A porous organic polymer with aminopyridine functionalities was designed to fabricate a stable, atomically dispersed Ir catalyst. This Ir-based SAC exhibits excellent catalytic activity during the liquid phase hydrogenation of CO 2 to formate, with a turnover number as high as 25,135 representing the best performance yet for a heterogeneous conversion of CO 2 to formate. The chemical structure of the Ir SAC is analogous to that of a homogeneous mononuclear complex catalyst, representing an intermediary between heterogeneous and homogeneous catalysis.
The lack of safe, efficient, and economical hydrogen storage technologies is a hindrance to the realization of the hydrogen economy. Reported herein is a reversible formate-based carbon-neutral hydrogen storage system that is established over a novel catalyst comprising palladium nanoparticles supported on nitrogen-doped mesoporous carbon. The support was fabricated by a hard template method and nitridated under a flow of ammonia. Detailed analyses demonstrate that this bicarbonate/formate redox equilibrium is promoted by the cooperative role of the doped nitrogen functionalities and the well-dispersed, electron-enriched palladium nanoparticles.
Here, luminol electrochemiluminescence was first applied to analyze intracellular molecules, such as glucose, at single cells. The individual cells were retained in cell-sized microwells on a gold coated indium tin oxide (ITO) slide, which were treated with luminol, triton X-100, and glucose oxidase simultaneously. The broken cellular membrane in the presence of triton X-100 released intracellular glucose into the microwell and reacted with glucose oxidase to generate hydrogen peroxide, which induced luminol luminescence under positive potential. To achieve fast analysis, the luminescences from 64 individual cells on one ITO slide were imaged in 60 s using a charge-coupled device (CCD). More luminescence was observed at all the microwells after the introduction of triton X-100 and glucose oxidase suggested that intracellular glucose was detected at single cells. The starvation of cells to decrease intracellular glucose produced less luminescence, which confirmed that our luminescence intensity was correlated with the concentration of intracellular glucose. Large deviations in glucose concentration at observed single cells revealed high cellular heterogeneity in intracellular glucose for the first time. This developed electrochemiluminescence assay will be potentially applied for fast analysis of more intracellular molecules in single cells to elucidate cellular heterogeneity.
Production of chemicals and fuels from renewable cellulosic biomass is important for the creation of a sustainable society, and it critically relies on the development of new and efficient transformation routes starting from cellulose. Here, a chemocatalytic conversion route from cellulosic biomass to methyl glycolate (MG), ethylene glycol (EG), and ethanol (EtOH) is reported. By using a tungsten-based catalyst, cellulose is converted into MG with a yield as high as 57.7 C % in a one-pot reaction in methanol at 240 °C and 1 MPa O , and the obtained MG can be easily separated by distillation. Afterwards, it can be nearly quantitatively converted to EG at 200 °C and to EtOH at 280 °C with a selectivity of 50 % through hydrogenation over a Cu/SiO catalyst. By this approach, the fine chemical MG, the bulk chemical EG, and the fuel additive EtOH can all be efficiently produced from renewable cellulosic materials, thus providing a new pathway towards mitigating the dependence on fossil resources.
Soil organic carbon (SOC) dynamics in croplands is a crucial component of global carbon (C) cycle. Depending on local environmental conditions and management practices, typical C input is generally required to reduce or reverse C loss in agricultural soils. No studies have quantified the critical C input for maintaining SOC at global scale with high resolution. Such information will provide a baseline map for assessing soil C dynamics under potential changes in management practices and climate, and thus enable development of management strategies to reduce C footprint from farm to regional scales. We used the soil C model RothC to simulate the critical C input rates needed to maintain existing soil C level at 0.1° × 0.1° resolution in global wheat systems. On average, the critical C input was estimated to be 2.0 Mg C ha−1 yr−1, with large spatial variability depending on local soil and climatic conditions. Higher C inputs are required in wheat system of central United States and western Europe, mainly due to the higher current soil C stocks present in these regions. The critical C input could be effectively estimated using a summary model driven by current SOC level, mean annual temperature, precipitation, and soil clay content.
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