Chemical Society Reviews最新文献

Zeolite-catalyzed methanol-to-olefin (MTO) and methanol-to-ethanol (MTE) reactions have achieved significant breakthroughs in both industry and academia, proving to be mature alternative pathways for producing basic chemicals from non-oil resources. The successful transition of these catalytic processes from laboratory to industrial implementation has been propelled by fundamental breakthroughs in the comprehensive understanding of reaction mechanisms. In this context, solid-state nuclear magnetic resonance (ssNMR) spectroscopy has emerged as an indispensable tool for elucidating catalyst structures, catalytic reaction mechanisms, and the interactions and dynamics of reactant molecules in these industrially important processes. This review specifically focuses on the application of ssNMR spectroscopy in industrially mature MTO and dimethyl ether (DME) carbonylation processes, which serve as representative examples of zeolite-catalyzed industrial processes. Based on this molecular-level information from spectroscopic observations combined with theoretical methods, this review aims to bridge the fundamental understandings of reaction mechanisms with practical applications, including the rationalization of catalysts, the optimization of catalytic performance, and the improvement of industrial processes.

Sulfur dioxide is a toxic atmospheric pollutant, primarily emitted from the combustion of sulfur-containing fossil fuels. The development of clean and cost-effective chemical processes for capturing SO₂ has garnered significant interest from both industry and academia. On the other hand, sulfonyl-derived functional groups occupy a significant position in pharmaceuticals, agrochemicals and materials science. As versatile building blocks, sulfonyl groups can be utilized in a variety of bond-forming reactions in modern organic chemistry. Thus, the direct synthesis of these SO₂-containing compounds from SO₂ under mild conditions represents a more atom-efficient and greener approach. Owing to the troublesome issue of using toxic and malodorous gaseous SO₂, sulfonylation reactions involving diverse SO₂ surrogates provide an efficient and promising method for the synthesis of SO₂-containing compounds. Since 2014, radical-mediated SO₂ insertion strategies have attracted significant attention. By using photocatalysis, electrochemistry, transition-metal catalysis, and thermal initiation, significant progress has been made toward radical sulfonylation with SO₂ surrogates. This review highlights the advances from the past decade that provide readers with essential tools for designing and implementing radical sulfonylation using SO₂ surrogates in organic synthesis.

This review outlines several linear optical effects featured by molecular polaritons arising in the collective strong light-matter coupling regime. Under weak laser irradiation and when the single-molecule light-matter coupling can be neglected (often in the limit when the number of molecules per photon mode is large), we show that the excited-state molecular dynamics under collective strong coupling can be exactly replicated without the cavity using a shaped (or "filtered") laser, whose field amplitude is enhanced by the cavity quality factor, shining on the bare molecules. As a consequence, the absorption within a cavity can be understood as the overlap between the polariton transmission and the bare molecular absorption, suggesting that polaritons act in part as optical filters. This framework demystifies and provides a straightforward explanation for a large class of experiments and theoretical models in molecular polaritonics, highlighting that the same effects can be achieved without the cavity with shaped laser pulses. With a few modifications, this simple conceptual picture can also be adapted to understand the incoherent nonlinear response of polaritonic systems. This review establishes a clear distinction between polaritonic phenomena that can be fully explained through classical linear optics and those that require a quantum electrodynamics approach. It also highlights the need to differentiate between effects that necessitate polaritons (i.e., hybrid light-matter states) and those that can occur in the weak coupling regime. We further discuss that certain quantum optical effects like fluorescence can be partially described as optical filtering, whereas some others like cavity-induced Raman scattering go beyond this. Further exploration in these areas is needed to uncover novel polaritonic phenomena beyond optical filtering.

This review explores the emerging field of supramolecular engineering in hybrid organic-inorganic perovskite optoelectronics. The incorporation of supramolecular agents has shown transformative effects on the crystallization, morphology, stability, and performance of perovskite-based materials and devices. We systematically review the types of supramolecular interactions, mechanisms of supramolecular engineering crystallization, synthesis of perovskite quantum dots, and interface engineering advancements for device stability. This comprehensive evaluation discusses the latest progress, challenges, and promising future directions, highlighting supramolecular engineering's potential in advancing hybrid organic-inorganic perovskite optoelectronic technologies.