Chemical Society Reviews最新文献

Perovskite/silicon tandem solar cells (PSTSCs) are among the most promising photovoltaic technologies for surpassing the efficiency limits of single-junction solar cells. A major breakthrough in this field has been the introduction of ultrathin hole-selective self-assembled monolayers (HS-SAMs). These molecular interfacial layers enable precise energy-level alignment, efficient hole extraction, and effective passivation of interfacial defects, while remaining compatible with textured silicon and large-area substrates. In this review, we discuss the molecular design principles of HS-SAMs, including anchoring groups, conjugated donor units, linkers, dipole engineering, wettability, and packing density, highlighting how these parameters influence charge extraction, perovskite crystallization, interfacial passivation, and device stability. We also summarize key advances in PSTSCs enabled by HS-SAMs, including a certified PCE of 29.2% with Me-4PACz and efficiencies above 32% with optimized PACz derivatives and 32.5% with 2PACz/IZO interlayers, together with operational stability exceeding 1000 h under damp-heat or continuous illumination conditions. By consolidating recent progress in molecular engineering, interfacial passivation, scalable deposition, and manufacturability, this review identifies HS-SAMs as a cornerstone for the development of efficient, stable, and commercially relevant perovskite and perovskite/silicon tandem photovoltaics.

Liquid hydrocarbon separation is in great demand in the modern petrochemical industry. Membrane-based liquid hydrocarbon separation has emerged as a next-generation technology with great potential to address energy and environmental challenges, representing one of the most rapidly evolving and demanding frontiers. Despite its promise to revolutionize energy-intensive processes, practical application remains hindered by the complexity of liquid hydrocarbon mixtures and the stringent requirements on membrane materials. In this review, microenvironment engineering is employed as the central concept to establish an integrated chain linking molecular transport mechanisms, material design, and industrial applications of liquid hydrocarbon separation membranes (LHSMs). Based on the molecular transmembrane transport mechanisms, we identify typical microenvironments in LHSMs and systematically classify liquid hydrocarbon separations into coarse, precise, and ultrafine regimes. This mechanism-based understanding of membrane microenvironments and separation regimes represents the first unified classification framework for LHSMs. Furthermore, we highlight membrane microenvironment engineering as a critical bridge connecting advanced membrane materials with practical separation performance. In particular, we propose the efficient management of membrane microenvironments, which enables the reproducibility and scalability of membrane fabrication while ensuring effective separation performance. Moreover, emerging techniques for microenvironment engineering are discussed, including in situ and operando monitoring techniques, as well as machine learning/artificial intelligence (AI)-assisted microenvironment engineering. Finally, future directions are outlined, including deeper mechanistic understanding, scalable membrane fabrication and process integration, LHSM-specific fouling understanding, and operando- and data-driven microenvironment engineering. Collectively, this review provides a coherent roadmap for the rational design and practical implementation of next-generation membranes for sustainable liquid hydrocarbon separations.

MXenes have emerged as highly promising two-dimensional materials for advanced sensing applications owing to their high electrical conductivity, rich surface chemistry, hydrophilicity, mechanical flexibility, and compositional diversity. While many MXene-based sensors have been interpreted primarily from the perspective of surface-mediated interactions on individual flakes, practical sensing devices are typically constructed from assembled architectures, including films, fibers, aerogels, hydrogels, and composite networks. In these systems, inter-flake regions can make important contributions to the generation and transmission of macroscopic sensing signals by influencing charge transport, ion and molecular diffusion, and local interfacial interactions at the device level. This review focuses on inter-flake modulation as a key design principle for MXene-based sensing systems. We begin by briefly outlining the intrinsic material properties that make MXenes attractive for sensing, then discuss the fundamental inter-flake properties of MXene assemblies, including interlayer spacing, flake orientation, structural porosity, and the chemical microenvironment, with emphasis on their characterization, modulation strategies, and impacts on sensing performance. We further summarize representative advances in inter-flake modulation of MXene assemblies for smart sensing scenarios, spanning piezoresistive sensing, chemiresistive sensing, and electrochemical sensing. Finally, we discuss key challenges and opportunities for optimizing inter-flake structures toward future MXene-based sensing systems. We believe this work will provide useful guidance and new perspectives for future advanced MXene materials and devices in smart sensing applications.

Physical mixing is one of the simplest ways to combine catalytic components, yet it has often been treated as an empirical formulation strategy rather than a rational design principle. This Review states that, when distinct solids are arranged to exchange intermediates, products, inhibitors, heat or local chemical potentials, a physical mixture can function as an interfacial reaction network rather than as a simple sum of independent catalysts. We define this concept as interfacial reaction-network catalysis (IRNC), in which complex transformations are spatially partitioned into coupled functional domains and steered through measurable interdomain exchange. After clarifying the boundaries between physical mixing, conventional bifunctional catalysis and chemically integrated architectures, we introduce three network-control modes: intermediate relay, catalytic shunting and thermodynamic cascading. Intermediate relay connects source and receiving domains through relayed intermediates. Catalytic shunting allocates branch-point flux among desired, side, escape and deactivation pathways. Thermodynamic cascading regulates local activities, residence times and deactivation exposure through enrichment, product removal and inhibitor buffering. We then discuss how these functions operate in oxide-zeolite, Fischer-Tropsch-zeolite and multicomponent systems, and how physical separation and chemical integration provide complementary coupling regimes. Finally, we highlight descriptor quantification, operando characterization, multiscale simulation and catalyst-reactor co-design as key requirements for moving IRNC from empirical combination to predictive network programming. This framework establishes physical mixing as a modular and scalable strategy for steering complex catalytic transformations across molecular, particle and reactor scales.