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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
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
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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
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。
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