Guangtao Li

Au/TiO2 is a promising photocatalyst for CO2 reduction, yet its performance is often limited by inefficient light utilization and insufficient local CO2 availability. Here, we present an integrated photocatalytic platform by embedding Au/TiO2 nanoparticles within imidazolium poly(ionic liquid) (PIL) nanocone arrays. The nanocone architecture provides broadband light harvesting with > 99% absorptivity, while the imidazolium PIL enriches CO2 near the catalytic sites, enabling synergistic enhancement of CO2 photoreduction. The intrinsic counter-anion exchangeability of the PIL further enables programmable regulation of the overall catalytic activity and product formation selectivity. By optimizing the counter anion and water supply, the system selectively produces CO (124.89 μmol·g–1·h–1, 94.2% selectivity) or CH4 (137.75 μmol·g–1·h–1, 100% selectivity). Metalloporphyrin counter anions additionally enable C2 product formation, while functional catalytic anions allow cascade conversion of CO2 into polymeric products. This work demonstrates an integrated strategy that couples light management, substrate enrichment, and reaction programmability for efficient and versatile solar-driven CO2 conversion.

Based on the synergetic integration of poly(ionic liquid)s and photonic structures, a photonic microsphere platform was developed for visually demonstrating and predicting ion effect of the Hofmeister Series in a robust and accurate fashion.

Plasmonic networks attract increasing attention owing to their strong plasmon coupling effects at hotspot regions, where intriguing, collective optical behavior and field enhancement occur. Engineering network architectures with flexible control over density and intensity of hotspots, thus fine‐tuning electromagnetic field is the prerequisite for fully exploiting their potential use in diverse plasmon‐based applications, but it represents a great challenge. Herein, a cage‐assisted bottom‐up self‐assembly strategy is proposed to construct a series of cage‐bridged complex network architectures with a high degree of flexibility in hotspot modulation. Critical parameters associated with plasmonic networks, including interparticle distance, the density and intensity of hotspots, as well as molecule accessibility of hotspot can be simultaneously and flexibly adjusted at will. Importantly, the integration of host–guest chemistry of molecular cages into interparticle regions of networks endows selective molecule trapping capability in hotspots, offering tremendous opportunities for broader plasmon‐based applications. The present study not only develops efficient plasmonic networks with enhanced density of hotspots and intense electromagnetic fields, but also provides new avenues for artificially engineering network architectures with advanced functionalities and facilitates further applications in sensing and optoelectronics.

Multicompartment assemblies attract much attention for their wide applications. However, the fabrication of multicompartment assemblies usually requires elaborately designed building blocks and careful controlling. The emergence of droplet networks has provided a facile way to construct multiple droplet architectures, which can further be converted to multicompartment assemblies. Herein, the bind motif‐free building blocks are presented, which consist of the hydrophobic Tf₂N⁻‐based ionic liquid (IL) dissolving LiTf₂N salt, that can conjugate via arrested coalescence in confined‐space templates to form IL droplet networks. Subsequent ultraviolent polymerization generates robust free‐standing multicompartment assemblies. The conjugation of building blocks relies not on the peripheral bind motif but on the interfacial instability‐induced arrested coalescence, avoiding tedious surface modification and assembly process. By tuning structures of templates and building blocks, multicompartment assemblies with 0D, 1D, 2D, and 3D structures are prepared in a facile and high‐throughput way. Importantly, the bottom‐up construction enables modular control over the compositions and spatial positions of individual building blocks. Combining with the excellent solvency of ILs, this system can serve as a general platform towards versatile multicompartment architectures. As demonstrations, by tailoring the chambers the multicompartment assemblies can spatiotemporally sense and report the chemical cues and perform various modes of motion.

Plasmonic dimers not only provide a unique platform for studying fundamental plasmonic behavior and effects but also are functional materials for numerous applications. The efficient creation of well-defined dimers with flexible control of structure parameters and thus tunable optical property is the prerequisite for fully exploiting the potential of this nanostructure. Herein, based on a polymer-assisted self-assembly approach in conjugation with molecular cage chemistry, a strategy was demonstrated for constructing cage-bridged plasmonic dimers with controlled sizes, compositions, shape, symmetry, and interparticle gap separation in a modular and high-yield manner. With a high degree of freedom and controllability, this strategy allows facilely accessing various symmetrical/asymmetrical dimers with sub-5 nm gap distance and tailored optical properties. Importantly, as the linkage of the two constituent elements, the molecular cages embedded in the junction endow the assembled dimers with the ability to precisely and reversibly host rich guest molecules in hotspot regions, offering great potential for creating various plasmon-mediated applications.

Patchy particles, defined as particles with one or more well-defined patches, have attracted much attention due to their anisotropic and directional interactions. The anisotropic nature of the patchy particle surface enables a certain degree of control over the assembly process. Enormous efforts have been carried out to design and explore the properties of patchy particles and their collective behaviour. However, the techniques to fabricate patchy particles are still limited in terms of tunability and scalability. In this work, an effective method of fabricating patchy particles with tunable spatial topology and chemical composition of patches is presented. The number, distribution and size of the patches can be tailored by adjusting the packing of the colloidal particles and the processing condition. The active secondary reaction on the polydopamine (PDA)-coated surface and silica surface could functionalize the obtained patchy particles with desired properties to meet different requirements. As a proof of principle, the PDA-coated patches were modified with thiol-based dye via the Michael reaction and the silica surfaces were functionalized with amine-terminated alkoxysilanes via the silane coupling reaction have been demonstrated. Furthermore, the unique properties of PDA, such as reductive ability, powerful adhesive capability and carbonizable feature, have also been proven to fabricate metallic nanoparticle-decorated patchy particles and anisotropic carbon nanocapsules. The well-defined patchy particles are templated from colloidal crystal and their gram-scale fabrication is easily achieved. These results indicate that our strategy will help access the transformative potential of patchy particles in the rational design and large-scale production of functional materials.