Sulfur-Modulated Tin Sites Enable Highly Selective Electrochemical Reduction of CO2 to Formate
2017; Elsevier BV; Volume: 1; Issue: 4 Linguagem: Inglês
10.1016/j.joule.2017.09.014
ISSN2542-4785
AutoresXueli Zheng, Phil De Luna, F. Pelayo Garcı́a de Arquer, Bo Zhang, Nigel Becknell, Michael B. Ross, Yifan Li, Mohammad Norouzi Banis, Yuzhang Li, Min Liu, Oleksandr Voznyy, Cao‐Thang Dinh, Tao‐Tao Zhuang, Philipp Stadler, Yi Cui, Xi‐Wen Du, Peidong Yang, Edward H. Sargent,
Tópico(s)Advanced Photocatalysis Techniques
ResumoElectrochemical reduction of carbon dioxide (CO2RR) to formate provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks powered using renewable electricity. Here, we hypothesized that the presence of sulfur atoms in the catalyst surface could promote undercoordinated sites, and thereby improve the electrochemical reduction of CO2 to formate. We explored, using density functional theory, how the incorporation of sulfur into tin may favor formate generation. We used atomic layer deposition of SnSx followed by a reduction process to synthesize sulfur-modulated tin (Sn(S)) catalysts. X-ray absorption near-edge structure (XANES) studies reveal higher oxidation states in Sn(S) compared with that of tin in Sn nanoparticles. Sn(S)/Au accelerates CO2RR at geometric current densities of 55 mA cm−2 at −0.75 V versus reversible hydrogen electrode with a Faradaic efficiency of 93%. Furthermore, Sn(S) catalysts show excellent stability without deactivation (<2% productivity change) following more than 40 hours of operation.
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