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1.
J Colloid Interface Sci ; 673: 616-627, 2024 Jun 17.
Article in English | MEDLINE | ID: mdl-38897063

ABSTRACT

Oxygen evolution reaction (OER) is the efficiency limiting half-reaction in water electrolysis for green hydrogen production due to the 4-electron multistep process with sluggish kinetics. The electrooxidation of thermodynamically more favorable organics accompanied by CC coupling is a promising way to synthesize value-added chemicals instead of OER. Efficient catalyst is of paramount importance to fulfill such a goal. Herein, a molybdenum iron carbide-copper hybrid (Mo2C-FeCu) was designed as anodic catalyst, which demonstrated decent OER catalytic capability with low overpotential of 238 mV at response current density of 10 mA cm-2 and fine stability. More importantly, the Mo2C-FeCu enabled electrooxidation assisted aldol condensation of phenylcarbinol with α-H containing alcohol/ketone in weak alkali electrolyte to selective synthesize cinnamaldehyde/benzalacetone at reduced potential. The hydroxyl and superoxide intermediate radicals generated at high potential are deemed to be responsible for the electrooxidation of phenylcarbinol and aldol condensation reactions to afford cinnamaldehyde/benzalacetone. The current work showcases an electrochemical-chemical combined CC coupling reaction to prepare organic chemicals, we believe more widespread organics can be synthesized by tailored electrochemical reactions.

2.
J Colloid Interface Sci ; 643: 292-304, 2023 Aug.
Article in English | MEDLINE | ID: mdl-37075538

ABSTRACT

The hierarchically nanostructured NiTe@CoxSy composites are constructed on a foamed nickel substrate by a two-step electrode preparation process. Structural characterization shows the dense growing of CoxSy nanosheets around NiTe nanorods forms a hierarchical nanostructure which possesses synergetic effects from both compositional and structural complementarity, more pathways for ion/electrolyte transport, richer redox active sites, and better conductivity. Thanks to the rational design of this hierarchical structure, NiTe@CoxSy delivers a high areal capacitance of 7.7F cm-2 at 3 mA cm-2 and achieves the improved capacitance retention of 97.9% after 10,000 cycles. Of particular importance is the successful fabrication of NiTe@CoxSy//activated carbon hybrid supercapacitors. This hybrid device has a wide operating voltage window, high areal energy density of 0.48 mWh cm-2 at 2.55 mW cm-2, impressive rate capability of 62.3% even after a 20-fold increase of the current density, and a 115.1% of initial capacitance retention after 15,000 cycles. Meanwhile, two tandem such hybrid devices can easily drive a pair of mini fans or light up a heart-like pattern assembled by 10 red LEDs. These experimental results not only demonstrate that the hierarchically nanostructured NiTe@CoxSy composites can serve as a prospective candidate electrode; but also develop a novel strategy about how to achieve high-performance stockpile equipment by rationale designing a desirable nanostructures.

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