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Integrating hydrogen production with anodic selective oxidation of sulfides over a CoFe layered double hydroxide electrode.

ABSTRACT: Replacing the sluggish oxygen evolution reaction (OER) with oxidation reactions for the synthesis of complex pharmaceutical molecules coupled with enhanced hydrogen evolution reaction (HER) is highly attractive, but it is rarely explored. Here, we report an electrochemical protocol for selective oxidation of sulfides to sulfoxides over a CoFe layered double hydroxide (CoFe-LDH) anode in an aqueous-MeCN electrolyte, coupled with 2-fold promoted cathodic H₂ productivity. This protocol displays high activity (85-96% yields), catalyst stability (10 cycles), and generality (12 examples) in selective sulfide oxidation. We demonstrate its applicability in the synthesis of four important pharmaceutical related sulfoxide compounds with scalability (up to 1.79 g). X-ray spectroscopy investigations reveal that the CoFe-LDH material evolved into amorphous CoFe-oxyhydroxide under catalytic conditions. This work may pave the way towards sustainable organic synthesis of valuable pharmaceuticals coupled with H₂ production.

SUBMITTER: Ma L

PROVIDER: S-EPMC8179046 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description: Not available

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A NiFe layered double hydroxide-decorated N-doped entangled-graphene framework: a robust water oxidation electrocatalyst.

Project description:Three dimensional (3D) porous carbon materials are highly desirable for electrochemical applications owing to their high surface area and porosity. Uniformly distributed porosity in the 3D architecture of carbon support materials allows reactant molecules to access more electrochemically active centres and simultaneously facilitate removal of the product formed during electrochemical reactions. Herein, we have prepared a nitrogen-doped entangled graphene framework (NEGF), decorated with NiFe-LDH nanostructures by an in situ solvothermal method followed by freeze-drying at high vacuum pressure and low temperature. The freeze-drying method helped to prevent the restacking of the graphene sheets and the formation of a high surface area nitrogen-doped entangled graphene framework (NEGF) supported NiFe-LDHs. The incorporation of the NEGF has significantly reduced the overpotential for the electrochemical oxygen evolution reaction (OER) in 1 M KOH solution. This corresponds to an overpotential reduction from 340 mV for NiFe-LDHs to 290 mV for NiFe-LDH/NEGF to reach the benchmark current density of 10 mA cm-2. The preparation of the catalyst is conceived through a low-temperature scalable process.

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Project description:Highly active Ru nanoparticles (Ru NPs) supported on NiFe layered double hydroxide (Ru/NiFe-LDH) are prepared easily using ultrasound-assisted reduction method without chemical reductants and stabilizers. The plentiful hydroxyls on NiFe-LDH are excited into hydrogen radicals (H) under the action of ultrasound for reducing Ru3+ to Ru0. Ru NPs with an average particle size of 1.26 nm highly disperse on the mesopore-like surface of NiFe-LDH, which improve the catalytic performance for N-ethylcarbazole (NEC) hydrogenation. The experimental results show that 5Ru/NiFe-LDH-300-60 exhibits the best catalytic performance with 100% conversion of NEC, 98.88% yield of dodecahydro-N-ethylcarbazole (12H-NEC) and 5.77 wt% mass hydrogen storage capacity under the reaction conditions of 110 ℃, 6 MPa and mRu:mNEC = 0.15 wt% for 80 min. The kinetics study shows that the apparent activation energy is only 25.15 kJ/mol, which is the lowest in the reported literatures. Ru complexes with O-contained groups on NiFe-LDH, improving the catalytic stability in NEC hydrogenation.

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Promoting electrocatalytic overall water splitting by sulfur incorporation into CoFe-(oxy)hydroxide.

Project description:The design and fabrication of highly cost-effective electrocatalysts with high activity, and stability to enhance the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) has been considered to be one of the most promising approaches toward overall water splitting. In this study, sulfur-incorporated cobalt-iron (oxy)hydroxide (S-(Co,Fe)OOH) nanosheets were directly grown on commercial iron foam via galvanic corrosion and hydrothermal methods. The incorporation of sulfur into (Co,Fe)OOH results in superior catalytic performance and high stability in both the HER and OER conducted in 1 M KOH. The incorporation of sulfur enhanced the electrocatalytic activity by modifying the electronic structure and chemical states of (Co,Fe)OOH. An alkaline water electrolyzer for overall water splitting was fabricated using a two-electrode configuration utilizing the S-(Co,Fe)OOH bifunctional electrocatalyst in both the HER and OER. The fabricated electrolyzer outperformed a precious metal-based electrolyzer using Pt/C as the HER electrocatalyst and IrO2 as the OER electrocatalyst, which are the benchmark catalysts. This electrolyzer provides a lower potential of 1.641 V at 10 mA cm-2 and maintains 98.4% of its performance after 50 h of durability testing. In addition, the S-(Co,Fe)OOH-based electrolyzer successfully generated hydrogen under natural illumination upon its combination with a commercial silicon solar cell and exhibited a solar to hydrogen (STH) efficiency of up to 13.0%. This study shows that S-(Co,Fe)OOH is a promising candidate for application in the future renewable energy industry due to its high cost-effectiveness, activity, and stability during overall water splitting. In addition, the combination of a commercial silicon solar cell with an alkaline water electrolyzer has great potential for the production of hydrogen.

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