Li Hongdong, Han Yi, Zhao Huan, Qi Wenjing, Zhang Dan, Yu Yaodong, Cai Wenwen, Li Shaoxiang, Lai Jianping, Huang Bolong, Wang Lei
Key Laboratory of Eco-chemical Engineering, Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life Science, Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, 266042, Qingdao, P. R. China.
College of Chemistry, Chongqing Normal University, 401331, Chongqing, P. R. China.
Nat Commun. 2020 Oct 28;11(1):5437. doi: 10.1038/s41467-020-19277-9.
Designing electrocatalysts with high-performance for both reduction and oxidation reactions faces severe challenges. Here, the uniform and ultrasmall (~3.4 nm) high-entropy alloys (HEAs) PtNiFeCoCu nanoparticles are synthesized by a simple low-temperature oil phase strategy at atmospheric pressure. The PtNiFeCoCu/C catalyst exhibits excellent electrocatalytic performance for hydrogen evolution reaction (HER) and methanol oxidation reaction (MOR). The catalyst shows ultrasmall overpotential of 11 mV at the current density of 10 mA cm, excellent activity (10.96 A mg at -0.07 V vs. reversible hydrogen electrode) and stability in the alkaline medium. Furthermore, it is also the efficient catalyst (15.04 A mg) ever reported for MOR in alkaline solution. Periodic DFT calculations confirm the multi-active sites for both HER and MOR on the HEA surface as the key factor for both proton and intermediate transformation. Meanwhile, the construction of HEA surfaces supplies the fast site-to-site electron transfer for both reduction and oxidation processes.
设计同时具有高性能还原和氧化反应的电催化剂面临着严峻挑战。在此，通过简单的常压低温油相策略合成了均匀且超小（约3.4纳米）的高熵合金（HEA）PtNiFeCoCu纳米颗粒。PtNiFeCoCu/C催化剂对析氢反应（HER）和甲醇氧化反应（MOR）表现出优异的电催化性能。该催化剂在10 mA cm的电流密度下显示出11 mV的超小过电位，在碱性介质中具有优异的活性（相对于可逆氢电极在-0.07 V时为10.96 A mg）和稳定性。此外，它也是在碱性溶液中报道过的用于MOR的高效催化剂（15.04 A mg）。周期性密度泛函理论计算证实，HEA表面上HER和MOR的多活性位点是质子和中间体转化的关键因素。同时，HEA表面的构建为还原和氧化过程提供了快速的位点间电子转移。
