Ruthenium/nitrogen-doped carbon as an electrocatalyst for efficient hydrogen evolution in alkaline solution
Ruthenium/nitrogen-doped carbon as an electrocatalyst for efficient hydrogen evolution in alkaline solution
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DOI：
10.1039/c7ta08764k
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发表时间：
2017-12
影响因子：
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通讯作者：
Jian Zhang;Pan Liu;Gang Wang;Panpan Zhang;Xiaodong Zhuang;Mingwei Chen;I. Weidinger;Xinliang Feng-Xinli
中科院分区：
文献类型：
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作者：
Jian Zhang;Pan Liu;Gang Wang;Panpan Zhang;Xiaodong Zhuang;Mingwei Chen;I. Weidinger;Xinliang Feng-Xinli
对于所有的电催化剂（甚至Pt），在碱性环境中的析氢反应（HER）的动力学是在酸性溶液中相比，由一个因素的两到三个更缓慢。在这里，我们展示了一种新的钌/氮掺杂的碳（Ru/NC）的泡沫石墨，其中丰富的，单一分散的钌原子螯合到氮掺杂的碳基质的电催化剂的制备。在1 M KOH水溶液中，所得Ru/NC电催化剂表现出优异的电催化HER活性，在10 mA cm-2下具有仅21 mV的极低过电位和在100 mV下高达8 A mgRu-1的优异质量电流密度，这上级于已报道的电催化剂的值（在10 mA cm−2时的过电位>50 mV），甚至是Pt催化剂（在10 mA cm−2时的过电位为1.36 mV）。重要的是，Ru/NC电催化剂的固有翻转频率（TOF）值（每个Ru原子）达到4.55 s-1，这是Pt催化剂的固有翻转频率（TOF）值（1.41 s-1）的3.2倍。电化学分析和结构表征表明，原子分散的Ru是负责出色的HER活性的Ru/NC电催化剂，因为一个大大加速的Volmer步骤。出色的HER性能使Ru/NC电催化剂在实际制氢应用中具有广阔的潜力。
For all electrocatalysts (even Pt), the kinetics of the hydrogen evolution reaction (HER) in alkaline environments are more sluggish by a factor of two to three compared to those in acidic solutions. Here, we demonstrated the preparation of a novel ruthenium/nitrogen-doped carbon (Ru/NC) electrocatalyst supported by graphite foam, in which abundant, singly dispersed Ru atoms were chelated to a nitrogen-doped carbon matrix. In a 1 M KOH aqueous solution, the resultant Ru/NC electrocatalyst exhibited excellent electrocatalytic HER activity with an extremely low overpotential of only 21 mV at 10 mA cm−2 and an excellent mass current density as high as 8 A mgRu−1 at 100 mV, which is superior to the values for reported electrocatalysts (overpotentials of >50 mV at 10 mA cm−2), even Pt catalysts (overpotential of ∼36 mV at 10 mA cm−2). Importantly, the inherent turnover frequency (TOF) value (per Ru atom) of the Ru/NC electrocatalyst reaches 4.55 s−1, which is 3.2 times higher than that of the Pt catalyst (1.41 s−1). Electrochemical analyses and structural characterization revealed that atomically dispersed Ru is responsible for the outstanding HER activity of the Ru/NC electrocatalyst because of a substantially accelerated Volmer step. The outstanding HER performance gives the Ru/NC electrocatalyst promising potential for practical hydrogen production applications.