Xu Weiwei, Chen Chongyang, Tang Chao, Li Youyong, Xu Lai
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, 199 Ren'ai Road, Suzhou, Jiangsu, 215123, PR China.
Sci Rep. 2018 Apr 4;8(1):5661. doi: 10.1038/s41598-018-24044-4.
Hydrogen evolution reaction (HER) via the electrocatalytic reduction of water on metal-free catalysts may become a promising method for a sustainable energy supply in the future. However, compared with noble metals or transition metals, the carbon-based metal-free electrocatalysts show poor activity. Here, a novel coplanar metal-free catalyst (CN-CN) was designed for the first time to achieve better efficiency for electron transfer and water reduction. Through the DFT calculations, we discovered that the unique coplanar CN-CN structure can promote the directional transfer of electrons from CN to CN under the drive of built-in electric potential in the π-conjugated plane. To achieve higher performance in HER, the single atom doping by the substitution of boron is carried out. Remarkably, after the boron is doped, the barrier in the Tafel step decreases from 2.35 eV to 0.86 eV. Our results indicate that the novel B-doped coplanar CN-CN structure is a promising metal-free catalyst for HER.
通过在无金属催化剂上对水进行电催化还原实现析氢反应（HER），可能会成为未来可持续能源供应的一种有前景的方法。然而，与贵金属或过渡金属相比，碳基无金属电催化剂表现出较差的活性。在此，首次设计了一种新型共面无金属催化剂（CN-CN），以实现更高的电子转移和水还原效率。通过密度泛函理论（DFT）计算，我们发现独特的共面CN-CN结构能够在π共轭平面内的内建电势驱动下促进电子从CN到CN的定向转移。为了在析氢反应中实现更高的性能，通过硼取代进行单原子掺杂。值得注意的是，硼掺杂后，塔菲尔步骤中的势垒从2.35 eV降至0.86 eV。我们的结果表明，新型硼掺杂共面CN-CN结构是一种有前景的析氢反应无金属催化剂。
