Electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural and furfural over oxygen vacancy-rich NiCoMn-layered double hydroxides nanosheets

Author(s): Biying Liu ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Shaojun Xu ⁶ ^, ⁷ ^, ⁸ ^, ⁹ ^, ¹⁰ , Man Zhang ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Xin Li ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Donato Decarolis ⁶ ^, ⁷ ^, ⁸ ^, ⁹ ^, ¹⁰ , Yuqian Liu ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Yuchen Wang ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Emma K. Gibson ¹⁰ ^, ¹¹ ^, ¹² ^, ¹³ ^, ⁹ , C. Richard A. Catlow ⁶ ^, ⁷ ^, ⁸ ^, ⁹ ^, ¹⁰ , Kai Yan ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵

Publication date (Electronic): 2021

Journal: Green Chemistry

Publisher: Royal Society of Chemistry (RSC)

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Abstract

Rational design of low-cost and active electrocatalysts is crucial for upgrading of biomass-derived chemicals.

Abstract

Rational design of low-cost and active electrocatalysts is crucial for upgrading of biomass-derived chemicals. Here, we report highly efficient catalysts ternary NiCoMn-layered double hydroxides (NiCoMn-LDHs) nanosheets which are oxygen vacancy-rich, produced under controllable conditions for the electrooxidation of both 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) and furfural to furoic acid (FurAc) under mild conditions, respectively. Electrochemical tests showed that the oxidation of HMF and furfural occurred prior to the oxidation of water at lower applied potentials with NiCoMn-LDHs catalysts. High yields of FDCA (91.7%) and FurAc (92.4%) were achieved in 2.5 h using 1.15 nm thick NiCoMn-LDHs nanosheets under the optimal conditions. The mechanism for the superior performance, high durability, and good faradaic efficiency has been elucidated by comprehensive characterization, which confirmed that ultrathin nanosheets expose more Co-NiOOH active sites with oxygen vacancies, facilitating the synergistic effect between HMF and furfural oxidation reaction on Co–Ni and Mn ²⁺ states. The oxygen vacancy-rich NiCoMn-LDHs nanosheet catalysts present a novel and energy-efficient solution to obtain upgraded biochemicals.

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Pierre Gallezot (2012)

This critical review provides a survey illustrated by recent references of different strategies to achieve a sustainable conversion of biomass to bioproducts. Because of the huge number of chemical products that can be potentially manufactured, a selection of starting materials and targeted chemicals has been done. Also, thermochemical conversion processes such as biomass pyrolysis or gasification as well as the synthesis of biofuels were not considered. The synthesis of chemicals by conversion of platform molecules obtained by depolymerisation and fermentation of biopolymers is presently the most widely envisioned approach. Successful catalytic conversion of these building blocks into intermediates, specialties and fine chemicals will be examined. However, the platform molecule value chain is in competition with well-optimised, cost-effective synthesis routes from fossil resources to produce chemicals that have already a market. The literature covering alternative value chains whereby biopolymers are converted in one or few steps to functional materials will be analysed. This approach which does not require the use of isolated, pure chemicals is well adapted to produce high tonnage products, such as paper additives, paints, resins, foams, surfactants, lubricants, and plasticisers. Another objective of the review was to examine critically the green character of conversion processes because using renewables as raw materials does not exempt from abiding by green chemistry principles (368 references).

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An investigation of thin-film Ni-Fe oxide catalysts for the electrochemical evolution of oxygen.

Mary W Louie, Alexis T Bell (2013)

A detailed investigation has been carried out of the structure and electrochemical activity of electrodeposited Ni-Fe films for the oxygen evolution reaction (OER) in alkaline electrolytes. Ni-Fe films with a bulk and surface composition of 40% Fe exhibit OER activities that are roughly 2 orders of magnitude higher than that of a freshly deposited Ni film and about 3 orders of magnitude higher than that of an Fe film. The freshly deposited Ni film increases in activity by as much as 20-fold during exposure to the electrolyte (KOH); however, all films containing Fe are stable as deposited. The oxidation of Ni(OH)2 to NiOOH in Ni films occurs at potentials below the onset of the OER. Incorporation of Fe into the film increases the potential at which Ni(OH)2/NiOOH redox occurs and decreases the average oxidation state of Ni in NiOOH. The Tafel slope (40 mV dec(-1)) and reaction order in OH(-) (1) for the mixed Ni-Fe films (containing up to 95% Fe) are the same as those for aged Ni films. In situ Raman spectra acquired in 0.1 M KOH at OER potentials show two bands characteristic of NiOOH. The relative intensities of these bands vary with Fe content, indicating a change in the local environment of Ni-O. Similar changes in the relative intensities of the bands and an increase in OER activity are observed when pure Ni films are aged. These observations suggest that the OER is catalyzed by Ni in Ni-Fe films and that the presence of Fe alters the redox properties of Ni, causing a positive shift in the potential at which Ni(OH)2/NiOOH redox occurs, a decrease in the average oxidation state of the Ni sites, and a concurrent increase in the activity of Ni cations for the OER.