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Mesoporous MoO3–x Material as an Efficient Electrocatalyst for Hydrogen Evolution Reactions
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2016-06-15 , DOI: 10.1002/aenm.201600528
Zhu Luo 1 , Ran Miao 2 , Tran Doan Huan 1 , Islam M. Mosa 2, 3 , Altug S. Poyraz 2 , Wei Zhong 1 , Jacqueline E. Cloud 1 , David A. Kriz 2 , Srinivas Thanneeru 2 , Junkai He 1 , Yashan Zhang 2 , Rampi Ramprasad 1 , Steven L. Suib 1, 2
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2016-06-15 , DOI: 10.1002/aenm.201600528
Zhu Luo 1 , Ran Miao 2 , Tran Doan Huan 1 , Islam M. Mosa 2, 3 , Altug S. Poyraz 2 , Wei Zhong 1 , Jacqueline E. Cloud 1 , David A. Kriz 2 , Srinivas Thanneeru 2 , Junkai He 1 , Yashan Zhang 2 , Rampi Ramprasad 1 , Steven L. Suib 1, 2
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A unique approach for the synthesis of nonstoichiometric, mesoporous molybdenum oxide (MoO3–x) with nanosized crystalline walls by using a soft template (PEO‐b‐PS) synthesis method is introduced. The as‐synthesized mesoporous MoO3–x is very active and stable (durability > 12 h) for the electrochemical hydrogen evolution reaction (HER) under both acidic and alkaline conditions. The intrinsic MoO3 serves as an HER electrocatalyst without the assistance of carbon materials, noble metals, or MoS2 materials. The results from transmission electron microscopy and N2 sorption techniques show that the as‐synthesized mesoporous MoO3–x has large accessible pores (20–40 nm), which are able to facilitate mass transport and charge transfer during HER. In terms of X‐ray diffraction, X‐ray photoelectron spectroscopy, temperature‐programmed oxidation, and diffusive reflectance UV–vis spectroscopy, the mesoporous MoO3–x exhibits mixed oxidation states (Mo5+, Mo6+) and an oxygen‐deficient structure. The as‐synthesized MoO3–x only requires a low overpotential (≈0.14 V) to achieve a 10 mA cm−2 current density in 0.1 m KOH and the Tafel slope is as low as 56 mV dec−1. Density functional theory calculations demonstrate a change of electronic structure and the possible reaction pathway of HER. Oxygen vacancies and mesoporosity serve as key factors for excellent performance.
中文翻译：
介孔MoO3-x材料可作为有效的氢析出反应电催化剂
介绍了一种使用软模板（PEO- b- PS）合成方法合成具有纳米尺寸晶体壁的非化学计量的中孔氧化钼（MoO 3- x）的独特方法。合成的中孔MoO 3 - x在酸性和碱性条件下对于电化学氢释放反应（HER）都非常活跃且稳定（耐用性> 12 h）。固有的MoO 3无需碳材料，贵金属或MoS 2材料即可用作HER电催化剂。透射电子显微镜和N 2吸附技术的结果表明，合成的中孔MoO 3– x具有大的可到达的孔（20–40 nm），能够在HER期间促进质量传输和电荷转移。在X射线衍射，X射线光电子能谱，程序升温氧化法和漫反射紫外可见光谱方面，中孔MoO 3– x表现出混合的氧化态（Mo 5+，Mo 6+）和氧-结构不足。合成后的MoO 3 - x仅需低过电位（≈0.14V）即可在0.1 m KOH中实现10 mA cm -2的电流密度，而Tafel斜率低至dec -1的56 mV。密度泛函理论计算证明了电子结构的变化以及HER可能的反应途径。氧空位和中孔性是获得优异性能的关键因素。
更新日期：2016-06-15
中文翻译：
介孔MoO3-x材料可作为有效的氢析出反应电催化剂
介绍了一种使用软模板（PEO- b- PS）合成方法合成具有纳米尺寸晶体壁的非化学计量的中孔氧化钼（MoO 3- x）的独特方法。合成的中孔MoO 3 - x在酸性和碱性条件下对于电化学氢释放反应（HER）都非常活跃且稳定（耐用性> 12 h）。固有的MoO 3无需碳材料，贵金属或MoS 2材料即可用作HER电催化剂。透射电子显微镜和N 2吸附技术的结果表明，合成的中孔MoO 3– x具有大的可到达的孔（20–40 nm），能够在HER期间促进质量传输和电荷转移。在X射线衍射，X射线光电子能谱，程序升温氧化法和漫反射紫外可见光谱方面，中孔MoO 3– x表现出混合的氧化态（Mo 5+，Mo 6+）和氧-结构不足。合成后的MoO 3 - x仅需低过电位（≈0.14V）即可在0.1 m KOH中实现10 mA cm -2的电流密度，而Tafel斜率低至dec -1的56 mV。密度泛函理论计算证明了电子结构的变化以及HER可能的反应途径。氧空位和中孔性是获得优异性能的关键因素。
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