemical ordering and understanding the correlation between the chemical ordering and catalytic property remain a challenge, yet represent an effective strategy to improve the performance of the nanoalloys. Herein, three AgPd-based nanoalloys with different composition-segregation types, namely, alloy (mixed-Ag19Pd72Ni9), core-shell (core-shell-Ag40Pd60) and janus (janus-Ag20Pd60Ni20) atomic arrangements, are developed via a successive co-reduction method and used in the formate oxidation reaction (FOR). The janus-Ag20Pd60Ni20 nanoalloy exhibits an electrocatalytic activity of 1.31 A mgPd−1 and remarkable long-term stability, outperforming the commercial Pd/C catalysts. The FOR activity follows the order of janus-Ag20Pd60Ni20 > core-shell-Ag40Pd60 > mixed-Ag19Pd72Ni9 nanoalloys. After galvanic replacement and acid treatment, the obtained galvanic-Ag20Pd60Ni20 and acid-Ag20Pd60Ni20 nanoalloys demonstrate 2.31 and 1.44 times higher mass activity than the janus-Ag20Pd60Ni20 nanoalloy. The improvements in the activity and stability can be attributed to largely increased Pd active sites on the surface of AgPd-based nanoalloys with optimal chemical ordering.



中文翻译:

Ni掺杂进行甲酰氧化从AgPd纳米合金从核-壳向Janus偏析的转变

开发具有良好设计的化学有序性的纳米合金并了解化学有序性和催化性能之间的相关性仍然是一个挑战,但仍代表着一种改善纳米合金性能的有效策略。本文中,三种具有不同组成-分离类型的基于AgPd的纳米合金分别为合金(混合Ag 19 Pd 72 Ni 9),核-壳(core-shell-Ag 40 Pd 60)和janus(janus-Ag 20 Pd 60) Ni 20原子排列是通过连续的共还原方法开发的,并用于甲酸氧化反应(FOR)中。janus-Ag 20 Pd 60 Ni20纳米合金具有1.31 A mg Pd -1的电催化活性和显着的长期稳定性,优于市售Pd / C催化剂。FOR活性遵循janus-Ag 20 Pd 60 Ni 20 >核-壳-Ag 40 Pd 60 >混合Ag 19 Pd 72 Ni 9纳米合金的顺序。经过电置换和酸处理后,得到的电-Ag 20 Pd 60 Ni 20和酸-Ag 20 Pd 60 Ni 20纳米合金的质量活性比janus-Ag 20 Pd 60 Ni 20纳米合金高2.31倍和1.44倍。活性和稳定性的改善可归因于具有最佳化学有序性的基于AgPd的纳米合金表面上Pd活性位点的大量增加。

更新日期:2020-03-06
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