Li Xiao, Wu Xingqiao, Li Junjie, Huang Jingbo, Ji Liang, Leng Zihan, Qian Ningkang, Yang Deren, Zhang Hui
State Key Laboratory of Silicon Materials and School of Materials Science and Engineering, Zhejiang University, Hangzhou, Zhejiang 310027, People's Republic of China.
Institute of Advanced Semiconductors, Hangzhou Innovation Center, Zhejiang University, Hangzhou, Zhejiang 310027, People's Republic of China.
Nanoscale. 2021 Dec 2;13(46):19610-19616. doi: 10.1039/d1nr06038d.
Electrocatalytic CO reduction to formate is considered as a perfect route for efficient conversion of the greenhouse gas CO to value-added chemicals. However, it still remains a huge challenge to design a catalyst with both high catalytic activity and selectivity for target products. Here we report a unique Sn-doped BiO nanosheet (NS) electrocatalyst with different atomic percentages of Sn (1.2, 2.5, and 3.8%) prepared by a simple solvothermal method for highly efficient electrochemical reduction of CO to formate. Of them, the 2.5% Sn-doped BiO NSs exhibited the highest faradaic efficiency (FE) of 93.4% with a current density of 24.3 mA cm for formate at -0.97 V in the H-cell and a maximum current density of nearly 50 mA cm was achieved at -1.27 V. The formate FE is stable maintained at over 90% in a wide potential range from -0.87 V to -1.17 V. Electrochemical and density functional theory (DFT) analyses of undoped and Sn doped BiO NSs indicated that the strong synergistic effect between Sn and Bi is responsible for the enhancement in the adsorption capacity of the OCHO* intermediate, and thus the activity for formate production. In addition, we coupled 2.5% Sn-doped BiO NSs with a dimensionally stable anode (DSA) to realize battery-driven highly active CORR and OER with decent activity and efficiency.
电催化将CO还原为甲酸盐被认为是将温室气体CO高效转化为增值化学品的理想途径。然而,设计一种对目标产物具有高催化活性和选择性的催化剂仍然是一个巨大的挑战。在此,我们报道了一种独特的Sn掺杂BiO纳米片(NS)电催化剂,通过简单的溶剂热法制备,其中Sn的原子百分比不同(1.2%、2.5%和3.8%),用于将CO高效电化学还原为甲酸盐。其中,2.5% Sn掺杂的BiO NSs在H型电池中于-0.97 V时对甲酸盐表现出最高的法拉第效率(FE)为93.4%,电流密度为24.3 mA cm ,在-1.27 V时实现了近50 mA cm 的最大电流密度。在-0.87 V至-1.17 V的宽电位范围内,甲酸盐FE稳定保持在90%以上。对未掺杂和Sn掺杂的BiO NSs进行的电化学和密度泛函理论(DFT)分析表明,Sn和Bi之间的强协同效应导致OCHO*中间体吸附能力增强,从而提高了甲酸盐生成活性。此外,我们将2.5% Sn掺杂的BiO NSs与尺寸稳定阳极(DSA)耦合,以实现电池驱动的高活性CO还原反应(CORR)和析氧反应(OER),具有良好的活性和效率。