Dopamine polymer derived isolated single-atom site metals/N-doped porous carbon for benzene oxidation

Article abstract of DOI:10.1039/d0cc03620j

Isolated single-atom site metals/nitrogen-doped porous carbon (ISAS M/NPC, M = Fe, Co, Ni) catalysts are successfully prepared by a top-down polymerization-pyrolysis-etching-activation (PPEA) strategy, which uses dopamine as the precursor. Due to the isolated single atom Fe active sites and porous structure, the ISAS Fe/NPC catalyst displays a high benzene conversion up to 42.6percent and nearly 100percent phenol selectivity.

Full text of DOI:10.1039/d0cc03620j

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DOI: 10.1039/D0CC03620J
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Dopamine polymer derived isolated single-atom sites metals/N-
doped porous carbon for benzene oxidation†
a,b,c
d
b
e
a
f
Konglin Wu,‡ Fei Zhan,‡ Renyong Tu, Weng-Chon Cheong, Yuansheng Cheng, Lirong Zheng,
Received 00th January 20xx,
Accepted 00th January 20xx
g
h
,c
,b
Wensheng Yan, Qinghua Zhang, Zheng Chen,* and Chen Chen*
DOI: 10.1039/x0xx00000x
Isolated single-atom sites metals/nitrogen-doped porous carbon
(
Recently, the isolated single-atom sites (ISAS) catalysts have
ISAS M/NPC, M = Fe, Co, Ni) catalyst are successfully prepared by attracted wide attention due to their numerous advantages,3
a top-down polymerization-pyrolysis-etching-activation (PPEA) such as low cost, clear catalytic activity center, specific catalytic
strategy, which use dopamine as precursors. Due to the isolated activity, 100% atom utilization, easy separation, etc. Many
single atom Fe active sites and porous structure, the ISAS Fe/NPC researches showed that the ISAS catalyst has become a
4
a
displayed a high benzene conversion up to 42.6% and nearly 100 % research hotspot in the fields of water gas conversion, gas-
4
b, 4c
4d
4e, 4f, 4g
phenol selectivity.
solid catalysis,
enzyme catalysis,
photocatalysis, electrocatalysis,
4
h, 4i
and so on. Meanwhile, the ISAS also brings
Catalysis is the soul of chemistry, the engine of chemical
engineering, and the eternal theme of chemistry and chemical
new opportunities and challenges to the field of organic
reaction, which act the role of bridging between the
homogeneous and heterogeneous catalysis. For example, the
1
engineering. It is generally known that the synthetic ammonia
5
2
and Fischer-Tropsch synthesis have a revolutionary impact on
single Pd atoms decorated on exfoliated graphitic carbon nitride
the human production and life. Thereby, the design and
preparation of catalytic materials is the core content of
catalysis. In many catalytic fields, the noble metal catalysts have
been playing a leading role. The noble metals are needed to be
used as catalysts in the fields of acetylene hydrochlorination,
automobile exhaust gas treatment, fuel cell, electrolytic water,
etc. However, due to the low reserves and high cost of precious
metals, its large-scale use is limited. Therefore, the
development of high-efficiency and low-cost non-noble metal
catalysts to replace or partially replace precious metal catalysts
has been the pursuit of researchers.
6
(
Pd-ECN) catalyst can be used in Suzuki reaction. It is found that
the catalyst has similar catalytic activity with homogeneous
7
catalyst. In the field of small molecule activation, the ISAS
Pt
1
/Ti3-x
C
2
T
y
MXene catalyst provides a green method to
via the high-efficiency formylation of amines
utilizing CO
2
8
reaction. Furthermore, the ISAS catalysts such as RGO@AC/Pd,
9
10
11a
Pt
Fe
1
/Ni nanocrystals,
1
Pt /FeO
x
,
CoSAs/NCNS,
and
/N−C11b can catalyze hydrogenation of nitro compounds with
1
good catalytic activity. Especially, when there are two type
unsaturated bonds in the substrate, i.e. C=C and N=O double
bonds, the selectivity of ISAS catalysts is higher than that of
1
2
commercial catalyst or micro/nanomaterials catalyst. A series
of ISAS catalysts have been used in the C-H activation and
a. Institute of Clean Energy and Advanced Nanocatalysis, School of Chemistry and
Chemical Engineering, Anhui University of Technology, Maanshan 243002, China.
Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China. E-
13–18
transformation,
which show high catalytic activity and
b.
selectivity. As an important reaction, the preparation of phenol
by oxidation of benzene has attracted wide attention. In
previous reports, the benzene can be oxidized to phenol by
mail: cchen@mail.tsinghua.edu.cn.
Center of Single-Atom, Clusters and Nanomaterials (CAN), College of Chemistry
c.
and Materials Science, Anhui Normal University, Wuhu 241002, China. E-mail:
chenzh07@mail.ahnu.edu.cn.
Chemistry and Chemical Engineering of Guangdong Laboratory, Shantou 515063,
1
9
homogeneous catalyst, but the conversion and selectivity are
not high. Thereby, the ISAS catalysts due to their high catalytic
activity and selectivity will bring new opportunities and
challenges for benzene oxidation reaction (BOR).
d.
China
e.
f.
Department of Physics and Chemistry, Faculty of Science and Technology,
University of Macau, Macao, China
Beijing Synchrotron Radiation Facility (NSRF), Chinese Academy of Science, Beijing
Here, we report a top-down polymerization-pyrolysis-
etching-activation (PPEA) strategy by using the dopamine as
basic structural units to construct isolated single-atom sites
metals/nitrogen-doped porous carbon (ISAS M/NPC, M = Fe, Co,
Ni) catalyst materials. The obtained ISAS Fe/NPC can be used as
1
00049, China
g.
National Synchrotron Radiation Laboratory (NSRL), University of Science and
Technology of China, Hefei, Anhui, 230029, China
Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
Electronic Supplementary Information (ESI) available: Experimental procedures,
h.
†
Figures S1-S8, and Tables S1-S6, See DOI: 10.1039/x0xx00000x
These authors contributed equally to this work.
‡
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Journal Name
low-cost heterogeneous catalyst in BOR, and displayed a high are no obvious Fe-based clusters in ISAS Fe/NPCV.ieTwhAerticfluerOtnhliener
conversion to phenol. The selectivity of phenol in ISAS Fe/NPC spherical aberration correction-scanningDtOraI:n1s0m.10is3s9i/oDn0CeCle0c3t6r2o0nJ
catalyst is significantly higher than that of nanoparticles microscope (AC-STEM) image exhibits the Fe atoms (bright
catalyst, which fully demonstrate the unique advantages of white spots in Figure 1d) in the ISAS Fe/NPC are atomically
atomically dispersed metal sites. Furthermore, the top-down dispersed on the substrate. The corresponding energy
PPEA strategy is also applicable to the preparation of other ISAS dispersion spectrum (EDS) elemental mapping results (Figure
catalysts (such as ISAS Co/NPC and ISAS Ni/NPC).
1e) show that Fe and N were observed in the ISAS Fe/NPC. The
metal content in ISAS Fe/NPC catalysts was quantitatively
analyzed by inductively coupled plasma optical emission
spectrometry (ICP-OES, Table S1, ESI†), and the metal loading
content is 1.75wt% for ISAS Fe/NPC. X-ray photoelectron
spectroscopy (XPS) results demonstrate that the Fe, N and C
were observed (Figure S3a, ESI†). The weak Fe2p signal was
obtained (Figure S3b, ESI†) because of the lower Fe loading and
atomically dispersed Fe atoms on the substrate. Figure S3c (ESI†)
shows the N1s spectrum, and three types of graphitic-N (401.7
eV), pyrrolic-N (400.1 eV), and pyridinic-N (398.5 eV) were
found.
Figure 2. (a) XANES spectra and (b) FT-EXAFS spectra for the Fe K-edge of ISAS Fe/NPC,
Figure 1. (a) Schematic illustration for the preparation of ISAS M/NPC catalysts, (b) XRD
patterns of Fe NPs/NPC and ISAS Fe/NPC, (c) TEM image of ISAS Fe/NPC, (d) AC-STEM
image of ISAS Fe/NPC, (e) HAADF-STEM image and the corresponding EDS elemental
mapping images.
Fe foil, FeO, and Fe
3
O
4
; (c) the corresponding EXAFS r space fitting curves of ISAS Fe/NPC,
catalytic site for ISAS Fe/NPC.
(d) structure diagram of Fe-N
4
In order to obtain the detailed structure information of ISAS
Fe/NPC, the X-ray absorption near-edge structure (XANES) and
extended X-ray absorption fine structure (EXAFS) were carried
out. As shown in Figure 2a and Figure S4 (ESI†), the XANES
Figure 1a shows the preparation process of ISAS M/NPC (M =
Fe, Co, Ni) catalysts by PPEA strategy, and the detailed
experimental procedures are shown in Electronic
Supplementary Information (ESI†). Here, we take the synthesis
of ISAS Fe/NPC catalyst as an example for illustration the PPEA
strategy: the dopamine and ferric salt were oxidization
polymerization under alkaline conditions in a mixture of ethanol
and water to form the Fe/polydopamine (FePDA) precursors,
and then the obtained FePDA precursors were pyrolyzed under
3 4
curves for Fe K-edge in ISAS Fe/NPC, Fe foil, FeO, and Fe O
demonstrates that the oxidation state of Fe in ISAS Fe/NPC is
between +2 and +3. This suggests that the Fe has a partial
positive charge due to the coordination of N around the
1
3
atomically dispersed Fe site. Fourier-transformed (FT) EXAFS
3
(
FT-EXAFS) spectrum (k -weighted) for ISAS Fe/NPC (Figure 2b)
shows a main peak at 1.5 Å, which can be attributed to the Fe–
N scattering path. No peak derived from Fe-Fe coordination is
found. The detailed structural parameters were obtained by
quantitative EXAFS fitting of the Fe K-edge in ISAS Fe/NPC, and
the corresponding fitting results are shown in Figure 2c, Figure
S5 (ESI†), and Table S2 (ESI†). The fitting data reveal that one Fe
atom is combined with four N atoms at the first coordination
shell in ISAS Fe/NPC, meanwhile the Fe-N bond length is about
2 2
H /Ar (5% H ) atmosphere at 500 °C for 3 h to get the Fe
nanoparticles/nitrogen doped porous carbon (Fe NPs/NPC,
Figure S1, ESI†). Subsequently, the Fe NPs/NPC were treated by
3
M HCl at 60 °C for 48 h to remove the Fe NPs, and then
products were activated by H /Ar (5% H ) atmosphere at 300 °C
2
2
for 2 h to obtain the ISAS Fe/NPC. For comparison, we also
obtained the nitrogen-doped porous carbon (NPC, Figure S2,
ESI†) without metals. XRD patterns (Figure 1b) show that the Fe
NPs can be removed by HCl treatment. Figure 1c displays there
1
.91 Å. These results further indicate that the atomically
dispersed Fe sites in the ISAS Fe/NPC catalyst are existed in the
2
| J. Name., 2012, 00, 1-3
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form of Fe-N
COMMUNICATION
moieties. Thereby, the possible structure model the ISAS Fe/NPC and NPC were studied by N adsorption–
4
2
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for ISAS Fe/NPC catalyst is shown in Figure 2d. Moreover, the desorption isotherm curves (Figure 3dDaOnI:d10F.1ig0u39r/eD0SC8C, 0E3S6I2†0)J.
ISAS Co/NPC (Figure S6, ESI†) and ISAS Ni/NPC (Figure S7, ESI†) Based on the Brunauer−Emmett−Teller (BET) evaluating
catalysts were also prepared by the same PPEA strategy. The method, the BET specific surface areas and pore sizes were
metal loading contents are 0.74wt% for ISAS Co/NPC and obtained (Table S5, ESI†). Obviously, the ISAS Fe/NPC shows a
0
.31wt% for ISAS Ni/NPC (Table S1, ESI†).
type IV feature (Figure 3d, red line) and the NPC displays a type
I feature (Figure 3d, black line). The BET specific surface area,
2
micropore size, and average pore size are 224 m /g, 1.1 nm, and
2
6
.8 nm for ISAS Fe/NPC, and are 370 m /g, 0.5 nm, and 1.97 nm
for pure NPC.
Table 1. Catalytic BOR by different catalysts.
O
OH
MeCN, catalyst
+
H2O2 , 60 °C, 24 h
O
Selectivityd
Benzene
conversion (%)
Catalyst
d
Phenol (%)
p-benzoquinone (%)
ISAS Fe/NPCa
ISAS Co/NPCa
ISAS Ni/NPCa
Fe NPs/NPCb
NPCa
42.6
16.3
7.1
6.5
1.6
0.4
-
>99
>99
>99
78
90
92
<1
<1
<1
22
10
8
Figure 3. (a) C K-edge and (b) N K-edge for pure NPC and ISAS Fe/NPC, (c) Raman spectra
for pure NPC and ISAS Fe/NPC; (f) N
ISAS Fe/NPC.
2
absorption and desorption curves for pure NPC and
FePDAa
Blankc
-
-
a
Conditions: catalyst, 50 mg; methyl cyanide (MeCN), 3 mL; benzene, 0.1 mL; H
reaction temperature, 60 °C; reaction time, 24 h. Conditions: catalyst, amount of Fe is
kept the same to that in 50 mg of ISAS Fe/NPC; MeCN, 3 mL; benzene, 0.1 mL; H
2
O
2
, 6 mL;
Near edge X-ray absorption fine structure (NEXAFS) was used
to test the structure information of ISAS Fe/NPC and pure NPC.
b
2
O
2
, 6
c
As shown in Figure 3a and Table S3 (ESI†), three distinct peaks mL; reaction temperature, 60 °C; reaction time, 24 h. Conditions: without catalyst;
MeCN, 3 mL; benzene, 0.1 mL; H
2
O
2
, 6 mL; reaction temperature, 60 °C; reaction time,
were observed in C K-edge spectra for ISAS Fe/NPC (red line)
and NPC (black line). The peaks at 283.6 eV and 290.6 eV are
d
2
4 h. Conversion and selectivity were determined by GC-MS and GC analysis.
2
attributed to the dipole transition sp -hybridized carbon of
The catalytic activities of the obtained ISAS M/NPC (M = Fe,
Co, Ni) catalysts in BOR were investigated. As shown in Table
, the catalytic BOR results show that the benzene conversion
for ISAS Fe/NPC is 42.6%, ISAS Co/NPC is 16.3%, and ISAS
Ni/NPC is 7.1%, which is higher than that of pure NPC (1.6%)
without ISAS metals and FePDA precursors (0.6%). Interestingly,
the selectivity of phenol was higher than 99% in all ISAS M/NPC
π*C=C and σ*C–C,20 while the sharp peak at 286.8 eV was sp -
3
1
3
2
0a, 20b
hybridized carbon of π*C–N-C/Fe was observed.
Due to
1
3
the strong interaction between C, N, and Fe, the peak of sp -
hybridized carbon in ISAS Fe/NPC is more sharp than that of
pure NPC, and the peak is also shifted to lower energy.
Meanwhile, the N K-edge spectra (Figure 3b) for ISAS Fe/NPC
(
red line) and NPC (black line) show that the resonances of
peaks a and peaks a , and peaks b are π*-transitions for
pyridinic-N and pyrrolic-N, and the peaks c are σ*-transitions for
(
M = Fe, Co, Ni) catalysts. When the Fe NPs/NPC catalyst was
1
2
used with equivalent Fe content, the benzene conversion and
phenol selectivity are significantly lower, only 6.5% and 78%,
respectively. This further proves that ISAS catalysts can achieve
high selectivity accompanied by high activity. Here, the rich
pore structures of the ISAS Fe/NPC catalyst are conducive to
mass transfer and provides favorable organic molecular
channels for the catalytic reaction. Compared with the
previously reported catalysts for BOR (Table S6, ESI†), the
obtained ISAS M/NPC (M = Fe, Co, Ni) catalysts exhibited
competitive catalytic activities. The above results indicate that
the ISAS catalysts are beneficial to improve the selectivity of
organic reactions.
2
0b, 20c
graphitic-N are observed.
1 2
The peak a and peak a in ISAS
Fe/NPC are sharper than that of NPC, but the peak b in ISAS
Fe/NPC is weaker than that of NPC. Here, the NEXAFS result is
consistent with that of XPS.
Raman spectroscopy was applied to characterize the ISAS
Fe/NPC and NPC. The D and G bands are observed in the Raman
spectra (Figure 3c). As shown in Figure 3c and Table S4 (ESI†),
-
1
-1
the D and G bands are 1348 cm and 1580 cm for NPC (black
-1
-1
line), and the D and G bands are 1353 cm and 1591 cm for
ISAS Fe/NPC (red line), respectively. Compared with pure NPC,
the D band of ISAS Fe/NPC is shifted to the higher wavenumber,
In summary, the high-efficient benzene oxidation catalysts of
isolated single-atom sites metals/nitrogen-doped porous
carbon (ISAS M/NPC-HA, M = Fe, Co, Ni) were successfully
synthesized by a polymerization-pyrolysis-etching-activation
1
3d, 21
indicating that there are abundant defects in ISAS Fe/NPC.
2
Furthermore, the strong G band is assigned to the sp -
hybridized carbon structure and the obvious broad 2D band
demonstrates the presence of layered structures in ISAS
Fe/NPC.21 Moreover, the specific surface areas and porosity of
(
PPEA) strategy. Among them, ISAS Fe/NPC could realize 42.6%
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J. Name., 2013, 00, 1-3 | 3
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Journal Name
6
7
Z. Chen, E. Vorobyeva, S. Mitchell, E. Fako, M. VAie.wOArrttiucleñOon,liNne.
DOI: 10.1039/D0CC03620J
Ramírez, Nat. Nanotech., 2018, 13, 702.
conversion, and the selectivity to phenol for all ISAS catalysts is
higher than 99%. These results show that ISAS catalysts have
high catalytic activity and selectivity in organic reactions, and
which have great potential industrial application value in the
future.
This work was supported by the National Key R&D Program
of China (2017YFA0700101, 2016YFA0202801), the National
Natural Science Foundation of China (21925202, 21872076,
López, S. M. Collins, P. A. Midgley, S. Richard, G. Vilé, J. Pérez-
D. Zhao, Z. Chen, W. Yang, S. Liu, X. Zhang, Y. Yu, W.-C.
Cheong, L. Zheng, F. Ren, G. Ying, X. Cao, D. Wang, Q. Peng, G.
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1590792, 21901007), Beijing Natural Science Foundation
(JQ18007) and Tsinghua University Initiative Scientific Research
Program. We acknowledge the Institute of Physics, Chinese
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Synchrotron Radiation Facility (BSRF), and National Synchrotron
Radiation Laboratory (NSRL).
1
Conflicts of interest
There are no conflicts to declare.
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