Ultralow Ru Single Atoms Confined in Cerium Oxide Nanoglues for Highly‐Sensitive and Robust H2O2‐Related Biocatalytic Diagnosis
Minjia Yuan,
Qian Li,
Zihe Wu
et al.
Abstract:Exploring highly efficient, portable, and robust biocatalysts is a great challenge in colorimetric biosensors. To overcome the challenging states in creating single‐atom biocatalysts, such as insufficient activity and stability, here, this work has engineered a unique CeO2 support as nanoglue to tightly anchor the Ru single‐atom sites (CeO2‐Ru) with strong electronic coupling for achieving highly sensitive and robust H2O2‐related biocatalytic diagnosis. The morphology and chemical/electronic structure analysis… Show more
“…The full XPS spectra reveal that the Ce-CDs were composed of five elements, including C, O, N, S, and Ce, thus proving the successful doping of Ce, N, S (Figure S2A). Additionally, the high-resolution spectrum of Ce 3d was divided into nine peaks (Figure E), with the peaks located at 904.1, 899.1, 885.4, 881.5 eV corresponding to Ce (III), and the remaining peaks representing Ce (IV), indicating the coexistence of Ce (IV) and Ce (III) on the surface of Ce-CDs. , The N 1s spectra exhibit two distinct peaks at 400.2 and 402.7 eV, attributed to pyrrolic-N and graphitic-N, respectively (Figure S2B). , The high-resolution C 1s spectra can be divided into three major peaks (Figure S2C), with the peak at 284.9 eV assigned to the CC structure, the peak at 286.5 eV indicating the presence of the C–N/C–O/C–S structure, and the peak at 288.7 eV attributed to the CO structure. , …”
Antimicrobial photodynamic therapy (aPDT) serves as a robust alternative to antibiotics, effectively facilitating the healing of infected wounds and circumventing the risk of resistance. However, the clinical application of aPDT is constrained by the local overproduction of reactive oxygen species (ROS) post-treatment and the deficiencies associated with traditional photosensitizers. Utilizing the self-assembly property of Pluronic F-127 (F127), we successfully achieved the efficient coassembly of cerium-doped carbon dots (Ce-CDs), significantly enhancing the photodynamic antimicrobial efficiency of carbon dots through a straightforward and effective method. Simultaneously, the introduction of cerium imparts outstanding antioxidant efficiency to F127-Ce-CDs (F-Ce-CDs), efficiently clearing overexpressed ROS at the site of infected wounds and protecting cells against oxidative stress. Moreover, F-Ce-CDs exhibit favorable biocompatibility and can significantly accelerate the migration of epithelial cells. In a murine model of infected wounds, F-Ce-CDs effectively inhibit bacterial activity and reduce inflammation, promoting collagen deposition and epithelial tissue regeneration, thereby accelerating the wound-healing process. With effective antimicrobial, anti-inflammatory, and antioxidant properties, coupled with excellent biocompatibility, F-Ce-CDs demonstrate substantial promise as a remarkably efficient application for safe and effective dressings in the healing of infected wounds.
“…The full XPS spectra reveal that the Ce-CDs were composed of five elements, including C, O, N, S, and Ce, thus proving the successful doping of Ce, N, S (Figure S2A). Additionally, the high-resolution spectrum of Ce 3d was divided into nine peaks (Figure E), with the peaks located at 904.1, 899.1, 885.4, 881.5 eV corresponding to Ce (III), and the remaining peaks representing Ce (IV), indicating the coexistence of Ce (IV) and Ce (III) on the surface of Ce-CDs. , The N 1s spectra exhibit two distinct peaks at 400.2 and 402.7 eV, attributed to pyrrolic-N and graphitic-N, respectively (Figure S2B). , The high-resolution C 1s spectra can be divided into three major peaks (Figure S2C), with the peak at 284.9 eV assigned to the CC structure, the peak at 286.5 eV indicating the presence of the C–N/C–O/C–S structure, and the peak at 288.7 eV attributed to the CO structure. , …”
Antimicrobial photodynamic therapy (aPDT) serves as a robust alternative to antibiotics, effectively facilitating the healing of infected wounds and circumventing the risk of resistance. However, the clinical application of aPDT is constrained by the local overproduction of reactive oxygen species (ROS) post-treatment and the deficiencies associated with traditional photosensitizers. Utilizing the self-assembly property of Pluronic F-127 (F127), we successfully achieved the efficient coassembly of cerium-doped carbon dots (Ce-CDs), significantly enhancing the photodynamic antimicrobial efficiency of carbon dots through a straightforward and effective method. Simultaneously, the introduction of cerium imparts outstanding antioxidant efficiency to F127-Ce-CDs (F-Ce-CDs), efficiently clearing overexpressed ROS at the site of infected wounds and protecting cells against oxidative stress. Moreover, F-Ce-CDs exhibit favorable biocompatibility and can significantly accelerate the migration of epithelial cells. In a murine model of infected wounds, F-Ce-CDs effectively inhibit bacterial activity and reduce inflammation, promoting collagen deposition and epithelial tissue regeneration, thereby accelerating the wound-healing process. With effective antimicrobial, anti-inflammatory, and antioxidant properties, coupled with excellent biocompatibility, F-Ce-CDs demonstrate substantial promise as a remarkably efficient application for safe and effective dressings in the healing of infected wounds.
“…The rapid and accurate detection of biomolecules is crucial to diagnose, track, and prevent varieties of diseases. − Recently, the colorimetric assay has received considerable attention for detecting different biological molecules owing to its easy operation, high efficiency, and “naked eye” visual detection. − It is worth mentioning that nanozymes have been widely studied as substitutes for natural enzymes in colorimetric assays, which can be attributed to the high enzyme-like activity, easy preparation, and strong stability in extreme conditions of nanozymes. − However, developing nanozymes with highly dispersed active sites and high enzyme-mimicking catalytic activities as well as robust structures for colorimetric biosensing diverse biomolecules still remains a substantial challenge. Metal–organic frameworks (MOFs) are porous organic–inorganic coordination materials with a large number of active sites that have been utilized as nanozymes in the fields of biotherapy, antibacterial, biosensors, and pollutant degradation. , Recently, Co nanoparticles derived from MOF with excellent enzyme-like activities have attracted considerable attention in many fields .…”
Designing a metal−organic framework (MOF)-derived nanozyme with highly dispersed active sites and high catalytic activity as well as robust structure for colorimetric biosensing of diverse biomolecules remains a substantial challenge. Here, an MOF-derived highly dispersed and pure α-cobalt confined in a nitrogen-doped carbon nanofiber (α-Co@NCNF) nanozyme with superior glucose oxidase (GOD)-and peroxidase (POD)-like activities was constructed for colorimetric assay of multiple biomolecules. Specifically, the α-Co@NCNF nanozyme was synthesized, utilizing in situ electrospinning Co-MOFs into polyacrylonitrile nanofiber (PAN) followed by a pyrolysis process. Taking advantage of the in situ electrospinning strategy, the α-Co nanoparticles were confined in continuous porous NCNF to restrict the growth and prevent the aggregation and oxidation during the pyrolysis process. The resulting special structure considerably improved the enzyme-like performance. A series of experiments validate that the enzyme-like activity of the α-Co@NCNF nanozyme was superior to that of Co@CoO@NCNF (derivatives from Co-MOFs grown on the surface of PAN nanofiber) and nature enzymes. Furthermore, α-Co@NCNF nanozymebased colorimetric biosensing was developed for monitoring glucose, hydrogen peroxide (H 2 O 2 ), and glutathione (GSH) and the corresponding linear ranges are 0.1−50 and 50−900 μM and 5−55 and 0.1−20 μM accompanied by the corresponding low detection of 0.03, 1.66, and 0.03 μM. The proposed method for the construction of α-Co@NCNF nanozyme with dual enzyme-like properties provides a new insight for designing novel nanozymes and has prospects for application in colorimetric biosensing.
Developing artificial enzymes based on organic molecules or polymers for reactive oxygen species (ROS)‐related catalysis has broad applicability. Herein, inspired by porphyrin‐based heme mimics, we report the synthesis of polyphthalocyanine‐based conjugated polymers (Fe‐PPc‐AE) as a new porphyrin‐evolving structure to serve as efficient and versatile artificial enzymes for augmented reactive oxygen catalysis. Owing to the structural advantages, such as enhanced π‐conjugation networks and π‐electron delocalization, promoted electron transfer, and unique Fe‐N coordination centers, Fe‐PPc‐AE showed more efficient ROS‐production activity in terms of Vmax and turnover numbers as compared with porphyrin‐based conjugated polymers (Fe‐PPor‐AE), which also surpassed reported state‐of‐the‐art artificial enzymes in their activity. More interestingly, by changing the reaction medium and substrates, Fe‐PPc‐AE also revealed significantly improved activity and environmental adaptivity in many other ROS‐related biocatalytic processes, validating the potential of Fe‐PPc‐AE to replace conventional (poly)porphyrin‐based heme mimics for ROS‐related catalysis, biosensors, or biotherapeutics. It is suggested that this study will offer essential guidance for designing artificial enzymes based on organic molecules or polymers.
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