Abstract：
Both the catalyst and electrolyte deeply impact the performance of the carbon dioxide reduction reaction (CO2RR). It remains a challenge to design the electrolyte compositions for promoting the CO2RR. Here, typical anionic surfactants, dodecylphosphonic acid (DDPA) and its analogues, are employed as electrolyte additives to tune the catalysis interface where the CO2RR occurs. Surprisingly, the anionic surfactant-tailored interfacial microenvironment enables a set of typical commercial catalysts for the CO2RR to deliver a significantly enhanced selectivity of carbon products in both neutral and acidic electrolytes. Mechanistic studies disclose that the DDPA addition restructures the interfacial hydrogen-bond environment via increasing the weak H-bonded water, thus promoting the CO2 protonation to CO. Specifically, in an H-type cell, the Faradaic efficiency of CO increases from 70 to 98% at -1.0 V versus the reversible hydrogen electrode. Furthermore, in a flow cell, the DDPA-containing electrolyte maintains over 90% FECO from 50-400 mA cm-2. Additionally, this electrolyte modulation strategy can be extended to acidic CO2RR with a pH of 1.5-3.5.
摘要：
催化剂和电解质都会对二氧化碳还原反应（CO2RR）的性能产生深远的影响。设计用于促进CO2RR的电解质组合物仍然是一个挑战。这里,典型的阴离子表面活性剂，十二烷基膦酸（DDPA）及其类似物，用作电解质添加剂以调节发生CO2RR的催化界面。令人惊讶的是,阴离子表面活性剂定制的界面微环境使得用于CO2RR的一组典型的商业催化剂能够在中性和酸性电解质两者中提供显著增强的碳产物选择性。机理研究表明，DDPA的加入通过增加弱H键合水来重构界面氢键环境，从而促进CO2质子化为CO。具体来说,在H型细胞中，与可逆氢电极相比，在-1.0V时，CO的法拉第效率从70％增加到98％。此外，在流动池中，含DDPA的电解质在50-400mAcm-2保持超过90%的FECO。此外,这种电解质调制策略可以扩展到pH为1.5-3.5的酸性CO2RR。
