Platinum Nanostructure/Nitrogen‐Doped Carbon Hybrid: Enhancing its Base Media HER/HOR Activity through Bi‐functionality of the Catalyst,ChemSusChem

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Platinum Nanostructure/Nitrogen‐Doped Carbon Hybrid: Enhancing its Base Media HER/HOR Activity through Bi‐functionality of the Catalyst
ChemSusChem ( IF 7.5 ) Pub Date : 2018-07-04 , DOI: 10.1002/cssc.201800856
Manas Kumar Kundu ₁ , Tanmay Bhowmik ₁ , Ranjit Mishra ₁ , Sudip Barman ₁

Affiliation

The design and synthesis of an active catalyst for the hydrogen evolution reaction/hydrogen oxidation reaction (HER/HOR) are important for the development of hydrogen‐based renewable technologies. The synthesis of a hybrid of platinum nanostructures and nitrogen‐doped carbon [Pt‐(PtO_x)‐NSs/C] for HER/HOR applications is reported herein. The HER activity of this Pt‐(PtO_x)‐NSs/C catalyst is 4 and 6.5 times better than that of commercial Pt/C in acids and bases, respectively. The catalyst exhibits a current density of 10 mA cm⁻² at overpotentials of 5 and 51 mV, with Tafel slopes of 29 and 64 mV dec⁻¹ in 0.5 m H₂SO₄ and 0.5 m KOH. This catalyst also showed superior HOR activity at all pH values. The HER/HOR activity of Pt‐(PtO_x)‐NSs/C and PtO_x‐free Pt‐nanostructures on carbon (PtNSs/C) catalysts are comparable in acid. The presence of PtO_x in Pt‐(PtO_x)‐NSs/C makes this Pt catalyst more HER/HOR‐active in basic media. The activity of the Pt‐(PtO_x)‐NSs/C catalyst is fivefold higher than that of the PtNSs/C catalyst in basic medium, although their activity is comparable in acid. The hydrogen‐binding energy and oxophilicity are two equivalent descriptors for HER/HOR in basic media. A bifunctional mechanism for the enhanced alkaline HER/HOR activity of the Pt‐(PtO_x)‐NSs/C catalyst is proposed. In the bifunctional Pt‐(PtO_x)‐NSs/C catalyst, PtO_x provides an active site for OH⁻ adsorption to form OH_ads, which reacts with hydrogen intermediate (H_ads), present at neighbouring Pt sites to form H₂O; this leads to enhancement of the HOR activity in basic medium. This work may provide an opportunity to develop catalysts for various renewable‐energy technologies.

中文翻译：

铂纳米结构/氮掺杂碳杂化物：通过催化剂的双功能增强其基础介质的HER / HOR活性

用于氢释放反应/氢氧化反应（HER / HOR）的活性催化剂的设计和合成对于氢基可再生技术的发展很重要。本文报道了用于HER / HOR应用的铂纳米结构和氮掺杂碳[Pt-（PtO _x）-NSs / C]杂化物的合成。这种Pt-（PtO _x）-NSs / C催化剂的HER活性分别比市售Pt / C在酸和碱中的活性高4倍和6.5倍。催化剂在5和51 mV的超电势下显示10 mA cm ^-2的电流密度，在0.5 m H ₂ SO ₄和0.5 m的Tafel斜率分别为29和64 mV dec ^-1KOH。该催化剂在所有pH值下均表现出优异的HOR活性。Pt-（PtO _x）-NSs / C和无PtO _x的碳纳米结构（PtNSs / C）的HER / HOR活性在酸中具有可比性。Pt-（PtO _x）-NSs / C中PtO _x的存在使该Pt催化剂在碱性介质中更具HER / HOR-活性。在碱性介质中，Pt-（PtO _x）-NSs / C催化剂的活性是PtNSs / C催化剂的活性的五倍，尽管它们的活性在酸中是可比的。氢结合能和亲氧性是基本介质中HER / HOR的两个等同描述词。双功能机制增强了Pt-（PtO _x的碱性HER / HOR活性）建议使用NSs / C催化剂。在双官能铂- （PTO _X）-NSs / C催化剂，PtO的_X为OH提供活性位点^-吸附以形成OH_广告，其中发生反应用氢气中间体（H_广告），存在于相邻的Pt位点以生成H ₂ ö ; 这导致基础培养基中HOR活性的增强。这项工作可能会为开发各种可再生能源技术的催化剂提供机会。

更新日期：2018-07-04

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