Bowen Zhou, Juping Wang, Lingfei Guo, Hongdong Li, Weiping Xiao, Guangrui Xu, Dehong Chen, Caixia Li, Yunmei Du, Hao Ding, Yihe Zhang, Zexing Wu, Lei Wang
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引用次数: 0
摘要
铂(Pt)基化合物是氢进化反应(HER)的基准催化剂,但在碱性环境中表现出缓慢的动力学特性。铂表面积累的 *OH 会阻塞活性位点,影响质子还原和水的再吸附。将钌(Ru)与铂位点合金化可显著调节水解离中间产物的吸附和解吸。选择合适的支持物并利用金属-支持物相互作用(MSI)对活性位点优化至关重要。通过超快微波辅助方法,制备出了锚定在富氧空位(OV)氧化钨(WO3)上的铂钌合金。得益于合金化和 MSI 之间的耦合效应,PtRu/WO3-OV 表现出极高的 HER 活性。在 1 m KOH、1 m KOH + 海水和 0.5 m H2SO4 中,它分别需要 9、26 和 6 mV 的超低过电位才能达到 10 mA cm-2。所设计的催化剂在质量活性方面超过了商用 Pt/C,在间歇式能源集成方面具有相当大的潜力。密度泛函理论显示,将 Ru 与铂位点合金化可显著降低*OH 解离的能量势垒,调节表面的阻塞,进而促进整个碱性 HER 过程。这项研究为快速合成具有铂位点调制功能的非碳支撑催化剂以用于碱性制氢提供了启示。
Microwave-Assisted PtRu Alloying on Defective Tungsten Oxide: A Pathway to Improved Hydroxyl Dynamics for Highly-Efficient Hydrogen Evolution Reaction
Platinum (Pt)-based compounds are the benchmarked catalysts for hydrogen evolution reaction (HER) but exhibit slow kinetics in alkaline environments. The *OH accumulation on Pt surface can block active sites, affecting proton reduction and water re-adsorption. Alloying Ruthenium (Ru) with Pt sites can significantly modulate the adsorption and desorption of water dissociation intermediates. Choosing suitable supports and utilizing metal-support interaction (MSI) is crucial for active site optimization. PtRu alloy anchored on tungsten oxide (WO3) with rich oxygen vacancies (OV) is prepared through an ultrafast microwave-assisted approach. Benefiting from the coupling effects between alloying and MSI, PtRu/WO3-OV exhibits exceptionally high HER activity. In 1 m KOH, 1 m KOH + seawater, and 0.5 m H2SO4, it requires ultralow overpotentials of 9, 26, and 6 mV to achieve 10 mA cm−2, respectively. The designed catalyst surpasses commercial Pt/C in mass activity and demonstrates considerable potential for intermittent energy integration. Density functional theory reveals that alloying Ru with Pt sites significantly reduces the energy barrier of dissociating *OH, modulating blockage on the surface and then promoting the overall alkaline HER process. This study offers insights into the rapid synthesis of non-carbon supported catalysts with Pt site modulation for alkaline hydrogen generation.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.