Hu Qi, Li Guomin, Liu Xiufang, Zhu Bin, Chai Xiaoyan, Zhang Qianling, Liu Jianhong, He Chuanxin
College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060, China.
Angew Chem Int Ed Engl. 2019 Mar 22;58(13):4318-4322. doi: 10.1002/anie.201900109. Epub 2019 Feb 20.
Recently, metal-free, heteroatom-doped carbon nanomaterials have emerged as promising electrocatalysts for the oxygen evolution reaction (OER), but their synthesis is a tedious process involving energy-wasting calcination. Molecular electrocatalysts offer attractive catalysts for the OER. Here, phytic acid (PA) was selected to investigate the OER activity of carbons in organic molecules by DFT calculations and experiments. Positively charged carbons on PA were very active towards the OER. The PA molecules were fixed into a porous, conductive hydrogel with a superhydrophilic surface. This outperformed most metal-free electrocatalysts. Besides the active sites on PA, the high OER activity was also related to the porous and conductive networks on the hydrogel, which allowed fast charge and mass transport during the OER. Therefore, this work provides a metal-free, organic-molecule-based electrocatalyst to replace carbon nanomaterials for efficient OER.
最近，无金属、杂原子掺杂的碳纳米材料已成为用于析氧反应（OER）的有前景的电催化剂，但其合成是一个涉及能源浪费的煅烧的繁琐过程。分子电催化剂为OER提供了有吸引力的催化剂。在此，通过密度泛函理论（DFT）计算和实验，选择植酸（PA）来研究有机分子中碳的OER活性。PA上带正电荷的碳对OER非常活跃。PA分子被固定在具有超亲水表面的多孔导电水凝胶中。这优于大多数无金属电催化剂。除了PA上的活性位点外，高OER活性还与水凝胶上的多孔导电网络有关，这使得在OER过程中能够快速进行电荷和质量传输。因此，这项工作提供了一种无金属、基于有机分子的电催化剂，以替代碳纳米材料用于高效的OER。
