Zhu Jingting, Cen Yingqian, Ma Haibin, Lian Weiguang, Liu Jidong, Ou Haohui, Ouyang Fangping, Zhang Lifu, Zhang Wenjing
State Key Laboratory of Radio Frequency Heterogeneous Integration, Shenzhen University, Shenzhen 518060, China.
International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, China.
Nanoscale Horiz. 2023 Aug 21;8(9):1273-1281. doi: 10.1039/d3nh00159h.
The electrochemical hydrogen evolution reaction (HER) effectively produces clean, renewable, and sustainable hydrogen; however, the development of efficient electrocatalysts is required to reduce the high energy barrier of the HER. Herein, we report two excellent single-atom (SA)/metal-organic framework (MOF) composite electrocatalysts (Pt-MIL100(Fe) and Pt-MIL101(Cr)) for HER. The obtained Pt-MIL100(Fe) and Pt-MIL101(Cr) electrocatalysts exhibit overpotentials of 60 and 61 mV at 10 mA cm, respectively, which are close to that of commercial Pt/C (38 mV); they exhibit overpotentials of 310 and 288 mV at 200 mA cm, respectively, which are comparable to that of commercial Pt/C (270 mV). Theoretical simulations reveal that Pt SAs modulate the electronic structures of the MOFs, leading to the optimization of the binding strength for H* and significant enhancement of the HER activity. This study describes a novel strategy for preparing desirable HER electrocatalysts based on the synergy between SAs and MIL-series MOFs. Using MIL-series MOFs to support SAs could be valuable for future catalyst design.
电化学析氢反应（HER）能有效产生清洁、可再生且可持续的氢气；然而，需要开发高效的电催化剂来降低HER的高能量势垒。在此，我们报道了两种用于HER的优异单原子（SA）/金属有机框架（MOF）复合电催化剂（Pt-MIL100(Fe)和Pt-MIL101(Cr)）。所制备的Pt-MIL100(Fe)和Pt-MIL101(Cr)电催化剂在10 mA cm时的过电位分别为60和61 mV，接近商业Pt/C（38 mV）的过电位；它们在200 mA cm时的过电位分别为310和288 mV，与商业Pt/C（270 mV）相当。理论模拟表明，Pt单原子调节了MOF的电子结构，导致H*结合强度的优化以及HER活性的显著增强。本研究描述了一种基于SA与MIL系列MOF之间协同作用制备理想HER电催化剂的新策略。使用MIL系列MOF来负载SA对未来的催化剂设计可能具有重要价值。
