Wang Xin,Miao Ming,Tang Bowen,Duan Haotian,Zhu Fulong,Zhang Huigang,Zhang Xian,Yin Wen-jin,Fu Yongzhu
Electrochemical conversion of CO 2 (CO 2 RR) into high-value fuel is identified as one of the promising approaches to achieve carbon neutrality. The synthesis of high-efficiency CO 2 reduction electrocatalysts with high C 2 :C 1 , selectivity remains a field of intense interest. Previous studies have shown that the presence of Cu(I) is beneficial for the reduction of CO 2 into C 2 products. However, the stable presence of Cu(I) remains controversial, especially in the negative potential window. Here we report a simple and easily scalable catalyst precursor Cu 2 (OH) 3 Cl/C, which automatically forms in-situ chlorine-doped Cu/Cu 2 O heterointerface during electrocatalysis. The catalyst not only exhibits a Faradaic efficiency of 33.03% but also provides a long-term stability of Cu + , gaining a stable electrolysis of 11 h, with an ethylene/methane ratio over 50. The experimental results and mechanistic studies confirm that the presence of Cl − inhibits the reduction of Cu + , inducing the formation of Cu 0 /Cu + , and reduces the reaction energy of the intermediate ⋆CO dimerization, thereby facilitating the formation of C 2 products. This work provides a feasible way to synthesize copper ions with long-term and stable positive charge in CO 2 RR and expands a new way to synthesize ethylene industrial products in the future.
Hydrogen generation through seawater electrolysis provides a promising, attractive pathway towards the utilization of sustainable energy. However, the catalytic activity and stability of oxygen evolution anode are severely limited by the chloride-induced corrosion and competitive oxidation reactions. In this work, we demonstrate an anion-assisted performance improvement strategy by quick and universal screening of electrolyte additive via correlating Cl − repellency with the anionic properties. Particularly, the addition of phosphate ions is found to enable highly stable alkaline seawater splitting at industry-level current density (0.5 A cm −2 ) over 500 h using transition metal hydroxides as anodic electrocatalysts. In situ experiments and theoretical simulations further reveal that the dynamic anti-corrosion behaviors of surface-adsorbed phosphate ions are attributed to three factors including repelling Cl − ions without significantly blocking OH − diffusion, preventing transition metal dissolution and acting as a local pH buffer to compensate the fast OH − consumption under high current electrolysis.
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