Interface-Engineered 2D Heterojunction with Photoelectric Dual Gain: Mxene@MOF-Enhanced SPR Spectroscopy for Direct Sensing of Exosomes.

MXene is widely used in the construction of optoelectronic interfaces due to its excellent properties. However, the hydrophilicity and metastable surface of MXene lead to its oxidation behavior, resulting in the degradation of its various properties, which seriously limits its practical application. In this work, a 2D metal-organic framework (2D MOF) with matching 2D morphology, excellent stability performance, and outstanding optoelectronic performance is grown in situ on the MXene surface through heterojunction engineering to suppress the direct contact between reactive molecules and the inner layer material without affecting the original advantages of MXene. The photoelectric dual gain MXene@MOF heterojunction is confirmed. As a photoelectric material, its properties are highly suitable for the demand of interface sensitization layer materials of surface plasmon resonance (SPR). Therefore, using SPR as a platform for the application of this interface material, the performance of MXene@MOF and its potential mechanism to enhance SPR are analyzed in depth using experiments combined with simulation calculations (FDTD/DFT). Finally, the MXene@MOF/peptides-SPR sensor is constructed for rapid and sensitive detection of the cancer marker exosomes to explore its potential in practical applications. This work offers a forward-looking strategy for the design of interface materials with excellent photoelectric performance.

Rational Construction of 3D Self-Supported MOF-Derived Cobalt Phosphide-Based Hollow Nanowall Arrays for Efficient Overall Water Splitting At large Current Density.

Developing efficient nonprecious bifunctional electrocatalysts for hydrogen and oxygen evolution reactions (HER and OER) in the same electrolyte with a low overpotential and large current density presents an appealing yet challenging goal for large-scale water electrolysis. Herein, a unique 3D self-branched hierarchical nanostructure composed of ultra-small cobalt phosphide (CoP) nanoparticles embedded into N, P-codoped carbon nanotubes knitted hollow nanowall arrays (CoPʘNPCNTs HNWAs) on carbon textiles (CTs) through a carbonization-phosphatization process is presented. Benefiting from the uniform protrusion distributions of CoP nanoparticles, the optimum CoPʘNPCNTs HNWAs composites with high abundant porosity exhibit superior electrocatalytic activity and excellent stability for OER in alkaline conditions, as well as for HER in both acidic and alkaline electrolytes, even under large current densities. Furthermore, the assembled CoPʘNPCNTs/CTs||CoPʘNPCNTs/CTs electrolyzer demonstrates exceptional performance, requiring an ultralow cell voltage of 1.50 V to deliver the current density of 10 mA cm-2 for overall water splitting (OWS) with favorable stability, even achieving a large current density of 200 mA cm-2 at a low cell voltage of 1.78 V. Density functional theory (DFT) calculation further reveals that all the C atoms between N and P atoms in CoPʘNPCNTs/CTs act as the most efficient active sites, significantly enhancing the electrocatalytic properties. This strategy, utilizing 2D MOF arrays as a structural and compositional material to create multifunctional composites/hybrids, opens new avenues for the exploration of highly efficient and robust non-noble-metal catalysts for energy-conversion reactions.

Fabrication of Carboxylate-Functionalized 2D MOF Nanosheet with Caged Cavity for Efficient and Selective Extraction of Uranium from Aqueous Solution.

The efficient removal of radioactive uranium from aqueous solution is of great significance for the safe and sustainable development of nuclear power. An ultrathin 2D metal-organic framework (MOF) nanosheet with cavity structures was elaborately fabricated based on a calix[4]arene ligand. Incorporating the permanent cavity structures on MOF nanosheet can fully utilize its structural characteristics of largely exposed surface area and accessible adsorption sites in pollutant removal, achieving ultrafast adsorption kinetics, and the functionalized cavity structure would endow the MOF nanosheets with the ability to achieve preconcentration and extraction of uranium from aqueous solution, affording ultrahigh removal efficiency even in ultra-low concentrations. Thus, more than 97% uranium can be removed from the concentration range of 50-500 µg L-1 within 5 min. Moreover, the 2D nano-material exhibits ultra-high anti-interference ability, which can efficiently remove uranium from groundwater and seawater. The adsorption mechanism was investigated by X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) analysis, and density functional theory (DFT) calculations, which revealed that the cavity structure plays an important role in uranium capture. This study not only realizes highly efficient uranium removal from aqueous solution but also opens the door to achieving ultrathin MOF nanosheets with cavity structures, which will greatly expand the applications of MOF nanosheets.

2D MOF-enhanced SPR detector based on tunable supramolecular probes for direct and sensitive detection of DOX in serum.

Therapeutic drug monitoring of doxorubicin (DOX) is important to study pharmacokinetics in patients undergoing chemotherapy for reduction of side effects and improve patient survival by rationally controlling the dose of DOX. A fast and ultra-sensitive surface plasmon resonance (SPR) detector without sample pre-handling was developed for DOX monitoring. First, the two-dimensional metal-organic framework was modified on the Au film to enhance SPR, and then, the supramolecular probes with tunable cavity structure were self-assembled at the sensing interface for direct detection of DOX through specific host-guest interactions with a low detection limit of 60.24 pM. The precise monitoring of DOX in serum proved the possibility of clinical application with recoveries in the range 102.86-109.47%. The mechanisms of host-guest interactions between supramolecular and small-molecule drugs were explored in depth through first-principles calculations combined with SPR experiments. The study paves the way for designing facile and sensitive detectors and provides theoretical support and a new methodology for the specific detection of small molecules through calixarene cavity modulation.

Ag Nanoparticles-Induced Metallic Conductivity in Thin Films of 2D Metal-Organic Framework Cu3(HHTP)2.

Two-dimensional (2D) metal-organic frameworks (MOFs) are usually associated with higher electrical conductivity and charge carrier mobility when compared with 3D MOFs. However, attaining metallic conduction in such systems through synthetic or postsynthetic modifications is extremely challenging. Herein, we present the fabrication of thin films of a 2D MOF, Cu3(HHTP)2 (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene), decorated with silver nanoparticles (AgNPs) exhibiting significant conductivity enhancement at room temperature. Variable-temperature electrical transport measurements across the low-temperature (200 K) to high-temperature (373 K) regime evidenced metallic conduction. Interestingly, thin films of a 3D MOF, CuTCNQ (TCNQ = 7,7,8,8-tetracyanoquinodimethane), upon decoration with AgNPs, disclosed a converse trend. The origin of such distinctive observations on AgNPs@Cu3(HHTP)2 and AgNPs@CuTCNQ systems was comprehended by using first-principles density functional theory (DFT) calculations and attributed to an interfacial electronic effect. Our work sheds new light on rationally designing synthetic modifications in thin films of MOFs to tune the electrical transport property.

Theoretical Prediction of Electrocatalytic Reduction of CO2 Using a 2D Catalyst Composed of 3 d Transition Metal and Hexaamine Dipyrazino Quinoxaline.

Transition metals and organic ligands combine to form metal-organic frameworks (MOFs), which possess distinct active sites, large specific surface areas and stable porous structures, giving them considerable promise for CO2 reduction electrocatalysis. In the present study, using spin polarisation density-functional theory, a series of 2D MOFs constructed from 3d transition metal and hexamethylene dipyrazoline quinoxaline(HADQ) were investigated. The calculated binding energies between HADQ and metal atoms for the ten TM-HADQ monolayers were strong sufficient to stably disperse the metal atoms in the HADQ monolayers. Of the ten catalysts tested, seven (Sc, Ni, Cu, Zn, Ti, V and Cr) exhibited high CO2 reduction selectivity, while Mn, Fe and Co required pH values above 2.350, 6.461 and 6.363, respectively, to exhibit CO2 reduction selectivity. HCOOH was the most important producer for Sc, Zn, Ni and Mn, while CH4 was the main producer for Ti, Cr, Fe and V. Cu and Co were less selective, producing HCHO, CH3 OH, and CH4 simultaneously at the same rate-determining step and limiting potential. The Cu-HADQ catalyst had a high overpotential for the HCHO product (1.022 V), while the other catalysts had lower overpotentials between 0.016 V and 0.792 V. Thus, these results predict TM-HADQ to show excellent activity in CO2 electrocatalytic reduction and to become a promising electrocatalyst for CO2 reduction.

Novel synthetic approach of 2D-metal-organic frameworks (MOF) for wastewater treatment.

In addition to their adjustable functionality, structural tunability, and compositional tunability, metal-organic frameworks (MOFs), often known as MOFs, are a distinct form of crystalline porous material. When reduced to two dimensions, ultrathin layers of MOF retain more of its fantastic external features, which is beneficial for a variety of technological applications. Due to their ultrathin atomic-level thickness, easily modifiable structure, and huge surface area, 2D MOF nanosheets and nanocomposites have been the subject of significant research. MOFs are considered intriguing materials for removing toxic contaminants among the novel technologies taken into account in water remediation processes because they exhibit numerous qualities that make them advantageous in water treatment: large surface area, easily functionalizable cavities, a few stable in water, large-scale synthesis, etc Nowadays, water pollution is a rising environmental concern that must be addressed. Due to their special qualities, which include chemical activities, a variety of functionalities, excellent stability, and the ability to be modified for the detection or adsorption of particular molecules, MOFs are widely used in detecting and removing contaminants from water. This review explores most recent wastewater treatment advancements (WWT) using the 2D MOFs mechanism.

Dominant Role of Hole Transport Pathway in Achieving Record High Photoconductivity in Two-Dimensional Metal-Organic Frameworks.

Metal-organic frameworks (MOFs) with mobile charges have attracted significant attention due to their potential applications in photoelectric devices, chemical resistance sensors, and catalysis. However, fundamental understanding of the charge transport pathway within the framework and the key properties that determine the performance of conductive MOFs in photoelectric devices remain underexplored. Herein, we report the mechanisms of photoinduced charge transport and electron dynamics in the conductive 2D M-HHTP (M=Cu, Zn or Cu/Zn mixed; HHTP=2,3,6,7,10,11-hexahydroxytriphenylene) MOFs and their correlation with photoconductivity using the combination of time-resolved terahertz spectroscopy, optical transient absorption spectroscopy, X-ray transient absorption spectroscopy, and density functional theory (DFT) calculations. We identify the through-space hole transport mechanism through the interlayer sheet π-π interaction, where photoinduced hole state resides in HHTP ligand and electronic state is localized at the metal center. Moreover, the photoconductivity of the Cu-HHTP MOF is found to be 65.5 S m-1 , which represents the record high photoconductivity for porous MOF materials based on catecholate ligands.

2D Zn-Porphyrin-Based Co(II)-MOF with 2-Methylimidazole Sitting Axially on the Paddle-Wheel Units: An Efficient Electrochemiluminescence Bioassay for SARS-CoV-2.

High electrocatalytic activity with tunable luminescence is crucial for the development of electrochemiluminescence (ECL) luminophores. In this study, a porphyrin-based heterobimetallic 2D metal organic framework (MOF), [(ZnTCPP)Co2(MeIm)] (1), is successfully self-assembled from the zinc(II) tetrakis(4-carboxyphenyl)porphine (ZnTCPP) linker and cobalt(II) ions in the presence of 2-methylimidazole (MeIm) by a facile one-pot reaction in methanol at room temperature. On the basis of the experimental results and the theoretical calculations, the MOF 1 contains paddle-wheel [Co2(-CO2)4] secondary building units (SBUs) axially coordinated by a MeIm ligand, which is very beneficial to the electron transfer between the Co(II) ions and oxygen. Combining the photosensitizers ZnTCPP and the electroactive [Co2(-CO2)4] SBUs, the 2D MOF 1 possesses an excellent ECL performance, and can be used as a novel ECL probe for rapid nonamplified detection of the RdRp gene of SARS-CoV-2 with an extremely low limit of detection (≈30 aM).

Ratiometric fluorescent sensor based on 2D MOF nanosheets modified by DNA for sensitive detection of Hg2.

Mercury is highly toxic and can accumulate throughout the food cycle, leading to water contamination and foodstuffs pollution. Therefore, increasing attention has been paid to explore effective detection of Hg2+. Here, we report a sensitive Hg2+sensor based on single-stranded DNA (ssDNA) modified two-dimensional (2D) MOF nanosheets by a ratiometric fluorescent method. The chosen 2D MOF nanosheets possess intrinsic peroxidase-like catalytic ability, ssDNA adsorption and fluorescence quenching. We demonstrate that the adsorption of ssDNA can significantly improve the peroxidase mimetic activity of 2D MOF nanosheets, enhancing the fluorescence of substrate Amplex Red. Taking advantages of the favorable characteristics above, we fabricate an efficient Hg2+sensor. In the presence of Hg2+, the ssDNA is released from 2D MOF nanosheets, which results in a decreasing of peroxidase mimetic activity of 2D MOF nanosheets and a fluorescence enhancement of attached fluorophore. A linear relationship between ratiometric fluorescence of substrate and fluorophore and Hg2+concentrations is obtained. The detection limit is 5 nM, which is much lower than the maximal contamination level in drinking water (30 nM) by Word Health Organization. These findings show 2D MOF based ratiometric fluorescent sensor is a convenient and efficient strategy to detect Hg2+.

2D Porphyrinic Metal-Organic Frameworks Featuring Rod-Shaped Secondary Building Units.

Metal-organic frameworks (MOFs) encompass a rapidly expanding class of materials with diverse potential applications including gas storage, molecular separation, sensing and catalysis. So-called 'rod MOFs', which comprise infinitely extended 1D secondary building units (SBUs), represent an underexplored subclass of MOF. Further, porphyrins are considered privileged ligands for MOF synthesis due to their tunable redox and photophysical properties. In this study, the CuII complex of 5,15-bis(4-carboxyphenyl)-10,20-diphenylporphyrin (H2L-CuII, where H2 refers to the ligand's carboxyl H atoms) is used to prepare two new 2D porphyrinic rod MOFs PROD-1 and PROD-2. Single-crystal X-ray analysis reveals that these frameworks feature 1D MnII- or CoII-based rod-like SBUs that are coordinated by labile solvent molecules and photoactive porphyrin moieties. Both materials were characterised using infrared (IR) spectroscopy, powder X-ray diffraction (PXRD) spectroscopy and thermogravimetric analysis (TGA). The structural attributes of PROD-1 and PROD-2 render them promising materials for future photocatalytic investigations.

Facile Synthesis of Two-Dimensional Iron/Cobalt Metal-Organic Framework for Efficient Oxygen Evolution Electrocatalysis.

A facile synthesis is reported of two-dimensional (2D) bimetallic (Fe/Co=1:2) metal-organic frameworks (MOF, ca. 2.2 nm thick) via simple stirring of the reaction mixture of Fe/Co salts and 1,4-benzene dicarboxylic acid (1,4-BDC) in the presence of triethylamine and water at room temperature. The mechanism of the 2D, rather than bulk, MOF was revealed by studying the role of each component in the reaction mixture. It was found that these 2D MOF-Fe/Co(1:2) exhibited excellent electrocatalytic activity for the oxygen evolution reaction (OER) under basic conditions. The electrocatalytic mechanism was disclosed via both experimental results and density functional theory (DFT) calculation. The 2D morphology and co-doping of Fe/Co contributed to the superior OER performance of the 2D MOF-Fe/Co(1:2). The simple and efficient synthetic method is suitable for the mass production and future commercialization of functional 2D MOF with low cost and high yield.

Two-Dimensional Metal-Organic Framework Nanosheets: A Rapidly Growing Class of Versatile Nanomaterials for Gas Separation, MALDI-TOF Matrix and Biomimetic Applications.

Two-dimensional (2D) metal-organic framework (MOF) nanosheets, as an emerging type of 2D materials, attract numerous attention due to their unique properties. First, the ultrathin thickness and nanoscale of the materials results in homogeneous dispersion in aqueous solution, giving the materials more opportunities to be utilized in solution chemistry, especially beneficial to the biomimetic catalysis and bio-related analytical applications. Second, the large surface area and accessible active sites of the MOF nanosheets are favorable to the binding between materials and the substrate, leading to their superior performance in catalysis, sensing and enzyme inhibition. Third, the suitable sizes of nanopores on the 2D MOF nanosheets give them the abilities to act as membranes for highly selective and energy-saving gas separation. This minireview covers the synthesis, characterization as well as bio-related and separation applications of 2D MOF nanosheets.

A fast hemostatic and enhanced photodynamic 2-dimensional metal-organic framework loaded aerogel patch for wound management.

Achieving rapid hemostasis and highly effective antibacterial holds significant importance in the early-stage treatment of wounds. In this study, a hybrid aerogel patch comprising carbon quantum dots (CQDs) modified 2-dimensional (2D) porphyrinic metal-organic framework (MOF) nanosheets was designed by incorporating gelatin methacrylate (GelMA) and polyacrylamide (PAM) based matrix. On one hand, CQDs were stably doped onto the surface of the 2D MOF nanosheets, thereby enhancing the photodynamic activity through fluorescence resonance energy transfer (FRET) process. After the preparation of hybrid aerogel patch, the patch loaded with CQDs-doped 2D MOF exhibited excellent photodynamic bactericidal activity against Gram-positive Staphylococcus aureus (>99.99 %) and Gram-negative Escherichia coli (>99.99 %). On the other hand, the hybrid patch with highly porous and absorbent structure can rapidly absorb blood to aggregate clotting components and form a hydration barrier covering the wound to enhance hemostasis. Besides, the hemolysis and cytotoxicity assays demonstrated a good biocompatibility of this designed patch. In summary, this 2D MOF-loaded aerogel patch holds a potential to achieve rapid hemostasis and effective anti-infection in the early-stage treatment of traumatic wounds.

A comparison between 2D and 3D cobalt-organic framework as catalysts for electrochemical CO2 reduction.

Electrocatalytic CO2 reduction, as an effective way to reduce the CO2 concentration, has gained attention. In this study, we prepared ZIF-67 nanoparticles and nanosheets and investigated them as electrocatalysts for CO2 reduction. It was found that ZIF-67 nanosheets, because of their two-dimensional morphologies, provide more under-coordinated cobalt nodes and have lower overpotentials for both hydrogen evolution and CO2 reduction reactions. Also, the rate-determining step for hydrogen evolution changes from Volmer for ZIF-67 nanoparticles to Hyrovsky for ZIF-67 nanosheets. Also, the presence of Mg2+ ions in solution causes more facile CO2 reduction, especially for ZIF-67 nanosheets.

Two-dimensional metal-organic framework nanozyme-mediated portable paper-based analytical device for dichlorophen assay.

The metal-organic frameworks (MOFs) nanozyme-mediated paper-based analytical devices (PADs) have shown great potential in portable visual determination of phenolic compounds in the environment. However, most MOF nanozymes suffer from poor dispersibility and block-like structure, which often prompts deposition and results in diminished enzymatic activity, severely hindering their environmental applications. Here, we proposed colorimetric PADs for the visual detection of dichlorophen (Dcp) based on its significant inhibitory effect on the two-dimensional (2D) MOF nanozyme activity. Specifically, we synthesized a 2D Cu TCPP (Fe) (defined as 2D-CTF) MOF nanozyme exhibiting excellent dispersibility and remarkable peroxidase-like (POD-like) activity, which could catalyze the oxidation and subsequent color change of 3,3',5,5'-tetramethylbenzidine even under neutral conditions. Notably, the POD-like activity of 2D-CTF demonstrated a unique response to Dcp because of the occupation of Fe-N4 active sites on the 2D-CTF. This property enables the use of 2D-CTF as a highly efficient catalyst to develop colorimetric PADs for naked-eye and portable detection of Dcp. We believe that the proposed colorimetric PADs offer an efficient method for Dcp assay and open fresh avenues for the advancement of colorimetric sensors for analyzing of phenolic toxic substances in real samples.

Transient paper-based electrochemical biosensor Fabricated by superadditive Cu-TCPP(Fe)/Mxene for Multipathway non-invasive, highly sensitive detection of Bodily metabolites.

Current advances in non-invasive fluid diagnostics highlight unique benefits for monitoring metabolic diseases. However, the low concentrations and complex compositions of biomarkers in fluids such as sweat, urine, and saliva impose stringent demands on the sensitivity and stability of detection technologies. Here, we developed a high-sensitivity, low-cost instantaneous electrochemical sensor based on the superadditive effect mechanism of Cu-TCPP(Fe)/Mxene (MMs Paper-ECL Sensor), which has been successfully applied for the simultaneous real-time detection of glucose and uric acid. Strong interfacial interactions between Mxene and Cu-TCPP(Fe) were revealed through precise simulation calculations and multi-dimensional characterization analysis, significantly enhancing the sensor's electrocatalytic performance and reaction kinetics. Experimentally, this exceptional electrocatalytic activity was demonstrated in its unprecedented high sensitivity and wide linear detection range for glucose and uric acid, with a non-invasive linear range from 0.001 nM to 5 mM, 0.025 nM-5 mM, detection limits as low as 1.88 aM and 5.80 pM, and stability extending up to 100 days. This represents not only a breakthrough in sensitivity and stability but also provides an effective, low-cost solution that overcomes the limitations of existing electronic devices, enabling multi-channel simultaneous detection. The universality of this sensor holds vast potential for application in the field of non-invasive fluid diagnostics.

2D MOF-enhanced SPR sensing platform: Facile and ultrasensitive detection of Sulfamethazine via supramolecular probe.

Sulfamethazine (SMZ) is widely present in the environment and can cause severe allergic reactions and cancer in humans. Accurate and facile monitoring of SMZ is crucial for maintaining environmental safety, ecological balance, and human health. In this work, a real-time and label-free surface plasmon resonance (SPR) sensor was devised using a two-dimensional metal-organic framework with superior photoelectric performance as an SPR sensitizer. The supramolecular probe was incorporated at the sensing interface, allowing for the specific capture of SMZ from other analogous antibiotics through host-guest recognition. The intrinsic mechanism of the specific interaction of the supramolecular probe-SMZ was elucidated through the SPR selectivity test in combination with analysis by density functional theory, including p-π conjugation, size effect, electrostatic interaction, π-π stacking, and hydrophobic interaction. This method facilitates a facile and ultrasensitive detection of SMZ with a limit of detection of 75.54 pM. The accurate detection of SMZ in six environmental samples demonstrates the potential practical application of the sensor. Leveraging the specific recognition of supramolecular probes, this direct and simple approach offers a novel pathway for the development of novel SPR biosensors with outstanding sensitivity.

High electrochemical active Au-NP/2D zinc-metal organic frameworks heterostructure-based ECL sensor for the miRNA-522 detection in triple negative breast cancer.

In this work, a novel electrochemiluminescence (ECL) sensor has been developed to detect the miRNA-522 in the tumor tissues of triple-negative breast cancer (TNBC) patients. Au NPs/Zn MOF heterostructure was obtained by in situ growth and used as novel luminescence probe. Firstly, zinc-metal organic framework nanosheets (Zn MOF NSs) were synthesized with Zn2+ as the central metal ion and 2-aminoterephthalic acid (NH2-BDC) as the ligand. 2D MOF nanosheets with ultra-thin layered structure and relatively large specific surface areas can enhance the catalytic activity in the ECL generation. Furthermore, the electron transfer capacity and the electrochemical active surface area of MOF were greatly improved by the growth of Au NPs. Therefore, Au NPs/Zn MOF heterostructure showed the significant electrochemical activity in the sensing process. In addition, the magnetic Fe3O4@SiO2@Au microspheres were used as capture units in the magnetic separation step. The magnetic spheres with hairpin aptamer H1 can capture target gene. Then the captured miRNA-522 triggered the target catalyzed hairpin assembly (CHA) sensing process and linked Au NPs/Zn MOF heterostructure. The concentration of miRNA-522 can be quantified by the ECL signal enhancement of the Au NPs/Zn MOF heterostructure. Due to the high catalytic activity of Au NPs/Zn MOF heterostructure and their unique structural and electrochemical properties, the prepared ECL sensor achieved high-sensitive detection of miRNA-522 in the range of 1 fM to 0.1 nM with the detection limit of 0.3 fM. This strategy can provide a potential alternative for miRNA detection in medical research and clinical diagnosis of triple negative breast cancer.

The development of a fluorescence/colorimetric biosensor based on the cleavage activity of CRISPR-Cas12a for the detection of non-nucleic acid targets.

Nano-biosensors are of great significance for the analysis and detection of important biological targets. Surprisingly, the CRISPR-Cas12a system not only provides us with excellent gene editing capabilities, it also plays an important role in biosensing due to its high base resolution and high levels of sensitivity. However, most CRISPR-Cas12a-based sensors are limited by their recognition and output modes, are therefore only utilized for the detection of nucleic acids using fluorescence as an output signal. In the present study, we further explored the potential application of CRISPR-Cas12a and developed a CRISPR-Cas12a-based fluorescence/colorimetric biosensor (UCNPs-Cas12a/hydrogel-MOF-Cas12a) that provides an efficient targeting system for small molecules and protein targets. These two sensors yield multiple types of signal outputs by converting the target molecule into a deoxyribonucleic acid (DNA) signal input system using aptamers, amplifying the DNA signal by catalyzed hairpin assembly (CHA), and then combining CRISPR-Cas12a with various nanomaterials. UCNPs-Cas12a/hydrogel-MOF-Cas12a exhibited prominent sensitivity and stability for the detection of estradiol (E2) and prostate-specific antigen (PSA), and was successfully applied for the detection of these targets in milk and serum samples. A major advantage of the hydrogel-MOF-Cas12a system is that the signal output can be observed directly. When combined with aptamers and nanomaterials, CRISPR-Cas12a can be used to target multiple targets, with a diverse array of signal outputs. Our findings create a foundation for the development of CRISPR-Cas12a-based technologies for application in the fields of food safety, environmental monitoring, and clinical diagnosis.