A series of carbon-based binary single-atom catalysts of Fe and Ni coordinated by nitrogen are fabricated using a glucose-chelating method. Depending on the Ni/Fe content, they exhibit a wide-range of controllable CO/H 2 ratio from 0.14 to 10.86, which is meaningful to specific chemical processes. The durability of the catalyst is evaluated over an 8-hour period with no significant degradation of activity. The variation of the faradaic efficiency with Ni/Fe content is justified by density-functional-theory based calculation of the reaction barrier in both hydrogen evolution and CO 2 reduction reactions.

Supramolecular luminescent hydrogels based on natural molecules have shown high potential for a variety of applications because of unique optical properties and biocompatibility, particularly serving as advanced biomaterials for bioimaging, biosensing, cell engineering, and so forth. A lanthanide complex-based system provides a promising way to prepare supramolecular luminescent hydrogels. Herein, we realize the creation of a luminescent hydrogel assembled from lanthanides and nucleosides. Nucleosides, the essential components of nucleic acids, functioning as the ligands, successfully chelate with lanthanides and form complexes in water. The complexes subsequently serve as building-blocks to form supramolecular hydrogels, which exhibit characteristic luminescent emission of lanthanides. The coordination modes and forming mechanism are studied by electrospray ionization time-of-flight mass spectrometry, matrix-assisted laser desorption/ionization time of flight mass spectrometry, 1 H NMR spectroscopy, and Fourier transform infrared spectroscopy; the corresponding molecular simulations are presented, and macro-/micro-morphologies, mechanical properties, and luminescent performances of hydrogels are systemically studied. Remarkably, these luminescent hydrogels show fluorochromic properties in response to external stimuli, including pH, temperature, anions, and cations, which are thus adopted to design smart luminescent switches and detect specific species such as Cu 2+ . Our work provides a feasible strategy to prepare stimuli-responsive luminescent hydrogels, reveals the diverse potential of nucleoside-based hydrogels, and exhibits a novel pathway for the preparation of smart optical materials.

Aerogels hold great promise as a lightweight replacement in materials fields. Dynamic fluorochromic aerogels that possess reversible stimuli responsiveness have been particularly attractive recently for new design opportunities in practical solid-state lighting and wide applications in advanced sensors/probe. In this study, we report a reversibly multiresponsive white-light-emitting (WLE) aerogel prepared with codoped lanthanide, thymidine, and carbon dots. By precisely modulating the stoichiometric ratio of lanthanide complexes and carbon dots, broad-spectrum output from purple to red is obtained, including pure white light (CIE (0.33, 0.32)). The freeze-drying process contributes to the elimination of hydration between water molecules and lanthanide ions, further preventing the quenching of lanthanide luminescence and preserving the high quantum yield (47.4%) of our aerogel. Moreover, the dynamic coordination bond between lanthanide (europium and terbium) and thymidine endows the aerogel with reversible responsiveness upon five different stimuli, including halide anions, metal ions, pH, temperature, and humidity. We envision that our WLE aerogel has considerable potential for use in various fields such as display devices, advanced sensors, and environmentally friendly probes where multiresponsiveness is required.

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