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Interaction Mediator Assisted Synthesis of Mesoporous Molybdenum Carbide: Mo-Valence State Adjustment for Optimizing Hydrogen Evolution.
ACS Nano ( IF 15.8 ) Pub Date : 2020-03-18 , DOI: 10.1021/acsnano.0c01285
Seongbeen Kim 1, 2 , Changhyeok Choi 2 , Jongkook Hwang 2, 3 , Jinkyu Park 2 , Jooyoung Jeong 1, 2 , Hyunwoo Jun 2 , Seonggyu Lee 1, 2 , Soo-Kil Kim 4 , Jong Hyun Jang 5 , Yousung Jung 2 , Jinwoo Lee 2
Affiliation  

To overcome inherent limitations of molybdenum carbide (MoxC) for hydrogen evolution reaction (HER), i.e., low density of active site and nonideal hydrogen binding strength, we report the synthesis of valence-controlled mesoporous MoxC as a highly efficient HER electrocatalyst. The synthesis procedure uses an interaction mediator (IM), which significantly increases the density of active site by mediating interaction between PEO-b-PS template and Mo source. The valence state of Mo is tuned by systematic control of the environment around Mo by controlled heat treatment under air before thermal treatment at 1100 °C. Theoretical calculations reveal that the hydrogen binding is strongly influenced by Mo valence. Consequently, MoxC achieves a significant increase in HER activity (exceeding that of Pt/C at high current density ∼35 mA/cm2 in alkaline solution). In addition, a volcano-type correlation between HER activity and Mo valence is identified with various experimental indicators. The present strategies can be applied to various carbide and Mo-based catalysts, and the established Mo valence and HER relations can guide development of highly active HER electrocatalysts.

中文翻译:

相互作用介体辅助的介孔碳化钼的合成:用于优化氢释放的钼价态调节。

为了克服碳化钼(MoxC)对于氢释放反应(HER)的固有局限性,即低的活性位点密度和非理想的氢键结合强度,我们报道了价态控制的介孔MoxC的合成,作为一种高效的HER电催化剂。合成过程使用相互作用介体(IM),该介体通过介导PEO-b-PS模板与Mo源之间的相互作用来显着增加活性位点的密度。在1100°C热处理之前,通过在空气中进行受控热处理,可以系统地控制Mo周围的环境,从而调节Mo的价态。理论计算表明,氢键受钼价的强烈影响。所以,MoxC的HER活性显着提高(在碱性溶液中,高电流密度〜35 mA / cm2时,超过了Pt / C的活性)。此外,还通过各种实验指标确定了HER活性与Mo价之间的火山类型相关性。本发明的策略可以应用于各种碳化物和基于Mo的催化剂,并且已建立的Mo价和HER关系可以指导高活性HER电催化剂的开发。
更新日期:2020-03-18
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