Coordination Chemistry Reviews 422 (2020) 213477

Contents lists available at ScienceDirect

Coordination Chemistry Reviews

journal homepage: www.elsevier.com/locate/ccr

Review

Removal of particulate matter with metal–organic

framework-incorporated materials
Dong Kyu Yoo, Ho Chul Woo, Sung Hwa Jhung ⇑
Department of Chemistry and Green-Nano Materials Research Center, Kyungpook National University, Daegu 41566, Republic of Korea

a r t i c l e i n f o a b s t r a c t

Article history: Recently, the contamination of air, both indoors and outdoors, has been severe, especially due to partic-
Received 29 May 2020 ulate matter (PM) in some cities and countries like India, China, and Korea. Therefore, both preventing the
Accepted 3 July 2020 evolution of PM and removing PM from air are highly important for sustainability. In this review, progress
regarding PM (especially 2.5 mm or less) removal via filtration is summarized. In particular, air filters
modified or composed with metal–organic frameworks (MOFs) or MOF-related materials are discussed,
Keywords: including preparation methods. Moreover, improved performances with the incorporation of MOFs and
Filter
mechanisms to explain the observations are discussed. Finally, perspectives in the field for effective
Mechanism
Metal–organic frameworks
PM capture/removal with MOF-incorporated filters are suggested after a brief summary of the researches.
Particulate matter Ó 2020 Elsevier B.V. All rights reserved.
Removal

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
1.1. Introduction to MOFs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
1.2. Filtration of particulate matter . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2. Preparation of MOF-incorporated filters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.1. In-situ synthesis in the presence of a substrate . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.2. Electrospinning . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2.3. Hot pressing. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2.4. Other methods. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
2.5. Comparison of various methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
3. Removal of PM with MOF-incorporated filters. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
3.1. Performances of MOF-incorporated filters. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
3.1.1. MOF incorporation for largely improving RE . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
3.1.2. MOF incorporation for complete removal of PM . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
3.2. Removal mechanisms . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
3.2.1. Electrostatic interaction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
3.2.2. High porosity and hierarchical pores . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
3.2.3. Functional groups of MOFs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
3.2.4. Other contributions of MOFs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
4. Summary and perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

⇑ Corresponding author.
E-mail address: sung@knu.ac.kr (S.H. Jhung).

https://doi.org/10.1016/j.ccr.2020.213477
0010-8545/Ó 2020 Elsevier B.V. All rights reserved.
2 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477

1. Introduction huge porosity, ready functionalization, designable pore and facile

Recently, there has been high interest in air quality because of
contamination of air, both indoors and outdoors, due to various
toxic substances, such as volatile organic compounds (VOCs),
NOx, SOx, and ozone. Air contamination with particulate matter
(PM) is especially severe, particularly in some countries including
India, China, and Korea. PM is composed of various chemical sub-
stances, such as nitrate, sulfate, silicate, carbon, and ammonium.
PM usually originates from industrial pollution, vehicular emis-
sions, soil dust, coal combustion, and biomass burning [1–9].
Moreover, secondary reactions among ammonia, SOx, NOx, and
VOCs produce PM [7,8]. Traditionally, PM has been classified based
on its size or aerodynamic diameter, with PM2.5 and PM10 usually
referring to materials smaller than 2.5 mm and 10 mm, respectively.
PM, especially PM2.5, has a devastating impact on human health,
particularly when it penetrates the human lungs and bronchi;
the negative effect of PM on health increases with decreasing PM
size. Therefore, PM, especially smaller ones, can cause health prob-
lems, ranging from lung cancer to mortality [1–9].
Because of the serious effect of PM on human lives, continuous
efforts have been made not only to prevent the possible evolution
of PM but also to remove it from air. Among removal methods, fil-
tration or air filters have been regarded as competitive and conve-
nient given their cost-effectiveness and versatility in shape/size for
various purposes [1,2,10–13]. Various materials [1,2], such as poly-
mers (for example, polypropylene, polyester, polyurethane,
polyetherimide [14], cellulose, lignin [15], and polybenzimidazole
[16]), fabrics (cotton), oxides, chitosan, silk, carbon (including acti-
vated carbon, carbon nanotubes [17], reduced graphene oxide [18],
graphene oxide [19]), amino acids [20], and metals, such as silver
[21]) have been used as raw materials or active components for fil-
ters. Even though filtration or air filters have advanced rapidly, fur-
ther improvements for high efficiency, low pressure drop, facile
reusability, and low cost are strongly required.
Air filters can be both porous filters and fibrous filters [10], and
porous materials have contributed considerably to air purification
[1]. So far, various porous materials [22–34] have advanced rapidly
mainly due to metal–organic frameworks (MOFs) [35–50], which
are composed of both inorganic and organic species. Because of
preparation, MOFs have been used for environmental remediation,
including CO2 capture, water purification and toxic chemical
removal [51–60]. Importantly, the performances of air filters have
been improved considerably by applying MOFs to make compos-
ites with conventional materials [61–64].
In this review, we summarize recent progress on air filters,
especially those modified or composed with MOFs. To the best of
our knowledge, there has been no review on this theme even
though (i) MOF-incorporated filters have rapidly advanced (vide
infra) and (ii) there are review articles on air filters [1,2] and MOFs
themselves [35–45]. Both improved performances (from the intro-
duction of MOFs) and preparation methods of MOF-incorporated
filters are explained. Moreover, reasoning for the origin of
improved performance (or the plausible mechanism for the contri-
bution of MOFs to PM removal) is dealt with. Finally, perspectives
in the field are suggested after a summary of the progress.
1.1. Introduction to MOFs
MOFs can be produced via a coordination bond between organic
linkers and metal ions or metal clusters [35–37]. Importantly,
many metallic species can be converted into MOFs with suitable
organic species, which is very different from conventional porous
materials such as zeolite or carbon [65–66]. MOFs have high poros-
ity and designable pores; therefore, they are highly attractive for
catalysis and adsorption. Because of their organic components,
MOFs can be facilely functionalized or modified [67,68]. Moreover,
MOFs can be synthesized under a wide range of conditions (includ-
ing ambient conditions [69]) or even with a continuous process
[70]. On the other hand, MOFs have been regarded as having low
thermal or chemical stability, even though several MOFs have been
reported to have appropriately high stability [71]. Table 1 shows a
comparison between MOFs, with both inorganic and organic com-
ponents, and zeolites as typical examples of inorganic porous
materials [66].
MOFs have several advantages in capturing various materials.
First, as mentioned above, modification or functionalization of
MOFs can be simple; therefore, the required property can be easily
obtained. Second, MOFs with a very similar crystal structure can be

Table 1
Properties of MOFs compared with the inorganic counterparts (zeolites) [66].

Item Inorg. mater. (zeolites) MOF Remarks for MOF

Central atom Si, Al, P, TMI* (small content) Almost all the cations (di, tri, tetra- Versatile functionality and
valent) isoreticular structures.
Central atom Atom Atom or clusters Versatile structures
state
Central atom Mainly tetrahedral Various Versatile functionality and easy
coordination coordination of chemicals
Linker -O-, -S- Carboxylates, phosphonates, Versatile functionality with wide
sulfonates, cyanides, imidazoles, pore openings and surface area
pyridines etc.
Frame flexibility Rigid Very flexible Show unusual behaviors such as
breathing
Structure Hundreds Infinite Ease of choice
Wall Thick Very thin Ready diffusion
Porosity Limited Very high Suitable for adsorption
Framework Negative Nearly neutral Sometimes positive
charge
Thermal stability Strong Weak Weak point (not serious in
adsorption/separation)
Synthesis Harsh or hydrothermal Very wide including hydrothermal
condition and room temperature synthesis
Special property OMS**, redox, breathing etc. Transition metals, lanthanides etc.
*
TMI: transition metal ions.
**
OMS: open metal sites.
 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477 3

MOFs with
different MOFs
metal ions MOFs with
functional or
tagged groups

MOFs with
different linkers
Fig. 1. Schematic presentations of analogous MOFs including (a) Analogous MOFs with different cations or cationic clusters; (b) Analogous MOFs with different linkers; (c)
Analogous MOFs with tagged functional groups. Redrawn, based on Ref. [73]. CopyrightÓ 2012, Royal Society of Chemistry.

Table 2
Comparison of porous and fibrous filters.

Item Porous filter Fibrous filter Ref.

Construction Creating very tiny pores on solid Stacking (random) of fibers (with diameter [2,13]
substrate from several microns to tens of microns)
Removal mechanism Size exclusion Diffusion, interception and impaction [2,10]
Porosity <30% >70% [13]
Advantage High filtration efficiency Good filtration capacity [2,13]
Disadvantage High cost, less effective for smaller Challenging in cleaning and reusing [1,2,5,13]
PMs
High pressure drop
Other characteristics Pressure drop can be increased very Usually thick, non-transparent filter [2,13]
rapidly when PMs attach to pores
(due to decreased surface porosity)

produced from several metal ions or linkers (for example, with dif- of air filters (porous and fibrous ones) have been utilized in PM
ferent sizes, such as benzene-, biphenyl-, and naphthalene- removal or capture. Table 2 shows a summary of the comparison
dicarboxylic acids). These MOFs, schemed in Fig. 1, are called anal- of the two filters [1,2,5,10,13]. Here, the two typical filters are
ogous, isomorphous, isoreticular, or isostructural MOFs and can be briefly explained. The first is the porous type (Fig. 2a) [10] and pro-
highly useful to study any effects of metal ions or linkers [72–76]. duced by creating tiny pores in solid substrates (therefore, this is
Third, MOFs can be composed easily with various materials to generally expensive [5]). Porous filters can remove PM with the
obtain composites with improved performances, including high
stability [77–80]. Finally, MOFs can be converted into other func-
tional materials, including MOF-derived materials or carbons
[81–85], since MOFs are composed of very well-dispersed or -
designed metallic and organic components. In summary, MOFs
are exceptionally attractive porous materials that can be applied
in various fields, including PM capture.

1.2. Filtration of particulate matter

As mentioned, PM can be removed from air via filtration with

suitable air filters made from various materials such as carbon, chi-
tosan, metal, oxide, polymer, silk and so on [1,2]. So far, two types Fig. 2. Illustrations of (a) porous air filter and (b) fibrous air filter. Adapted with
permission from Ref. [10]. CopyrightÓ 2017, American Chemical society.
4 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477

Fig. 3. (a) Filtration efficiency with different PM sizes, (b) PM2.5 filtration efficiency, (c) pressure drop, and (d) PM2.5 filtration QF of the membranes with different ZIF-8
precursor concentrations. The terminologies of ‘BISG’ and ‘AISG’ in (c) mean ‘before in situ growth’ and ‘after in situ growth’, respectively. Reproduced with permission from
Ref. [91] CopyrightÓ 2020, American Chemical society.

size exclusion principle; therefore, pores should be smaller than REð%Þ ¼ C i  C f =C i  100% ð1Þ
the size of target PM [2]. Generally, the porosity of this filter is
low (<30%) [13]; therefore, the pressure drop is high even though where, Ci (mg/m3) and Cf (mg/m3) are the concentrations of PM par-
the filtration efficiency can be also high [13]. The most serious ticles before and after passing through air filters, respectively.
thing of porous filters is that the removal degree should be The QF, one of the most important factors for air filters [1], can
decreased with decreasing PM size [1]. Moreover, the pressure be calculated using Eq. (2) [1,2]:
drop can be increased very rapidly when PM attaches to pores
because of decreased surface porosity [2]. QF ¼ lnð1  REð%Þ=100Þ=DP ð2Þ
The second type is the fibrous filter (Fig. 2b) [10], which is pro-
duced by randomly stacking fibers with a diameter from several where, RE (%) is the removal efficiency (%) of PM and DP is the pres-
microns to tens of microns [2,13]. The porosity of this filter is high sure drop (Pa) of the filters.
(>70%) [13], and the filtration mechanism is based on diffusion, Finally, pressure drop (the pressure difference between before
interception, and impaction [2,10]. Generally, fibrous filters have and after passing through a filter) is also important for estimating
good filtration capacity [2]; however, it is challenging to clean the performance of a filter.
and reuse fibrous filters [2]. Moreover, this type of filter is usually
thick and non-transparent [13].
Considering the inefficiency, such as poor removal efficiency
2. Preparation of MOF-incorporated filters
especially for small PM (<0.3 mm) [14,17], ready blocking, high
pressure drop, low air flux, and poor reusability, of commercial
Since the pioneering work of Wang et al. in 2016 [61], there
air filters [5], further improvement is essential, and developing
have been continuous efforts to improve air filters via the incorpo-
new materials and surface modification are recommended for
ration of MOFs into substrates. As has been reviewed by Qui et al.
effective filters [1,2]. Moreover, so far, the exact mechanism to
[86], the preparation of the MOF membrane, especially on sub-
remove PM via filtration is not fully elucidated [1,2]. Therefore, fur-
strates, has been studied for various MOFs by using several meth-
ther works are required to develop advanced air filters and to
ods including direct synthesis with or without the modification of
understand the removal mechanism.
supports. Since readers can refer to review articles on MOF mem-
Finally, the performances of air filters can be estimated using
branes or films [86–88], in this section, methods to introduce MOFs
several factors, such as the removal efficiency (RE), pressure drop,
to filters or base materials (for filters such as fabrics) that have
and quality factor (QF).
been applied only for PM removal will be discussed (with some
The RE (%) is obtained by Eq. (1) [2]:
reported results and reasoning).
 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477
2.1. In-situ synthesis in the presence of a substrate
The incorporation of MOFs into filter materials has been
achieved mainly via in-situ synthesis, probably because of the
facile synthesis of some MOFs (especially ZIF-8) under mild condi-
tions [89,90]. For example, ZIF-8 nanocrystals were loaded onto
polypropylene–polycarbonate (PPC) fibrous membranes via the
simple mixing of ZIF-8 precursors and methanol in the presence
of PPC at room temperature [91]. Even though the quantity of
loaded ZIF-8 was very small (<1%), the RE of PM2.5 was increased
significantly (Fig. 3a and 3b) due to the defect and positive charge
of highly porous ZIF-8. Curiously, there was no increase in pressure
drop (actually, there were slight decreases in the pressure drop)
even after the introduction of ZIF-8 (Fig. 3c); therefore, the QF
was increased considerably or more than doubled (for example,
from 0.026 to 0.055 Pa1, for the best case) (Fig. 3d) [91].
ZIF-8 was also introduced to cellulose fibers via in-situ synthe-
sis at 70–75 °C [92–94]. Another MOF, Ag-MOF [Ag2(HBTC)(im),
im: imidazole] was also included for antibacterial activity [91].
By loading MOFs, the RE was increased considerably (~44 to
94.3% [92], ~65 to 99.94% [93]); however, the pressure drop
increased much (19 to 158 Pa [92]; 21 to 134 Pa [93]) because of
the very high deposition ratio of MOFs (>70%). Much ZIF-8 (depo-
sition rate > 90%) could be loaded onto cellulose fiber [94], and
the growth mechanism was explained by electrostatic and hydro-
gen bonding interactions. With the ZIF-8 coating, the filtration effi-
ciency of PM0.3 was 99.9%, a slightly improved efficiency from that
of pristine cellulose (99.5%). However, the pressure drop increased
greatly (from 198 to 681 Pa), which is understandable given the
high ZIF-8 loading [94]. The improved performances were
explained by (i) the complex tortuous channel and the increased
specific surface area of filters [92] and (ii) the complex porous
structure with a 3D filter network [93]. Su et al. explained the rea-
son in a similar way or interpreted it with the increased specific
surface area of the filter [94].
Graphene or reduced graphene oxide aerogel (rGA) was modi-
fied with ZIF-8 via in situ crystallization (after dipping Zn2+@rGO
in methylimidazole) under ambient conditions [95]. The removal
efficiencies of the produced filter for PM2.5 and PM10 were
>99.3% and >99.6%, respectively, and the high efficiency could be
attributed to (i) the high specific surface area and well-connected
porous network of graphene aerogel and (ii) many metal sites from
ZIF-8/rGA [95]. Importantly, the pressure drop of the aerogel filter
was relatively low of 22 Pa (when the filter thickness was 4 mm
and the air flow velocity was 1.4 m s1).
ZIF-8 was loaded onto polyester (PET) [96] via in-situ synthesis
at 120 °C (after modifying the polyester fiber with aminopropyltri-
Fig. 4. PM removal efficiencies of pure cottons and UiO-66-coated cottons. The ‘‘10” or ‘‘20%” over the bar charts means the crude quantity of coated MOFs. Figures (a, b) show
the removal efficiency for PM2.5 and PM10, respectively. Adapted with permission from Ref. [99] CopyrightÓ 2019, American Chemical society.
5
ethoxysilane). The removal efficiencies (for PM2.5) of the neat PET
and ZIF-8/PET were 38.30% and 77.15%, respectively. The increased
efficiency was explained by the porosity and functional group of
the MOF and electrostatic interactions. The pressure drop
increased slightly (from ~5 to ~8 Pa) due to the ZIF-8 loading.
Moreover, both PET and ZIF-8/PET had a relatively small pressure
drop (<15 Pa) even after the second recycling (after washing in
50% methanol).
ZIF-8@SiO2 composite nanofiber membrane was obtained via
controlled crystallization at room temperature (using contra diffu-
sion) [97]. By increasing the crystallization time from 0.5 to 2 h, the
deposition rate increased monotonically from 20 to 48%. The PM RE
of ZIF-8@SiO2 was as high as 99.96%, which was explained by the
high surface area of ZIF-8 and electrostatic interactions (due to
unbalanced metal ions and defects of the MOF). Interestingly, the
increase in pressure drop (with increasing processing time)
through ZIF-8@SiO2 was very slow compared with that thorough
SiO2 even though ZIF-8@SiO2 had higher pressure drop than SiO2
(before filtering) [97].
UiO-66 with or without functional groups such as –NH2 was
loaded onto CNT-PTFE [98] or cotton fabric [99] via in-situ synthe-
sis. Feng et al. synthesized UiO-66-NH2 in the presence of CNT-
PTFE at 120 °C for 24 h. The obtained filter (the UiO-66-NH2 load-
ing amount was ~9%, after 24 h) was very effective (99.997%, which
was increased from 99.94% with pristine PTFE) in the removal of
ultrafine dust (PM0.3) because of sieving effects [98]. However,
the pressure drop of UiO-66-NH2@CNTs/PTFE membrane (110 Pa)
was considerably higher than that of PTFE membrane (70 Pa) [98].
Yoo and Jhung prepared UiO-66- or UiO-66-NH2-coated cotton
by using a two-step procedure [99]. The preparation of MOF was
conducted at 50 °C for 18 h, and the coated quantity of MOF was
~10% or ~20%, which could be controlled by changing the quantity
of the modulator (acetic acid) in the first step of the synthesis.
Moreover, UiO-66-NH-SO3H, with both -NH- and -SO3H groups,
could be obtained by a reaction between UiO-66-NH2 and 1,4-
butane-sultone. By loading UiO-66-NH-SO3H, the RE for PM2.5
could be increased to 80% (from 35% with pure cotton) as a result
of facile charge separation on the functional group of -SO3H (and,
accordingly, effective electrostatic interaction). The importance of
charge separation in PM removal is supported by the tendency
shown in Fig. 4. The UiO-66-NH-SO3H/cotton and pure cotton
showed QFs of 0.042 and 0.014 Pa1, respectively. The highly
increased (or, tripled) QF with UiO-66-NH-SO3H was because of
the relatively small increase in pressure drop (even with a consid-
erably increased RE (%)) [99].
Hierarchical ZIF-L, together with ZIF-8, was assembled over
glass, polyurethane (three-dimensional foam), nylon microfibers,
6 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477
Fig. 5. Schematic representation of the fabrication procedure for ZIF-67@PAN filters, from PAN and precursors for ZIF-67. Reproduced with permission from Ref. [109].
CopyrightÓ 2020, Elsevier B.V.
and nonwoven fabrics (PP microfibers) via in-situ synthesis for 6 h
at room temperature (without stirring) [100]. The H-ZIF-L_PP
microfiber-based filter showed improved RE (92.5%) for PM2.5
compared with 73.8% with a pure PP-based filter. The increased
efficiency was attributed to (i) the increase of the interception
and impaction of PM from the structure of 2D ZIF-L (or, each side
of the 2D ZIF-L could be used) and (ii) the positively charged sur-
face of 2D ZIF-L. The pressure drop with the H-ZIF-L_PP
microfiber-based filter (10.5 Pa at 0.2 m s1 of face velocity) was
comparable to that of the pristine PP-based filter (9.0 Pa) due to
the hierarchically assembled structure and microporous nature of
ZIF-L [100].
2.2. Electrospinning
Electrospinning is a production method for fibers (especially
ultrafine fibers with a diameter from a few nm to a few tens of
mm) that uses a high-voltage electric force to draw charged threads
from a viscous polymer melt or solution. The electrospinning tech-
nique has also been applied to produce MOF-incorporated and
MOF-derived materials [101,102]. Here, the electrospinning
method to prepare an MOF-incorporated filter, especially for PM
removal, will be discussed.
Since 2016, when electrospun MOFs (20–60%)/polymers (PAN,
PS, and PVP) were applied in PM filtration [61], several filters, mod-
ified with MOFs, have been reported. Hao et al. prepared ZIF-8-
incorporated polyimide (PI) membrane by electrospinning the
mixture of ZIF-8 powder and soluble PI [103]. The prepared mem-
brane showed high RE (96.6%, pure PI’s efficiency was 83.2%) for
PM2.5 (Ci > 300 mg/m3), flexibility, and transmittance. However,
there was only a slight increase in the pressure drop (from 69 to
72 Pa) with ZIF-8 incorporation; therefore, the QF was nearly dou-
bled (from 0.0258 to 0.0470 Pa1), showing the beneficial contribu-
tion of ZIF-8 to PM removal [103]. The improved performances
were explained by (1) the surface charge of ZIF-8; (2) rough mor-
phology of the filter; and (3) ultrathin fiber (suitable for strong
adhesion).
Dai et al. prepared ZIF-8-incorporated porous polylactic acid
(PLA) membrane in a similar manner [104]. Curiously, the addition
of the ZIF-8 nanoparticles promoted the formation of pores on the
surface of fibers. The ZIF-8/PLA membrane showed higher PM2.5
capture efficiency (~95%) than pure PLA (~85%), which was
explained by the functional groups and open metal sites of ZIF-8.
Importantly, the recyclable ZIF-8/PLA had lower pressure drop
than PLA, probably because of the increased porosity [104].
Wang et al. prepared ZIF-8-incorporated polyacrylonitrile (PAN)
with electrospinning and showed nearly perfect (>99.9%) removal
(with a pressure drop of 80.1 Pa and a QF of ~0.1 Pa1) of PM0.3
(Ci > 300 mg/m3) [105]. Synthesized ZIF-67 and polystyrene (PS)
were also electrospun to obtain hierarchical porous nanofiber
membrane [106]. The RE of ZIF-67/PS membrane for PM0.3 was
higher than 99.9% (Ci ~ 200 mg/m3) (because ZIF-67 increased elec-
trostatic interaction), and the pressure drop was 91 Pa [106].
ZIF-67@PAN filters were prepared via electrospinning and the
immersion method [107]. Or, cobalt acetate and PAN were first
electrospun to gain PAN/Co-acetate films, which were immersed
in 2-methylimidazole/ethanol solution for 10 h at room tempera-
ture to obtain ZIF-67@PAN filters [107]. By integrating ZIF-67 into
the electrospun PAN nanofibers, the filtration efficiency for PM2.5
increased from 74.5 to 87.2% (with a pressure drop of 81 Pa). The
improved performance could be explained by enhanced electro-
static interaction owing to the unbalanced metal ions and defects
of MOFs [107].
MIL-53(Al)–NH2-loaded PAN membranes (30% or 60% MOF)
were prepared by electrospinning the mixture of MIL-53(Al)–NH2
and PAN [108]. Moreover, a similar membrane (MOF ~ 30%) was
prepared via the in-situ synthesis of MIL-53(Al)–NH2 in the pres-
ence of an as-spun PAN membrane or heating the mixture of
MOF precursors and PAN membrane for 16 h at 100 °C. This mem-
brane, prepared via the in situ method, was effective in the
removal of fine PM (99.99%) with a pressure drop of 30.5 Pa
[108]. The effective removal was attributed to (i) dipole–dipole
interaction between PM and the MOF or polymer and (ii) physical
adsorption (due to small holes with a large surface area) [108].
Very recently, ZIF-67@PAN filter was prepared via electrospinning
of both PAN and precursors for ZIF-67 (Fig. 5) [109]. ZIF-67 could
be prepared, after spinning the precursors, at room temperature
because no heating was required for the synthesis; and the ZIF-
67@PAN filter was effective in removal of PMs with wide range
of sizes (15 nm to 10 lm).
2.3. Hot pressing
Earlier, Chen et al. coated ZIF-8, ZIF-67, and Ni-ZIF-8 on sub-
strates such as plastic mesh, glass cloth, metal mesh, nonwoven
fabric, and melamine foam using the hot-pressing technique [63].
Or, MOF precursors were first casted onto rolling substrates and
heated to produce MOF-based filters. With increasing cycle times
(casting and heating), the quantity of loaded MOF was increased
linearly despite transmittance decreasing slightly. The ZIF-
 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477 7

Fig. 6. (top) Schematic Presentation of the Hot-Pressing Preparation Method for Various Textiles/MOFs Composites Air Filters for PM Removal. Structures of Four MOFs are
also shown. (bottom) PM removal efficiency for the pure textiles and MOFs@textiles composites. Reproduced with permission from Ref. [111]. CopyrightÓ 2019, American
Chemical society.

8@plastic mesh showed highly improved (~4-fold) RE for PM2.5
compared with the bare plastic mesh. Moreover, the ZIF-
8@plastic mesh can be readily recycled after brush cleaning and
further washing with water/ethanol [63].
A ZIF-8-coated filter was also prepared from zinc acetate and
methylimidazole after loading onto non-woven fabrics (NWFs)
via hot pressing at 100 °C [110]. Interestingly, ZIF-8 composed of
Zn showed bactericidal activity under solar irradiation [110]. The
filter also showed higher PM RE than bare NWF (from ~52 to
96.8% for PM2.5 and from ~62 to 97.7% for PM10) with a low pres-
sure drop of 64 Pa at a 0.7 m s1 flow rate [110].
MOF (such as MIL-53(Al), ZIF-8, UiO-66, or MFM-300(In))-
loaded textiles were prepared with hot pressing [111]. Metal pre-
cursors and organic ligands were mixed, ground, and loaded onto
cotton, aramid, or polyester and heated (80–130 °C) for 10 min
(Fig. 6, top). The MOF-loaded textiles showed highly improved
PM removal efficiencies. For example, MIL-53(Al)@aramid
removed > 95% (from < 50% with aramid) of PM2.5 (and > 96% of
PM10) particles (initial PM2.5 > 280 mg/m3; PM10 > 360 mg/m3)
(Fig. 6, bottom) and was reusable five times [111].
A Zn(II)–organic complex (imidazole-based)-coated air filter
was also prepared via hot pressing [112]. A substrate such as car-
bon fiber cloth was covered with precursors (such as zinc chloride)
of metal–organic complex (named PBM-Zn) and heated for 5 min
at 80 °C. PBM-Zn2@melamine foam-4 showed high removal rates
(PM2.5: 99.5% and PM10: 99.3%) when the initial concentration
was high (PM2.5 > 500 lg/m3; PM10 > 800 lg/m3). These removal
rates were higher than that of base melamine (PM2.5, 79.6%;
PM10, 82.3%) [112]. These good performances were explained by
the higher electrostatic potential f and electron cloud-exposed
metal [112].
2.4. Other methods
Several other methods have been used to prepare air filters
incorporating MOFs or MOF-related materials. Composite filters
8 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477
composed of unconventional MOFs and various substrates were
prepared via vacuum filtration [113]. Or, a selected substrate was
applied to the cooled mother liquor of the MOF synthesis. The
mother liquor was obtained from MOF synthesis after removing
solid portions via filtration and cooling to room temperature. After
maintaining the substrate in mother liquor for 2 h, the substrate
was placed in a vacuuming device. Because of the high zeta poten-
tial and microporous framework (or high porosity), MOF-
incorporated filters showed good performance in PM removal (or
>99.9% for car exhaust gas) [113].
An assembly of MOF crystal on substrate was also applied [114].
Pre-synthesized MOF (NH2-MIL-101(Cr)) crystals were assembled
on PI fibers at ambient temperature in order to achieve ‘‘MOF-
cloth” on PI fibers. The obtained composite showed RE (even at
260 °C) of ~93% (with a pressure drop of 57.5 Pa) for PM0.3. The
RE was highly improved from <50% with pristine PI paper [114].
This good performance was explained by the polar –NH2 group
and surface charge of the MOF, which is helpful for electrostatic
interaction (ESI). Moreover, the large surface area and high f poten-
tial of the MOF crystals might be helpful [114].
MOF-based hollow tubes were prepared via templated freeze-
drying [62]. Various MOFs, such as UIO-66, UiO-66-NH2, ZIF-8,
MIL-101-NH2, and MOF-74, can be formed in hollow tubes, which
leads to low pressure drop and good performance. For example, a
‘‘cellular” hollow tube showed high efficiency (>92%) in PM filtra-
tion with low pressure drop (12 Pa, 0.1 m s1) [62].
Fig. 7. (a) Photograph of a water drop on the N-PUA-NON-2 film and the engineering schemes for PUA-NON and N-PUA-NON films. (b) PM removal efficiencies of PUA, PUA-
NON, N-PUA, and N-PUA-NONs. (c) Recyclability of N-PUA-NON-2 for the removal of PM. Reproduced with permission from Ref. [117]. CopyrightÓ 2019, American Chemical
society.
Flexible self-supported mats of various MOFs, such as MIL-53
(Al), MIL-53(Al)–NH2, Cu-BTC, ZIF-8, ZIF-67, UiO-66, and MIL-88B
(Fe), were obtained from the complete phase transformation (via
hydro/solvothermal reaction) of electrospun metal oxide fibrous
mats [115]. An MOF in a fibrous mat (FM) showed greatly
increased PM RE compared with a metal oxide FM (the precursor
for an MOF FM). For example, FS-MIL-53(Al)-FM showed higher
RE than the precursor Al2O3 FM. Or, the REs increased from 63 to
89% and 67 to 91% for PM2.5 and PM10, respectively, when the ini-
tial concentration was high (PM2.5 = 410 mg/m3, PM10 = 710 mg/
m3) [115].
Porous cellulose nanofiber (CNF) stringed Cu-BTC (polyhedron
membrane on a stainless-steel screen) was obtained via a
filtration-assisted gelation process [116]. The RE of the prepared
hierarchical membrane for PM2.5 was above 95% for a long time,
when the initial concentration of PM2.5 was very high, at
>999 mg/m3. The hierarchical porous structures of Cu-BTC might
contribute to effective PM removal [116].
Sonogashira coupling was applied to coat the nanoporous
organic network (NON) on polyurethane acrylate (PUA) film
[117]. After coating, the PUA film changed into a superhydrophobic
surface and showed highly improved performance in capturing PM
with recyclability (through water washing) (Fig. 7) [117]. The
improved performances were explained by the porosity and high
surface areas of the coated NON [117]. However, unfortunately,
there was no description of the pressure drop or QF in that study.
 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477 9

OH OCH3
Toluene O
Cotton OH + Cotton O Si Cl
Si Cl
OH H3CO OCH3
-3CH3OH O

O O
Zr Toluene Zr
Cotton O Si Cl HO OH Cotton O Si O OH
O O -HCl O O
Zr Zr
O Zr O
Zr Zr Zr
O Zr O
Zr
O O
OH HO OH
HO Zr
Zr
Zr-MOF coated cotton
Zr-MOF

Fig. 8. A scheme to introduce CPTMS onto cotton; and Zr-MOF coating onto cotton by using the introduced CPTMS. Adapted with permission from Ref. [118]. CopyrightÓ
2020, American Chemical society.

Very recently, MOFs were loaded onto substrates via a covalent
bonding between the MOFs and a substrate [118]. Or, we could
coat several UiO-66s on cotton via reactions (by using (3-chloropro
pyl)trimethoxysilane (CPTMS) as a linker) shown in Fig. 8 [118].
2.5. Comparison of various methods
In this section, the advantages and disadvantages of each
method, especially in-situ synthesis, electrospinning, and hot
pressing, will be discussed. First, in-situ synthesis has the advan-
tage of versatility in MOF structures. Or, most MOFs, irrespective
of metal/linker and structure, can be synthesized if the intended
MOFs were reported earlier and synthesis conditions are well
adjusted. Importantly, compatibility between the substrate and
MOF should be considered for homogeneous growth, high disper-
sion, and good adhesion. The weak points of in-situ synthesis
might be that (i) the synthesis of some MOFs requires high-
pressure vessels, for example; therefore, the cost can be high; (ii)
it is not very suitable for mass production; and (iii) pretreatment
of the substrate might be needed for compatibility between the
MOF and substrate.
Second, the electrospinning method also has the advantage of
versatility in MOF structures. Or, any MOF, if already synthesized,
can be introduced to polymers before spinning. However, nano-
sized MOFs and high MOF–polymer compatibility are important
for the homogeneous dispersion of MOFs. Instead of MOF/polymer
spinning, MOFs might also be grown on an electrospun MOF pre-
cursor (metal or linker)/polymer. Electrospinning also has weak
points. Small or nano-sized MOFs are required since big particles
will decrease the efficiency of the introduced MOFs. Moreover,
MOFs may be embedded in the inner part of the polymer; there-
fore, the efficiency of MOFs in interacting with PM might be low,
especially when electrospun polymers are thick. Making porous
polymer, as reported [104], might be one option for utilizing MOFs
effectively in PM capturing.
The hot-pressing method has the advantage of in-situ synthesis
(from precursors) on a solid substrate. However, depending on the
intended MOFs, the heating temperature will be not high enough
for the ready synthesis of MOFs. Or, the temperature cannot be

Table 3
Comparison of preparation methods for MOF-incorporated filters.

Method Advantage Disadvantage Remarks

In situ Possible synthesis of most MOFs - Synthesis of some MOFs needs high
pressure vessels, for example,
therefore, cost can be high.
- Not very suitable for mass
production.
- Pretreatment of substrate might be
needed for compatibility between
MOF and substrate.
Electrospinning* Any MOF, if synthesized, can be -Small or nano-sized MOFs are
introduced onto polymers, before required since big particles will
spinning. decrease the efficiency of MOFs.
-MOFs may be embedded in the inner
part of polymer; therefore, efficiency
of MOFs to interact with PM might be
not high.
Hot pressing Possible in situ synthesis (from -Some MOFs might be not easily
precursors) on solid substrate. produced.
-Substrate might be burned or
destroyed, especially under high
temperature.
*
In electrospinning, a high MOF loading of 60 wt% can be achieved by controlling the particle size and morphology of different MOF crystals [61].
Compatibility between substrate and
MOF is important for homogeneous
growth, high dispersion and good
adhesion.
Instead of spinning of MOF/polymer,
MOFs might be grown on electrospun
MOF precursor (metal or linker)/
polymer.
Nano-sized MOFs and high
compatibility (between MOFs and the
polymers) are important for
homogeneous dispersion of MOFs.
Depending on MOFs, heating
temperature will be not high enough
for ready synthesis.
10 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477
Fig. 9. Proposed capture mechanism of the MOFilter for air pollutants such as PM and SO2. Inset is the SEM image of the surface of the MOF/polymer composite fiber.
Reproduced with permission from Ref. [61]. CopyrightÓ 2016, American Chemical society.
increased to be sufficiently high for the synthesis of a special MOF
such as MIL-101 (which usually requires 220 °C [119]) since sub-
strate such as fabrics can be burnt or destroyed. Conclusively, some
MOFs might not be easily produced via hot pressing. The character-
istics, including advantages and disadvantages, of the three major
methods are summarized in Table 3.
3. Removal of PM with MOF-incorporated filters
3.1. Performances of MOF-incorporated filters
As described, air filters have been advanced by incorporating
MOFs into conventional filters or base materials, such as fabrics.
The developments can be classified into two categories based on
purpose: (i) improving the removal efficiencies significantly and
(ii) perfectly removing PM or securing very high RE (for example,
>99.5%). In this section, advancements will be discussed based on
this classification, especially for removing PM2.5 or smaller PM.
3.1.1. MOF incorporation for largely improving RE
The incorporation of MOFs into substrates was highly effective
in improving RE considerably, irrespective of the loading method
(in situ preparation, electrospinning, hot pressing, and so on) and
substrates, such as synthetic polymers and celluloses. The range
of RE increase was wide (from ~10% [104] to ~50% [92,111,112]).
However, it should be mentioned that low pressure drop is impor-
tant since high RE is not very meaningful if the pressure drop
increases too much. Increases in pressure drops, by loading MOFs,
also ranged widely, from a negligible increase [91,100,103] to a
large increase of ~500 Pa (from 198 Pa with cellulose filter to
681 Pa with cellulose filter @ZIF-8) [94]. Zhu et al. [97]. showed
an interesting trend in the pressure drop of SiO2 fiber (with or
without ZIF-8 loading) with increasing operation time. Even
though ZIF-8@SiO2 had a higher pressure drop than SiO2 before
PM filtration, the increase in pressure drop with ZIF-8@SiO2 due
to increasing quantity of captured PM was very slow compared
with that of SiO2 as a result of the relatively stable fiber structure
of ZIF-8@SiO2 composite membrane [97].
When the increase in pressure drop is very small even with
MOF loading, the QF can be increased considerably because of
the increased RE, as has been observed frequently. For example,
the QF was more than doubled by ZIF-8 and UiO-66-NH-SO3H
loading onto PPC [91] and cotton [99], respectively. Even though
QF is one of the most important parameters for air filters [1], the
values are not always provided in open literatures. In summary,
the incorporation of MOFs into the filter has been highly effective
in increasing the RE considerably.
3.1.2. MOF incorporation for complete removal of PM
The PM RE could be >99.5% or near-perfect by loading MOFs
onto conventional filters. In some cases, the increase in RE was
quite high (~20% [112] or ~35% [93]); however, generally, the RE
was not increased by much (~0.5% [94] or ~0.06% [98]). Irrespective
of the amount of increase in RE, several composite filters (with
MOFs) have shown a RE of >99.9% [93,94,97,98,105,106,108,116].
Therefore, PM of 2.5 mm or less can be removed completely with
MOF-incorporated filters. However, the pressure drop was gener-
ally high (for example, 110 Pa [98] and 134 Pa [93]) for the perfect
removal of PM, excluding MIL-53(Al)–NH2 grown on PAN (MGP),
which had a pressure drop of 30.5 Pa [108]. It is understandable
to have high pressure drop for the complete removal of PM. Unfor-
tunately, there are several reports without data on pressure drop
for both pristine and modified filters. In summary, the modification
of filters with MOFs has been highly effective in the perfect
removal of PM; however, pressure drop can be considerable in
some cases.
3.2. Removal mechanisms
Understanding the PM removal mechanism is very important
not only for fundamental studies but also for practical applications.
Here, the mechanisms that were applied to explain the contribu-
tion of incorporated MOFs to PM removal will be described. As
summarized in Table 2, the removal mechanism with a porous fil-
ter and a fibrous filter was explained traditionally by size exclusion
and diffusion/interception/impaction, respectively.
After loading MOFs onto conventional filters, other mechanisms
were suggested to explain the improved performances. In 2016, for
the first time, Zhang et al. not only showed improved filters by
MOF loading but also suggested plausible mechanisms (Fig. 9),
such as (i) electrostatic interactions between polar PM and positive
MOFs (due to the unbalanced metal ions and defects of MOFs), (ii)
interacting PM with highly polar functional groups (like –OH) of
MOFs, and (iii) the binding of PM to the open metal sites of MOFs
[61]. After the suggestion of the mechanism by Zhang et al. [61],
many researches relied on it when there was a discussion on the
mechanism for PM capturing (with introduced MOFs). Next, sug-
gested mechanisms will be described individually.
 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477
Fig. 10. Plausible interactions between –SO3H of UiO-66-NH-SO3H and three types of PMs: (a) carbonaceous PMs, (b) NO–3, and (c) NH+4 species. Adapted with permission from
Ref. [99]. CopyrightÓ 2019, American Chemical society.
3.2.1. Electrostatic interaction
As mentioned, Zhang et al. [61] previously suggested the ESI
mechanism based on polar PM and the high efficiency of ZIF-8 with
high f potential. After that, there were similar explanations. For
example, Bian et al. suggested enhanced electrostatic interaction
owing to the unbalanced metal ions and defects of ZIF-67 [107].
Wang et al. explained the favorable contribution of Zn-based
metal–organic complexes to PM removal with higher electrostatic
potential and an electron cloud-exposed metal center [112]. Simi-
lar ESI was suggested in effective PM removal with ZIF-8 [96,97].
Moreover, similar dipole–dipole interaction between PM and
MIL-53(Al)-NH2 was suggested [108].
Recently, Yoo and Jhung systematically investigated PM
removal with cotton coated with UiO-66s with a few functional
groups [99]. The RE of coated UiO-66s was in the order of UiO-
66 < UiO-66-NH2 < UiO-66-NH-SO3H, and they pointed out the
importance of charge separations in functional groups of UiO-66.
They also explained the high RE of UiO-66-NH-SO3H with the pos-
sible charge separation of the -SO3H group (and, eventually via
ESI). Moreover, they suggested that any MOF that can have a pos-
sible charge separation can be used to remove any PM, including
nitrate, sulfate, ammonium, and carbons, as shown in Fig. 10
[99]. Very recently, we have also suggested the possible favorable
interaction (via ESI), which can be effective in PM removal,
between charged PMs and MOFs that can have large charge sepa-
ration (like –NO2 group) [118].
3.2.2. High porosity and hierarchical pores
Considering the importance of porosity in adsorption (espe-
cially physical adsorption), porosity and hierarchical pores were
suggested as the driving force for PM capture. For example,
improved PM removal with PUA (coated with NONs) was
explained by the porosity and high surface area of coated NONs
[117]. Wang et al. suggested the contribution of physical adsorp-
tion (because fibers had small holes with a large surface area) in
PM removal with MIL-53(Al)–NH2 [108]. Zhao et al. pointed out
the importance of the hierarchical porous structures of Cu-BTC in
11
PM removal [116]. Moreover, the complex porous structure [94],
high specific surface area/well-connected porous network of gra-
phene aerogel [95], and microporous framework (or high porosity)
of unconventional MOFs [113] were also suggested. Very recently,
the importance of porosity of MOFs in PM removal was confirmed
by us by using isostructural Zr-MOFs such as UiO-66, UiO-67 and
DUT-52 [120]. In that study, we demonstrated that the QF or RE
increased linearly with increasing the surface area of all the stud-
ied MOFs, irrespective of the applied linkers (for synthesizing three
isostructural Zr-MOFs) and synthesis conditions for one MOF UiO-
66 (Fig. 11, for QF). We also suggested why PMs, with much bigger
size than the pore size (with nanometer range) of conventional
MOFs, could be captured readily with MOFs. We explained the
observation with (i) relatively small quantity of captured PM (com-
pared with the weight of filter or MOF) and (ii) contribution of
polar functional groups or polar parts (with very small size) of
PMs in interaction with porous filter containing MOFs [120].
3.2.3. Functional groups of MOFs
As mentioned above, functional groups (especially polar ones),
such as –OH [61] and -SO3H [99], were effective in increasing the
performance in PM capture. Similarly, the polar –NH2 group was
also suggested as a possible strategy for increasing PM removal
[108,114]. Very recently, we have also shown that the PM removal
efficiency and quality factor (as illustrated in Fig. 12 (top)) in of Zr-
MOF-containing filters monotonously increased with increasing
developed charges (in total, ~ 0 to 2.0) on functional groups (such
as –NH+3Cl- and –NO2) of MOFs or UiO-66s [118]. As mentioned,
these functional groups, with charge separations shown in Fig. 12
(bottom), eventually contribute to the favorable ESI with polar or
charged PM. In other words, polar or charged FGs are very effective
in PM removal mainly because of efficient ESI between the FGs and
charged PMs.
3.2.4. Other contributions of MOFs
Given the specific structure of 2D ZIF-L (i.e., each side of 2D ZIF-
L can be used for interaction), the interception and impaction of
12 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477

0.05
(a) PM2.5
Quality factor (Pa )

0.04
-1

2
R =0.997

0.03

Cotton
0.02
UiO-66/cotton
DUT-52/cotton
UiO-67/cotton
0.01
0 1000 2000 3000
2 -1
Surface areaBET (m ·g )

0.06
(b) PM10
Quality factor (Pa )
-1

2
0.04 R =0.970

Cotton
0.02 UiO-66/cotton
DUT-52/cotton
UiO-67/cotton
0 1000 2000 3000
2 -1
Surface areaBET (m ·g ) Fig. 12. (top) Effect of charge separation of FGs (loaded onto Zr-MOF or UiO-66) on
the quality factors of Zr-MOFs/cotton for PM2.5 and PM10 removal. The quantities
Fig. 11. Effect of surface area of isostructural Zr-MOFs, that were coated onto (total, in absolute value) of charge separation of FGs are shown in parentheses,
cotton, on quality factor in removal of PMs. Figures (a) and (b) show the quality below the name of FGS (right of bar charts). (bottom) A Scheme to show the charge
factor for PM2.5 and PM10, respectively. Adapted with permission from Ref. [120]. separations of FGs loaded onto Zr-MOFs or UiO-66s. Adapted with permission from
CopyrightÓ 2020, American Chemical society. Ref. [118]. CopyrightÓ 2020, American Chemical society.

PM could be enhanced [100]. Even though it is not related to the

MOF (here, ZIF-8) itself, the rough morphology of the filter and
ultrathin PI fiber (which is suitable for strong adhesion) have also
been suggested as important factors in PM removal [103].
The open metal sites of MOFs, especially ZIF-8, have been said
to be important in PM capture [91,104]. Traditionally, some MOFs,
such as Cu-BTC, MOF-74, MIL-100, and MIL-101, have been well-
known for OMSs [121]. However, it should be mentioned that gen-
eral MOFs (well crystallized ones) do not have OMSs (even though
defected sites can lead to open or unbalanced metal ions) or a spe-
cial treatment is required for OMS generation [121–123]. More-
over, OMSs, even if present, can be readily saturated by H2O
vapor when filters are in humid conditions [61]. Therefore, it is rec-
ommended that the contribution of OMSs is checked carefully if
these sites are important for PM removal.
4. Summary and perspectives
Based on the above discussion, the following is a summary of
the studies on PM removal from air with MOF-incorporated filters.
MOFs, due to their high porosity, polar functional groups, and pos-
sible high surface charge (e.g., ZIF-8), can be recommended as a
component of a PM filter. MOFs with defects or OMSs are also very
effective in PM capture because of the possible formation of unbal-
anced metal ions or capturing sites, respectively. However, ade-
quate loading (for highly dispersed and good adhesion with the
substrate) is essential for utilizing the porosity and functionality
of MOFs. In particular, approiate bonding or high compatibility
between MOFs and base materials for filters is highly important
for longevity, reusability, low pressure drop, the good dispersion
of MOFs, and cost reduction.
Even though there have been continuous efforts to improve PM
removal from air with MOF-incorporated filters, there is a high
probability of more advanced filters being developed. The follow-
ing are perspectives in the field for both a fundamental under-
standing and commercial applications.
First, more diverse MOFs can be investigated considering the
preparation of many MOF structures, especially with high porosity
and OMSs, such as MIL-100 [124]. Moreover, some MOFs with Ti
(such as MIL-125 [125]) and Ag (such as MIL-101-SO3Ag
[126,127]) might also be interesting for other functionalities (to-
gether with PM capture), such as photocatalysis (to remove other
pollutants) and antibiotics. Highly porous and stable MOFs like
Zr-MOFs [71] can be also recommendable for effective PM removal.
Second, hierarchical MOFs are very interesting even though
there have been a few studies on this or relevant ideas
[94,95,116]. PM particles (of a micron or less) are much larger than
the pore sizes (less than a few nm in general cases) of MOFs; there-
fore, hierarchical MOFs with micro-, meso-, and macro-pores
might be more effective than general/microporous MOFs. Or,
well-dispersed and small-sized MOFs (on substrates) with a large
external surface will show high efficiency.
 D.K. Yoo et al. / Coordination Chemistry Reviews 422 (2020) 213477
Fig. 13. A Scheme to summarize perspectives and interesting research themes on PM removal with MOFs.
Third, surface modification or functionalization is recom-
mended to improve the performances in PM removal, as illustrated
by Jhung et al. [99,118]. Considering the facile functionalization of
MOFs by both direct synthesis and post-synthetic modification,
this is one way of further improving the function of an MOF.
Fourth, several parameters should be considered in the prepara-
tion and operation of MOF-incorporated filters. The weight % of
loaded MOFs and average size of MOF particles may be considered
in the preparation. In the operation to remove PM, RE, pressure
drop, flow rate (both face velocity and volume flow rate), the initial
concentration of PM, the size distributions of PM, and the main
composition (and origin [128,129]) of PM should be accurately
described. These will be helpful for comparing several results and
duplicating other works.
Fifth, the degree of exposure of MOFs should be considered,
especially when prepared via electrospinning and hot pressing.
Electrospun MOFs might be embedded inside of a substrate (and
the MOF thickness might be excessively high if hot pressing is used
to prepare MOFs in large quantity); therefore, the utilization will
not be very high. Accordingly, efforts to increase the degree of
exposure are required, including using porous polymers [104] or
fibrous polymers with small fiber diameter.
Sixth, theoretical calculations to understand both the selective
interaction between PMs and MOFs and preferential loading of
MOFs onto substrates are recommended to understand the PM
removal with MOFs in more detail. However, so far, there was little
attempt to understand PM removal (with MOFs) by using
calculations.
Seventh, fundamental studies, including development of new
materials for air filters and basic study on removal mechanism,
are highly recommended, since further developments for air filters
(especially new functional materials) are required and exact mech-
anisms for PM capture, so far, are not fully understood [1,2].
Based on above, it can be summarized that MOFs will be highly
effective in the removal of PMs (especially, small-sized ones) con-
sidering highly porous MOFs with preferable FGs and preferable
interactions, such as ESI. Since PM with smaller diameters
(0.3 mm or less) has a more serious impact on health and is hard
to capture or remove via simple filtration [14,17], effective removal
of PMs (even small sized) via special interactions will be the strong
point of MOF-based filters. Moreover, MOFs have been and will be
13
advanced very rapidly for various crystal structures, compositions,
functionality, styles (like composite, core–shell, and hollow struc-
ture), and huge porosity; therefore, it can be suggested that
MOF-based filters might have a huge potential for both research/
development and application for PM removal. Finally, perspectives
and interesting research themes on PM removal with MOFs are
summarized as Fig. 13.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgement
This work was supported by Basic Science Research Program
through the National Research Foundation of Korea (NRF) funded
by the Ministry of Science, ICT and future Planning (grant number:
2017R1A2B2008774).
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