Accelerating Anode Reaction with Electro-oxidation of Alcohols over Ru Nanoparticles to Reduce the Potential for Water Splitting.
Accelerating Anode Reaction with Electro-oxidation of Alcohols over Ru Nanoparticles to Reduce the Potential for Water Splitting.
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DOI：
10.1021/acsami.1c20511
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发表时间：
2021-12
影响因子：
9.5
通讯作者：
Pei Zhu;Yongli Shen;Linxiu Dai;Qiuyuan Yu;Zhi‐Ming Zhang;Changhua An
中科院分区：
文献类型：
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作者：
Pei Zhu;Yongli Shen;Linxiu Dai;Qiuyuan Yu;Zhi‐Ming Zhang;Changhua An
水电解制氢是生产绿色能源载体的一种有前途和可持续的方法，但阳极析氧反应（OER）动力学缓慢导致工作电位高。用低电位驱动有机物的电氧化代替OER是加速缓慢阳极反应的有效途径，从而增加了水分解过程中的析氢量。在此，我们在n掺杂碳纳米管（Ru-NPs@NCNTs）上制备了Ru纳米颗粒，以实现苯甲醇的电氧化，以降低水分解中的阳极电位。在Ru-NPs催化剂的帮助下，在电流密度为10 mA cm-2的情况下，阳极反应电位从1.76 V vs RHE显著降低到1.19 V vs RHE。同时，有价苯甲醛的选择性为100%，收率为95%。Ru-NPs还表现出良好的耐久性和对其他醇的广泛适用性。Ru- nps的高性能主要归功于苯甲醇与催化剂表面原子的独特水平吸附构型，缩短了•OH基团与Ru原子之间的距离，提高了•OH基团的活化速率。这项工作提出了一种可行的策略，以提高水分解性能，同时在温和的条件下生产增值有机物。
Generating hydrogen by water electrolysis is a promising and sustainable approach to the production of a green energy carrier, but the sluggish kinetics of the oxygen evolution reaction (OER) at anode leads to a high working potential. Replacing OER with electro-oxidation of organics driven at a low potential offers an effective way to accelerate the sluggish anode reaction, and thus increase hydrogen evolution in water-splitting. Herein, we have prepared a Ru nanoparticles on N-doped carbon nanotubes (Ru-NPs@NCNTs) to implement electro-oxidation of benzyl alcohol toward reducing the anodic potential in watersplitting. The potential of the anode reaction is remarkably decreased from 1.76 to 1.19 V vs RHE at a current density of 10 mA cm-2 with the assistance of a Ru-NPs catalyst. Furthermore, 100% selectivity and 95% yield of valuable benzaldehyde were achieved simultaneously. The Ru-NPs also exhibits good durability and wide applicability to other alcohols. The high performance of Ru-NPs is mainly attributed to the unique horizontal adsorption configuration of benzyl alcohol with surface atoms of the catalyst, shortening the distance between the •OH group and Ru atoms, and increasing the activation rate of the •OH group. This work presents a feasible strategy to boost water-splitting performance and concurrently produce value-added organics under mild conditions.