Song Yanfang, Junqueira João R C, Sikdar Nivedita, Öhl Denis, Dieckhöfer Stefan, Quast Thomas, Seisel Sabine, Masa Justus, Andronescu Corina, Schuhmann Wolfgang
Analytical Chemistry-Center for Electrochemical Sciences (CES), Faculty of Chemistry and Biochemistry, Ruhr University Bochum, Universitätsstrasse 150, 44780, Bochum, Germany.
CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 99 Haike Road, Shanghai, 201203, P. R. China.
Angew Chem Int Ed Engl. 2021 Apr 12;60(16):9135-9141. doi: 10.1002/anie.202016898. Epub 2021 Mar 10.
Electroreduction of CO to multi-carbon products has attracted considerable attention as it provides an avenue to high-density renewable energy storage. However, the selectivity and stability under high current densities are rarely reported. Herein, B-doped Cu (B-Cu) and B-Cu-Zn gas diffusion electrodes (GDE) were developed for highly selective and stable CO conversion to C products at industrially relevant current densities. The B-Cu GDE exhibited a high Faradaic efficiency of 79 % for C products formation at a current density of -200 mA cm and a potential of -0.45 V vs. RHE. The long-term stability for C formation was substantially improved by incorporating an optimal amount of Zn. Operando Raman spectra confirm the retained Cu species under CO reduction conditions and the lower overpotential for *OCO formation upon incorporation of Zn, which lead to the excellent conversion of CO to C products on B-Cu-Zn GDEs.
将CO电还原为多碳产物作为一种实现高密度可再生能源存储的途径已引起了广泛关注。然而,在高电流密度下的选择性和稳定性却鲜有报道。在此,我们开发了B掺杂的Cu(B-Cu)和B-Cu-Zn气体扩散电极(GDE),用于在与工业相关的电流密度下将CO高选择性且稳定地转化为C产物。B-Cu GDE在电流密度为-200 mA cm且相对于可逆氢电极(RHE)的电位为-0.45 V时,对C产物形成表现出79%的高法拉第效率。通过加入适量的Zn,C形成的长期稳定性得到了显著提高。原位拉曼光谱证实了在CO还原条件下保留的Cu物种,以及加入Zn后*OCO形成的过电位降低,这导致了B-Cu-Zn GDEs上CO向C产物的优异转化。