Computational chemistry methods are playing an increasingly pivotal role in chemical experiments. From quantum chemistry simulations to finite element simulations, researchers can always find an appropriate simulation method to elucidate the specific mechanisms at a certain resolution scale. However, in organic or inorganic synthesis, the synthesis mechanisms span multiple spatial and temporal scales of chemical experiments. Furthermore, the intricate nature of these mechanisms renders it impossible for any single simulation method to provide a comprehensive depiction of the entire process. In this perspective, using zeolite and polymer synthesis simulations as examples, we stress the significance of fullscale modeling techniques for chemical experiments and urge the corresponding sophisticated simulation platform.
This comprehensive review delves into a unique intersection of hydrogels as smart molecules and their transformative applications in ophthalmology. Beginning with the foundational definition, properties, and classification of hydrogels, the review explores their synthesis and responsive capabilities. Specific applications examined encompass topical drug delivery, contact lenses, intravitreal drug delivery, ocular adhesives, vitreous substitutes, and cell-based therapy. A methodical analysis, including an overview of relevant ocular structures and a comparative evaluation of hydrogel-based solutions against traditional treatments, is conducted. Additionally, potential constraints, translation challenges, knowledge gaps, and research areas are identified. Our methodical approach, guided by an extensive literature review from 2017 to 2023, illuminates the unprecedented opportunities offered by hydrogels, along with pinpointing areas for further inquiry to facilitate their transition into clinical practice.
It is a great challenge to discover novel chemical reactions suitable for biological analysis in a living system. The development of novel protein thiol blocking agents is a crucial need for exploring protein thiol functions in protein refolding, signal transduction, and redox regulation. We are always keen on seeking novel chemical reactions applied to endogenous biological macromolecules or protein thiol sensing, blocking, and labeling. In the present work, we have successfully developed a novel agent to block protein thiol by enhanced electron-withdrawing inductive effects. This sensing and blocking process was detailedly monitored by UV-vis, fluorescent spectra, and SDS-Page gel separation. The spectral studies demonstrated that the agent could react ultrafastly with thiol within seconds at μM level. Furthermore, fluorescent imaging in cells and in vivo was further used for the validation of its ability to sensing and blocking thiol, providing evidence of downregulated protein thiols in Parkinson’s disease. The enhanced electronwithdrawing inductive effect strategy in this work may provide a general guideline for designing protein thiol agent.
Stimuli-responsive DNA-based logic gates have emerged as a promising field at the intersection of synthetic biology and nanotechnology. These gates exploit the unique properties of DNA molecules to perform programmable computational operations in response to specific stimuli. This review provides a comprehensive overview of recent advancements in the design, working principles, and applications of stimuli-responsive DNA-based logic gates. The progress made in developing various types of logic gates triggered by metal ions, pH, oligonucleotides, small molecules, proteins, and light is highlighted. The applications of these logic gates in imaging and biosensing, drug delivery, synthetic biology and molecular computing are discussed. This review underscores the significant contributions and future prospects of stimuli-responsive DNA-based logic gates in advancing the field of nanotechnology.
Glutathione (GSH)-activated prodrugs are promising for overcoming the limitations of conventional anti-tumor drugs. However, current GSH-responsive disulfide groups exhibit unregulated reactivity, making it impossible to precisely control the drug release rate. We herein report a series of GSH-responsive prodrugs with a “three-in-one” molecular design by integrating a fluorescence report unit, stimuliresponsive unit and chemodrug into one scaffold with tunable aromatic nucleophilic substitution (SNAr) reactivity. The drug release rate of these prodrugs is tailored by modification of substituent groups with different electron-withdrawing or -donating abilities on the BODIPY core. Furthermore, the prodrugs self-assemble in water to form nanoparticles that serve as photosensitizers to produce reactive oxygen species upon irradiation for photodynamic therapy (PDT). The PDT process also increases the concentration of GSH in cells, further promoting the release of drugs for chemotherapy. This strategy provides a powerful platform for sequential photodynamic and chemotherapy with tunable drug release rates and synergistic therapeutic effects.
Smart chiral liquid crystal elastomers are a class of soft photonic crystals with periodic nanostructures. There are two kinds of chiral liquid crystal elastomers with structural colors: cholesteric liquid crystal elastomers with a one-dimensional helical nanostructure and blue-phase liquid crystal elastomers with a three-dimensional photonic crystal nanostructure. The self-assembled nanostructure of chiral liquid crystal elastomers can be dynamically controlled under external stimulation, and the reflected color can be adjusted throughout the visible light range. Along with the development of innovative material systems and cutting-edge manufacturing technologies, researchers have proposed diverse strategies to design and synthesize chiral liquid crystal elastomers and have thoroughly investigated their properties and potential applications. Here, we provide a systematic review of the progress in the design and fabrication of smart chiral liquid crystal elastomers, focusing on the cholesteric liquid crystal elastomers via surface-enforced alignment, bar coating, 3D printing, anisotropic deswelling methods as well as the three-dimensional self-assembly of blue-phase liquid crystal elastomers without additional alignment. Smart chiral liquid crystal elastomers are able to respond quickly to external stimuli and have a wide range of applications in areas such as adaptive optics, color-changing camouflage, soft robotics, and information encryption. This review concludes with a perspective on the opportunities and challenges for the future development of smart chiral liquid crystal elastomers.
The multifaceted switches are part of our everyday life from the macroscopic to the molecular world. A molecular switch operating in the solution and in the crystalline state is very different. In this review, we summarize the state-of-the-art of smart molecular crystal switches based on molecular martensites. These crystal switches respond to external stimuli and reversibly change between states, retaining their macroscopic integrity. The operation of the switches predominantly relies on temperature alterations or mechanical stress, with emerging methods based on photothermal effects, photoisomerization, and host-guest chemistry. The capability of changing the molecular orientation and interaction in smart molecular crystal switches offers opportunities in several applications, including actuators, reversibly shaping structural materials, optoelectronic and magnetic materials, as well as switchable porous materials. Smart molecular crystal switches have vast potential in modern scientific and technological progress. The ongoing research shapes a rich landscape for innovation and future scientific exploration across diverse disciplines.
Precise design and control of molecular self-assembly as living creatures are exciting ideas in the field of nanotechnology. Characterized with predesigned geometries and accurate spatial addressability, programmable DNA origami nanostructures have been recognized as optimized tools for assembling multiple functional components. A variety of biomolecules can be attached to the nanoscale drawing boards in a site-specific fashion, thus facilitating the precise construction of DNA origami-based materials for studies on biological interface. In this minireview, we highlight the recent advances in the precise construction of DNA origami-based materials with artificial bio-structures and/or biomimicking functions. The regulation of biological functions by these DNA origami-engineered assemblies at the bio-interface has been summarized and discussed.