Peroxidase-mimicking Activity Research Articles

Biomimetic synergistic effect of redox site and Lewis acid for construction of efficient artificial enzyme

In enzymatic catalysis, the redox site and Lewis acid are the two main roles played by metal to assist amino acids. However, the reported enzyme mimics only focus on the redox-active metal as redox site, while the redox-inert metal as Lewis acid has, to the best of our knowledge, not been studied, presenting a bottleneck of enzyme mimics construction. Based on this, a series of highly efficient MxV2O5·nH2O peroxidase mimics with vanadium as redox site and alkaline-earth metal ion (M2+) as Lewis acid are reported. Experimental results and theoretical calculations indicate the peroxidase-mimicking activity of MxV2O5·nH2O show a periodic change with the Lewis acidity (ion potential) of M2+, revealing the mechanism of redox-inert M2+ regulating electron transfer of V-O through non-covalent polarization and thus promoting H2O2 adsorbate dissociation. The biomimetic synergetic effect of redox site and Lewis acid is expected to provide an inspiration for design of enzyme mimics.

Surface gold atoms determine peroxidase mimic activity in gold alloy nanoparticles.

The development of peroxidase mimic nanocatalysts is relevant for oxidation reactions in biosensing, environmental monitoring and green chemical processes. Several nanomaterials have been proposed as peroxidase mimic, the majority of which consists of noble metals and oxide nanoparticles (NPs). Yet, there is still limited information about how the change in the composition influences their catalytic activity. Here, the peroxidase mimic behaviour of gold NPs is compared to a traditional nanoalloy as Au-Ag and to the Au-Fe and the Au-Co nanoalloys, which were not tested before as oxidation catalysis. Since the alloys of gold with iron and cobalt are thermodynamically unstable, laser ablation in liquid (LAL) is exploited for the synthesis of these NPs. Using LAL, no chemical stabilizers or capping agents are present on the NPs surface, allowing the evaluation of the oxidation behaviour as a function of the alloy composition. The results point to the importance of surface gold atoms in the catalytic process, but also indicate the possibility of obtaining active nanocatalysts with a lower content of Au by alloying it with iron, which is earth-abundant, non-toxic and low cost. Overall, Au nanoalloys are worth consideration as a more sustainable alternative to pure Au nanocatalysts for oxidation reactions.

NIR-II-Responsive Versatile Nanozyme Based on H2O2 Cycling and Disrupting Cellular Redox Homeostasis for Enhanced Synergistic Cancer Therapy.

Disturbing cellular redox homeostasis within malignant cells, particularly improving reactive oxygen species (ROS), is one of the effective strategies for cancer therapy. The ROS generation based on nanozymes presents a promising strategy for cancer treatment. However, the therapeutic efficacy is limited due to the insufficient catalytic activity of nanozymes or their high dependence on hydrogen peroxide (H2O2) or oxygen. Herein, we reported a nanozyme (CSA) based on well-defined CuSe hollow nanocubes (CS) uniformly covered with Ag nanoparticles (AgNPs) to disturb cellular redox homeostasis and catalyze a cascade of intracellular biochemical reactions to produce ROS for the synergistic therapy of breast cancer. In this system, CSA could interact with the thioredoxin reductase (TrxR) and deplete the tumor microenvironment-activated glutathione (GSH), disrupting the cellular antioxidant defense system and augmenting ROS generation. Besides, CSA possessed high peroxidase-mimicking activity toward H2O2, leading to the generation of various ROS including hydroxyl radical (•OH), superoxide radicals (•O2-), and singlet oxygen (1O2), facilitated by the Cu(II)/Cu(I) redox and H2O2 cycling, and plentiful catalytically active metal sites. Additionally, due to the absorption and charge separation performance of AgNPs, the CSA exhibited excellent photothermal performance in the second near-infrared (NIR-II, 1064 nm) region and enhanced the photocatalytic ROS level in cancer cells. Owing to the inhibition of TrxR activity, GSH depletion, high peroxidase-mimicking activity of CSA, and abundant ROS generation, CSA displays remarkable and specific inhibition of tumor growth.

Silver Nanoparticle-Immobilized Schiff-Base Macrocycles as Nanozymes with Peroxidase Mimic Activity for Antibacterial Films

Silver Nanoparticle-Immobilized Schiff-Base Macrocycles as Nanozymes with Peroxidase Mimic Activity for Antibacterial Films

Synthesis, Structural Analysis, and Peroxidase-Mimicking Activity of AuPt Branched Nanoparticles.

Bimetallic nanomaterials have generated significant interest across diverse scientific disciplines, due to their unique and tunable properties arising from the synergistic combination of two distinct metallic elements. This study presents a novel approach for synthesizing branched gold-platinum nanoparticles by utilizing poly(allylamine hydrochloride) (PAH)-stabilized branched gold nanoparticles, with a localized surface plasmon resonance (LSPR) response of around 1000 nm, as a template for platinum deposition. This approach allows precise control over nanoparticle size, the LSPR band, and the branching degree at an ambient temperature, without the need for high temperatures or organic solvents. The resulting AuPt branched nanoparticles not only demonstrate optical activity but also enhanced catalytic properties. To evaluate their catalytic potential, we compared the enzymatic capabilities of gold and gold-platinum nanoparticles by examining their peroxidase-like activity in the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB). Our findings revealed that the incorporation of platinum onto the gold surface substantially enhanced the catalytic efficiency, highlighting the potential of these bimetallic nanoparticles in catalytic applications.

Iron/Molybdenum Sulfide Nanozyme Cocatalytic Fenton Reaction for Photothermal/Chemodynamic Efficient Wound Healing.

The issue of bacterial infectious diseases remains a significant concern worldwide, particularly due to the misuse of antibiotics, which has caused the emergence of antibiotic-resistant strains. Fortunately, the rapid development of nanomaterials has propelled significant progress in antimicrobial therapy, offering promising solutions. Among them, the utilization of nanoenzyme-based chemodynamic therapy (CDT) has become a highly hopeful approach to combating bacterial infectious diseases. Nevertheless, the application of CDT appears to be facing certain constraints for its low efficiency in the Fenton reaction at the infected site. In this study, we have successfully synthesized a versatile nanozyme, which was a composite of molybdenum sulfide (MoS2) and iron sulfide (FeS2), through the hydrothermal method. The results showed that iron/molybdenum sulfide nanozymes (Fe/Mo SNZs) with desirable peroxidase (POD) mimic activity can generate cytotoxic reactive oxygen species (ROS) by successfully triggering the Fenton reaction. The presence of MoS2 significantly accelerates the conversion of Fe2+/Fe3+ through a cocatalytic reaction that involves the participation of redox pairs of Mo4+/Mo6+, thereby enhancing the efficiency of CDT. Additionally, based on the excellent photothermal performance of Fe/Mo SNZs, a near-infrared (NIR) laser was used to induce localized temperature elevation for photothermal therapy (PTT) and enhance the POD-like nanoenzymatic activity. Notably, both in vitro and in vivo results demonstrated that Fe/Mo SNZs with good broad-spectrum antibacterial properties can help eradicate Gram-negative bacteria like Escherichia coli and Gram-positive bacteria like Staphylococcus aureus. The most exciting thing is that the synergistic PTT/CDT exhibited astonishing antibacterial ability and can achieve complete elimination of bacteria, which promoted wound healing after infection. Overall, this study presents a synergistic PTT/CDT strategy to address antibiotic resistance, providing avenues and directions for enhancing the efficacy of wound healing treatments and offering promising prospects for further clinical use in the near future.

Silver nanoparticles loaded carbon-magnetic nanocomposites: A nanozyme for colorimetric detection of dopamine

Dopamine (DA) is catecholamine neurotransmitters that play an important role in the central nervous system. In recent years people started to intentionally add DA to animal feed to enhance muscle development and increase their profit margin. Human consumption of the residual DA from animal tissues has been reported to be associated with the development of such diseases as Parkinson’s disease, epilepsy, senile dementia, and schizophrenia and pose serious human health risks. These require development of rapid, cheap, and sensitive methods for detection of DA from animal tissue. Compared to other techniques that require access to expensive instruments, skilled human power, and tiresome routine procedures, colorimetric methods provide cheap and reliable options for detection of DA. Here we report a colorimetric method based on the peroxidase-mimic activity of Fe3O4@C@AgNPs for the detection of DA. A simple wet chemical method was employed to synthesize AgNPs on hydrophilic carbon coated Fe3O4. The produced nanocomposites were characterized by transmission electron microscopy (TEM), Fourier Transform infrared spectroscopy (FTIR), and surface-enhanced Raman spectroscopy (SERS). The detection of DA was done based on inhibition of the peroxidase-like activity of Fe3O4@C@AgNPs using 3, 3, 5, 5′-tetramethylbenzidine (TMB) as a substrate. In the presence of DA, however, the peroxidase-like activity started to decrease. The decrease in activity was concentration dependent showing a linear relationship in the range of 0.5-80 µM. In this linear range, the limit of detection (LOD) was computed and found to be as low as 0.12 µM. Therefore, we propose that the peroxidase-like activity of Fe3O4@C@AgNPs could be used for quantitative detection of DA from different samples.

Multifunctional nanoenzyme lateral flow immunoassay strip for rapid and ultrasensitive detection of carbofuran in vegetables

A lateral flow immunoassay strip (LFIAS) is one of the most frequently rapid test technologies for carbofuran (CAR). Nevertheless, the LFIAS has a poor quantitative capability and low sensitivity. And, it also requires often complex sample handling steps, making testing time longer. In this study, Fe3O4 nanoparticles were successively modified with MIL-100(Fe)-based metal-organic framework (MOF) and chloroplatinic acid hexahydrate to obtain a core-shell complex of Fe3O4-MOF-Pt. The complex had a peroxidase-mimicking activity catalytic function that enabled signal amplification and sensitivity enhancement. Upon coupling with carbofuran monoclonal antibody (CAR-mAb), the magnetic separation properties of the probe enabled target-specific enrichment. The LFIAS based on Fe3O4-MOF-Pt nanocomposites could detect CAR in the range of 0.25–50 ng mL−1 with a limit of detection (LOD) of 0.15 ng mL−1, enabling colorimetric and catalytic analysis. In addition, the method showed high specificity and stability for detecting CAR in various vegetables, and recovery rates of the spiked samples were 91.40%−102.40%. In conclusion, this study provided one-stop detection of “target enrichment-visual inspection”. While lowering the LOD, it reduced the detection time and improved the detection efficiency. The multifunctional Fe3O4-MOF-Pt nanocomposite provides an idea for the construction of novel multifunctional probes to improve the detection performance of conventional LFIAS.

Synchronously Sensitive Immunoassay and Efficient Inactivation of Living Zika Virus via DNAzyme Catalytic Amplification and In Situ Aggregation-Induced Emission Photosensitizer Generation.

Sensitive identification and effective inactivation of the virus are paramount for the early diagnosis and treatment of viral infections to prevent the risk of secondary transmission of viruses in the environment. Herein, we developed a novel two-step fluorescence immunoassay using antibody/streptavidin dual-labeled polystyrene nanobeads and biotin-labeled G-quadruplex/hemin DNAzymes with peroxidase-mimicking activity for sensitive quantitation and efficient inactivation of living Zika virus (ZIKV). The dual-labeled nanobeads can specifically bind ZIKV through E protein targeting and simultaneously accumulate DNAzymes, leading to the catalytic oxidation of Amplex Red indicators and generation of intensified aggregation-induced emission fluorescence signals, with a detection limit down to 66.3 PFU/mL and 100% accuracy. Furthermore, robust reactive oxygen species generated in situ by oxidized Amplex Red upon irradiation can completely kill the virus. This sensitive and efficient detection-inactivation integrated system will expand the viral diagnostic tools and reduce the risk of virus transmission in the environment.

A bimetallic peroxidase-mimicking nanozyme with antifouling property for construction of sensor array to identify phosphoproteins and diagnose cancers

Protein phosphorylation is a significant post-translational modification that plays a decisive role in the occurrence and development of diseases. However, the rapid and accurate identification of phosphoproteins remains challenging. Herein, a high-throughput sensor array has been constructed based on a magnetic bimetallic nanozyme (Fe3O4@ZNP@UiO-66) for the identification and discrimination of phosphoproteins. Attributing to the formation of Fe–Zr bimetallic dual active centers, the as-prepared Fe3O4@ZNP@UiO-66 exhibits enhanced peroxidase-mimicking catalytic activity, which promotes the electron transfer from Zr center to Fe(II)/Fe(III). The catalytic activity of Fe3O4@ZNP@UiO-66 can be selectively inhibited by phosphoproteins due to the strong interaction between phosphate groups and Zr centers, as well as the ultra-robust antifouling capability of zwitterionic dopamine nanoparticle (ZNP). Considering the diverse binding affinities between various proteins with the nanozyme, the catalytic activity of Fe3O4@ZNP@UiO-66 can be changed to various degree, leading to the different absorption responses at 420 nm in the hydrogen peroxide (H2O2) - 2, 2′-azino-bis (3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) system. By simply extracting different absorbance intensities at various time points, a sensor array based on reaction kinetics for the discrimination of phosphoproteins from other proteins is constructed through linear discriminant analysis (LDA). Besides, the quantitative determination of phosphoproteins and identification of protein mixtures have been realized. Further, based on the differential level of phosphoproteins in cells, the differentiation of cancer cells from normal cells can also be implemented by utilizing the proposed sensor array, showing great potential in disease diagnosis.

Glutathione‑iron hybrid nanozyme-based colorimetric sensor for specific and stable detection of thiram pesticide on fruit juices

Given the potential dangers of thiram to food safety, constructing a facile sensor is significantly critical. Herein, we presented a colorimetric sensor based on glutathione‑iron hybrid (GSH-Fe) nanozyme for specific and stable detection of thiram. The GSH-Fe nanozyme exhibits good peroxidase-mimicking activity with comparable Michaelis constant (Km = 0.551 mM) to the natural enzyme. Thiram pesticides can specifically limit the catalytic activity of GSH-Fe nanozyme via surface passivation, causing the change of colorimetric signal. It is worth mentioning that the platform was used to prepare a portable hydrogel kit for rapid qualitative monitoring of thiram. Coupling with an image-processing algorithm, the colorimetric image of the hydrogel reactor is converted into the data information for accurate quantification of thiram with a detection limit of 0.3 μg mL−1. The sensing system has good selectivity and high stability, with recovery rates in fruit juice samples ranging from 92.4% to 106.9%.

Pore-Forming Toxin-Driven Recovery of Peroxidase-Mimicking Activity in Biomass Channels for Label-Free Electrochemical Bacteria Sensing.

The development of sensitive, selective, and rapid methods to detect bacteria in complex media is essential to ensuring human health. Virulence factors, particularly pore-forming toxins (PFTs) secreted by pathogenic bacteria, play a crucial role in bacterial diseases and serve as indicators of disease severity. In this study, a nanochannel-based label-free electrochemical sensing platform was developed for the detection of specific pathogenic bacteria based on their secreted PFTs. In this design, wood substrate channels were functionalized with a Fe-based metal-organic framework (FeMOF) and then protected with a layer of phosphatidylcholine (PC)-based phospholipid membrane (PM) that serves as a peroxidase mimetic and a channel gatekeeper, respectively. Using Staphylococcus aureus (S. aureus) as the model bacteria, the PC-specific PFTs secreted by S. aureus perforate the PM layer. Now exposed to the FeMOF, uncharged 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) molecules in the electrolyte undergo oxidation to cationic products (ABTS•+). The measured transmembrane ionic current indicates the presence of S. aureus and methicillin-resistant S. aureus (MRSA) with a low detection limit of 3 cfu mL-1. Besides excellent specificity, this sensing approach exhibits satisfactory performance for the detection of target bacteria in the complex media of food.

Graphene quantum dots on TiO2 nanotubes as a light-assisted peroxidase nanozyme

Hybrid nanozyme graphene quantum dots (GQDs) deposited TiO2 nanotubes (NTs) on titanium foil (Ti/TiO2 NTs-GQDs) were manufactured by bestowing the hybrid with the advantageous porous morphology, surface valence states, high surface area, and copious active sites. The peroxidase-like activity was investigated through the catalytic oxidation of chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2, which can be visualized by the eyes. TiO2 NTs and GQDs comprising oxygen-containing functional groups can oxidize TMB in the presence of H2O2 by mimicking peroxidase enzymes. The peroxidase-mimicking activity of hybrid nanozyme was significantly escalated by introducing light illumination due to the photosensitive features of the hybrid material. The peroxidase-like activity of Ti/TiO2 NTs-GQDs enabled H2O2 determination over the linear range of 7 to 250 μM, with a LOD of 2.1 µM. The satisfying peroxidase activity is possibly due to the unimpeded access of H2O2 to the catalyst’s active sites. The porous morphology provides the easy channeling of reactants and products. The periodic structure of the material also gave rise to acceptable reproducibility. Without material functionalization, the Ti/TiO2 NTs-GQDs can be a promising substitute for peroxidases for H2O2 detection.Graphical abstract

Gold-silver-platinum trimetallic nanozyme-based dual-mode immunosensor for ultrasensitive osteoprotegerin detection

In this study, we report a novel gold-silver-platinum nanocomposite (AuNP-AgNP-PtNP), which displayed excellent peroxidase-mimicking activity because of the synergistic effect involving three metals. The nanozyme allowed the development of a sensitive and specific dual-mode immunodetection system to detect protein using electrochemical and colourimetric assays. The developed ultrasensitive dual-mode immunosensor was based on the anti-osteoprotegerin antibody-linked nanozyme interaction with recombinant osteoprotegerin (rOPG) protein coated over a microtiter plate. Based on the excellent electrocatalytic activity of the trimetallic nanozyme towards reducing hydrogen peroxide (H2O2), the trimetallic nanozyme could be employed towards electrochemical immunodetection of the rOPG proteins. The proposed dual-mode biosensor allowed enhanced sensitive determination of rOPG proteins with a wide linear range of 0.1 fg/mL to 10 ng/mL for electrochemical detection and 1 fg/mL to 100 ng/mL for colourimetrically detecting rOPG proteins. Moreover, the dual-mode sensor could detect rOPG proteins with a LOD of 1.81 pg/mL using the electrochemical mode and 1.87 pg/mL using the colourimetric detection mode. Moreover, the study demonstrates outstanding selectivity, sensitivity, and specificity, yielding robust recoveries in human serum samples.

S-Doping Regulated Iron Spin States in Fe-N-C Single-Atom Material for Enhanced Peroxidase-Mimicking Activity at Neutral pH.

Designing biomimetic nanomaterials with peroxidase (POD)-like activity at neutral pH remains a significant challenge. An S-doping strategy is developed to afford an iron single-atom nanomaterial (Fe1@CN-S) with high POD-like activity under neutral conditions. To the best of knowledge, there is the first example on the achievement of excellent POD-like activity under neutral conditions by regulating the active site structure. S-doping not only promotes the dissociation of the N─H bond in 3,3″,5,5″-tetramethylbenzidine (TMB), but also facilitates the desorption of OH* by the transformation of iron species' spin states from middle-spin (MS FeII) to low-spin (LS FeII). Meanwhile, LS FeII sites typically have more unfilled d orbitals, thereby exhibiting stronger interactions with H2O2 than MS FeII, which can enhance POD-like activity. Finally, a one-pot visual detection of glucose at pH 7 is performed, demonstrating the best selectivity and sensitivity than previous reports.

Colorimetric Detection of Acid Phosphatase and Malathion Using NiCo2O4 Nanosheets as Peroxidase-Mimicking Activity

Colorimetric Detection of Acid Phosphatase and Malathion Using NiCo2O4 Nanosheets as Peroxidase-Mimicking Activity

Bimetallic PtPd Atomic Clusters as Apoptosis/Ferroptosis Inducers for Antineoplastic Therapy through Heterogeneous Catalytic Processes.

Active polymetallic atomic clusters can initiate heterogeneous catalytic reactions in the tumor microenvironment, and the products tend to cause manifold damage to cell metabolic functions. Herein, bimetallic PtPd atomic clusters (BAC) are constructed by the stripping of Pt and Pd nanoparticles on nitrogen-doped carbon and follow-up surface PEGylation, aiming at efficacious antineoplastic therapy through heterogeneous catalytic processes. After endocytosed by tumor cells, BAC with catalase-mimic activity can facilitate the decomposition of endogenous H2O2 into O2. The local oxygenation not only alleviates hypoxia to reduce the invasion ability of cancer cells but also enhances the yield of •O2- from O2 catalyzed by BAC. Meanwhile, BAC also exhibit peroxidase-mimic activity for •OH production from H2O2. The enrichment of reactive oxygen species (ROS), including the radicals of •OH and •O2-, causes significant oxidative cellular damage and triggers severe apoptosis. In another aspect, intrinsic glutathione (GSH) peroxidase-like activity of BAC can indirectly upregulate the level of lipid peroxides and promote ferroptosis. Such deleterious redox dyshomeostasis caused by ROS accumulation and GSH consumption also results in immunogenic cell death to stimulate antitumor immunity for metastasis suppression. Collectively, this paradigm is expected to inspire more facile designs of polymetallic atomic clusters in disease therapy.

The peroxidase-like activity of Au NPs deposited inverse opal CeO2 nanozyme for rapid and sensitive H2O2 sensing

In this study, the hybrid nanozyme gold nanoparticles deposited CeO2 inverse opal photonic crystals (IOPCs) on the glass slide was fabricated by bestowing the hybrid with the beneficial porous morphology with its unique advantages: its surface valence states, high surface area, and copious active sites. The oxidase and peroxidase-mimicking activity was studied by observing the catalytic oxidation of chromogenic substrate 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid (ABTS) in the presence of H2O2, which can be visualized by the eyes. Au NPs and CeO2 IOPCs consisting of Ce3+ and Ce4+ can oxidize ABTS in the presence of H2O2 by mimicking peroxidase enzymes. The peroxidase-like activity of nanozyme was substantially improved by introducing light irradiation due to the photosensitive nature of the hybrid. The peroxidase-like activity of nanozyme enabled H2O2 linear detection over the range 9 to 500 μM, with a LOD of 2.7 µM. The acceptable nanozyme activity is probably owing to the easy access of H2O2 to the active sites of nanozyme. The porous architecture led to the easy channeling of reactants and products. The periodic architecture of the nanozyme also led to decent reproducibility. Without functionalization, the nanozyme can be a promising alternative to peroxidase enzymes for hydrogen peroxide measurements.

Simultaneous electrochemical and colorimetric detection of tri-heavy metal ions in environmental water samples employing 3D-MOF/nickel selenide as a synergistic catalyst

The detrimental growth of water pollutants such as heavy metal ions (HMI) has become a life-threatening problem in the modern era. Therefore, developing more efficient strategies to detect such compounds requires increased attention. In this study, we designed a dual-mode assay for electrochemical sensing and naked-eye (colorimetric) detection of HMI using the peroxidase mimic activity of the developed nanozyme. The nanozyme of choice, which possesses both the necessary electrochemical properties and the ability to be oxidized with 3,3′,5,5′-tetramethylbenzidine (TMB), was determined and studied. Flower-like nickel selenide (NiSe) was integrated with a zeolitic imidazole framework (ZIF-67) to enable its wider applicability. HMI detection with a wide linear range of about 0.029–764.8 µM (Cd2+), 0.299–355.5 µM (Pb2+), and 0.29–153.2 µM (Hg2+) with NiSe/ZIF showed excellent electrochemical performances, while the linear range in colorimetric detection was about 0.199–429.9 µM (Cd2+), 0.199–90.8 µM (Pb2+), and 0.149–276.8 µM (Hg2+). The limit of detection for the simultaneous detection was 5.2 nM (Cd2+), 4.7 nM (Pb2+), and 6.2 nM (Hg2+) for electrochemical sensing. The LOD obtained for the colorimetric analyses were 0.043 µM (Cd2+), 0.050 µM (Pb2+), and 0.091 µM (Hg2+). The real sample analysis of the environmental water samples showed good results for trace heavy metal ions. Thus, the developed NiSe/ZIF catalyst is more effective with dual detection and can be used for portable analysis of several targets with further modifications.

Portable hydrogel kit driven by bimetallic carbon dots nanozyme for H2O2-self-supplying dual-modal monitoring of atmospheric CH3SH

Due to the typical volatility of gaseous pollutant methyl mercaptan (CH3SH), the development of a facile, reliable, and accurate onsite environmental surveillance of highly toxic CH3SH faces many challenges, but it is critical to environmental atmosphere assessment and safeguarding public health. Here, we prepared a novel bimetallic carbon dots (Fe&Cu@CDs) nanozyme with high peroxidase-mimicking activity to design a portable hydrogel kit for onsite visual H2O2-self-supplying enzymatic cascade catalytic colorimetric and photothermal signal synergistic amplification dual-modal monitoring of CH3SH in atmospheric environment. Assisted by alcohol oxidase (AOX), CH3SH could be specifically converted into H2O2 for oxidizing chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) catalyzed by Fe&Cu@CDs to produce dark blue ox-TMB with absorption at 652 nm and photothermal characters. Consequently, a CH3SH concentration-dependent change both in naked-eye color and photothermal effect-triggered temperature were observed. By hybridizing AOX-assisted Fe&Cu@CDs + TMB with agarose, a H2O2-self-supplying colorimetric and photothermal signal synergistic amplification sensory hydrogel kit integrated with Color Picker APP-installed smartphone and 660 nm laser-equipped handheld thermal imager for CH3SH was proposed with acceptable results in atmospheric environment around wastepile (e.g., solid waste and food waste piles), which exhibited great potentials to further develop commercial onsite monitoring platforms in warning-early abnormal atmospheric CH3SH for safeguarding environmental health.