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缺氧氧化钨诱导电子和质子转移:在宽pH值和碱性海水中激活钌位点用于析氢

Oxygen-deficient tungsten oxide inducing electron and proton transfer: Activating ruthenium sites for hydrogen evolution in wide pH and alkaline seawater.

作者信息

Zhou Bowen, Ding Hao, Jin Wei, Zhang Yihe, Wu Zexing, Wang Lei

机构信息

Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences, Xueyuan Road, Haidian District, Beijing 100083, PR China.

School of Environmental Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, PR China.

出版信息

J Colloid Interface Sci. 2024 Apr 15;660:321-333. doi: 10.1016/j.jcis.2024.01.064. Epub 2024 Jan 13.

DOI:10.1016/j.jcis.2024.01.064
PMID:38244499
Abstract

The design of electrocatalysts for the hydrogen evolution reaction (HER) that perform effectively across a broad pH spectrum is paramount. The efficiency of hydrogen evolution at ruthenium (Ru) active sites, often hindered by the kinetics of water dissociation in alkaline or neutral conditions, requires further enhancement. Metal oxides, due to superior electron dynamics facilitated by oxygen vacancies (O) and shifts in the Fermi level, surpass carbon-based materials. In particular, tungsten oxide (WO) promotes the directed migration of electrons and protons which significantly activates the Ru sites. Ru/WO-O is prepared through a simple hydrothermal and low-temperature annealing process. The prepared catalyst achieves 10 mA cm at overpotentials of 23 mV (1 M KOH), 36 mV (0.5 M HSO), 62 mV (1 M PBS), and 38 mV (1 M KOH + seawater). At an overpotential corresponding to 10 mA cm in 1 M KOH and 1 M KOH + seawater, the mass activity of Ru/WO-O is about 7.7 and 7.86 times that of 20 wt% Pt/C. The improvement in activity and stability arises from electronic modifications attributed to metal-support interaction. This work offers novel insights for modulating the HER activity of Ru sites across a wide pH range.

摘要

设计能够在广泛的pH范围内有效进行析氢反应(HER)的电催化剂至关重要。在钌(Ru)活性位点上析氢的效率,在碱性或中性条件下常常受到水离解动力学的阻碍,需要进一步提高。由于氧空位(O)促进了优越的电子动力学以及费米能级的移动,金属氧化物优于碳基材料。特别是,氧化钨(WO)促进电子和质子的定向迁移,从而显著激活Ru位点。通过简单的水热和低温退火工艺制备了Ru/WO-O。所制备的催化剂在23 mV(1 M KOH)、36 mV(0.5 M HSO)、62 mV(1 M PBS)和38 mV(1 M KOH + 海水)的过电位下实现了10 mA cm。在1 M KOH和1 M KOH + 海水中对应于10 mA cm的过电位下,Ru/WO-O的质量活性分别约为20 wt% Pt/C的7.7倍和7.86倍。活性和稳定性的提高源于金属-载体相互作用引起的电子修饰。这项工作为在宽pH范围内调节Ru位点的HER活性提供了新的见解。

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