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DOI: 10.1039/x0xx00000x
Published on 22 November 2019. Downloaded on 11/27/2019 6:49:19 AM.
Constructing 2D MOFs from 2D LDHs: highly efficient and durable
electrocatalyst for water oxidation
Mengke Cai,a Qinglin Liu,a Ziqian Xue,a Yinle Li,a Yanan Fan,a Aiping Huang,b Man-Rong Li,a Mark
Croft,c Trevor A. Tyson,d Zhuofeng Kee and Guangqin Li*a
Two-dimensional (2D) materials have been widely applied to electrochemical conversion technologies, especially toward
the water oxidation reactions (WOR) in metal-air batteries and water splitting. Here, we demonstrate a facile ligand-assisted
synthetic method, promoting the transformation from 2D layered double hydroxides (LDHs) to 2D metal-organic frameworks

(MOFs). CoFe-LDH precursor performs as an adjustable metal release source, controlling heterogeneous nucleation for 2D
MOFs. Compared with most cobalt-based electrocatalysts, the optimized CoFe 2D MOFs exhibits a superior WOR
performance on glassy-carbon electrodes (overpotential of 274 mV at 10 mA cm-2, a Tafel slope of 46.7 mV dec-1) and long-
term stability, due to the unique 2D characteristics and coupling effect between Co and Fe ions. More importantly, this work
highlights the ability to transformation from 2D LDHs to 2D MOFs, and reveals the intrinsic factors for excellent performance
in WOR.

Additionally, how to rationally design and synthesize 2D

Introduction materials is also of great interest and challenge. The synthesis
of 2D materials usually depend on chemical vapor deposition
Water splitting by electrolysis (2H2O → O2 + 2H2) provides a
and physical exfoliation, involving both top-down and bottom-
potential and encouraging path for the generation of efficient,
up approaches.31-33 Recently, 2D materials such as TMDs with
clean and renewable H2 fuel to support human civilization.1-3
unique microstructure were obtained by means of precursor
However, the efficiency of water electrolysis is limited by large
transformation, exhibiting superior catalytic properties
overpotentials, especially for water oxidation reaction (WOR),
compared with direct synthesis.21,26,34 Therefore, getting 2D
and the use of expensive noble electrocatalysts hinders the
materials through precursor transformation are promising to
long-term development for water electrolysis application.4-9 In
significantly broaden the design and synthesis of
recent years, further research has been conducted to explore
electrocatalysts for energy storage and conversion.
cost-effective and efficient non-noble electrocatalysts for
MOFs are constructed by coordination bonds between metal
WOR.10-12 Notably, two-dimensional (2D) materials have
nodes/clusters and organic ligands with periodic reticular
attracted very significant attention in the field of
chemistry.35 Due to precise periodicity, nano-dimensional MOFs
heterogeneous electrocatalysis due to their unique physical,
possess definite accessible active sites and well-defined
chemical, and electronic properties. As a result, graphene,13-15
structures, which have exhibited promising performance
graphitic C3N4,16,17 transition metal dichalcogenides (TMDs),18-20
towards water oxidation.24-26 However, the poor conductivity,
layered double hydroxides (LDHs),21-23 2D metal-organic
low mass permeability and stability have limited its
frameworks (MOFs)24-28 and 2D covalent-organic frameworks
development in electrocatalysis. Thus, to design highly efficient
(COFs)29,30 are considered as promising water splitting catalysts.
electrocatalysts, construction of 2D MOFs with nanosheets
could be an appropriate strategy to satisfy the followings:
nanolayer to strengthen electron transfer and mass
a MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of transport;24,25,36,37 large surface area exposed active sites, and
Functional Materials, School of Chemistry, Sun Yat-Sen University, Guangzhou coordinative unsaturated metal sites.24,26,38-43
510275, People’s Republic of China. E-mail: liguangqin@mail.sysu.edu.cn Here, we report a CoFe bimetal 2D MOFs as electrocatalysts
b Key Laboratory of Polymer Composites and Functional Materials of Ministry of

Education, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, People’s for WOR, for the first time, prepared from the transformation
Republic of China of precursor CoFe-LDHs as the template. So far, there are
c Department of Physics and Astronomy, Rutgers, The State University of New Jersey,

136 Frelinghuysen Road, Piscataway, New Jersey 08854, United States

extensive reports on 2D-LDHs containing Ni, Co, Fe and Mn
d Department of Physics, New Jersey Institute of Technology, Newark, New Jersey exhibiting excellent catalytic properties in WOR, especially for
07102, United States NiFe-LDHs known as the most promising catalyst.10,12,13,20,22,23
e Key Laboratory for Polymeric Composite and Functional Materials of Ministry of

Education, School of Materials Science and Engineering, Sun Yat-Sen University, For Ni-based materials, the addition of Fe dramatically
Guangzhou 510275, People’s Republic of China enhances WOR activity. But for Co-based materials, it is not
Electronic Supplementary Information (ESI) available:. See
DOI: 10.1039/x0xx00000x well-documented and CoFe-based materials usually show more

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modest WOR activity compared with NiFe-based materials.49-53
So it is a significant challenge to construct novel CoFe-based
materials with better activity than CoFe-LDHs and explore the
relevant mechanism. More importantly, LDHs own adjustable
and reasonable layer spacing, allowing ligands to attack inner
Co and Fe from interlayer, which makes it as a good candidate
to form 2D MOFs. Thus CoFe 2D-LDHs are chosen as precursors
since its bimetallic Co/Fe composition and 2D layered
characteristics. Interestingly, with the transformation from 2D
LDHs to 2D MOFs, the obtained electrocatalyst loaded on
glassy-carbon (GC) electrodes demonstrate a low overpotential
of 274 mV at 10 mA cm-2 in alkaline conditions. During the long-
term stability test, the 2D MOFs loaded on nickel foam (NF)
maintain highly stable activity for 70 h at a constant
overpotential of 271 mV.
Results and discussion
Published on 22 November 2019. Downloaded on 11/27/2019 6:49:19 AM.
The transformation were conducted via ligand-assisted procedure by
mixing precursor CoFe-layered double hydroxide (CoFe-LDH) and
terephthalic acid in DMF at various temperature and time (Fig. 1),
and correspondingly transformed specimens were named as LM-T-t
(T: temperature/°C, t: time/hour). To clearly understand the process
from CoFe-LDH transformed to bimetallic 2D MOFs, powder X-ray
diffraction (PXRD) tests were carried out on all specimens. In Fig. S1
a, the (003) and (006) diffractions can be observed at 2θ = 11.51° and
23.18° for prepared CoFe-LDH, indexed as a bimetal ferrocobalt
hydroxide with CO32- (carbonate) as interlayer counterion.
Interestingly, the (003) and (006) diffractions shifted to lower angle,
indicating the interlayer ion-exchange for CoFe-LDH. The basal
interlayer spacing was calculated to be 0.77 nm for the pristine CoFe-
LDH, shifting to 0.84 nm for both LM-100-12 and LM-130-12 based
on Bragg equation (2dsinθ = nλ). The PXRD patterns showed that the
characteristic diffraction peaks of the (003) and (006) planes of CoFe-
LDH disappeared, while the (200), (201) and (-201) facets of the 2D
Co-MOFs emerged and became stronger with the increase of
reaction temperature and time (Fig. S1 a-b). Finally, with excessive
transformation time, another MOFs phase diffraction peaks arose in
PXRD patterns, which was usually obtained by the coordination of
Fe3+ with terephthalic acid and named as MIL-88B(Fe) (Fig. S1 b) (No.
Fig. 1 Schematic illustration for the ligand-assisted transformation to prepare
2D-MOF.
1415803, space group of P63/mmc, Cambridge Crystallographic Date
Centre).44-46
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DOI: 10.1039/C9TA09397D
Journal of Materials Chemistry A Accepted Manuscript
Fig.2 SEM images of (a) CoFe-LDH and (b) LM-160-12. TEM images of (c) CoFe-
LDH and (d) LM-160-12. HRTEM image (e), HAADF-STEM image (f) and EDXS
mapping images of LM-160-12 for Co (g), Fe (h) and O (i). AFM image (j) and
the height curves (k) of the as-prepared LM-160-12, showing measured
dimensions of nanosheets.
Furthermore, the N2-adsorption/desorption isotherms were shown
in Fig. S2 a-b. The specimens LM-160-12, LM-160-24 and LM-160-36
all exhibited reversible microporous regions and adsorption
hysteresis loops, categorized as microporous type-IV isotherms
unlike those of precursor CoFe-LDH, LM-100-12 and LM-130-12.
Moreover, the hysteresis loop area of LM-160-12 was larger than
others, indicating the presence of multilevel pores and unique
hierarchical structure. Additionally, the Brunauer-Emmet-Teller
(BET) surface areas of LM-160-12 was calculated to be 105.1 m2 g-1 in
Fig. S3, higher than those of CoFe-LDH (39.2 m2 g-1), LM-100-12 (39.8
m2 g-1) and LM-130-12(43.2 m2 g-1), lower than LM-160-24 (174.5 m2
g-1) and LM-160-36 (247.8 m2 g-1), which was consistent well with
XRD results. The total pore volume of specimens was shown in Fig.
S3, both LM-160-12 (0.151 cm3 g-1) and LM-160-24 (0.154 cm3 g-1)
possessed nearly twice pore volume of precursor CoFe-LDH (0.085
cm3 g-1). The pore sizes of specimens (Fig. S4-5) were calculated by
nonlocal density functional theory (NLDFT), showing that the
mesoporous distribution of LM-160-12 was the largest compared
with other specimens. The coexistence of unique microporous and
mesoporous structure in LM-160-12 may make it positive in
electrocatalysis.
The morphology was characterized by scan field-emission scanning
electron microscopy (SEM), transmission electron microscopy (TEM),
and atomic force microscopy (AFM). The SEM image (Fig. 2a)
indicated that the CoFe-LDH nanosheets possessed a hexagonal
shape with lateral mean diameter about 50-500 nm, consistent with
reported work.21 After transformation via ligand-assisted method
under 160 °C for 12 hours (Fig. 2b), spindle-like thin nanosheets were
obtained for LM-160-12. The TEM images (Fig. 2c-d) also revealed the
large morphological changes and coinciding well with Fig. 2a and 2b.
Interestingly, tracking the morphology of the transformation (Fig. S6-
7), it suggested that the ligand-assisted transformation from 2D
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CoFe-LDH to 2D MOFs resulted in obvious crystal dissociation,
recrystallization, and irregular growth. Due to a lack of solution
agitation and lack of surfactants in solid-liquid reaction system,
agglomeration and disorder growth happened in long-term reaction,
such as LM-160-24 and LM-160-36. Encouragingly, High resolution
transmission electron microscopy (HRTEM) and High angle annular
dark field scanning transmission electron microscopy (HAADF-SEM)
images clearly elucidated the spindle-like shape for LM-160-12 (Fig.
2e-f), and the nanosheets possessed a homogeneous distribution of
Co, Fe and O elements, which was illuminated by energy-dispersive
X-ray spectroscopy (EDXS) (Fig. 2g-i). Moreover, AFM image of LM-
160-12 in Fig. 2j showed the nanosheets consisted of ultrathin sheets
apparently in red dashed circle, and the thickness of ultrathin sheets
was determined to be 4.84-7.39 nm (Fig. 2k). The thickness of single
coordination structural layer was calculated about 0.97 nm in
reported CoNi 2D MOFs,24 suggesting that LM-160-12 ultrathin
nanosheets included 5-8 coordination layers. The above results also
Published on 22 November 2019. Downloaded on 11/27/2019 6:49:19 AM.
revealed that LM-160-12 owned characteristics of inherent 2D
structural periodicity, which may provide exposed active surfaces for
MOFs-based electrocatalysts.47,49
To further identify the transformation process from LDH to 2D MOFs,
active metal content and ratio of all specimens were measured by
inductively coupled plasma-mass spectrometer (ICP-MS). Both Co
and Fe content showed a downward trend with increase of
transformation temperature and time (Fig. 3a-b), because of Co and
Fig. 3 Identification of the transformation process by comparing active metal
content and ratio. Measured metal content of Co (a), Fe (b) and molar ratio
of Co/Fe (c). The dissociation of cations for CoFe-LDH soaked in DMF at 160
°C (d). Schematic diagram of structural transformation from LDH to 2D MOFs
(e). Local unsaturated (green dashed circle) model for the metals on surface
of LM-160-12 (f) and four sets of non-equivalent [MO6] octahedra (g). Blue
for Co, orange for Fe, red for O, grey for C, and white for H.
Fe ions only from precursors CoFe-LDH in the transformation
process. The molar ratio for Co/Fe, however, varied between 2.2 for
the LM-160-12 with the most 2D characteristics to 1.5 for LM-160-36
(Fig. 3c). It coincided well with the PXRD results that high proportion
of iron content tends to form microporous structure MIL-88B(Fe).
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DOI: 10.1039/C9TA09397D
Journal of Materials Chemistry A Accepted Manuscript
Fig. 4 (a) LSV curves, (b) comparison of WOR overpotential at 10 and 100 mA
cm-2, (c) Tafel plots and (d) EIS curves (the equivalent circuit diagram is shown
inset, dots represent raw data and dashed lines represent fitted data) of
various specimens. RHE denotes the reversible hydrogen electrode.
The excessive doping of trivalent iron affected the coordination
environment between bivalent cobalt and terephthalic acid to form
2D MOFs. Next, we carried out a dissociation experiment to monitor
the cations release of precursors CoFe-LDH, soaked in DMF at 160 °C
measured by ICP-MS. Shown in Fig. 3d, the dissociation ratio of Co/Fe
was between 3.5 for the initial 6 hours and decreased to 2.9 after 42
hours, which significantly exceeded the the initial ratio of Co/Fe 2.0
for precursor CoFe-LDH. In other words, the dissociation of cobalt
was faster than iron in the beginning, which facilitated that ligand
terephthalic was more inclined to coordinate with cobalt in the early
stage of heterogeneous nucleation. These suggested that precursor
CoFe-LDH, an adjustable metal release source, played a key role in
the ligand-mediated transformation process (Fig. 3e). Shown in Fig.
3e-f and S8, ligand terephthalic molecules separated the 2D bimetal
layers along a axis, which were composed of pseudo octahedral
[CoO6] and [FeO6]. Here, the unsaturated metal sites (green dashed
circle) on the surface of LM-160-12 satisfied the desirable four-
electron pathway for WOR (Fig. 3f). However, there were four sets of
non-equivalent octahedral [MO6], derived from different metal
centers and ligands containing oxygen (Fig. 3g). So it is an enormous
challenge to clarify the specific reaction pathways and active centers
(Co or Fe).49-53
All electrochemical measurements for WOR were performed with
1.0 M KOH solutions as electrolyte. As shown in Fig. 4a, the linear
sweep voltammetry (LSV) curves were investigated to compare each
specimen’s WOR catalytic activity. It should be noted that a rather
small overpotential (274 mV) was required for the LM-160-12 to
deliver a current density of 10 mA cm-2 (Fig. 4b), which is comparable
with commercial RuO2 (271 mV) and superior to most cobalt-based
and pristine MOFs electrocatalysts (Table S1 and S2). Interestingly,
the specimen LM-160-24, possessing better crystallinity and specific
surface than LM-160-12, exhibited lower WOR catalytic activity. To
understand how and why weakly crystalline 2D MOFs LM-160-12
possess the best WOR electrocatalytic activity, correlative Tafel
slopes was performed in Fig. 4c. The LM-160-12 showed the smallest
Tafel slope (46.7 mV dec-1) compared with isostructural LM-160-24
(46.9 mV dec-1) and the other specimens, indicating better kinetic
activity possibly due to fast mass transport and electron transfer.
Electrochemical impedance spectroscopy (EIS) was also conducted to
evaluate the electron transfer ability and understand reaction
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kinetics (Fig. 4d). The equivalent circuit model (the inset of Fig. 4d) to higher valence state Co was induced by the π-donation between
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was set to fit the impedance responses, where Rs represents solution Fe3+ and bridging O2-, because enhanced π-donation triggered more
DOI: 10.1039/C9TA09397D
resistance, Rct represents electron transfer resistance, Rp represents partial charge transfer from Co2+ to O2-, which may contribute to the
surface porosity and CPE stands for the constant phase element. The LM-160-12 with best activity.
Rct and Rp value of the LM-160-12 (47.8 and 3.4 ohm) was smaller To probe the electronic and local structural motifs, X-ray absorption

Journal of Materials Chemistry A Accepted Manuscript

than isostructural LM-160-24 (49.8 and 9.4 ohm), also suggesting
faster electron transfer and ion diffusion in WOR process (Table S3).
Furthermore, the electrochemical surface area (ECSA) was measured
by evaluating electrochemical double-layer capacitance (Cdl), which
was proportional to the slope of current differences plotted against
scanning rates. The LM-160-12 possessed a Cdl value of 25.4 mF cm-
2, nearly twice as LM-160-24 (14.7 mF cm-2), significantly exceeding
other specimens (Fig. S9-11). This ESCA result showed a volcanic type
trend, differing from the observed ascending type for BET surface
area. It was clear that ESCA is not simply up to the BET specific
surface, so the unique 2D nanosheets morphological characteristics
had a vital impact in electrocatalytic process. In addition, we
Published on 22 November 2019. Downloaded on 11/27/2019 6:49:19 AM.
near-edge structure (XANES) was performed on the specimens. As
shown in Fig. 5c and S19 a, the X-ray absorption curves of both LM-
160-12 and LM-160-24 show Fe K-edge shifts quite close to, albeit
somewhat lower, compared with the reference La2FeVO6. This
supports a formal chemical Fe valence state close to Fe3+ in both
materials. At the Co K-edge, the XANES spectra of both specimens
showed Co atoms oxidation state is higher than +2 (Fig. 5d and S19
b). This is consistent with partial substitution of Fe in Co sites in
MOFs, which led to charge transfer between both atoms, in

compared the LSV curves normalized by ECSA for all samples in Fig.
S12, where the LM-160-12 was superior to others in intrinsic WOR
activity and their WOR activity tendency was not entirely consistent
with the LSV curves in Fig. 4a. Interestingly, the results indicate that
the differences in the WOR performance are not only originated from
exposed active sites but also the intrinsic activity. To investigate the
long-term electrocatalytic stability, we took chronopotentiometric
measurement to evaluate the 2D MOFs LM-160-12 loaded on both
glassy carbon electrode (GCE) and nickel foam (NF). As revealed in
Fig. S13, the durability of LM-160-12 loaded on GCE maintained a 10
h stability with slight decrease in activity, and it was supposed that
bubble breakup resulted in catalyst shedding due to fast oxygen
evolution. When replaced with applicable NF as support, a highly
stable current density of 10 mA cm-2 was obtained for at least 70 h.
Importantly, the HRTEM, HAADF-STEM and EDXS mapping images
(Fig. S14) of LM-160-12 nanosheets loaded on NF after long-term
stability test were consistent with observation before pre-reaction.
The PXRD pattern results (Fig. S15) also illustrated that the diffraction
peaks of 2D MOFs, (200), (201) and (-201) facets, were still retained
modestly after long-term reaction. Moreover, the valence electron
structures before and after electrocatalysis were further confirmed
by XPS. From XPS results (Fig. S16), the binding energy of Fe 2p3/2
shifted to low binding energy, while opposite up-shift was observed Fig. 5 (a) Fe 2p3/2 and (b) Co 2p3/2 high resolution XPS spectra of precursor
for Co 2p3/2 at the same time. It suggested that long-term CoFe-LDH, LM-160-12 and LM-160-24. (c) The Fe K-edge and (d) Co K-edge
electrocatalysis promoted the charge transfer from Fe to Co by the XANES spectra for LM-160-12 and LM-160-24, and standard FeO, La2FeVO6,
ligands containing oxygen, and deeper study on electronic structures CoO and LaCoO3. (e), (f) Expanded pre-edge peaks comparison of LM-160-12
and LM-160-24, respectively.
should be implemented.
accordance with previous report on metal doping engineering in
Next, to further verify the bimetal interaction, the XPS survey was
MOFs.54 The broad unresolved Co-K main edge peak near 7725 eV in
carried out. As shown in Fig. S17, four elements Co, Fe, O and C were
LM-160-12, compared to the sharper features in the LM-160-24
detected on the surface for all specimens. And the molar ratio of
spectrum (Fig. 5d) should also be noted. This broadening is
Co/Fe measured by XPS was consistent with that detected by ICP-MS
consistent with a significant structural distortion of nearest
(Table S4). After the transform from LDH to 2D MOFs, the O2- 1s
neighbours to Co sites in the former system compared to the latter.55
(530.7 eV for CoFe-LDH) peak shifted to higher binding energies
In the Fe and Co pre-edge region, two pre-edge peaks around 7114.2
(531.2 eV for LM-160-12 and LM-160-24), respectively (Fig. S18).
eV and 7709.8 eV were shown both in the LM-160-12 and LM-160-
Meantime, the Fe3+ 2p3/2 shifted to low binding energy (Fig. 5a), and
24 (Fig. 5e-f). Both peaks were derived from the transition, from
the same up-shift was obtained for Co2+ 2p3/2 (Fig. 5b). The above
quadrupole allowed 1s to 3d and dipole allowed 1s to 3d-4p hybrid
results indicated that part of electron was transferred from Co2+ to
orbitals.56 Here non-centrosymmetric distortions enhance the
Fe3+ through the bridging oxygen, which could adjust the electron
stronger transitions into the 3d-4p hybrid orbitals, and the enhanced
density of the metal sites. It is obvious that the peroxidation of Co2+

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pre-edge feature spectral weight for the LM-160-12 material 4 M. T. M. Koper, J. Electroanal. Chem., 2011, 660,View 254-260.
Article Online
supports a more strongly distorted and unsaturated local 5 J. Zhang, Q. Zhang and X. Feng, Adv. Mater., 31, 1808167.
DOI: 10.1039/C9TA09397D
6 C. Tang, H.-F. Wang and Q. Zhang, Acc. Chem. Res., 2018, 51,
environment. In general, the combination of XANES, ESCA and 881-889.
morphology characterization clearly revealed that the existence of 7 F. Song, L. Bai, A. Moysiadou, S. Lee, C. Hu, L. Liardet and X.
more coordination unsaturated metal sites and local structural Hu, J. Am. Chem. Soc., 2018, 140, 7748-7759.

Journal of Materials Chemistry A Accepted Manuscript

distortion on LM-160-12 surfaces, compared with LM-160-24,
resulted in excellent WOR activity. Hence, we propose that the
excellent catalytic performance may mainly originate from the
unique 2D characteristics rather than the coupling effect between Co
and Fe, which not only provide more coordination unsaturated metal
sites but also facilitate electron transport, transfer and ion
diffusion.57-59
Conclusions
In summary, a novel ligand-assisted synthetic strategy is
demonstrated to prepare bimetal 2D MOFs nanosheets as
Published on 22 November 2019. Downloaded on 11/27/2019 6:49:19 AM.
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highly active and durable electrocatalysts for the WOR, by the
transformation from 2D LDHs. Furthermore, the precursor LDHs 14
serve as an adjustable metal release source to control the
heterogeneous nucleation process, forming layered bimetal 2D 15
MOFs. The coupling effect between Co and Fe promotes the 16
delocalization Co 3d electron and enhances the WOR activity.
More importantly, the layered bimetal 2D CoFe-MOFs possess 17
more exposed active sites, rapid electron transfer and faster ion
diffusion, which makes major contributions to superior activity 18
in our work. We believe that the unique ligand-assisted
synthetic strategy will extend opportunity towards constructing 19
2D MOFs-based materials for wide applications such as energy
storage and conversion.
20
21
Conflicts of interest
The authors declare no conflict of interest. 22
23
Acknowledgements
24
This work was supported by The 100 Talents Plan Foundation of
Sun Yat-sen University, the Program for Guangdong Introducing
Innovative and Entrepreneurial Teams (2017ZT07C069), 25
Guangdong Natural Science Funds for Distinguished Young
Scholar (No. 2015A030306027), and the NSFC Projects
(201875287, 21821003, and 21890380). Part of this research
26
used the QAS, 7-BM beamline at the National Synchrotron Light
Source II, a U.S. Department of Energy (DOE) Office of Science 27
User Facility operated for the DOE Office of Science by 28
Brookhaven National Laboratory under Contract No. DE-
SC0012704. 29
Notes and references 30
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 Page 7 of 7 Journal of Materials Chemistry A

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DOI: 10.1039/C9TA09397D
Table of Contents

Journal of Materials Chemistry A Accepted Manuscript

We demonstrate a facile ligand-assisted synthetic method, promoting the
transformation from 2D layered double hydroxides (LDHs) to 2D metal-organic
frameworks (MOFs). The optimized CoFe 2D MOFs transformed from CoFe-LDH
Published on 22 November 2019. Downloaded on 11/27/2019 6:49:19 AM.

precursor performs exhibits a superior water oxidation reaction performance and

durable stability.