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@ARTICLE{Yin:631478,
author = {Yin, Zhaohui and Gao, Zirui and Luo, Lan and Zhang, Xiaohui
and Hou, Wenxiang and Dai, Wenjing and Tian, Shuheng and
Qin, Xuetao and Wang, Maolin and Peng, Mi and Li, Kaihua and
Wang, Songbo and Zhang, Lei and Wang, Hong and Li, Jianxin
and Zhu, Qingjun and Cheng, Bowen and Yin, Zhen and Ma,
Ding},
title = {{A} {G}reen and {E}fficient {E}lectrocatalytic {R}oute for
the {H}ighly‐{S}elective {O}xidation of {C}−{H} {B}onds
in {A}romatics over 1{D} {C}o$_3${O}$_4$ ‐{B}ased
{N}anoarrays},
journal = {Angewandte Chemie},
volume = {137},
number = {3},
issn = {0932-2132},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {PUBDB-2025-01990},
pages = {e202415044},
year = {2025},
note = {Waiting for fulltext},
abstract = {Electrocatalytic oxidation of C−H bonds in hydrocarbons
represents an efficient and sustainable strategy for the
synthesis of value-added chemicals. Herein, a highly
selective and continuous-flow electrochemical oxidation
process of toluene to various oxygenated products (benzyl
alcohol, benzaldehyde, and benzyl acetate) is developed with
the electrocatalytic membrane electrodes (ECMEs). The
selectivity of target products can be manipulated via
surface and interface engineering of Co$_3$O$_4$-based
electrocatalysts. We achieved a high benzaldehyde
selectivity of 90 \% at a toluene conversion of 47.6 \%
using 1D Co$_3$O$_4$ nanoneedles (NNs) loaded on a
microfiltration (MF) titanium (Ti) membrane, i.e,
Co$_3$O$_4$ NNs/Ti. In contrast, the main product shifted to
benzyl alcohol with a selectivity of 90.1 \% at a
conversion of 32.1 \% after modifying MnO2 nanosheets
(NSs) on Co3O4 NNs/Ti (Co$_3$O$_4$@MnO$_2$/Ti) catalyst.
Moreover, benzyl acetate product can be obtained with a
selectivity of 92 \% at a conversion of 58.5 \% at high
current density (>1.5 mA cm−2), demonstrating that the
pathway of toluene oxidation is readily maneuvered. DFT
results reveal that modifying MnO$_2$ on Co$_3$O$_4$
optimizes the electron structure of Co$_3$O$_4$@MnO$_2$/Ti
and modulates the adsorption behavior of intermediate
species. This work demonstrates a sustainable, efficient,
and continuous-flow process for precise control over the
production selectivity of value-added oxygenated derivatives
in the electrochemical oxidation of aromatic hydrocarbons.},
cin = {$Z_PITZ$},
ddc = {660},
cid = {$I:(DE-H253)Z_PITZ-20210408$},
pnm = {621 - Accelerator Research and Development (POF4-621)},
pid = {G:(DE-HGF)POF4-621},
experiment = {EXP:(DE-MLZ)NOSPEC-20140101},
typ = {PUB:(DE-HGF)16},
doi = {10.1002/ange.202415044},
url = {https://bib-pubdb1.desy.de/record/631478},
}