Ultrathin ferroic HfO2-ZrO2 superlattice gate stack for advanced transistors.

With the scaling of lateral dimensions in advanced transistors, an increased gate capacitance is desirable both to retain the control of the gate electrode over the channel and to reduce the operating voltage1. This led to a fundamental change in the gate stack in 2008, the incorporation of high-dielectric-constant HfO2 (ref. 2), which remains the material of choice to date. Here we report HfO2-ZrO2 superlattice heterostructures as a gate stack, stabilized with mixed ferroelectric-antiferroelectric order, directly integrated onto Si transistors, and scaled down to approximately 20 ångströms, the same gate oxide thickness required for high-performance transistors. The overall equivalent oxide thickness in metal-oxide-semiconductor capacitors is equivalent to an effective SiO2 thickness of approximately 6.5 ångströms. Such a low effective oxide thickness and the resulting large capacitance cannot be achieved in conventional HfO2-based high-dielectric-constant gate stacks without scavenging the interfacial SiO2, which has adverse effects on the electron transport and gate leakage current3. Accordingly, our gate stacks, which do not require such scavenging, provide substantially lower leakage current and no mobility degradation. This work demonstrates that ultrathin ferroic HfO2-ZrO2 multilayers, stabilized with competing ferroelectric-antiferroelectric order in the two-nanometre-thickness regime, provide a path towards advanced gate oxide stacks in electronic devices beyond conventional HfO2-based high-dielectric-constant materials.

Confinement of Ultrasmall Bimetallic Nanoparticles in Conductive Metal-Organic Frameworks via Site-Specific Nucleation.

Conductive metal-organic frameworks (cMOFs) are emerging materials for various applications due to their high surface area, high porosity, and electrical conductivity. However, it is still challenging to develop cMOFs having high surface reactivity and durability. Here, highly active and stable cMOF are presented via the confinement of bimetallic nanoparticles (BNPs) in the pores of a 2D cMOF, where the confinement is guided by dipolar-interaction-induced site-specific nucleation. Heterogeneous metal precursors are bound to the pores of 2D cMOFs by dipolar interactions, and the subsequent reduction produces ultrasmall (≈1.54 nm) and well-dispersed PtRu NPs confined in the pores of the cMOF. PtRu-NP-decorated cMOFs exhibit significantly enhanced chemiresistive NO2 sensing performances, owing to the bimetallic synergies of PtRu NPs and the high surface area and porosity of cMOF. The approach paves the way for the synthesis of highly active and conductive porous materials via bimetallic and/or multimetallic NP loading.

Large-area synthesis of nanoscopic catalyst-decorated conductive MOF film using microfluidic-based solution shearing.

Conductive metal-organic framework (C-MOF) thin-films have a wide variety of potential applications in the field of electronics, sensors, and energy devices. The immobilization of various functional species within the pores of C-MOFs can further improve the performance and extend the potential applications of C-MOFs thin films. However, developing facile and scalable synthesis of high quality ultra-thin C-MOFs while simultaneously immobilizing functional species within the MOF pores remains challenging. Here, we develop microfluidic channel-embedded solution-shearing (MiCS) for ultra-fast (≤5 mm/s) and large-area synthesis of high quality nanocatalyst-embedded C-MOF thin films with thickness controllability down to tens of nanometers. The MiCS method synthesizes nanoscopic catalyst-embedded C-MOF particles within the microfluidic channels, and simultaneously grows catalyst-embedded C-MOF thin-film uniformly over a large area using solution shearing. The thin film displays high nitrogen dioxide (NO2) sensing properties at room temperature in air amongst two-dimensional materials, owing to the high surface area and porosity of the ultra-thin C-MOFs, and the catalytic activity of the nanoscopic catalysts embedded in the C-MOFs. Therefore, our method, i.e. MiCS, can provide an efficient way to fabricate highly active and conductive porous materials for various applications.

Chemiresistive Hydrogen Sensors: Fundamentals, Recent Advances, and Challenges.

Hydrogen (H2) is one of the next-generation energy sources because it is abundant in nature and has a high combustion efficiency that produces environmentally benign products (H2O). However, H2/air mixtures are explosive at H2 concentrations above 4%, thus any leakage of H2 must be rapidly and reliably detected at much lower concentrations to ensure safety. Among the various types of H2 sensors, chemiresistive sensors are one of the most promising sensing systems due to their simplicity and low cost. This review highlights the advances in H2 chemiresistors, including metal-, semiconducting metal oxide-, carbon-based materials, and other materials. The underlying sensing mechanisms for different types of materials are discussed, and the correlation of sensing performances with nanostructures, surface chemistry, and electronic properties is presented. In addition, the discussion of each material emphasizes key advances and strategies to develop superior H2 sensors. Furthermore, recent key advances in other types of H2 sensors are briefly discussed. Finally, the review concludes with a brief outlook, perspective, and future directions.

Single-Atom Pt Stabilized on One-Dimensional Nanostructure Support via Carbon Nitride/SnO2 Heterojunction Trapping.

Catalysis with single-atom catalysts (SACs) exhibits outstanding reactivity and selectivity. However, fabrication of supports for the single atoms with structural versatility remains a challenge to be overcome, for further steps toward catalytic activity augmentation. Here, we demonstrate an effective synthetic approach for a Pt SAC stabilized on a controllable one-dimensional (1D) metal oxide nano-heterostructure support, by trapping the single atoms at heterojunctions of a carbon nitride/SnO2 heterostructure. With the ultrahigh specific surface area (54.29 m2 g-1) of the nanostructure, we obtained maximized catalytic active sites, as well as further catalytic enhancement achieved with the heterojunction between carbon nitride and SnO2. X-ray absorption fine structure analysis and HAADF-STEM analysis reveal a homogeneous atomic dispersion of Pt species between carbon nitride and SnO2 nanograins. This Pt SAC system with the 1D nano-heterostructure support exhibits high sensitivity and selectivity toward detection of formaldehyde gas among state-of-the-art gas sensors. Further ex situ TEM analysis confirms excellent thermal stability and sinter resistance of the heterojunction-immobilized Pt single atoms.

Hydrogen Sensors Based on MoS2 Hollow Architectures Assembled by Pickering Emulsion.

For rapid hydrogen gas (H2) sensing, we propose the facile synthesis of the hollow structure of Pt-decorated molybdenum disulfide (h-MoS2/Pt) using ultrathin (mono- or few-layer) two-dimensional nanosheets. The controlled amphiphilic nature of MoS2 surface produces ultrathin MoS2 NS-covered polystyrene particles via one-step Pickering emulsification. The incorporation of Pt nanoparticles (NPs) on the MoS2, followed by pyrolysis, generates the highly porous h-MoS2/Pt. This hollow hybrid structure produces sufficiently permeable pathways for H2 and maximizes the active sites of MoS2, while the Pt NPs on the hollow MoS2 induce catalytic H2 spillover during H2 sensing. The h-MoS2/Pt-based chemiresistors show sensitive H2 sensing performances with fast sensing speed (response, 8.1 s for 1% of H2 and 2.7 s for 4%; and recovery, 16.0 s for both 1% and 4% H2 at room temperature in the air). These results mark the highest H2 sensing speed among 2D material-based H2 sensors operated at room temperature in air. Our fabrication method of h-MoS2/Pt structure through Pickering emulsion provides a versatile platform applicable to various 2D material-based hollow structures and facilitates their use in other applications involving surface reactions.

The Design and Science of Polyelemental Nanoparticles.

Polyelemental nanoparticles (PE NPs) containing four or more elements in a single NP have intriguing intrinsic properties compared to their single-element counterparts. The fusion of diverse elements induces synergistic effects including new physical and chemical phenomena. However, conventional methods have not offered effective strategies for the uniform creation of PE NPs with high reproducibility. Recently, with advances in nanoscience, several new methods have been developed using both thermodynamic and kinetic approaches and, often, the interplay between them. In this Perspective, we highlight recent key advances in the design of PE NPs and their underlying formation mechanisms. We discuss the potential applications of PE NPs and the outlook and future directions for this field.

Pore-Size-Tuned Graphene Oxide Membrane as a Selective Molecular Sieving Layer: Toward Ultraselective Chemiresistors.

Conventional graphene oxide (GO)-based gas membranes, having a narrow pore-size range of less than 0.3 nm, exhibit limited gas molecular permeability because of the kinetic diameters of most volatile organic and sulfur compound (VOCs/VSCs) molecules being larger than 0.3 nm. Here, we employ GO nanosheets (NSs) with a tunable pore-size distribution as a molecular sieving layer on two-dimensional (2D) metal oxide NSs-based gas sensors, i.e., PdO-sensitized WO3 NSs to boost selectivity toward specific gas species. The pore size, surface area, and pore density of GO NSs were simply manipulated by controlling H2O2 concentration. In addition, the pore size-tuned GO NSs were coated on cellulose filtering paper as a free-standing nanoporous membrane. Holey GO membrane showed a highly selective H2S permeability characteristic, exhibiting superior cross-selectivity to CH3COCH3 (0.46 nm), C2H5OH (0.45 nm), and C7H8 (0.59 nm) with larger kinetic diameters compared with H2S (0.36 nm). Such pore-size-tuned GO nanoporous layer is scalable and robust, highlighting a great promise for designing low cost and highly efficient gas-permeable membrane for outstanding selective gas sensing platform.

Catalytic Metal Nanoparticles Embedded in Conductive Metal-Organic Frameworks for Chemiresistors: Highly Active and Conductive Porous Materials.

Conductive porous materials having a high surface reactivity offer great promise for a broad range of applications. However, a general and scalable synthesis of such materials remains challenging. In this work, the facile synthesis of catalytic metal nanoparticles (NPs) embedded in 2D metal-organic frameworks (MOFs) is reported as highly active and conductive porous materials. After the assembly of 2D conductive MOFs (C-MOFs), i.e., Cu3(hexahydroxytriphenylene)2 [Cu3(HHTP)2], Pd or Pt NPs are functionalized within the cavities of C-MOFs by infiltration of metal ions and subsequent reduction. The unique structure of Cu3(HHTP)2 with a cavity size of 2 nm confines the bulk growth of metal NPs, resulting in ultra-small (≈2 nm) and well-dispersed metal NPs loaded in 2D C-MOFs. The Pd or Pt NPs-loaded Cu3(HHTP)2 exhibits remarkably improved NO2 sensing performance at room temperature due to the high reactivity of catalytic metal NPs and the high porosity of C-MOFs. The catalytic effect of Pd and Pt NPs on NO2 sensing of Cu3(HHTP)2, in terms of reaction rate kinetics and activation energy, is demonstrated.

Universal Synthesis of Porous Inorganic Nanosheets via Graphene-Cellulose Templating Route.

Two-dimensional (2D) inorganic nanomaterials have attracted enormous interest in diverse research areas because of their intriguing physicochemical properties. However, reliable method for the synthesis and composition manipulation of polycrystalline inorganic nanosheets (NSs) are still considered grand challenges. Here, we report a robust synthetic route for producing various kinds of inorganic porous NSs with desired multiple components and precise compositional stoichiometry by employing tunicin, i.e., cellulose extracted from earth-abundant marine invertebrate shell waste. Cellulose fibrils can be tightly immobilized on graphene oxide (GO) NSs to form stable tunicin-loaded GO NSs, which are used as a sacrificial template for homogeneous adsorption of diverse metal precursors. After a subsequent pyrolysis process, 2D metallic or metal oxide NSs are formed without any structural collapse. The rationally designed tunicin-loaded GO NS templating route paves a new path for the simple preparation of multicompositional inorganic NSs for broad applications, including chemical sensing and electrocatalysis.

High-Resolution, Fast, and Shape-Conformable Hydrogen Sensor Platform: Polymer Nanofiber Yarn Coupled with Nanograined Pd@Pt.

We report a flexible hydrogen sensing platform based on a single-strand yarn consisting of high-density electrospun nanofibers, on which nanograined Pd or Pd@Pt is coated via yarn spinning followed by sputter deposition. In general, Pd undergoes a phase transition to PdH x (α-PdH x at [H2] < 1% and ß-PdH x at [H2] > 2%), in which H atoms act as electron scattering centers, thus increasing the resistance. In our system, the sensors exhibit switchable H2 sensing behaviors, that is, (i) Δ R/ R0 > 0 at [H2] > 1% by the active electron scattering and (ii) Δ R/ R0 < 0 at [H2] < 1% derived from nanograined Pd effects. Due to high mechanical stability stemming from nanogranular morphologies of Pd, which is essential for enduring a huge volume expansion upon exposure to high-concentration H2, we could obtain a wide concentration range (4-0.0001%) H2 detection resolution. Moreover, an ultrathin Pt overlayer coated on Pd offers an accelerated H2 detection capability based on effective gas dissociation and activation properties. Furthermore, by virtue of the core (thread)-shell (nanofiber yarn) scaffold, long cycling reliability and flexibility were achieved. This facile and low-cost yarn fabrication method offers the development of single-strand thread-type wearable chemiresistors that possess a high surface area and open porosity, facilitating gas diffusion and reaction.

Heterogeneous Metal Oxide-Graphene Thorn-Bush Single Fiber as a Freestanding Chemiresistor.

The development of freestanding fiber-type chemiresistors, having high integration ability with various portable electronics including smart clothing systems, is highly demanding for the next-generation wearable sensing platforms. However, critical challenges stemming from the irreversible chemical sensing kinetics and weak reliability of the freestanding fiber-type chemiresistor hinder their practical use. In this work, for the first time, we report on the potential suitability of the freestanding and ultraporous reduced graphene oxide fiber functionalized with WO3 nanorods (porous WO3 NRs-RGO composite fiber) as a sensitive nitrogen dioxide (NO2) detector. By employing a tunicate cellulose nanofiber (TCNF), which is a unique animal-type cellulose, the numerous mesopores are formed on a wet-spun TCNF-GO composite fiber, unlike a bare GO fiber with dense surface structure. More interestingly, due to the superior wettability of TCNF, the aqueous tungsten precursor is uniformly adsorbed on an ultraporous TCNF-GO fiber, and subsequent heat treatment results in the thermal reduction of a TCNF-GO fiber and hierarchical growth of WO3 NRs perpendicular to the porous RGO fiber (porous WO3 NRs-RGO fiber). The freestanding porous WO3 NRs-RGO fiber shows a notable response to 1 ppm NO2. Furthermore, we successfully demonstrate reversible NO2 sensing characteristics of the porous WO3 NRs-RGO fiber, which is integrated on a wrist-type wearable sensing device.

Glass-Fabric Reinforced Ag Nanowire/Siloxane Composite Heater Substrate: Sub-10 nm Metal@Metal Oxide Nanosheet for Sensitive Flexible Sensing Platform.

The development of flexible chemiresistors is imperative for real-time monitoring of air quality and/or human physical conditions without space constraints. However, critical challenges such as poor sensing characteristics, vulnerability under toxic chemicals, and weak reliability hinder their practical use. In this work, for the first time, an ultrasensitive flexible sensing platform is reported by assembling Pt loaded thin-layered (≈10 nm) SnO2 nanosheets (Pt-SnO2 NSs) based 2D sensing layers on Ag nanowires embedded glass-fabric reinforced vinyl-phenyl siloxane hybrid composite substrate (AgNW-GFRVPH film) as a heater. The thermally stable AgNW-GFRVPH film based heater is fabricated by free radical polymerization of vinyl groups in vinyl-phenyl oligosiloxane and phenyltris(dimethylvinylsiloxy)silane with Ag NW and glass-fabric, showing outstanding heat generation (≈200 °C), high dimensional stability (13 ppm °C-1), and good thermal stability (≈350 °C). The Pt-SnO2 NSs, which are synthesized by calcination of Sn precursor coated graphene oxide (GO) sheets and subsequent Pt functionalization, exhibit high mechanical flexibility and superior response (Rair/Rgas = 4.84) to 1 ppm level dimethyl sulfide. Taking these advantages, GO-templated oxide NSs combined with a highly stable AgNW-GFRVPH film heater exhibits the best dimethyl sulfide sensing performance compared to state-of-the-art flexible chemiresistors, enabling them as a superior flexible gas sensing platform.

Pt-Functionalized PdO Nanowires for Room Temperature Hydrogen Gas Sensors.

In this work, we prepared a well-aligned palladium oxide nanowire (PdO NW) array using the lithographically patterned Pd nanowire electrodeposition (LPNE) method followed by subsequent calcination at 500 °C. Sensitization with platinum (Pt) nanoparticles (NPs), which were functionalized on PdO NWs through a simple reduction process, significantly enhanced the detection capability of the Pt-loaded PdO NWs (Pt-PdO NWs) sensors toward hydrogen gas (H2) at room temperature. The well-distributed Pt NPs, which are known chemical sensitizers, activated the dissociation of H2 and oxygen molecules through the spillover effect with subsequent diffusion of these products to the PdO surface, thereby transforming the entire surface of the PdO NWs into reaction sites for H2. As a result, at a high concentration of H2 (0.2%), the Pt-PdO NWs showed an enhanced sensitivity of 62% (defined as Δ R/ Rair × 100%) compared to that (6.1%) of pristine PdO NWs. The Pt-PdO NWs exhibited a response time of 166 s, which was 2.68-fold faster than that of pristine PdO NWs (445 s). In addition, the Pt-PdO NWs responded to a very low concentration of H2 (10 ppm) with a sensitivity of 14%, unlike the pristine PdO NWs, which did not exhibit any response at that concentration. These outstanding results are mainly attributed to a homogeneous decoration of Pt NPs on the surface of well-aligned PdO NWs. In this work, we demonstrated the potential suitability of Pt-PdO NWs as a highly sensitive H2 sensing layer at room temperature.

In Situ Coupling of Multidimensional MOFs for Heterogeneous Metal-Oxide Architectures: Toward Sensitive Chemiresistors.

Metal-organic frameworks (MOFs) are used as a new intriguing class of templates, which enable the creation of porous inorganic nanostructures via calcination. In this work, we first introduce in situ coupling of multidimensional MOFs for producing heterogeneous metal-oxide composite with multiple p-n junctions. Controlling relative ratios of two mixed solvents (water and ethanol), in zeolitic imidazolate framework (ZIF) growth, leads to the distinctive morphological evolution such as rod, sheet, and polyhedron particles. One-pot hybridization of ZIF-8 (sheet) with ZIF-67 (rods) results in the generation of hierarchically assembled 1D ZIF-67 rods anchored on a 2D ZIF-8 sheet. Through the calcination of such hybridized ZIFs, we successfully prepared hierarchically assembled 1D Co3O4 rods immobilized in a 2D ZnO sheet, possessing numerous n-type ZnO/p-type Co3O4 heterogeneous interfaces. This unique structure offers a remarkably enhanced chemiresistive sensing performance (Ra/Rg = 29 at 5 ppm acetone).

Chitosan-templated Pt nanocatalyst loaded mesoporous SnO2 nanofibers: a superior chemiresistor toward acetone molecules.

In this work, we introduce a chitosan-Pt complex (CS-Pt) as an effective template for catalytic Pt sensitization and creation of abundant mesopores in SnO2 nanofibers (NFs). The Pt particles encapsulated by the CS exhibit ultrasmall size (∼2.6 nm) and high dispersion characteristics due to repulsion between CS molecules. By combining CS-Pt with electrospinning, mesoporous SnO2 NFs uniformly functionalized with the Pt catalyst (CS-Pt@SnO2 NFs) are synthesized. Particularly, numerous mesopores with diameters of ∼20 nm form through the decomposition of CS, while a small SnO2 grain size (14.32 nm) is achieved by the pinning effect of CS. It is observed that CS-Pt@SnO2 NFs exhibit outstanding response (Rair/Rgas = 141.92 at 5 ppm), excellent selectivity, stability, and fast response (12 s)/recovery (44 s) speed toward 1 ppm of acetone at 350 °C and high humidity (90% RH). In addition, by applying an exponential fitting tool to experimental response values toward 0.1-5 ppm of acetone, it is estimated that CS-Pt@SnO2 NFs can detect 5 ppb of acetone with a notable response (Rair/Rgas = 2.9). Furthermore, the sensor array based on CS-Pt@SnO2 NFs, CS-driven SnO2 NFs, polyol-Pt loaded SnO2 NFs, and dense SnO2 NFs obviously classifies simulated diabetic breath and healthy human breath by using a pattern recognition tool. These results clearly demonstrate that mesoporous SnO2 NFs, particularly functionalized with CS-Pt templated nanocatalysts, open up a new class of sensing layers offering high sensitivity and selectivity.

An Impedance-Transduced Chemiresistor with a Porous Carbon Channel for Rapid, Nonenzymatic, Glucose Sensing.

A new type of chemiresistor, the impedance-transduced chemiresistor (ITCR), is described for the rapid analysis of glucose. The ITCR exploits porous, high surface area, fluorine-doped carbon nanofibers prepared by electrospinning of fluorinated polymer nanofibers followed by pyrolysis. These nanofibers are functionalized with a boronic acid receptor and stabilized by Nafion to form the ITCR channel for glucose detection. The recognition and binding of glucose by the ITCR is detected by measuring its electrical impedance at a single frequency. The analysis frequency is selected by measuring the signal-to-noise ( S/ N) for glucose detection across 5 orders of magnitude, evaluating both the imaginary and real components of the complex impedance. On the basis of this analysis, an optimal frequency of 13 kHz is selected for glucose detection, yielding an S/ N ratio of 60-100 for [glucose] = 5 mM using the change in the total impedance, Δ Z. The resulting ITCR glucose sensor shows a rapid analysis time (<8 s), low coefficient of variation for a series of sensors (<10%), an analysis range of 50 µM to 5 mM, and excellent specificity versus fructose, ascorbic acid, and uric acid. These metrics for the ITCR are obtained using a sample size as small as 5 µL.

Bimodally Porous WO3 Microbelts Functionalized with Pt Catalysts for Selective H2S Sensors.

Bimodally meso- (2-50 nm) and macroporous (>50 nm) WO3 microbelts (MBs) functionalized with sub-3 nm Pt catalysts were fabricated via the electrospinning technique followed by subsequent calcination. Importantly, apoferritin (Apo), tea saponin and polystyrene colloid spheres (750 nm) dispersed in an electrospinning solution acted as forming agents for producing meso- and macropores on WO3 MBs during calcination. Particularly, mesopores provide not only numerous reaction sites for effective chemical reactions, but also facilitate gas diffusion into the interior of the WO3 MBs, dominated by Knudsen diffusion. The macropores further accelerate gas permeability in the interior and on the exterior of the WO3 MBs. In addition, Pt nanoparticles with mean diameters of 2.27 nm were synthesized by using biological protein cages, such as Apo, to further enhance the gas sensing performance. Bimodally porous WO3 MBs functionalized by Pt catalysts showed remarkably high hydrogen sulfide (H2S) response ( Rair/ Rgas = 61 @ 1 ppm) and superior selectivity to H2S against other interfering gases, such as acetone (CH3COCH3), ethanol (C2H5OH), ammonia (NH3), and carbon monoxide (CO). These results demonstrate a high potential for the feasibility of catalyst-loaded meso- and macroporous WO3 MBs as new sensing platforms for the possibility of real-time diagnosis of halitosis.

Feasible Defect Engineering by Employing Metal Organic Framework Templates into One-Dimensional Metal Oxides for Battery Applications.

Facile synthesis of rationally designed nanostructured electrode materials with high reversible capacity is highly critical to meet ever-increasing demands for lithium-ion batteries. In this work, we employed defect engineering by incorporating metal organic framework (MOF) templates into one-dimensional nanostructures by simple electrospinning and subsequent calcination. The introduction of Co-based zeolite imidazole frameworks (ZIF-67) resulted in abundant oxygen vacancies, which induce not only more active sites for Li storage but also enhanced electrical conductivity. Moreover, abundant mesoporous sites are formed by the decomposition of ZIF-67, which are present both inside and outside the resultant SnO2-Co3O4 nanofibers (NFs). Attributed to the creation of vacancy sites along with the synergistic effects of SnO2 and Co3O4, SnO2-Co3O4 NFs exhibit an excellent reversible capacity for 300 cycles (1287 mA h g-1 at a current density of 500 mA g-1) along with superior rate capabilities and improved initial Coulombic efficiency compared with pristine SnO2 NFs. This is an early report on utilizing MOF structures as the defect formation platform into one-dimensional nanostructures, which is expected to result in superior electrochemical performances required for advanced electrodes.

Hierarchical Metal-Organic Framework-Assembled Membrane Filter for Efficient Removal of Particulate Matter.

Here, we propose heterogeneous nucleation-assisted hierarchical growth of metal-organic frameworks (MOFs) for efficient particulate matter (PM) removal. The assembly of two-dimensional (2D) Zn-based zeolite imidazole frameworks (2D-ZIF-L) in deionized water over a period of time produced hierarchical ZIF-L (H-ZIF-L) on hydrophilic substrates. During the assembly, the second nucleation and growth of ZIF-L occurred on the surface of the first ZIF-L, leading to the formation of flowerlike H-ZIF-L on the substrate. The flowerlike H-ZIF-L was easily synthesized on various substrates, namely, glass, polyurethane three-dimensional foam, nylon microfibers, and nonwoven fabrics. We demonstrated H-ZIF-L-assembled polypropylene microfibers as a washable membrane filter with highly efficient PM removal property (92.5 ± 0.8% for PM2.5 and 99.5 ± 0.2% for PM10), low pressure drop (10.5 Pa at 25 L min-1), long-term stability, and superior recyclability. These outstanding particle filtering properties are mainly attributed to the unique structure of the 2D-shaped H-ZIF-L, which is tightly anchored on individual fibers comprising the membrane.