Chemical Reviews最新文献

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.

Transmission electron microscopy (TEM) is an indispensable analytical technique in materials research as it probes material information down to the atomic level and can be utilized to examine dynamic phenomena during material transformations. In situ TEM resolves transient metastable states via direct observation of material dynamics under external stimuli. With innovative sample designs developed over the past decades, advanced in situ TEM has enabled emulation of battery operation conditions to unveil nanoscale changes within electrodes, at interfaces, and in electrolytes, rendering it a unique tool to offer unequivocal insights of battery materials that are beam-sensitive, air-sensitive, or that contain light elements, etc. In this review, we first briefly outline the history of advanced electron microscopy along with battery research, followed by an introduction to various in situ TEM sample cell configurations. We provide a comprehensive review on in situ TEM studies of battery materials for lithium batteries and beyond (e.g., sodium batteries and other battery chemistries) via open-cell and closed-cell in situ TEM approaches. At the end, we raise several unresolved points regarding sample preparation protocol, imaging conditions, etc., for in situ TEM experiments. We also provide an outlook on the next-stage development of in situ TEM for battery material study, aiming to foster closer collaboration between in situ TEM and battery research communities for mutual progress.

Hydrogen produced with no greenhouse gas emissions is termed “green hydrogen” and will be essential to reaching decarbonization targets set forth by nearly every country as per the Paris Agreement. Proton exchange membrane water electrolyzers (PEMWEs) are expected to contribute substantially to the green hydrogen market. However, PEMWE market penetration is insignificant, accounting for less than a gigawatt of global capacity. Achieving substantive decarbonization via green hydrogen will require PEMWEs to reach capacities of hundreds of gigawatts by 2030. This paper serves as an overarching roadmap for cell-level improvements necessary for gigawatt-scale PEMWE deployment, with insights from three well-established hydrogen technology companies included. Analyses will be presented for economies of scale, renewable energy prices, government policies, accelerated stress tests, and component-specific improvements.