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Theoretical and Experimental Insight into the Effect of Nitrogen Doping on Hydrogen Evolution Activity of Ni3S2 in Alkaline Medium
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2018-03-15 , DOI: 10.1002/aenm.201703538 Tianyi Kou 1 , Tyler Smart 1, 2 , Bin Yao 1 , Irwin Chen 1 , David Thota 1 , Yuan Ping 1 , Yat Li 1
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2018-03-15 , DOI: 10.1002/aenm.201703538 Tianyi Kou 1 , Tyler Smart 1, 2 , Bin Yao 1 , Irwin Chen 1 , David Thota 1 , Yuan Ping 1 , Yat Li 1
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Nickel sulfide (Ni3S2) is a promising hydrogen evolution reaction (HER) catalyst by virtue of its metallic electrical conductivity and excellent stability in alkaline medium. However, the reported catalytic activities for Ni3S2 are still relatively low. Herein, an effective strategy to boost the H adsorption capability and HER performance of Ni3S2 through nitrogen (N) doping is demonstrated. N‐doped Ni3S2 nanosheets achieve a fairly low overpotential of 155 mV at 10 mA cm−2 and an excellent exchange current density of 0.42 mA cm−2 in 1.0 m KOH electrolyte. The mass activity of 16.9 mA mg−1 and turnover frequency of 2.4 s−1 obtained at 155 mV are significantly higher than the values reported for other Ni3S2‐based HER catalysts, and comparable to the performance of best HER catalysts in alkaline medium. These experimental data together with theoretical analysis suggest that the outstanding catalytic activity of N‐doped Ni3S2 is due to the enriched active sites with favorable H adsorption free energy. The activity in the Ni3S2 is highly correlated with the coordination number of the surface S atoms and the charge depletion of neighbor Ni atoms. These new findings provide important guidance for future experimental design and synthesis of optimal HER catalysts.
中文翻译：
碱性介质中氮掺杂对Ni3S2析氢活性影响的理论和实验研究
硫化镍（Ni 3 S 2）凭借其金属导电性和在碱性介质中的出色稳定性而成为一种很有前途的放氢反应（HER）催化剂。但是，据报道对Ni 3 S 2的催化活性仍然较低。在本文中，展示了通过掺杂氮（N）来提高Ni 3 S 2的H吸附能力和HER性能的有效策略。N掺杂的Ni 3 S 2纳米片在10 mA cm -2时实现了155 mV的相当低的过电势，在1.0 m中具有0.42 mA cm -2的出色交换电流密度KOH电解质。在155 mV下获得的16.9 mA mg -1的质量活度和2.4 s -1的周转频率显着高于其他基于Ni 3 S 2的HER催化剂报道的值，与碱性条件下最佳HER催化剂的性能相当中等的。这些实验数据和理论分析表明，N掺杂的Ni 3 S 2的出色催化活性是由于富集的活性中心具有良好的H吸附自由能。Ni 3 S 2中的活性与表面S原子的配位数和相邻Ni原子的电荷耗竭高度相关。这些新发现为将来的实验设计和最佳HER催化剂的合成提供了重要的指导。
更新日期：2018-03-15
中文翻译：
碱性介质中氮掺杂对Ni3S2析氢活性影响的理论和实验研究
硫化镍（Ni 3 S 2）凭借其金属导电性和在碱性介质中的出色稳定性而成为一种很有前途的放氢反应（HER）催化剂。但是，据报道对Ni 3 S 2的催化活性仍然较低。在本文中，展示了通过掺杂氮（N）来提高Ni 3 S 2的H吸附能力和HER性能的有效策略。N掺杂的Ni 3 S 2纳米片在10 mA cm -2时实现了155 mV的相当低的过电势，在1.0 m中具有0.42 mA cm -2的出色交换电流密度KOH电解质。在155 mV下获得的16.9 mA mg -1的质量活度和2.4 s -1的周转频率显着高于其他基于Ni 3 S 2的HER催化剂报道的值，与碱性条件下最佳HER催化剂的性能相当中等的。这些实验数据和理论分析表明，N掺杂的Ni 3 S 2的出色催化活性是由于富集的活性中心具有良好的H吸附自由能。Ni 3 S 2中的活性与表面S原子的配位数和相邻Ni原子的电荷耗竭高度相关。这些新发现为将来的实验设计和最佳HER催化剂的合成提供了重要的指导。
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