Bao Deyu, Huang Linsen, Gao Yingjie, Davey Kenneth, Zheng Yao, Qiao Shi-Zhang
School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia.
J Am Chem Soc. 2024 Dec 18;146(50):34711-34719. doi: 10.1021/jacs.4c13036. Epub 2024 Nov 22.
Electrolysis of natural seawater driven by renewable energy is practically attractive for green hydrogen production. However, because precipitation initiated by an increase in local pH near to the cathode deactivates catalysts or blocks electrolyzer channels, limited catalysts are capable of operating with untreated, natural seawater (., pH 8.2 to 8.3 and . 35 g salts L); most are used in strongly alkaline or acidic seawater. Here, we report a new natural seawater electrolysis cathode with precipitation-suppression via a Pt/WO catalyst to create a dynamically local acid-like environment. The formed hydrogen tungsten bronze (HWO) phase via continuous hydrogen insertion from water acts as a proton reservoir. As a result, dynamically stored protons create a local acid-like environment near the Pt active sites. We evidence that this tailored acid-like environment boosts the hydrogen evolution reaction in natural seawater splitting and neutralizes generated OH species to restrict precipitation formations. Consequently, a long-term stability of >500 h at 100 mA cm was exhibited in direct seawater electrolysis.
由可再生能源驱动的天然海水电解对于绿色制氢具有实际吸引力。然而,由于靠近阴极处局部pH值升高引发的沉淀会使催化剂失活或堵塞电解槽通道,因此只有有限的催化剂能够在未经处理的天然海水中运行(例如,pH值为8.2至8.3且盐含量为35 g/L);大多数催化剂用于强碱性或酸性海水中。在此,我们报道了一种新型的天然海水电解阴极,通过Pt/WO催化剂抑制沉淀,以创建动态局部类酸环境。通过水的持续氢插入形成的氢钨青铜(HWO)相充当质子库。结果,动态存储的质子在Pt活性位点附近创建了局部类酸环境。我们证明,这种定制的类酸环境促进了天然海水分解中的析氢反应,并中和了生成的OH物种以限制沉淀形成。因此,在直接海水电解中,在100 mA/cm²的电流密度下表现出超过500小时的长期稳定性。