Carbon dots (CDs), comprising crystalline graphitized carbon cores and polymer surface groups, are currently attracting a lot of interest in biological fields owing to their fluorescent properties, high photostability, biocompatibility and low toxicity. In addition, the easy preparation and functionalization of CDs stimulate the development of CDs‐based composite materials with specific functions. Presently, the biological applications of CDs are growing at a remarkable speed, justifying the need for up‐to‐date review articles that capture recent progress in this blossoming field. In this review, breakthroughs in the synthesis, modification, optical properties, toxicology and biocatalytic platforms of CDs are described. Further, recent research related to bioimaging, biosensing, drug delivery, antibacterial, anticancer (photothermal therapy, photodynamic therapy and synergistic therapy) and antiviral therapies involving CDs are discussed in detail. Finally, a perspective on the prospects and challenges of CDs in the fields of biomedicine and biotechnology is provided.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/smsc.202200012

Carbon Dots in Bioimaging, Biosensing and Therapeutics: A Comprehensive Review

Millions of families around the world remain vulnerable to water scarcity and have no access to drinking water. Advanced oxidation processes (AOPs) are an effective way towards water purification with qualified reactive oxygen species (ROSs) while are impeded by the high-cost and tedious process in either input of consumable reagent, production of ROSs, and the pre-treatment of supporting electrolyte. Herein, we couple solar light-assisted H2O2 production from water and photo-Fenton-like reactions into a self-cyclable system by using an artificial leaf, achieving an unassisted H2O2 production rate of 0.77 μmol/(min·cm2) under 1 Sun AM 1.5 illumination. Furthermore, a large (70 cm2) artificial leaf was used for an unassisted solar-driven bicarbonate-activated hydrogen peroxide (BAP) system with recycled catalysts for real-time wastewater purification with requirements for only water, oxygen and sunlight. This demonstration highlights the feasibility and scalability of photoelectrochemical technology for decentralized environmental governance applications from laboratory benchtops to industry. 

/pdf/self-cycled-photo-fenton-like-system-based-on-an-artificial-3fx32g0q.pdf

Self-cycled photo-Fenton-like system based on an artificial leaf with a solar-to-H_2O_2 conversion efficiency of 1.46%

MetalN‐coordinated centers supported by carbonaceous substrates have emerged as promising artificial metalloenzymes (AMEs) to mimic the biocatalytic effects of their natural counterparts. However, the synthesis of well‐defined AMEs that contain different atomic metalN centers but present similar physicochemical and coordination structures remains a substantial challenge. Here, 20 different types of AMEs with similar geometries and well‐defined atomic metalN‐coordinated centers are synthesized to compare and disclose the catalytic activities, substrate selectivities, kinetics, and reactive oxygen species (ROS) products. Their oxidase (OXD)‐, peroxidase (POD)‐, and halogen peroxidase (HPO)‐mimetic catalytic behaviors are systematically explored. The Fe‐AME shows the highest OXD‐ and HPO‐mimetic activities compared to the other AMEs due to its high vmax (0.927 × 10−6 m s−1) and low Km (1.070 × 10−3 m), while the Cu‐AME displays the best POD‐like performance. Furthermore, theoretical calculation reveals that the ROS‐catalytic paths and activities are highly related to the electronic structures of the metal centers. Benefiting from its facile adsorption of H2O2 molecule and lower energy barrier to generating •O2−, the Fe‐AME displays higher ROS‐catalytic performances than the Mn‐AME. The engineered AMEs show not only remarkably high ROS‐catalytic performances but also provide new guidance toward developing metalN‐coordinated biocatalysts for broad application fields.

A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers

Plasmon stimulation represents an appealing way to modulate enzyme mimic functions, but utilization efficiency of plasmon excitation remains relatively low. To overcome this drawback, a heterojunction composite based on graphdiyne nanowalls wrapped hollow copper sulfide nanocubes (CuS@GDY) with strong localized surface plasmon resonance (LSPR) response in the near‐infrared (NIR) region is developed. This nanozyme can concurrently harvest LSPR induced hot carriers and produce photothermal effects, resulting in dramatically increased peroxidase‐like activity when exposed to 808 nm light. Both experimental results and theoretical calculations show that the remarkable catalytic performance of CuS@GDY is due to the unique hierarchical structure, narrow bandgap of GDY nanowalls, LSPR effect of CuS nanocages, fast interfacial electron transfer dynamics, and carbon vacancies on CuS@GDY. This plasmonic nanozyme exhibits rapid, efficient, broad‐spectrum antibacterial activity (>99.999%) against diverse pathogens (methicillin‐resistant Staphylococcus aureus, Staphylococcus aureus, and Escherichia coli). This study not only sheds light on the mechanism of the nanozyme‐/photocatalysis coupling process, but also opens up a new avenue for engineering plasmonic NIR light driven nanozymes for rapid synergistic photothermal and photo‐enhanced nanozyme therapy.

Plasmonic Nanozyme of Graphdiyne Nanowalls Wrapped Hollow Copper Sulfide Nanocubes for Rapid Bacteria‐Killing

Nanomaterials‐based artificial enzymes (AEs) have flourished for more than a decade. However, it is still challenging to further enhance their biocatalytic performances due to the limited strategies to tune the electronic structures of active centers. Here, a new path is reported for the de novo design of the d electrons of active centers by modulating the electron transfer in vanadium‐based AEs (VOx‐AE) via a unique Zn–O–V bridge for efficient reactive oxygen species (ROS)‐catalysis. Benefiting from the electron transfer from Zn to V, the V site in VOx‐AE exhibits a lower valence state than that in V2O5, which results in charge‐filled V‐dyz orbital near the Fermi level to interfere with the formation of sigma bonds between the V‐ dz2 and O‐pz orbitals in H2O2. The VOx‐AE exhibits a twofold Vmax and threefold turnover number than V2O5 when catalyzing H2O2. Meanwhile, the VOx‐AE shows enhanced catalytic eradication of drug‐resistant bacteria and achieves comparable wound‐treatment indexes to vancomycin. This modulating charge‐filling of d electrons provides a new direction for the de novo design of nanomaterials‐based AEs and deepens the understanding of ROS‐catalysis.

Modulating Electron Transfer in Vanadium‐Based Artificial Enzymes for Enhanced ROS‐Catalysis and Disinfection

ROS-Catalytic Transition-Metal-Based Enzymatic Nanoagents for Tumor and Bacterial Eradication

The invention belongs to the field of ultrasound imaging diagnosis, and particularly relates to a phospholipid-like amphiphilic comb-shaped graft copolymer-based ultrasound contrast agent and a preparation method thereof. The invention provides the phospholipid-like amphiphilic comb-shaped graft copolymer-based ultrasound contrast agent compriisng a shell and an inner core, and the shell is an amphiphilic comb-shaped graft copolymer polycaprolactone-g-polymethacryloxyethyl phosphorylcholine, and the inner core is an ultrasound response substance. The prepared phospholipid-like amphiphilic comb-shaped graft copolymer-based ultrasound contrast agent has relatively uniform particle size distribution, is significantly better than phospholipid-based ultrasound contrast agent in stability, and is more suitable for ultrasound diagnosis and treatment research; and the phospholipid-like amphiphilic comb-shaped graft copolymer-based ultrasound contrast agent can solve the problem of the pressureresistance and mechanical index change of an existing ultrasound contrast agent and expands the application range of ultrasound contrast agents.

Phospholipid-like amphiphilic comb-shaped graft copolymer-based ultrasound contrast agent and preparation method thereof

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ROS-Catalytic Transition-Metal-Based Enzymatic Nanoagents for Tumor and Bacterial Eradication

Phospholipid-like amphiphilic comb-shaped graft copolymer-based ultrasound contrast agent and preparation method thereof