Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2023-06-17 , DOI: 10.1016/j.apcatb.2023.123015 Jianpeng Sun , Shiyu Qin , Zisheng Zhang , Chunhu Li , Xiaofeng Xu , Zizhen Li , Xiangchao Meng
Herein, through a rapid Joule heating method, we have successfully prepared well lattice-matched Co2Mo3O8/MoO2 heterointerfaces on Ni foam (Co2Mo3O8/MoO2/NF) in only 130 s. Notably, the rapid Joule heating can effectively avoid oxidation of catalyst caused by prolonged heating and achieve rich uncoordinated Mo4+ sites, which contributed to the enhanced electrocatalytic performance in hydrogen evolution reaction (HER). As-prepared Co2Mo3O8/MoO2 delivered remarkable HER activity (23 mV at 10 mA cm−2), which was comparable to Pt-based electrocatalyst. As-prepared sample also revealed excellent stability at 200-h test in electrocatalytic splitting of alkaline seawater. Of particular note, the solar-driven H2O-H2 electrolyzer also showed a promising solar-to-hydrogen (STH) efficiency of 12.4 %. The cell voltage for the home-made anion exchange membrane (AEM) seawater electrolyzer was only 2.13 V at 200 mA·cm−2 at 50 °C, and only 4.7 kW-h required to produce 1 m3 of H2. DFT calculations revealed that the electron redistribution spontaneously takes place at Co–O–Mo bonds at Co2Mo3O8/MoO2 heterointerfaces, which could regulate the electronic structure and d-band center of Mo sites, and then achieve high-efficiency adsorption of H2O on Mo sites and near-zero hydrogen-adsorption free energy on O sites. This study provided a new strategy to regulate the chemical states via Joule heating for highly efficient seawater splitting to evolve H2.
中文翻译:
焦耳热合成良好晶格匹配的 Co2Mo3O8/MoO2 异质界面,大大改善了碱性海水电解中的析氢反应,STH 效率为 12.4%
在此,通过快速焦耳加热方法,我们仅在130秒内就成功在泡沫镍上制备了晶格匹配良好的Co 2 Mo 3 O 8 /MoO 2异质界面(Co 2 Mo 3 O 8 /MoO 2 /NF)。值得注意的是,快速焦耳加热可以有效避免长时间加热引起的催化剂氧化,并获得丰富的不配位Mo 4+位点,这有助于增强析氢反应(HER)中的电催化性能。所制备的 Co 2 Mo 3 O 8 /MoO 2具有显着的 HER 活性(10 mA cm 时为 23 mV)-2 ),与 Pt 基电催化剂相当。所制备的样品在碱性海水电催化分解的 200 小时测试中也显示出优异的稳定性。特别值得注意的是,太阳能驱动的 H 2 O-H 2电解槽还显示出令人鼓舞的太阳能制氢 (STH) 效率,高达 12.4%。自制的阴离子交换膜(AEM)海水电解槽在50℃、200mA·cm -2条件下的电池电压仅为2.13V,产生1m 3 H 2仅需4.7kW-h 。DFT 计算表明电子重新分布自发地发生在 Co 2 Mo 3 O 8 /MoO 2的 Co-O-Mo 键上异质界面可以调节Mo位点的电子结构和d带中心,从而实现H 2 O在Mo位点上的高效吸附和O位点上氢吸附自由能接近于零的效果。这项研究提供了一种通过焦耳热调节化学态的新策略,以实现高效海水分解以产生 H 2。