Xing Gengyu, Tong Miaomiao, Yu Peng, Wang Lei, Zhang Guangying, Tian Chungui, Fu Honggang
Key Laboratory of Functional Inorganic Materials Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin, 150080, China.
Key Laboratory for Photonic and Electronic Bandgap Materials, Ministry of Education, School of Physics and Electronic Engineering, Harbin Normal University, Harbin, 150025, China.
Angew Chem Int Ed Engl. 2022 Oct 4;61(40):e202211098. doi: 10.1002/anie.202211098. Epub 2022 Sep 5.
The emerging star of single atomic site (SAS) catalyst has been regarded as the most promising Pt-substituted electrocatalyst for oxygen reduction reaction (ORR) in anion-exchange membrane fuel cells (AEMFCs). However, the metal loading in SAS directly affects the whole device performance. Herein, we report a dual nitrogen source coordinated strategy to realize high dense Cu-N SAS with a metal loading of 5.61 wt% supported on 3D N-doped carbon nanotubes/graphene structure wherein simultaneously performs superior ORR activity and stability in alkaline media. When applied in H /O AEMFC, it could reach an open-circuit voltage of 0.90 V and a peak power density of 324 mW cm . Operando synchrotron radiation analyses identify the reconstruction from initial Cu-N to Cu-N /Cu-nanoclusters (NC) and the subsequent Cu-N /Cu-NC under working conditions, which gradually regulate the d-band center of central metal and balance the Gibbs free energy of *OOH and *O intermediates, benefiting to ORR activity.
单原子位点（SAS）催化剂这一新兴明星已被视为阴离子交换膜燃料电池（AEMFC）中用于氧还原反应（ORR）最具前景的铂替代电催化剂。然而，SAS中的金属负载量直接影响整个器件性能。在此，我们报道一种双氮源配位策略，以实现负载于三维氮掺杂碳纳米管/石墨烯结构上、金属负载量为5.61 wt%的高密度Cu-N SAS，其在碱性介质中同时具有优异的ORR活性和稳定性。当应用于氢/氧AEMFC时，它可达到0.90 V的开路电压和324 mW cm 的峰值功率密度。原位同步辐射分析确定了在工作条件下从初始的Cu-N到Cu-N /Cu纳米团簇（NC）以及随后的Cu-N /Cu-NC的重构，这逐渐调节中心金属的d带中心并平衡OOH和O中间体的吉布斯自由能，有利于ORR活性。
