Zhang Mou, Su Mengfei, Zhang Chunyan, Gao Feng, Lu Qingyi
State Key Laboratory of Coordination Chemistry, Coordination Chemistry Institute, Collaborative Innovation Center of Advanced Microstructures, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.
Jiangsu Key Laboratory of Artificial Functional Materials, Department of Materials Science and Engineering, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing 210023, China.
Molecules. 2024 Sep 26;29(19):4570. doi: 10.3390/molecules29194570.
Platinum (Pt)-based materials are among the most competitive electrocatalysts for the hydrogen evolution reaction (HER) due to suitable hydrogen adsorption energy. Due to the rarity of Pt, it is desirable to develop cost-effective Pt-based electrocatalysts with low Pt loading. Herein, Pt/PtS electrocatalysts on S-doped carbon nanofilms (PPS/C) have been successfully fabricated through a precursor reduction route with a complex of Pt and 1-dodecanethiol (1-DDT) as the precursor. The PPS/C achieved at 400 °C (PPS/C-400) exhibits excellent HER performances with an ultralow overpotential of 41.3 mV, a low Tafel slope of 43.1 mV dec at a current density of 10 mA cm, and a long-term stability of 10 h, superior to many recently reported Pt-based HER electrocatalysts. More importantly, PPS/C-400 shows a high mass-specific activity of 0.362 A mg at 30 mV, which is 1.88 times of that of commercial 20% Pt/C (0.193 A mg). The introduction of sulfur leads to the formation of PtS, which not only reduces the content of Pt but also realizes the interface regulation of Pt/PtS, as well as the doping of carbon. Both regulations make the resulting catalyst have abundant active centers and rapid electron transfer/transport, which is conducive to balancing the adsorption and resolution of intermediate products, and finally achieving great mass-specific activity and stability. The research work may provide ideas for designing effective Pt-based multi-interface electrocatalysts.
基于铂（Pt）的材料因其合适的氢吸附能，是析氢反应（HER）中最具竞争力的电催化剂之一。由于Pt的稀有性，开发低Pt负载量的具有成本效益的Pt基电催化剂是很有必要的。在此，通过以Pt与1-十二烷硫醇（1-DDT）的络合物为前驱体的前驱体还原路线，成功制备了S掺杂碳纳米薄膜上的Pt/PtS电催化剂（PPS/C）。在400℃下制备的PPS/C（PPS/C-400）表现出优异的HER性能，在10 mA cm的电流密度下，过电位超低，为41.3 mV，塔菲尔斜率低至43.1 mV dec，长期稳定性达10 h，优于许多最近报道的基于Pt的HER电催化剂。更重要的是，PPS/C-400在30 mV时显示出0.362 A mg的高质量比活性，是商业20% Pt/C（0.193 A mg）的1.88倍。硫的引入导致形成PtS，这不仅降低了Pt的含量，还实现了Pt/PtS的界面调控以及碳的掺杂。这两种调控使得所得催化剂具有丰富的活性中心和快速的电子转移/传输，有利于平衡中间产物的吸附和解析，最终实现了高的质量比活性和稳定性。该研究工作可为设计有效的基于Pt的多界面电催化剂提供思路。
