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Investigation on Electron Distribution and Synergetic to Enhance Catalytic Activity in Bimetallic Ni(II)/Pd(II) Molecular Monolayer
Author(s) -
Huang Pingping,
Xue Ziqian,
Li Tiesheng,
Liu Zhongyi,
Wei Donghui,
Liu Minghua,
Wu Yangjie
Publication year - 2018
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201801350
Subject(s) - diimine , bimetallic strip , catalysis , palladium , nickel , materials science , monolayer , electron transfer , inorganic chemistry , photochemistry , chemistry , nanotechnology , organic chemistry , metallurgy
Novel graphene oxide (GO)‐supported ordered diimine Ni/Pd bimetallic monolayers with ratio of Ni to Pd atomic ratios (2136 : 1, 333 : 1 and 97 : 1) (denoted as GO‐Diimine‐Ni/Pd1, GO‐Diimine‐Ni/Pd2, GO‐Diimine‐Ni/Pd3) were fabricated and their catalytic performances and synergetic mechanism were systematic investigated. For the as‐prepared GO‐Diimine‐Ni/Pd1, that trace palladium complex was responded for changing the electronic environment, tuning catalytic actives and modifying the electronic states which could enhance the highlighted catalytic activity. The more dramatic aspect of the GO‐Diimine‐Ni/Pd1 with high efficient catalytic activity could be achieved even with atom ratio of Ni/Pd even in 2136 : 1 (TOF Ni =21277 h −1 ; TOF Pd =4.545×10 7 h −1 ), in which the noble Pd could almost be replaced by non‐noble Ni according to requirement for economic chemistry. Interestingly, the synergetic mechanism between nickel and palladium was that the electron of Pd may transfer to Ni, which is different from the conventional Pd/Ni for catalyzing coupling reaction. Especially, the formation of Ni 0 around Pd (II) as active centers was proposed and its size could be controlled with adjusting the palladium content on the surface. The results exhibited that the synergic effect between Ni and Pd made it easy for Ni 2+ reduced into Ni 0 . It was crucial for adjusting the catalytic activity by designing the fine structure of ligand, the supports selection and modulating the Pd content at the molecular level.