The Role of Active Oxide Species for Electrochemical Water Oxidation on the Surface of 3d‐Metal Phosphides,Advanced Energy Materials

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The Role of Active Oxide Species for Electrochemical Water Oxidation on the Surface of 3d‐Metal Phosphides
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2018-02-12 , DOI: 10.1002/aenm.201703290
Kaili Liu _{1,

2,

3} , Fengmei Wang ₁ , Peng He ₁ , Tofik Ahmed Shifa _{1,

2} , Zhenxing Wang ₁ , Zhongzhou Cheng ₁ , Xueying Zhan ₁ , Jun He _{1,

2}

Affiliation

Transition metal phosphides (TMPs) have recently been utilized as promising electrocatalysts for oxygen evolution reaction (OER) in alkaline media. The metal oxides or hydroxides formed on their surface during the OER process are hypothesized to play an important role. However, their exact role is yet to be elucidated. Here unambiguous justification regarding the active role of oxo(hydroxo) species on O‐Ni₍₁₋_x₎Fe_xP₂ nanosheet with pyrite structure is shown. These O‐Ni₍₁₋_x₎Fe_xP₂ (x = 0.25) nanosheets demonstrate greatly improved OER performance than their corresponding hydroxide and oxide counterparts do. From density function theory (DFT) calculations, it is found that the introduction of iron into the pyrite‐phased NiP₂ alters OER steps occurred on the surface. Notably, the partially oxidized surface of O‐Ni₍₁₋_x₎Fe_xP₂ nanosheets is vital to improve the local environment and accelerate the reaction steps. This study sheds light on the OER mechanism of the 3d TMP electrocatalyst and opens up a way to develop efficient and low‐cost electrocatalysts.

中文翻译：

活性氧化物在3d金属磷酸盐表面电化学水氧化中的作用

过渡金属磷化物（TMP）最近已被用作在碱性介质中用于氧释放反应（OER）的有前途的电催化剂。假设在OER过程中在其表面形成的金属氧化物或氢氧化物起重要作用。但是，它们的确切作用还有待阐明。在此显示了关于氧（氢氧）物种在具有黄铁矿结构的O‐Ni _（1-_x_） Fe _x P ₂纳米片上的积极作用的明确论据。这些O‐Ni _（1-_x_） Fe _x P ₂（x= 0.25）纳米片证明了其相应的氢氧化物和氧化物对应物大大提高了OER性能。根据密度函数理论（DFT）计算，发现将铁引入到黄铁矿相NiP _2中会改变表面上发生的OER阶跃。值得注意的是，O-Ni _（1-_x_） Fe _x P ₂纳米片的部分氧化表面对于改善局部环境和加快反应步骤至关重要。这项研究揭示了3d TMP电催化剂的OER机理，并开辟了开发高效和低成本电催化剂的途径。

更新日期：2018-02-12

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