%0 Journal Article
%T Breaking Trade©\Off between Selectivity and Activity of Nickel©\Based Hydrogenation Catalysts by Tuning Both Steric Effect and d©\Band Center
%A Huiwen Wang
%A Li Wang
%A Lun Pan
%A Ruijie Gao
%A Xiangwen Zhang
%A Yunduo Yao
%J Archive of "Advanced Science".
%D 2019
%R 10.1002/advs.201900054
%X For selective hydrogenation of chemicals the high selectivity is always at the expense of activity and improving both selectivity and activity is challenging. Here, by chelating with p©\fluorothiophenol (SPhF)©\arrays, both steric and electronic effects are created to boost the performance of cheap nickel©\based catalysts. Compared with dinickel phosphide, the SPhF©\chelated one exhibits nearly 12 times higher activity and especially its selectivity is increased from 38.1% and 21.3% to nearly 100% in hydrogenations of 3©\nitrostyrene and cinnamaldehyde. Commercial catalysts like Raney Ni chelating with SPhF©\array also exhibits an enhanced selectivity from 20.5% and 23.4% to ¡Ö100% along with doubled activity. Both experimental and density functional theory (DFT) calculation prove that the superior performance is attributed to the confined flat adsorption by ordered SPhF©\arrays and downshifted d©\band center of catalysts, leading to prohibited hydrogenation of the vinyl group and accelerative H2 activation. Such a surface modification can provide an easily©\realized and low©\cost way to design catalysts for the selective hydrogenation
%K d©\band center
%K Ni2P
%K selective hydrogenation
%K steric effects
%K thiol©\arrays
%U https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6523378/