TY - JOUR
T1 - Construction of Highly Active and Selective Molecular Imprinting Catalyst for Hydrogenation
AU - He, Dongcheng
AU - Li, Teng
AU - Dai, Xingchao
AU - Liu, Shujuan
AU - Cui, Xinjiang
AU - Shi, Feng
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/9/27
Y1 - 2023/9/27
N2 - Surface molecular imprinting (MI) is one of the most efficient techniques to improve selectivity in a catalytic reaction. Heretofore, a prerequisite to fabricating selective catalysts by MI strategies is to sacrifice the number of surface-active sites, leading to a remarkable decrease of activity. Thus, it is highly desirable to design molecular imprinting catalysts (MICs) in which both the catalytic activity and selectivity are significantly enhanced. Herein, a series of MICs are prepared by sequentially adsorbing imprinting molecules (nitro compounds, N) and imprinting ligand (1,10-phenanthroline, L) over the copper surface of Cu/Al2O3. The resulting Cu/Al2O3-N-L MICs not only offer promoted catalytic selectivity but also enhance catalytic activity for nitro compounds hydrogenation by an creating imprinting cavity derived from the presorption of N and forming new active Cu-N sites at the interface of the copper sites and L. Characterizations by means of various experimental investigations and DFT calculations disclose that the molecular imprinting effect (promoted activity and selectivity) originates from the formation of new active Cu-N sites and precise imprinting cavities, endowing promoted catalytic selectivity and activity on the hydrogenation of nitro compounds.
AB - Surface molecular imprinting (MI) is one of the most efficient techniques to improve selectivity in a catalytic reaction. Heretofore, a prerequisite to fabricating selective catalysts by MI strategies is to sacrifice the number of surface-active sites, leading to a remarkable decrease of activity. Thus, it is highly desirable to design molecular imprinting catalysts (MICs) in which both the catalytic activity and selectivity are significantly enhanced. Herein, a series of MICs are prepared by sequentially adsorbing imprinting molecules (nitro compounds, N) and imprinting ligand (1,10-phenanthroline, L) over the copper surface of Cu/Al2O3. The resulting Cu/Al2O3-N-L MICs not only offer promoted catalytic selectivity but also enhance catalytic activity for nitro compounds hydrogenation by an creating imprinting cavity derived from the presorption of N and forming new active Cu-N sites at the interface of the copper sites and L. Characterizations by means of various experimental investigations and DFT calculations disclose that the molecular imprinting effect (promoted activity and selectivity) originates from the formation of new active Cu-N sites and precise imprinting cavities, endowing promoted catalytic selectivity and activity on the hydrogenation of nitro compounds.
UR - http://www.scopus.com/inward/record.url?scp=85172711784&partnerID=8YFLogxK
U2 - 10.1021/jacs.3c04576
DO - 10.1021/jacs.3c04576
M3 - 文章
C2 - 37722009
AN - SCOPUS:85172711784
SN - 0002-7863
VL - 145
SP - 20813
EP - 20824
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 38
ER -