Wang Songrui, Wang Minmin, Liu Zhi, Liu Shoujie, Chen Yanju, Li Min, Zhang Hui, Wu Qikang, Guo Jiahui, Feng Xueqing, Chen Zheng, Pan Yuan
School of Chemistry and Materials Science, Anhui Normal University, Wuhu 241000, China.
State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, China.
ACS Appl Mater Interfaces. 2022 Apr 6;14(13):15250-15258. doi: 10.1021/acsami.2c00652. Epub 2022 Mar 25.
Hydrogen production by water splitting and seawater electrolysis is a promising alternative to develop clean hydrogen energy. The construction of high-efficiency and durable electrocatalysts for the hydrogen evolution reaction (HER) in a wide pH range and seawater is critical to overcoming the sluggish kinetic process. Herein, we develop an efficient catalytic material composed of a single-atom Ru-N site and Ru nanoparticles anchored on nitrogen-doped carbon (Ru/N-C) through the coordination-pyrolysis strategy of the melamine formaldehyde resin. The Ru/N-C catalyst shows outstanding HER activity with the smallest overpotentials, the lowest Tafel slopes, the highest mass activity and turnover frequency, as well as excellent stability in both acidic and alkaline media. Moreover, Ru/N-C shows comparable hydrogen production performance and a higher faradic efficiency to 20% Pt/C in natural seawater and artificial simulated seawater. Theoretical calculations demonstrate that the strong synergistic effects between the Ru-N site and Ru nanoparticles modify the electronic structure to accelerate the HER kinetics. Ru nanoparticles can effectively realize dissociation of HO to generate adsorbed hydrogen and also promote the single-atom Ru-N site to combine adsorbed hydrogen to H and desorption. This work provides a new perspective for designing high-efficiency hydrogen production electrocatalysts for large-scale seawater electrolysis.
通过水分解和海水电解制氢是开发清洁氢能的一种有前景的替代方法。构建在宽pH范围和海水中用于析氢反应（HER）的高效耐用电催化剂对于克服缓慢的动力学过程至关重要。在此，我们通过三聚氰胺甲醛树脂的配位热解策略开发了一种由单原子Ru-N位点和锚定在氮掺杂碳（Ru/N-C）上的Ru纳米颗粒组成的高效催化材料。Ru/N-C催化剂表现出出色的HER活性，具有最小的过电位、最低的塔菲尔斜率、最高的质量活性和周转频率，以及在酸性和碱性介质中均具有出色的稳定性。此外，Ru/N-C在天然海水和人工模拟海水中显示出与20% Pt/C相当的产氢性能和更高的法拉第效率。理论计算表明，Ru-N位点和Ru纳米颗粒之间的强协同效应改变了电子结构，从而加速了HER动力学。Ru纳米颗粒可以有效地实现HO的解离以产生吸附氢，还促进单原子Ru-N位点将吸附氢结合为H并解吸。这项工作为设计用于大规模海水电解的高效产氢电催化剂提供了新的视角。
