TY - JOUR
T1 - Solid Base Bi24O31Br10(OH)δ with Active Lattice Oxygen for the Efficient Photo-Oxidation of Primary Alcohols to Aldehydes
AU - Dai, Yitao
AU - Ren, Pengju
AU - Li, Yaru
AU - Lv, Dongdong
AU - Shen, Yanbin
AU - Li, Yongwang
AU - Niemantsverdriet, Hans
AU - Besenbacher, Flemming
AU - Xiang, Hongwei
AU - Hao, Weichang
AU - Lock, Nina
AU - Wen, Xiaodong
AU - Lewis, James P.
AU - Su, Ren
N1 - Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2019/5/6
Y1 - 2019/5/6
N2 - The selective oxidation of primary alcohols to aldehydes by O2 instead of stoichiometric oxidants (for example, MnVII, CrVI, and OsIV) is an important but challenging process. Most heterogeneous catalytic systems (thermal and photocatalysis) require noble metals or harsh reaction conditions. Here we show that the Bi24O31Br10(OH)δ photocatalyst is very efficient in the selective oxidation of a series of aliphatic (carbon chain from C1 to C10) and aromatic alcohols to their corresponding aldehydes/ketones under visible-light irradiation in air at room temperature, which would be challenging for conventional thermal and light-driven processes. High quantum efficiencies (71 % and 55 % under 410 and 450 nm irradiation) are reached in a representative reaction, the oxidation of isopropanol. We propose that the outstanding performance of the Bi24O31Br10(OH)δ photocatalyst is associated with basic surface sites and active lattice oxygen that boost the dehydrogenation step in the photo-oxidation of alcohols.
AB - The selective oxidation of primary alcohols to aldehydes by O2 instead of stoichiometric oxidants (for example, MnVII, CrVI, and OsIV) is an important but challenging process. Most heterogeneous catalytic systems (thermal and photocatalysis) require noble metals or harsh reaction conditions. Here we show that the Bi24O31Br10(OH)δ photocatalyst is very efficient in the selective oxidation of a series of aliphatic (carbon chain from C1 to C10) and aromatic alcohols to their corresponding aldehydes/ketones under visible-light irradiation in air at room temperature, which would be challenging for conventional thermal and light-driven processes. High quantum efficiencies (71 % and 55 % under 410 and 450 nm irradiation) are reached in a representative reaction, the oxidation of isopropanol. We propose that the outstanding performance of the Bi24O31Br10(OH)δ photocatalyst is associated with basic surface sites and active lattice oxygen that boost the dehydrogenation step in the photo-oxidation of alcohols.
KW - active lattice oxygen
KW - photo-oxidation
KW - primary alcohols
KW - solid base
KW - visible-light photocatalysis
UR - https://www.scopus.com/pages/publications/85062374118
U2 - 10.1002/anie.201900773
DO - 10.1002/anie.201900773
M3 - 文章
C2 - 30737874
AN - SCOPUS:85062374118
SN - 1433-7851
VL - 58
SP - 6265
EP - 6270
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 19
ER -