Confining Nickel Nanoparticles in Hierarchical Nitrogen-Doped Carbon Nanocages for Efficient Electrochemical CO 2 Reduction to CO

作者：Ruonan Cui, Biao Feng, Tao Sun, Fengfei Xu, Jiao Liu, Zi‐Xuan Sun, Changkai Zhou, Yao Yu, Lijun Yang, Xizhang Wang, Hsien‐Yi Hsu, Qiang Wu, Zheng Hu · 发表于：The Journal of Physical Chemistry Letters · 年份：2025 · DOI：10.1021/acs.jpclett.5c00842 · 被引用次数：6 · 研究领域：CO2 Reduction Techniques and Catalysts、Advanced Thermoelectric Materials and Devices、Advanced battery technologies research

Electrochemical CO 2 reduction (CO 2 RR) represents an attractive strategy for achieving carbon neutrality. Nevertheless, developing efficient and inexpensive catalysts is still challenging. Herein, we report a yolk–shell catalyst consisting of Ni nanoparticles (NPs) confined in hierarchical nitrogen-doped carbon nanocages (Ni@hNCNC) for efficient CO 2 RR, which demonstrates high CO faradaic efficiency of 98% and impressive CO partial current density of 195 mA cm –2 at −1.4 V (versus reversible hydrogen electrode) in neutral electrolyte and 352 mA cm –2 at −1.1 V in alkaline electrolyte, outperforming the counterparts of Ni NPs supported on the outer surface of hNCNC (Ni/hNCNC) and confined in undoped hierarchical carbon nanocages. The combined experimental and theoretical studies reveal that the main active sites are the pyridinic N and Ni atoms at the interfaces of the Ni–hNCNC composite. The exceptional performance of Ni@hNCNC is attributed to the electronic interaction between N dopants and Ni NPs, the efficiently exposed interfacial active sites, as well as the confinement of hNCNC to keep a stable structure during CO 2 RR. This study provides an efficient route to enhance the electrocatalytic CO 2 -to-CO performance in neutral solution by confining a low-cost Ni catalyst in N-doped carbon nanocages.