Chemical Reviews最新文献

Therapeutic reprogramming represents a transformative paradigm in regenerative medicine, developing new approaches in cell therapy, small molecule drugs, biologics, and gene therapy to address unmet medical challenges. This paradigm encompasses the precise modulation of cellular fate and function to either generate safe and functional cells ex vivo for cell-based therapies or to directly reprogram endogenous cells in vivo or in situ for tissue repair and regeneration. Building on the discovery of induced pluripotent stem cells (iPSCs), advancements in chemical modulation and CRISPR-based gene editing have propelled a new iterative medicine paradigm, focusing on developing scalable, standardized cell therapy products from universal starting materials and enabling iterative improvements for more effective therapeutic profiles. Beyond cell-based therapies, non-cell-based therapeutic strategies targeting endogenous cells may offer a less invasive, more convenient, accessible, and cost-effective alternative for treating a broad range of diseases, potentially rejuvenating tissues and extending healthspan.

The growing interest in thermoelectric energy conversion technologies has recently extended to the molecular scale, with molecular tunnel junctions emerging as promising platforms for energy harvesting from heat in a quantum-tunneling regime. This Review explores the advances in thermoelectricity within molecular junctions, highlighting the unique ability of these junctions to exploit charge tunneling and controlled molecular structure to enhance thermoelectric performance. Molecular thermoelectrics, which bridge nanoscale material design and thermoelectric applications, utilize tunneling mechanisms, such as coherent tunneling and hopping processes, including coherent and incoherent pathways, to facilitate energy conversion. Complementing these mechanisms is an array of high-precision fabrication techniques for molecular junctions, from single-molecule break junctions to large-area liquid metal-based systems, each tailored to optimize heat and charge transfer properties. With novel design strategies such as the incorporation of electron-dense ligands, customizable anchor groups, and advanced junction architectures, molecular tunnel junctions hold promise for addressing challenging targets in thermoelectricity. This Review focuses on theoretical models, experimental methodologies, and design principles aimed at understanding the thermoelectric function in molecular junctions and enhancing the performance.

Accurate models for open quantum systems─quantum states that have nontrivial interactions with their environment─may aid in the advancement of a diverse array of fields, including quantum computation, informatics, and the prediction of static and dynamic molecular properties. In recent years, quantum algorithms have been leveraged for the computation of open quantum systems as the predicted quantum advantage of quantum devices over classical ones may allow previously inaccessible applications. Accomplishing this goal will require input and expertise from different research perspectives, as well as the training of a diverse quantum workforce, making a compilation of current quantum methods for treating open quantum systems both useful and timely. In this Review, we first provide a succinct summary of the fundamental theory of open quantum systems and then delve into a discussion on recent quantum algorithms. We conclude with a discussion of pertinent applications, demonstrating the applicability of this field to realistic chemical, biological, and material systems.

Water is a salient component in catalytic systems and acts as a reactant, product and/or spectator species in the reaction. Confined water in distinct local environments can display significantly different behaviors from that of bulk water. Therefore, the wide-ranging chemistry of confined water can provide tremendous opportunities to tune the reaction kinetics. In this review, we focus on drawing the connection between confined water properties and reaction kinetics for heterogeneous (electro)catalysis. First, the properties of confined water are presented, where the enthalpy, entropy, and dielectric properties of water can be regulated by tuning the geometry and hydrophobicity of the cavities. Second, experimental and computational studies that investigate the interactions between water and inorganic materials, such as carbon nanotubes (1D confinement), charged metal or metal oxide surfaces (2D), zeolites and metal–organic frameworks (3D) and ions/solvent molecules (0D), are reviewed to demonstrate the opportunity to create confined water structures with unique H-bonding network properties. Third, the role of H-bonding structure and dynamics in governing the activation free energy, reorganization energy and pre-exponential factor for (electro)catalysis are discussed. We highlight emerging opportunities to enhance proton-coupled electron transfer by optimizing interfacial H-bond networks to regulate reaction kinetics for the decarbonization of chemicals and fuels.

Solid-state batteries (SSBs) could offer improved energy density and safety, but the evolution and degradation of electrode materials and interfaces within SSBs are distinct from conventional batteries with liquid electrolytes and represent a barrier to performance improvement. Over the past decade, a variety of imaging, scattering, and spectroscopic characterization methods has been developed or used for characterizing the unique aspects of materials in SSBs. These characterization efforts have yielded new understanding of the behavior of lithium metal anodes, alloy anodes, composite cathodes, and the interfaces of these various electrode materials with solid-state electrolytes (SSEs). This review provides a comprehensive overview of the characterization methods and strategies applied to SSBs, and it presents the mechanistic understanding of SSB materials and interfaces that has been derived from these methods. This knowledge has been critical for advancing SSB technology and will continue to guide the engineering of materials and interfaces toward practical performance.