NiCo LDH nanozymes with selective antibacterial activity against Gram-negative bacteria for wound healing.

Bacterial infections have been a major threat to human health. Especially, Gram-negative (G-) bacterial infections have been an increasing problem worldwide. The overuse of antibiotics leads to an emergence of drug resistance, and thus the development of novel antimicrobial agents is important, particularly against G- bacteria. Nanozymes use reactive oxygen species (ROS) to kill bacteria, reducing the risk of bacterial resistance and providing new opportunities to meet the challenges of strain selectivity. Here, we synthesized NiCo layered double hydroxide (LDH) nanozymes, which exhibit selective antibacterial activity based on their peroxide-like (POD-like) activity. To obtain the highest antibacterial activity, the POD-like activity of NiCo LDH nanozyme was further optimized by tuning the ratio of nickel and cobalt, and Ni4Co6 LDHs showed the highest POD activity and antibacterial activity. More importantly, Ni4Co6 LDHs can achieve selective sterilization of G- bacteria due to their electrostatic adsorption and hydrophilic interactions with the bacterial cell wall. Animal experiments further indicated that the healing of G- bacteria-infected wounds was effectively promoted without damaging their normal biological tissues. In conclusion, we provide a selective antibacterial agent through a simple strategy, which provides a new direction for the application of nanozymes.

Alkaline-promoted regulation of the peroxidase-like activity of Ni/Co LDHs and development bioassays.

Nanozymes' activities could be regulated by a simple and effective pH change in an in situ manner. In this work, for the first time, the peroxidase-like activity of Ni/Co layered double hydroxides (LDHs) was regulated via the alkaline-promoted reaction of fluorogenic substrate homovanillic acid and H2O2, and a promising tool for pH sensing was developed over the pH range of 8.3-9.6. As peroxidase nanozyme model, Ni/Co LDHs showed ease of preparation, low-cost, and water-solubility, which played an important role in this luminescence system. Based on the pH-dependent regulation of the Ni/Co LDHs activity, we constructed the bioassay platform for the determination urea, urease, penicillin G, and penicillinase with a wide linear range of 17-1000 µM, 3.3-270 mU mL-1, 3.3-1300 µM and 3.3-100 mU mL-1, respectively. This study not only demonstrated the alkaline-promoted modulation the nanozymes' activities, but also established a facile approach to develop novel bioassays.

Evaluation of fluorogenic substrates for Ni/Co LDHs peroxidase mimic and application for determination of inhibitory effects of antioxidant.

Nanomaterial-based peroxidase-mimetics are an emerging research field that promises to produce alternatives to horseradish peroxidase for a variety of applications. Generally, some peroxidase-mimetics substrates are used in acidic condition (pH ≤ 7). Then, it is necessary to screen some peroxidase-mimetics substrates suitable for basic condition because that some peroxidase-mimetics leached ions in acidic solution. In this paper, using Ni/Co layered double hydroxides (LDHs) as a nano-peroxidase mimic model, we evaluated three fluorogenic substrates suitable for basic condition though experimental conditions, reaction kinetic and glucose detection assay. And the detection of glucose method based on homovanillic acid (HVA) as fluorescent substrate gave wide linear range (0.02-20 µM) and low detection limit (0.01 µM). We also developed a novel platform that could study the inhibitory effects of ascorbic acid and glutathione based on the system of Ni/Co LDHs-HVA-H2O2.

One-step analysis of glucose and acetylcholine in water based on the intrinsic peroxidase-like activity of Ni/Co LDHs microspheres.

In the present study, a simple strategy was developed for Ni/Co layered double hydroxides (LDHs) as a substitute for natural peroxidase. The obtained Ni/Co LDHs exhibited ease of preparation, low-cost, and water-solubility; importantly, this material showed high catalytic activity in neutral pH solutions (phosphate buffer, Tris-HCl buffer, and even water). Benefitting from Ni/Co LDHs having a similar pH and temperature with specificity oxidase, such as glucose oxidase, choline oxidase, acetylcholinesterase, etc., a novel one-step method for a biosensor was developed in water. Glucose detection was selected as an application model system to evaluate the performance of this method, which showed a linear detection range from 0.5 µM to 100 µM with a detection limit (DL) of 0.1 µM. We also extended the one-step method to detect acetylcholine (ACh) by taking advantage of the specific catalytic reaction of acetylcholinesterase (AChE) and choline oxidase (ChOx). The linear detection range was from 10 µM to 150 µM with the DL of 1.62 µM. The proposed method had ease of operation, simple steps, and was rapid for glucose and ACh detection in real samples. On the basis of these advantages and virtues, Ni/Co LDHs could become attractive nanozymes in biotechnology and bioassays, and create a great influence on the next generation of enzyme mimetic systems.