Metal-Organic Framework-Derived Three-Dimensional Macropore Nitrogen-Doped Carbon Frameworks Decorated with Ultrafine Ru-Based Nanoparticles for Overall Water Splitting.
Metal-Organic Framework-Derived Three-Dimensional Macropore Nitrogen-Doped Carbon Frameworks Decorated with Ultrafine Ru-Based Nanoparticles for Overall Water Splitting.
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DOI：
10.1021/acs.inorgchem.2c01151
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发表时间：
2022-06
影响因子：
4.6
通讯作者：
Di Li;Xiangli Shi;Shichao Sun;Xinyu Zheng;Daniel Tian;Deli Jiang
中科院分区：
文献类型：
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作者：
Di Li;Xiangli Shi;Shichao Sun;Xinyu Zheng;Daniel Tian;Deli Jiang
氢能以其绿色、可持续、高能量密度等优点被认为是化石燃料能源的替代能源。电解水制氢是一种很有前途的能量转换技术，但受限于过电位大，因此迫切需要高效的电催化剂。在本文中，首先使用Zn中心金属有机骨架（MOF，ZIF-8）作为前体制备包括双Ru/三维（3D）大孔N掺杂碳骨架（Ru/3DMNC）和双RuO 2/3D大孔N掺杂碳骨架（RuO 2/3DMNC）的Ru基电催化剂。超薄3D大孔骨架结构加上N掺杂，使合成的Ru基电催化剂具有丰富的暴露催化活性位点、良好的导电性和优异的电子/质量传输性能，实现了更高的析氢反应（HER）、析氧反应（OER）活性。和总体水分解。Ru/3DMNC和RuO 2/3DMNC呈现50.96和216.74 mV的低过电位，以达到10 mA cm-2的电流密度。此外，由Ru/3DMNC和RuO 2/3DMNC分别作为阴极和阳极催化剂构建的整个水裂解装置仅在1.51 V下提供10 mA cm-2的电流密度，这上级Pt/C|| RuO 2电池（1.573 V）。本工作为以MOFs为前驱体设计和构建高效的骨架结构水裂解电催化剂提供了一种合理的策略。
Hydrogen energy with the advantages of green, sustainability, and high energy density has been considered as an alternative to fossil fuel energy. Water electrolysis to produce hydrogen is a promising energy conversion technology but limited to the large overpotential; thus, a highly efficient electrocatalyst is urgently needed. Herein, Ru-based electrocatalysts including an ultrathin Ru/three-dimensional (3D) macropore N-doped carbon framework (Ru/3DMNC) and ultrathin RuO2/3D macropore N-doped carbon framework (RuO2/3DMNC) are first prepared using a Zn-centered metal-organic framework (MOF, ZIF-8) as the precursor. The ultrathin 3D macropore framework structure together with N doping endows the as-synthesized Ru-based electrocatalysts with abundant exposed catalytic active sites, good electroconductivity, and excellent electron/mass transport, accomplishing improved activities for hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and overall water splitting. The Ru/3DMNC and RuO2/3DMNC present low overpotentials of 50.96 and 216.74 mV to reach a current density of 10 mA cm-2. Moreover, the overall water splitting device constructed by Ru/3DMNC and RuO2/3DMNC as the cathode and anode catalysts, respectively, affords a current density of 10 mA cm-2 only at 1.51 V, which is superior to the Pt/C||RuO2 cell (1.573 V). This work provides a rational strategy to design and construct the efficient framework structure electrocatalysts for water splitting using MOFs as the precursor.