Kang Lan, Zhang Yonghao, Dong Lihui, Yin Shibin, Li Bin, Fan Minguang, He Huibing, Chen Zhengjun
Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi Colleges and Universities Key Laboratory of Applied Chemistry Technology and Resource Development, School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, P. R. China.
State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi University, Nanning, 530004, P. R. China.
Small. 2024 Dec;20(50):e2406510. doi: 10.1002/smll.202406510. Epub 2024 Oct 8.
The limited adsorption and activation of CO on catalyst and the high energy barrier for intermediate formation hinder the development of electrochemical CO reduction reactions (CORR). Herein, this work reports a boron (B) doping engineering in AgCd bimetals to alleviate the above limitations for efficient CO electroreduction to CO and aqueous Zn-CO batteries. Specifically, the B-doped AgCd bimetallic catalyst (AgCd-B) is prepared via a simple reduction reaction at room temperature. A combination of in situ experiments and density functional theory (DFT) calculations demonstrates that B-doping simultaneously enhances the adsorption and activation of CO and reduces the binding energy of the intermediates by moderating the electronic structure of bimetals. As a result, the AgCd-B catalyst exhibits a high CO Faraday efficiency (FE) of 99% at -0.8 V versus reversible hydrogen electrode (RHE). Additionally, it maintains a FE over 92% at a wide potential window of 600 mV (-0.6 to -1.1 V versus RHE). Furthermore, the AgCd-B catalyst coupled with the Zn anode to assemble aqueous Zn-CO batteries shows a power density of 20.18 mW cm and a recharge time of 33 h.
一氧化碳在催化剂上的有限吸附和活化以及中间体形成的高能垒阻碍了电化学一氧化碳还原反应(CORR)的发展。在此,这项工作报道了在银镉双金属中进行硼(B)掺杂工程,以缓解上述限制,实现高效的一氧化碳电还原为一氧化碳以及水系锌-一氧化碳电池。具体而言,通过室温下的简单还原反应制备了硼掺杂的银镉双金属催化剂(AgCd-B)。原位实验和密度泛函理论(DFT)计算相结合表明,硼掺杂通过调节双金属的电子结构,同时增强了一氧化碳的吸附和活化,并降低了中间体的结合能。结果,AgCd-B催化剂在相对于可逆氢电极(RHE)为-0.8 V时表现出99%的高一氧化碳法拉第效率(FE)。此外,在600 mV的宽电位窗口(相对于RHE为-0.6至-1.1 V)内,其法拉第效率保持在92%以上。此外,AgCd-B催化剂与锌阳极耦合组装水系锌-一氧化碳电池时,功率密度为20.18 mW cm,充电时间为33小时。