Molten Electrolyte-Modulated Electrosynthesis of Multi-Anion Mo-Based Lamellar Nanohybrids Derived from Natural Minerals for Boosting Hydrogen Evolution,ACS Applied Materials & Interfaces

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Molten Electrolyte-Modulated Electrosynthesis of Multi-Anion Mo-Based Lamellar Nanohybrids Derived from Natural Minerals for Boosting Hydrogen Evolution
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-12-15 , DOI: 10.1021/acsami.0c17137
Rui Jiang ₁ , Bowen Deng ₁ , Liu Pi ₁ , Liangyou Hu ₁ , Di Chen ₁ , Yanpeng Dou ₁ , Xuhui Mao ₁ , Dihua Wang ₁

Affiliation

The multi-anion molybdenum-based nanohybrids, N-doped β-Mo₂C/MoP/MoO_x (denoted as MoCPO), serving as a highly efficient catalyst for hydrogen evolution reaction (HER), are fabricated via a simple and scalable electrosynthesis in molten NaCl–KCl, which integrates pyrolysis/electroreduction/compounding into a one-pot strategy using polyphosphazenes (PPAs) and earth-abundant molybdenite (mainly MoS₂) as precursors. The deliberately selected PPA and molten electrolyte ensure the unique lamellar nanostructures and the blending of multiple anions of C, N, P, and O in the obtained catalyst, specifically, triggering the in situ formation of the structural oxygen vacancies (V_O) in MoCPO. The nature of the hybrids can be regulated by adjusting the synthesis condition. The optimized hybrid displays a low overpotential of 99.2 mV at 10 mA cm^–2 for HER in 0.5 M H₂SO₄ and stays active over a broad pH range. The theoretical calculations reveal that V_O in the hybrids serves as favorable active sites, thus contributing to the superior HER activity. Moreover, MoCPO is also effective for overall water splitting as a bifunctional catalyst.

中文翻译：

天然矿物衍生的多阴离子钼基层状纳米杂化物的熔融电解质调制电合成，以促进氢的释放

多阴离子钼系纳米复合物，N掺杂β-沫₂ C / MOP /的MoO _X（表示为MoCPO），用作析氢反应高效率的催化剂（HER），通过一个简单的，可扩展的电合成制造在熔融的NaCl–KCl中，它使用聚磷腈（PPAs）和富含地球的辉钼矿（主要为MoS ₂）为前体，将热解/电还原/化合物整合为一锅法。精心选择的PPA和熔融电解质可确保独特的层状纳米结构以及所获得的催化剂中C，N，P和O的多个阴离子的掺混，特别是触发了结构氧空位（V _O的原位形成））。杂种的性质可以通过调节合成条件来调节。经过优化的混合动力电池在0.5 MH ₂ SO _4中的HER电流为10 mA cm ^–2时显示99.2 mV的低过电势，并在宽pH范围内保持活性。理论计算表明，杂种中的V _O可以作为有利的活性位点，从而促进其优异的HER活性。此外，MoCPO作为双功能催化剂对整体水分解也有效。

更新日期：2020-12-30

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