Negative Electrocatalytic Effects of p-Doping Niobium and Tantalum on MoS2 and WS2 for the Hydrogen Evolution Reaction and Oxygen Reduction Reaction
Negative Electrocatalytic Effects of p-Doping Niobium and Tantalum on MoS2 and WS2 for the Hydrogen Evolution Reaction and Oxygen Reduction Reaction
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DOI：
10.1021/acscatal.6b01593
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发表时间：
2016-09-01
期刊：
影响因子：
12.9
通讯作者：
Pumera, Martin
中科院分区：
文献类型：
--
作者：
Chua, Xing Juan;Luxa, Jan;Pumera, Martin
过渡金属二硫属化合物（TMDs）因其良好的催化性能和独特的材料性能而成为研究的前沿。随着对单层或多层TMD研究的极大兴趣，我们试图从根本上探索掺杂对体TMD的影响，特别是MoS 2和WS 2与p型掺杂剂Nb和Ta的析氢反应（HER）和氧还原反应（ORR）。尽管在HER上掺杂的TMD的计算研究中报告的承诺，我们的结果表明，否则。掺杂的本体TMD与其未掺杂的对应物相比对于HER显示出更低的催化活性。对于ORR催化观察到类似的效果。进行表征以阐明其表面元素组成、性质和形态。发现掺杂的WS 2具有高百分比的IT相，但这与HER在-10 mA cm（-2）下的较低过电位无关，这与普遍的共识相矛盾。因此，我们表明，p型掺杂剂有一个负的电催化效应的HER. These研究结果是非常重要的TMD电化学领域，因为他们挑战了目前的共识，即掺杂总是提高TMD的电催化。
Transition-metal dichalcogenides (TMDs) are at the forefront of research for their promising catalytic abilities and unique materials properties. With great interest in the study of mono- or few-layered TMDs, we seek to fundamentally explore the effects of doping on bulk TMDs, particularly MoS2 and WS2 for the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) with p-dopants Nb and Ta. Despite promises reported in the computational studies of doped TMDs on the HER, our results show otherwise. Doped bulk TMDs display less catalytic activity in comparison to their undoped counterparts for the HER A similar effect is observed for ORR catalysis. Characterization was done to shed light on its surface elemental composition, properties, and morphologies. It was found that doped WS2 has a high percentage of IT phase but this does not correlate with a lower overpotential for the HER at -10 mA cm(-2), which contradicts the general consensus. We therefore show that p-dopants have a negative electrocatalytic effect on the HER. These findings are of high importance for the field of TMD electrochemistry, as they challenge the current consensus that doping always improves the electrocatalysis of TMDs.