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1.
Angew Chem Int Ed Engl ; 62(37): e202306754, 2023 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-37464925

RESUMO

Despite the recent progress in increasing the power generation of Anion-exchange membrane fuel cells (AEMFCs), their durability is still far lower than that of Proton exchange membrane fuel cells (PEMFCs). Using the complementary techniques of X-ray micro-computed tomography (CT), Scanning Electron Microscopy (SEM) and Energy Dispersive X-ray (EDX) spectroscopy, we have identified Pt ion migration as an important factor to explain the decay in performance of AEMFCs. In alkaline media Pt+2 ions are easily formed which then either undergo dissolution into the carbon support or migrate to the membrane. In contrast to PEMFCs, where hydrogen cross over reduces the ions forming a vertical "Pt line" within the membrane, the ions in the AEM are trapped by charged groups within the membrane, leading to disintegration of the membrane and failure. Diffusion of the metal components is still observed when the Pt/C of the cathode is substituted with a FeCo-N-C catalyst, but in this case the Fe and Co ions are not trapped within the membrane, but rather migrate into the anode, thereby increasing the stability of the membrane.

2.
Materials (Basel) ; 16(1)2023 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-36614733

RESUMO

Sustainable production of renewable carbon-based fuels and chemicals remains a necessary but immense challenge in the fight against climate change. Bio-oil derived from lignocellulosic biomass requires energy-intense upgrading to produce usable fuels or chemicals. Traditional upgrading methods such as hydrodeoxygenation (HDO) require high temperatures (200−400 °C) and 200 bar of external hydrogen. Electrochemical hydrogenation (ECH), on the other hand, operates at low temperatures (<80 °C), ambient pressure, and does not require an external hydrogen source. These environmental and economically favorable conditions make ECH a promising alternative to conventional thermochemical upgrading processes. ECH combines renewable electricity with biomass conversion and harnesses intermediately generated electricity to produce drop-in biofuels. This review aims to summarize recent studies on bio-oil upgrading using ECH focusing on the development of novel catalytic materials and factors impacting ECH efficiency and products. Here, electrode design, reaction temperature, applied overpotential, and electrolytes are analyzed for their impacts on overall ECH performance. We find that through careful reaction optimization and electrode design, ECH reactions can be tailored to be efficient and selective for the production of renewable fuels and chemicals. Preliminary economic and environmental assessments have shown that ECH can be viable alternative to convention upgrading technologies with the potential to reduce CO2 emissions by 3 times compared to thermochemical upgrading. While the field of electrochemical upgrading of bio-oil has additional challenges before commercialization, this review finds ECH a promising avenue to produce renewable carbon-based drop-in biofuels. Finally, based on the analyses presented in this review, directions for future research areas and optimization are suggested.

4.
Anal Chem ; 80(6): 2042-9, 2008 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-18275165

RESUMO

An ultrasensitive chronoamperometric method for quantitative determination of trace amounts of lead (down to 20 ppb) in acidic solutions is proposed in this paper. The method is based on observations that a complete underpotentially deposited (UPD) lead layer inhibits the electroreduction of nitrate on a bare Cu(111) electrode. To asses the limits of the method, both the electroreduction of nitrate and UPD of lead monolayer on copper single (111) and polycrystalline electrodes in perchloric acidic solution are studied by means of cyclic voltammetry, chronoamperometry, and rotating disk electrode (RDE) experiments. It is found that an inexpensive polycrystalline copper electrode is sensitive enough for analytical detection of lead traces in electrolytes down to 1 x 10(-8) M. Analytical results obtained by the proposed method in 2 orders of magnitude concentration range are compared to atomic absorption spectroscopy measurements to evaluate and assess the sensitivity of the employed experimental protocol. The excellent match between both analytical approaches validates the applicability of the proposed method.

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