Two-dimensional materials, such as layered compounds and nanosheets, have attracted interest for their characteristic structures and properties. If layered materials containing functional organic molecules are synthesized, designed nanosheets can be obtained by exfoliation. Here we show the design and synthesis of an amorphous organic layered material containing a conjugated-polymer network, its exfoliation into nanosheets, and their applications. Copolymerization of benzoquinone and pyrrole generates random stacks of the conjugated polymer layers through successive CC bond formation and pericyclic reaction under mild conditions at 60°C. The amorphous organic layered materials are efficiently exfoliated into nanosheets in 44.6% after 1 h. The nanosheets are used as a metal-free electrocatalyst for hydrogen evolution reaction with the overpotential 0.28 V (vs. RHE). The present approach may be applied to the design of functional nanosheets with graphenelike structures under mild conditions.

Water pollution, evident by negative values of redox potential in waters, occurs at the lagoonal coast located near the densely populated area of Fongafale Islet on Funafuti Atoll, Tuvalu, Central Pacific. Sediment microbial quinone analysis revealed that these coastal sediments exhibit 2.7-10.4 times more microbial biomass, significantly different microbial community structure and low microbial diversity, when compared to an undisturbed natural coastal sediment. Thus, the pollution is chronic. By considering the total land use/coverage on the islet, the situation of septic tank installations, temporal changes in water redox potential and Escherichia coli numbers in the coastal waters and the spatial distribution of acid volatile sulfide in the sediments, we conclude that domestic wastewater is the primary source of pollution. This pollution is proposed to occur via the following mechanism: during ebb tides, domestic wastewater leaking from bottomless septic tanks and pit toilets run off into the lagoonal coast. Tide changes control the pollution load of domestic wastewater.

Novel tert-alkoxysilanetriols (ROSi(OH)(3), R=adamantyl and 3-ethyl-3-pentyl) have been prepared from the corresponding tert-alkoxytrichlorosilanes and successfully used as molecular building blocks to produce ordered siloxane-based nanomaterials. Controlled hydrolysis of the alkoxytrichlorosilanes led to the formation of crystalline powders of alkoxysilanetriols that were stable under ambient conditions. Solid-state polycondensation of the alkoxysilanetriols occurred upon heating, which led to the formation of ordered silica-organic nanocomposites with laminated morphologies. On the other hand, silylation of the tert-alkoxysilanetriols with chlorotrimethoxysilane enabled us to synthesize well-defined oligomeric alkoxysilanes (ROSi[OSi(OMe)(3)](3)). Hydrolysis and polycondensation of these oligomers followed by acid treatment gave microporous silica with narrow pore size distributions. Thus, tert-alkoxy groups serve not only as protecting groups of siloxane species to regulate hydrolysis and polycondensation, but also as templates to generate micropores thereby providing unique synthetic pathways for the design of ordered silica-based materials.

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Amorphous flexible covalent organic networks containing functional molecules were synthesized by consecutive and multiple reactions at different rates and in multiple directions.

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