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Dissecting the role of anions in surface reconstruction in urea oxidation to maximize assisted hydrogen production
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2024-11-05 , DOI: 10.1039/d4qi02333a
Weiwei Bao, Mameng Yang, Taotao Ai, Jie Han, Zhifeng Deng, Xiangyu Zou, Peng Jiang, Junjun Zhang

Transition metal chalcogenides (TMCs) are a category of electrocatalysts with favorable catalytic activity, however, the impact of oxidation and the leaching of chalcogens on the urea oxidation reaction (UOR) is not clear. Herein, 3D nanostructures of Mo-Ni3S2 nanowire arrays densely grown on nickel foam (NF) were conceived and produced using a hydrothermal treatment. During the UOR process, S and Mo are electrooxidized to generate sulfite (SO32−) and molybdate (MoO42−), with SO32− further oxidized to sulfate (SO42−). Experiments proved that adding molybdate and sulfate actively improves the oxidation activity of Ni(OH)2 and optimizes the adsorption/desorption of the UOR intermediates. The well-conceived Mo-Ni3S2 bifunctional catalyst performs well in urea-aided hydrolysis at up to 82 mA cm−2 at a voltage of 1.57 V with little performance degradation over 50 h. A promising avenue for new insights into the mechanisms underlying anionic surface reconstruction in the UOR process is offered in this work.

中文翻译:


剖析阴离子在尿素氧化表面重建中的作用,以最大限度地辅助制氢



过渡金属硫属化物 (TMC) 是一类具有良好的催化活性的电催化剂,然而,硫属化合物的氧化和浸出对尿素氧化反应 (UOR) 的影响尚不清楚。在此,构思了密集生长在泡沫镍 (NF) 上的 Mo-Ni3S2 纳米线阵列的 3D 纳米结构,并使用水热处理生产。在 UOR 过程中,S 和 Mo 被电氧化生成亚硫酸盐 (SO32−) 和钼酸盐 (MoO42−),SO32− 进一步氧化成硫酸盐 (SO42−)。实验证明,添加钼酸盐和硫酸盐可积极提高 Ni(OH)2 的氧化活性,并优化 UOR 中间体的吸附/解吸。构思完善的 Mo-Ni3S2 双功能催化剂在 1.57 V 电压下以高达 82 mA cm-2 的尿素辅助水解表现良好,在 50 小时内性能下降很小。这项工作为深入了解 UOR 过程中阴离子表面重建机制提供了一条有前途的途径。
更新日期:2024-11-06
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