Paired Electrocatalytic Oxygenation and Hydrogenation of Organic Substrates with Water as the Oxygen and Hydrogen Source

Zhang, Peili; Sheng, Xia; Chen, Xiaoyu; Fang, Zhiyong; Jiang, Jian; Wang, Mei; Li, Fusheng; Fan, Lizhou; Ren, Yansong; Zhang, Biaobiao; Timmer, Brian J. J.; Ahlquist, Mårten S. G.; Sun, Licheng

doi:10.1002/ange.201903936

Cited by 61 publications

(32 citation statements)

References 31 publications

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“…For example, the oxidation of glycerol to glyceraldehyde (GLAD) and/or 1,3dihydroxyacetone (DHA) could essentially increase the commercial value by thousands of times [4,5]. The oxidation of other biomass-derived alcohols (benzylic alcohols and 5-hydroxymethylfurfural) [6,7], the activation of C-H bonds [8], as well as the production of various oxidizing reagents (S2O8 2− , ClO − , and H2O2) [9] are also of significant importance for the chemical industry. However, the commonly employed thermo-and electrochemical routes not only rely greatly on adscititious oxidants and noble metal catalysts (e.g., Pt, Pd, and Au), but also require massive energy consumption, thus seriously hindering their potential applications [3,[10][11][12].…”

Section: Introductionmentioning

confidence: 99%

Interface-modulated nanojunction and microfluidic platform for photoelectrocatalytic chemicals upgrading

Liu

et al. 2021

Applied Catalysis B: Environmental

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Photoelectrocatalytic oxidation provides a technically applicable way for solar-chemical synthesis, but its efficiency and selectivity are moderate. Herein, a microfluidic photoelectrochemical architecture with 3-D microflow channels is constructed by interfacial engineering of defective WO3/TiO2 heterostructures on porous carbon fibers. Kelvin probe force microscopy and photoluminescence imaging visually evidence the charge accumulation sites on the nanojunction. This efficient charge separation contributes to 3-fold enhancement in the yield of glyceraldehyde and 1,3-dihydroxyacetone during glycerol upgrading, together with nearly doubled production of high value-added KA oil and S2O8 2− oxidant through cyclohexane and HSO4 − oxidization, respectively. More importantly, the microfluidic platform with enhanced mass transfer exhibits a typical reaction selectivity of 85%, which is much higher than the conventional planar protocol. Integrating this microfluidic photoanode with an oxygen reduction cathode leads to a self-sustained photocatalytic fuel cell with remarkably high open-circuit voltage (0.9 V) and short-circuit current (1.2 mA cm −2 ).

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Section: Introductionmentioning

confidence: 99%

Interface-modulated nanojunction and microfluidic platform for photoelectrocatalytic chemicals upgrading

Liu

et al. 2021

Applied Catalysis B: Environmental

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“…The latter can be readily realized by using D 2 O to replace H 2 O, in sharp contrast to previous –ND 2 synthesis using expensive and hard-to-obtain deuterated D 2 , LiAlD 4 and DCl [ 32 , 33 ]. Currently, the electrochemical reduction of nitro compounds relies on the use of noble metal electrodes and suffers from low conversion, narrow substrate scopes and poor selectivity [ 34 , 35 ]. Furthermore, the operational conditions in acidic solutions (such as HClO 4 ) make it impractical and challenging to synthesize –ND 2 with a high deuteration content [ 36 , 37 ].…”

Section: Introductionmentioning

confidence: 99%

Potential-tuned selective electrosynthesis of azoxy-, azo- and amino-aromatics over a CoP nanosheet cathode

Chong

Liu

Huang

et al. 2019

National Science Review

116

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Azoxy-, azo- and amino-aromatics are among the most widely used building blocks in materials science pharmaceuticals and synthetic chemistry, but their controllable and green synthesis has not yet been well established. Herein, a facile potential-tuned electrosynthesis of azoxy-, azo- and amino-aromatics via aqueous selective reduction of nitroarene feedstocks over a CoP nanosheet cathode is developed. A series of azoxy-, azo- and amino-compounds with excellent selectivity, good functional group tolerance and high yields are produced by applying different bias input. The synthetically significant and challenging asymmetric azoxy-aromatics can be controllably synthesized in moderate to good yields. The use of water as the hydrogen source makes this strategy remarkably fascinating and promising. In addition, deuterated aromatic amines with a high deuterium content can be readily obtained by using D2O. By pairing with anodic oxidation of aliphatic amines to nitriles, synthetically useful building blocks can be simultaneously produced in a CoP||Ni2P two-electrode electrolyzer. Only 1.25 V is required to achieve a current density of 20 mA cm−2, which is much lower than that of overall water splitting (1.70 V). The paired oxidation and reduction reactions can also be driven using a 1.5 V battery to synthesize nitrile and azoxybenzene with good yields and selectivity, further emphasizing the flexibility and controllability of our method. This work paves the way for a promising approach to the green synthesis of valuable chemicals through potential-controlled electrosynthesis.

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“… 8 Recent efforts demonstrated the effective utilization of both anodic and cathodic sides for the simultaneous ECH and ECO of bio-oil compounds. 8 , 9 In particular, the bio-oil compounds, such as furfural (FF) and 5-hydroxymethylfurfural (HMF), and phenolic compounds have been successfully converted into alcohols, fuels, and oxidative reactive products using paired electrolyzers. 5 , 9 − 14 …”

Section: Introductionmentioning

confidence: 99%

“… 8 , 9 In particular, the bio-oil compounds, such as furfural (FF) and 5-hydroxymethylfurfural (HMF), and phenolic compounds have been successfully converted into alcohols, fuels, and oxidative reactive products using paired electrolyzers. 5 , 9 − 14 …”

Section: Introductionmentioning

confidence: 99%

High-Grade Biofuel Synthesis from Paired Electrohydrogenation and Electrooxidation of Furfural Using Symmetric Ru/Reduced Graphene Oxide Electrodes

Bharath

Banat

2021

ACS Appl. Mater. Interfaces

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Electrochemical hydrogenation is a challenging technoeconomic process for sustainable liquid fuel production from biomass-derived compounds. In general, half-cell hydrogenation is paired with water oxidation to generate the low economic value of O 2 at the anode. Herein, a new strategy for the rational design of Ru/reduced graphene oxide (Ru/RGO) nanocomposites through a cost-effective and straightforward microwave irradiation technique is reported for the first time. The Ru nanoparticles with an average size of 3.5 nm are well anchored into the RGO frameworks with attractive nanostructures to enhance the furfural’s paired electrohydrogenation (ECH) and electrooxidation (ECO) process to achieve high-grade biofuel. Furfural is used as a reactant with the paired electrolyzer to produce furfuryl alcohol and 2-methylfuran at the cathode side. Simultaneously, 2-furic acid and 5-hydroxyfuroic acid along with plenty of H + and e – are generated at the anode side. Most impressively, the paired electrolyzer induces an extraordinary ECH and ECO of furfural, with the desired production of 2-methylfuran (yield = 91% and faradic efficiency (FE) of 95%) at X FF = 97%, outperforming the ECH half-cell reaction. The mechanisms of the half-cell reaction and paired cell reaction are discussed. Exquisite control of the reaction parameters, optimized strategies, and the yield of individual products are demonstrated. These results show that the Ru/RuO nanocomposite is a potential candidate for biofuel production in industrial sectors.

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Paired Electrocatalytic Oxygenation and Hydrogenation of Organic Substrates with Water as the Oxygen and Hydrogen Source

Abstract: Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.org/10.

Cited by 61 publications

References 31 publications

Interface-modulated nanojunction and microfluidic platform for photoelectrocatalytic chemicals upgrading

Interface-modulated nanojunction and microfluidic platform for photoelectrocatalytic chemicals upgrading

Potential-tuned selective electrosynthesis of azoxy-, azo- and amino-aromatics over a CoP nanosheet cathode

High-Grade Biofuel Synthesis from Paired Electrohydrogenation and Electrooxidation of Furfural Using Symmetric Ru/Reduced Graphene Oxide Electrodes

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