Strain induced rich planar defects in heterogeneous WS2/WO2 enable efficient nitrogen fixation at low overpotential,Journal of Materials Chemistry A

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Strain induced rich planar defects in heterogeneous WS2/WO2 enable efficient nitrogen fixation at low overpotential
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-04-29 , DOI: 10.1039/c9ta13812a
Ying Ling _{1,

2,

3,

4,

5} , Farhad M. D. Kazim _{1,

2,

3,

4,

5} , Shuangxiu Ma _{1,

2,

3,

4,

5} , Quan Zhang _{1,

2,

3,

4,

5} , Konggang Qu _{5,

6,

7,

8} , Yangang Wang _{5,

9,

10,

11} , Shenglin Xiao _{1,

2,

3,

4,

5} , Weiwei Cai _{1,

2,

3,

4,

5} , Zehui Yang _{1,

2,

3,

4,

5}

Affiliation

Suppression of the competitive hydrogen evolution reaction (HER) and creation of new active sites have been considered to be the most effective methodology to design efficient electrocatalysts for the nitrogen reduction reaction (NRR). Here, we report a heterogeneous WS₂/WO₂ electrocatalyst with abundant planar defects at the heterointerface ascribed to the strain effect induced by the mismatched lattice spacing between WS₂ and WO₂, which enables efficient electrocatalysis toward the NRR with a faradaic efficiency of 13.5% and an NH₃ yield rate of 8.53 μg_NH₃ h⁻¹ mg_cat.⁻¹ at −0.1 V vs. RHE in acidic medium compared to bare WS₂ with a faradaic efficiency of 7.87% and an NH₃ yield rate of 6.99 μg_NH₃ h⁻¹ mg_cat.⁻¹. The superior NRR electrocatalytic activity of heterostructured WS₂/WO₂ is attributed to the introduction of WO₂ effectively impeding the HER catalysis because of the blocking of edge defects in WS₂ and simultaneously creating planar defects at the WS₂/WO₂ heterointerface as active sites for stable NRR catalysis. The extraordinary NRR electrocatalytic activity of WS₂/WO₂ is further confirmed by NMR measurements and density functional theory (DFT) calculations demanding comparably lower uphill free energy for the rate-determining step of NRR catalysis, i.e. formation of NNH species. This work offers useful information for constructing efficient NRR electrocatalysts.

中文翻译：

异质WS2 / WO2中应变诱导的丰富平面缺陷使低过电势下的固氮效率更高

抑制竞争性氢释放反应（HER）和创建新的活性位点被认为是设计用于氮还原反应（NRR）的高效电催化剂的最有效方法。在此，我们报道了一种异质WS ₂ / WO ₂电催化剂，该异质WS ₂ / WO ₂电催化剂在异质界面处具有大量平面缺陷，这归因于WS ₂和WO ₂之间晶格间距失配引起的应变效应，从而能够以13.5的法拉第效率对NRR进行有效的电催化。％和NH ₃ 8.53微克的产率_{NH ₃} ħ ^-1毫克_猫。^-1在-0.1 V下vs.RHE在酸性介质相比裸WS ₂用的7.87％一法拉第效率和NH ₃ 6.99微克的产率_{NH ₃} ħ ^-1毫克_猫。^-1。异质结构的优异NRR电催化活性WS ₂ / WO ₂归因于引入的WO ₂有效地阻碍HER催化作用因为在WS边缘缺陷的阻挡₂和同时产生的WS面缺陷₂ / WO ₂异质界面作为活性稳定的NRR催化位点。WS ₂ / WO具有非凡的NRR电催化活性通过NMR测量和密度泛函理论（DFT）计算进一步证实了图₂，这对于NRR催化的速率确定步骤（即NNH物种的形成）要求相对较低的上坡自由能。这项工作为构建有效的NRR电催化剂提供了有用的信息。

更新日期：2020-07-07

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