Bulk layered heterojunction as an efficient electrocatalyst for hydrogen evolution.
Bulk layered heterojunction as an efficient electrocatalyst for hydrogen evolution.
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DOI：
10.1126/sciadv.1602215
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发表时间：
2017-03
期刊：
影响因子：
13.6
通讯作者：
Shin H
中科院分区：
文献类型：
--
作者：
Bae C;Ho TA;Kim H;Lee S;Lim S;Kim M;Yoo H;Montero-Moreno JM;Park JH;Shin H
一种具有大块层状异质结的复合硫系化合物具有良好的催化产氢活性。我们描述了由分散在体中的二维（2D）材料组成的硫族化合物复合材料的自发形成及其在析氢反应（HERs）中应用的不同寻常的电荷输运性质。当以MoS2为代表的二维材料以受控的方式沉积在过渡金属（如Cu）上时，金属也会发生硫化反应。这一过程产生了非常独特的结构，即Cu-Mo-S的大块层状异质结（BLHJs），其内部含有MoS2薄片，均匀地分散在Cu2S基体中。所得到的结构有望通过层状框架诱导不对称电荷转移，并作为HERs的电催化剂进行了测试。经过适当的热处理，与可逆氢电极相比，BLHJ表面在−0.1 V电位下表现出约10 mA/cm2的高效HER性能。塔菲尔斜率约为每十年30至40毫伏。通过证明BLHJs在其他过渡金属（如Ni）上的形成，进一步推广了目前的策略。所制备的Ni-Mo-S BLHJs也表现出了卓越的HER性能，并且在不使用Pt对电极的情况下稳定运行了10天以上，消除了任何可能的Pt污染问题。
A composite chalcogenide with bulk layered heterojunctions exhibits an excellent catalytic activity for hydrogen production. We describe the spontaneous formation of composite chalcogenide materials that consist of two-dimensional (2D) materials dispersed in bulk and their unusual charge transport properties for application in hydrogen evolution reactions (HERs). When MoS2 as a representative 2D material is deposited on transition metals (such as Cu) in a controlled manner, the sulfidation reactions also occur with the metal. This process results in remarkably unique structures, that is, bulk layered heterojunctions (BLHJs) of Cu–Mo–S that contain MoS2 flakes inside, which are uniformly dispersed in the Cu2S matrix. The resulting structures were expected to induce asymmetric charge transfer via layered frameworks and tested as electrocatalysts for HERs. Upon suitable thermal treatments, the BLHJ surfaces exhibited the efficient HER performance of approximately 10 mA/cm2 at a potential of −0.1 V versus a reversible hydrogen electrode. The Tafel slope was approximately 30 to 40 mV per decade. The present strategy was further generalized by demonstrating the formation of BLHJs on other transition metals, such as Ni. The resulting BLHJs of Ni–Mo–S also showed the remarkable HER performance and the stable operation over 10 days without using Pt counter electrodes by eliminating any possible issues on the Pt contamination.