Integrated electrocatalytic processing of levulinic acid and formic acid to produce biofuel intermediate valeric acid

Literature Information

Publication Date 2013-11-21
DOI 10.1039/C3GC42254B
Impact Factor 10.182
Authors

Yang Qiu, Le Xin, David J. Chadderdon, Ji Qi, Changhai Liang, Wenzhen Li


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Abstract

Herein, we report integrated electrocatalytic processing of simulated acid-catalyzed cellulose hydrolysis downstream (levulinic acid + formic acid) to the biofuel intermediate valeric acid (VA). This green electro-biorefining process does not require complex steps to separate levulinic acid and formic acid (FA) from H2SO4; instead it couples electrocatalytic hydrogenation (ECH) of levulinic acid (LA) in a single electrocatalytic flow cell reactor and electrocatalytic oxidation of formic acid in a proton exchange membrane-direct formic acid fuel cell (DFAFC). The presence of FA has shown no negative effect on the ECH of LA and a high VA selectivity of >90% can be achieved on a non-precious Pb electrode while the Faradaic efficiency remains >47% during 8 hours of reaction in the single electrocatalytic flow cell reactor. This stream is fed directly to the DFAFC with a Pd/C anode catalyst to self-sustainably remove FA where 47% conversion of FA can be reached in 6 hours. However, electro-oxidation of FA over Pd/C appears to be reversibly inhibited by the product VA produced during ECH of LA. The electro-oxidation of FA + C2–C5 alkyl carboxylic acid in the half cell study shows that such an inhibition effect could have originated from the –COOH adsorption on the Pd surface. Higher carboxylic acid concentration and longer carbon chain lead to more serious loss of the electrocatalytic surface area (ECSA) of Pd/C.

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Green Chemistry
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Green Chemistry provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on, but not limited to, the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998). Green chemistry is the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry is at the frontiers of this continuously-evolving interdisciplinary science and publishes research that attempts to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. Submissions on all aspects of research relating to the endeavour are welcome. The journal publishes original and significant cutting-edge research that is likely to be of wide general appeal. To be published, work must present a significant advance in green chemistry. Papers must contain a comparison with existing methods and demonstrate advantages over those methods before publication can be considered. For more information please see this Editorial. Coverage includes the following, but is not limited to: Design (e.g. biomimicry, design for degradation/recycling/reduced toxicity…) Reagents & Feedstocks (e.g. renewables, CO2, solvents, auxiliary agents, waste utilization…) Synthesis (e.g. organic, inorganic, synthetic biology…) Catalysis (e.g. homogeneous, heterogeneous, enzyme, whole cell…) Process (e.g. process design, intensification, separations, recycling, efficiency…) Energy (e.g. renewable energy, fuels, photovoltaics, fuel cells, energy storage, energy carriers…) Applications (e.g. electronics, dyes, consumer products, coatings, pharmaceuticals, preservatives, building materials, chemicals for industry/agriculture/mining…) Impact (e.g. safety, metrics, LCA, sustainability, (eco)toxicology…) Green chemistry is, by definition, a continuously-evolving frontier. Therefore, the inclusion of a particular material or technology does not, of itself, guarantee that a paper is suitable for the journal. To be suitable, the novel advance should have the potential for reduced environmental impact relative to the state of the art. Green Chemistry does not normally deal with research associated with 'end-of-pipe' or remediation issues.

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