* S Supporting Information CONSPECTUS: The total world energy demand is predicted to rise significantly over the next few decades, primarily driven by the continuous growth of the developing world. With rapid depletion of nonrenewable traditional fossil fuels, which currently account for almost 86% of the worldwide energy output, the search for viable alternative energy resources is becoming more important from a national security and economic development standpoint. Nuclear energy, an emission-free, high-energy-density source produced by means of controlled nuclear fission, is often considered as a clean, affordable alternative to fossil fuel. However, the successful installation of an efficient and economically viable industrial-scale process to properly sequester and mitigate the nuclear-fission-related, highly radioactive waste (e.g., used nuclear fuel (UNF)) is a prerequisite for any further development of nuclear energy in the near future. Reprocessing of UNF is often considered to be a logical way to minimize the volume of high-level radioactive waste, though the generation of volatile radionuclides during reprocessing raises a significant engineering challenge for its successful implementation. The volatile radionuclides include but are not limited to noble gases (predominately isotopes of Xe and Kr) and must be captured during the process to avoid being released into the environment. Currently, energy-intensive cryogenic distillation is the primary means to capture and separate radioactive noble gas isotopes during UNF reprocessing. A similar cryogenic process is implemented during commercial production of noble gases though removal from air. In light of their high commercial values, particularly in lighting and medical industries, and associated high production costs, alternate approaches for Xe/Kr capture and storage are of contemporary research interest. The proposed pathways for Xe/Kr removal and capture can essentially be divided in two categories: selective absorption by dissolution in solvents and physisorption on porous materials. Physisorption-based separation and adsorption on highly functional porous materials are promising alternatives to the energy-intensive cryogenic distillation process, where the adsorbents are characterized by high surface areas and thus high removal capacities and often can be chemically fine-tuned to enhance the adsorbate−adsorbent interactions for optimum selectivity. Several traditional porous adsorbents such as zeolites and activated carbon have been tested for noble gas capture but have shown low capacity, selectivity, and lack of modularity. Metal− organic frameworks (MOFs) or porous coordination polymers (PCPs) are an emerging class of solid-state adsorbents that can be tailor-made for applications ranging from gas adsorption and separation to catalysis and sensing. Herein we give a concise summary of the background and development of Xe/Kr separation technologies with a focus on UNF reprocessing and the prospects of MOF-based adsorbents for that particular appl...

A breathing 2-fold interpenetrated microporous metal-organic framework was synthesized with a flexible tetrahedral organic linker and Zn(2) clusters that sorb CO(2) preferably over N(2) and H(2).

Access to nitrogen-based fertilizers is critical to maximize agricultural yield, as nitrogen is the most common rate-limiting nutrient. Nearly all nitrogenbased fertilizers rely on ammonia and nitric acid as feedstocks, and thus the demand for these chemicals is heavily dependent on the global population and food demand. Over the next three decades, the global population will continue to dictate the market size and value for ammonia and nitric acid, which consequently will have a significant impact on our energy infrastructure. Here, we discuss the potential for carbon-free electrocatalytic nitrogen reduction, nitrogen oxidation, and nitrate reduction to meet fertilizer manufacturing demands. We also explore various growth scenarios to predict the 2050 market size and value for ammonia and nitric acid. We highlight that if the current approaches for manufacturing ammonia and nitric acid remain constant, carbon emissions from the production of fixed fertilizer feedstocks could exceed 1300 Mt CO 2eq /yr, prompting a strong need for green alternatives.

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The considerable number of important physical properties, including optical, electronic, and magnetic properties, of Prussian blue (PB) analogues have attracted fundamental and industrial interest. Nevertheless, the gas sorption properties of PB coordination compounds were only investigated very recently. In this work, we report the synthesis and gas sorption properties of PB nanocomposites with different size and shape obtained by using poly(vinylpyrrolidone) (PVP), chitosan, and dioctyl sodium sulfosuccinate (AOT) as stabilizers and structure directing agents. All three porous nanocrystals show high and selective CO(2) adsorption over CH(4) or N(2). No distinct relationship was found between the size (or shape) of the nanosorbents and their gas uptake capacities. To our knowledge, this is the first report on the use of PB nanocomposites for CO(2) capture applications.

Krypton (Kr) and xenon (Xe) adsorption on two partially fluorinated metal-organic frameworks (FMOFCu and FMOFZn) with different cavity size and topologies are reported. FMOFCu shows an inversion in sorption selectivity toward Kr at temperatures below 0 °C while FMOFZn does not. The 1D microtubes packed along the (101) direction connected through small bottleneck windows in FMOFCu appear to be the reason for this peculiar behavior. The FMOFCu shows an estimated Kr/Xe selectivity of 36 at 0.1 bar and 203 K.

Low-cost renewable lignin has been used as a precursor to produce porous carbons. However, to date, it has not been easy to obtain high surface area porous carbon without activation processes or templating agents. Here, we demonstrate that low molecular weight lignin yields highly porous carbon with more graphitization through direct carbonization without additional activation processes or templating agents. We found that molecular weight and oxygen consumption during carbonization are critical factors to obtain high surface area, graphitized porous carbons. This highly porous carbon from low-cost renewable lignin sources is a good candidate for supercapacitor electrode materials.

Adsorption isotherms of pure gases present in flue gas including CO(2), N(2), SO(2), NO, H(2)S, and water were studied using prussian blues of chemical formula M(3)[Co(CN)(6)](2).nH(2)O (M = Co, Zn) using an HPVA-100 volumetric gas analyzer and other spectroscopic methods. All the samples were characterized, and the microporous nature of the samples was studied using the BET isotherm. These materials adsorbed 8-10 wt % of CO(2) at room temperature and 1 bar of pressure with heats of adsorption ranging from 200 to 300 Btu/lb of CO(2), which is lower than monoethanolamine (750 Btu/lb of CO(2)) at the same mass loading. At high pressures (30 bar and 298 K), these materials adsorbed approximately 20-30 wt % of CO(2), which corresponds to 3 to 5 molecules of CO(2) per formula unit. Similar gas adsorption isotherms for SO(2), H(2)S, and NO were collected using a specially constructed volumetric gas analyzer. At close to 1 bar of equilibrium pressure, these materials sorb around 2.5, 2.7, and 1.2 mmol/g of SO(2), H(2)S, and NO. In particular, the uptake of SO(2) and H(2)S in Co(3)[Co(CN)(6)](2) is quite significant since it sorbs around 10 and 4.5 wt % at 0.1 bar of pressure. The stability of prussian blues before and after trace gases was studied using a powder X-ray diffraction instrument, which confirms these materials do not decompose after exposure to trace gases.