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Register a new userEfficient Electrocatalytic Reduction of CO2 by Nitrogen-Doped Nanoporous Carbon-Carbon Nanotube Membranes - A Step Towards the Electrochemical CO2 Refinery
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The search for earth abundant, efficient and stable electrocatalysts that can enable the chemical reduction of CO2 to value-added chemicals and fuels at an industrially relevant scale, is a high priority for the development of a global network of renewable energy conversion and storage systems that can meaningfully impact greenhouse gas induced climate change. Here we introduce a straightforward, low cost, scalable and technologically relevant method to manufacture an all-carbon, electroactive, nitrogen-doped nanoporous carbon-carbon nanotube composite membrane, dubbed HNCM-CNT. The membrane is demonstrated to function as a binder-free, high-performance electrode for the electrocatalytic reduction of CO2 to formate. The Faradaic efficiency for the production of formate is 81%. Furthermore, the robust structural and electrochemical properties of the membrane endow it with excellent long-term stability.
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Electrochemical reduction of CO2 to CO is a promising strategy. However, achieving high Faradaic efficiency with high current density using ILs electrolyte remains a challenge. In this study, the IL N octyltrimethyl 1,2,4 triazole ammonium shows outstanding performance for electrochemical reduction of CO2 to CO on the commercial Ag electrode, and the current density can be up to 50.8 mA cm-2 with a Faradaic efficiency of 90.6%. The current density of CO is much higher than those reported in the ILs electrolyte. In addition, the density functional theory calculation further proved that IL interacts with CO2 to form IL CO2 complex which played a key role in reducing the activation energy of CO2. According to the molecular orbital theory, the electrons obtained from ILs was filled in the anti bonding orbit of the CO2, resulting in reducing the C=O bond energy. This work provides a new strategy to design novel ILs for high efficiency electrochemical reduction of CO2 to CO.
The low efficiency of commercially-used reverse osmosis (RO) membranes has been the main obstacle in seawater desalination application. Here, we report the auspicious performance, through molecular dynamics simulations, of a seawater desalination filter based on the recently-synthesized graphene-like carbon nitride (g-C2N) [Nat. Commun., 2015, 6, 6486]. Taking advantage of the inherent nanopores and excellent mechanical properties of g-C2N filter, highly efficient seawater desalination can be achieved by modulating the nanopores under tensile strain. The water permeability can be improved by two orders of magnitude compared to RO membranes, which offers a promising approach to the global water shortage solution.
The technical and economic feasibility to deliver sustainable liquid biocrude through hydrothermal liquefaction (HTL) while enabling negative carbon dioxide emissions is evaluated in this paper, looking into the potential of the process in the context of negative emission technologies (NETs) for climate change mitigation. In the HTL process, a gas phase consisting mainly of carbon dioxide is obtained as a side product driving a potential for the implementation of carbon capture and storage in the process (BECCS) that has not been explored yet in the existing literature and is undertaken in this study. To this end, the process is divided in a standard HTL base and a carbon capture add-on, having forestry residues as feedstock. The Selexol technology is adapted in a novel scheme to simultaneously separate the CO2 from the HTL gas and recover the excess hydrogen for biocrude upgrading. The cost evaluation indicates that the additional cost of the carbon capture can be compensated by revenues from the excess process heat and the European carbon allowance market. The impact in the MFSP of the HTL base case ranges from -7% to 3%, with -15% in the most favorable scenario, with a GHG emissions reduction potential of 102-113% compared to the fossil baseline. These results show that the implementation of CCS in the HTL process is a promising alternative from technical, economic and environmental perspective in future scenarios in which advanced liquid biofuels and NETs are expected to play a role in the decarbonization of the energy system.
We use quantum chemical calculations to elucidate a viable homogeneous mechanism for pyridine-catalyzed reduction of CO2 to methanol. In the first component of the catalytic cycle, pyridine (Py) undergoes a H+ transfer (PT) to form pyridinium (PyH+) followed by an e- transfer (ET) to produce pyridinium radical (PyH0). Examples of systems to effect this ET to populate the LUMO of PyH+(E0calc ~ -1.3V vs. SCE) to form the solution phase PyH0 via highly reducing electrons include the photo-electrochemical p-GaP system (ECBM ~ -1.5V vs. SCE at pH= 5) and the photochemical [Ru(phen)3]2+/ascorbate system. We predict that PyH0 undergoes further PT-ET steps to form the key closed-shell, dearomatized 1,2-dihydropyridine (PyH2) species. Our proposed sequential PT-ET-PT-ET mechanism transforming Py into PyH2 is consistent with the mechanism described in the formation of related dihydropyridines. Because it is driven by its proclivity to regain aromaticity, PyH2 is a potent recyclable organo-hydride donor that mimics the role of NADPH in the formation of C-H bonds in the photosynthetic CO2 reduction process. In particular, in the second component of the catalytic cycle, we predict that the PyH2/Py redox couple is kinetically and thermodynamically competent in catalytically effecting hydride and proton transfers (the latter often mediated by a proton relay chain) to CO2 and its two succeeding intermediates, namely formic acid and formaldehyde, to ultimately form CH3OH. The hydride and proton transfers for the first reduction step, i.e. reduction of CO2, are sequential in nature; by contrast, they are coupled in each of the two subsequent hydride and proton transfers to reduce formic acid and formaldehyde.
However, their electrocatalytic activity is still poorly understood. This work deciphers the origin of the catalytic activity of counter-electrodes (CEs)/current collectors made of self-standing carbon nanotubes fibers (CNTfs) using Co$^(+2)$/Co$^(+3)$ redox couple electrolytes. This is based on comprehensive electrochemical and spectroscopic characterizations of fresh and used electrodes applied to symmetric electrochemical cells using platinum-based CEs as a reference. As the most relevant findings, two straight relationships were established: i) the limiting current and stability increase rapidly with surface concentration of oxygen-containing functional groups, and ii) the catalytic potential is inversily related to the amount of residual metallic Fe catalyst nanoparticles interspersed in the CNTf network. Finally, the fine tune of the metallic nanoparticle content and the degree of functionalization enabled fabrication of efficient and stable dye-sensitized solar cells with cobalt electrolytes and CNTf-CE outperforming those with reference Pt-CEs.
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