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oxygenated boron-doped carbon via polymer dehalogenation as an electrocatalyst for high-efficiency O_(2)reduction to H_(2)O_(2)

引用

Science China Materials 2022年第5期65卷 1276-1284页

作者： Yingna Chang Jiawei Li Jun Ma Yu Liu Rong Xing Yaqun Wang Guoxin Zhang Institute of New Energy on Chemical Storage and Power Sources College of Applied Chemistry and Environmental EngineeringYancheng Teachers UniversityYancheng 224000China Shandong University of Science and Technology Department of Electrical Engineering and AutomationQingdao 266590China College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China

The direct electrochemical synthesis of H_(2)O_(2)from O_(2)is currently the most promising alternative to energyintensive industrial anthraquinone oxidation/reduction methods. However, its widespread use is hampered by the lack of efficient low-cost electrocatalysts. In the current study,oxygenated boron-doped carbon(O-BC) materials were realized via a green synthetic strategy involving polymer dehalogenation and employed as electrode materials for the electrochemical synthesis of H_(2)O_(2)via a 2 e-oxygen *** catalytic activity of the O-BC materials was optimized through systematic variation of the boron source(H_(2)BO_(2))dosage and annealing temperature. Electrochemical measurements revealed that the optimal sample(O-BC-2-650)exhibited a selectivity of 98% for the 2 e-oxygen reduction to H2 O_(2)and an average H_(2)O_(2)production rate of412.8 mmol g_(cat)^(-1) h^(-1)in an H-type alkaline electrolyzer. Density functional theory simulations indicated that the functionalization of active B sites with one oxygen atom provides the lowest Gibbs free energy change(ΔG) of 0.03 e V for the hydrogenation of*O_(2), while functionalization with zero or two O atoms results in much larger ΔG values(0.08 and 0.10 e V,respectively). Thus, this work details a new type of green, lowcost, and metal-free electrocatalyst for H_(2)O_(2)production.

关键词： doped carbon material oxygenated dopant boron oxygen reduction reaction hydrogen peroxide

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