Confinement Effect of Mesopores: In Situ Synthesis of Cationic Tungsten-Vacancies for a Highly Ordered Mesoporous Tungsten Phosphide Electrocatalyst.,ACS Applied Materials & Interfaces

当前位置： X-MOL 学术 › ACS Appl. Mater. Interfaces › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Confinement Effect of Mesopores: In Situ Synthesis of Cationic Tungsten-Vacancies for a Highly Ordered Mesoporous Tungsten Phosphide Electrocatalyst.
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-05-11 , DOI: 10.1021/acsami.9b22761
Feng Li ₁ , Chengru Wang ₁ , Xiaocang Han ₁ , Xiaoqian Feng ₁ , Yuqi Qu ₁ , Jing Liu ₁ , Wenlong Chen ₁ , Liping Zhao ₁ , Xuefeng Song ₁ , Hong Zhu ₁ , Han Chen ₁ , Min Zhao ₂ , Zhao Deng ₃ , Jianbo Wu _{1,

4} , Peng Zhang ₁ , Lian Gao ₁

Affiliation

Engineering defects in crystalline electrocatalysts is an effective approach to tailor the electronic structure and number of active sites, which are essential for the intrinsic activity of the hydrogen evolution reaction (HER). Unlike previously reported methods, we demonstrate a confinement effect using a mesoporous template for in situ fabrication of cationic W vacancies in as-prepared ordered mesoporous tungsten phosphide (WP) nanostructures by adjusting the nonstoichiometric ratio of the precursor elements. With a plenty of W vacancies and ordered mesoporosity, the as-prepared catalyst WP-Mesop exhibits better catalytic performance than the catalysts without mesopores and/or vacancies. The WP-Mesop shows an ultralow overpotential of 175 mV in acid and 229 mV in alkaline at 100 mA cm-2 and stability of 48 h without structural collapse in both acid and alkaline media. Meanwhile, density functional theory calculations further reveal that the activation barrier for HER can be lowered by introducing cationic W vacancies. This strategy can be extended to generate cationic defects in other transition metal phosphides to improve their HER activities.

中文翻译：

中孔的约束作用：高阶介孔磷化钨电催化剂的阳离子钨空位的原位合成。

晶体电催化剂中的工程缺陷是调整电子结构和活性位点数量的有效方法，这对于析氢反应（HER）的固有活性至关重要。与以前报道的方法不同，我们证明了通过调节前体元素的非化学计量比，在制备的有序介孔磷化钨（WP）纳米结构中使用介孔模板原位制备阳离子W空位的限制效应。制备的催化剂WP-Mesop具有大量W的空位和有序的介孔性，其催化性能比没有介孔和/或空位的催化剂要好。WP-Mesop在100 mA cm-2时显示出在酸中为175 mV和在碱中为229 mV的超低超电势，并且在酸和碱介质中均具有48 h的稳定性而无结构塌陷。同时，密度泛函理论计算进一步揭示，通过引入阳离子W空位可以降低HER的激活势垒。可以扩展该策略以在其他过渡金属磷化物中产生阳离子缺陷，以改善其HER活性。

更新日期：2020-05-01

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南