Rhodium metal–rhodium oxide (Rh–Rh2O3) nanostructures with Pt-like or better activity towards hydrogen evolution and oxidation reactions (HER, HOR) in acid and base: correlating its HOR/HER activity with hydrogen binding energy and oxophilicity of the catalyst†,Journal of Materials Chemistry A

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Rhodium metal–rhodium oxide (Rh–Rh2O3) nanostructures with Pt-like or better activity towards hydrogen evolution and oxidation reactions (HER, HOR) in acid and base: correlating its HOR/HER activity with hydrogen binding energy and oxophilicity of the catalyst†
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2018-10-25 00:00:00 , DOI: 10.1039/c8ta07028h
Manas Kumar Kundu _{1,

2,

3,

4,

5} , Ranjit Mishra _{1,

2,

3,

4,

5} , Tanmay Bhowmik _{1,

2,

3,

4,

5} , Sudip Barman _{1,

2,

3,

4,

5}

Affiliation

Design and synthesis of HER/HOR catalysts are of crucial importance for the development of polymer fuel cells and water electrolyzers. We report the synthesis of Rh–Rh₂O₃ nanoparticles/nitrogen-doped carbon composite (Rh–Rh₂O₃-NPs/C) for HER/HOR applications. The HER activity of this catalyst is ∼2.2 times and 1.43 times better than that of commercial Pt/C in base and acid, respectively. Rh–Rh₂O₃-NPs/C exhibited 10 mA cm⁻² current density at an overpotential of 63 mV and 13 mV with Tafel slopes of 70 mV dec⁻¹ and 32 mV dec⁻¹ in base and acid, respectively. The catalyst showed superior HOR activity at all pH values. The exchange current densities were ∼0.425 mA cm_Rh⁻² and ∼0.43 mA cm_Rh⁻² in base and acid, respectively. In base, the HOR and HER activities of Rh–Rh₂O₃-NPs/C are 50-fold and 10-fold higher, respectively, in comparison with those of the Rh₂O₃-free RhNPs/C catalyst, although the HER/HOR activity of both the catalysts is comparable in acid. In base, the adsorption of OH⁻ species (OH_ads) on Rh₂O₃ sites increases the reactivity of hydrogen intermediate (H_abs), which leads to the enhancement of HOR activity of Rh–Rh₂O₃-NPs/C. For HER in base, the adsorptive dissociation of water occurs on the Rh₂O₃ sites to form H_ads on the neighboring Rh sites and then, the recombination of H_ads results in the formation of hydrogen molecules. This study may provide an opportunity to develop an efficient catalyst for hydrogen-based renewable energy technologies.

中文翻译：

铑金属–铑氧化物（Rh–Rh ₂ O ₃）纳米结构，在酸和碱中对氢的释放和氧化反应（HER，HOR）具有类Pt或更好的活性：将其HOR / HER活性与氢的结合能和亲氧性相关催化剂†

HER / HOR催化剂的设计与合成对于聚合物燃料电池和水电解槽的开发至关重要。我们报告了用于HER / HOR应用的Rh–Rh ₂ O ₃纳米颗粒/氮掺杂碳复合材料（Rh–Rh ₂ O ₃ -NPs / C）的合成。该催化剂在碱和酸中的HER活性分别比市售Pt / C的HER活性高约2.2倍和1.43倍。Rh–Rh ₂ O ₃ -NPs / C在63 mV和13 mV的过电势下表现出10 mA cm ^-2的电流密度，Tafel斜率分别为dec m - _1和mm dec ^{-1 -1}和32 mV dec ^-1分别在碱和酸中。该催化剂在所有pH值下均表现出优异的HOR活性。在碱和酸中的交换电流密度分别为〜0.425mA·cm _Rh^-2和〜0.43mA·cm _Rh^-2。在基础上，与不含Rh ₂ O _3的RhNPs / C催化剂相比，Rh–Rh ₂ O ₃ -NPs / C的HOR和HER活性分别高50倍和10倍。两种催化剂的HER / HOR活性在酸中均相当。在基，OH的吸附^-物种（OH_广告上的Rh）₂ ö ₃位点增加氢中间体的反应性（H_abs），导致Rh–Rh₂ O₃ -NPs / C的HOR活性增强。她在碱，水的吸附解离发生在Rh₂ ø₃位点以H型_广告在相邻的Rh位点，然后，H的重组_广告中氢分子的形成的结果。这项研究可能为开发基于氢的可再生能源技术的有效催化剂提供机会。

更新日期：2018-10-25

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