The rational construction of covalent or noncovalent organic two-dimensional nanosheets is a fascinating target because of their promising applications in electronics, membrane technology, catalysis, sensing, and energy technologies. Herein, a large-area (square millimeters) and free-standing 2D supramolecular polymer (2DSP) single-layer sheet (0.7-0.9 nm in thickness), comprising triphenylene-fused nickel bis(dithiolene) complexes has been readily prepared by using the Langmuir-Blodgett method. Such 2DSPs exhibit excellent electrocatalytic activities for hydrogen generation from water with a Tafel slope of 80.5 mV decade(-1) and an overpotential of 333 mV at 10 mA cm(-2) , which are superior to that of recently reported carbon nanotube supported molecular catalysts and heteroatom-doped graphene catalysts. This work is promising for the development of novel free-standing organic 2D materials for energy technologies.

A general strategy for the synthesis of porous, fluorescent, triazine-framework-based membranes with intrinsic porosity through an aromatic nitrile trimerization reaction is presented. The essence of this strategy lies in the use of a superacid to catalyze the cross-linking reaction efficiently at a low temperature, allowing porous polymer membrane architectures to be facilely derived. With functionalized triazine units, the membrane exhibits an increased selectivity for membrane separation of CO(2) over N(2). The good ideal CO(2)/N(2) selectivity of 29 ± 2 was achieved with a CO(2) permeability of 518 ± 25 barrer. Through this general synthesis protocol, a new class of porous polymer membranes with tunable functionalities and porosities can be derived, significantly expanding the currently limited library of polymers with intrinsic microporosity for synthesizing functional membranes in separation, catalysis, and energy storage/conversion.

Phenolic ionic liquids for the efficient and reversible capture of CO(2) were designed and prepared from phosphonium hydroxide and substituted phenols. The electron-withdrawing or electron-donating ability, position, and number of the substituents on the anion of these ionic liquids were correlated with the physicochemical properties of the ionic liquids. The results show that the stability, viscosity, and CO(2)-capturing ability of these ionic liquids were significantly affected by the substituents. Furthermore, the relationship between the decomposition temperature, the CO(2)-absorption capacity, and the basicity of these ionic liquids was quantitatively correlated and further rationalized by theoretical calculation. Indeed, these ionic liquids showed good stability, high absorption capacity, and low absorption enthalpy for CO(2) capture. This method, which tunes the physicochemical properties by making use of substituent effects in the anion of the ionic liquid, is important for the design of highly efficient and reversible methods for CO(2)-capture. This CO(2) capture process using diverse phenolic ionic liquids is a promising potential method for CO(2) absorption with both high absorption capacity and good reversibility.