关键词: Ammonia synthesis Heterojunction Interface reconstruction Photocatalysis

来  源:   DOI:10.1016/j.jcis.2024.07.008

Abstract:
Prospective photocatalytic ammonia synthesis process has received more attentions but quite challenging with the low visible light utilization and weak N2 molecule absorption ability around the photocatalysts. Herein, interface reconstruction of MXene-Ti3C2/CeO2 composites with high-concentration active sites through the carbon-doped process are presented firstly, and obvious transition zones with the three-phase reaction interface are formed in the as-prepared catalysts. The optimal co-doped sample demonstrates an excellent photo response in the visible light region, the strongest chemisorption activity and the most active sites. Moreover, much more in-situ extra oxygen defects are also produced under light irradiation. It is expected that the double decorated catalyst shows a remarked ammonia production rate of above 0.76 mmol gcal-1·h-1 under visible-light illumination and a higher apparent quantum efficiency of 1.08 % at 420 nm, which is one of the most completive properties for the photocatalytic N2 fixation at present.
摘要:
有前景的光催化氨合成过程受到了更多的关注,但由于光催化剂周围的可见光利用率低和N2分子吸收能力弱,因此具有挑战性。在这里,首先提出了通过碳掺杂工艺重建具有高浓度活性位点的MXene-Ti3C2/CeO2复合材料的界面,在所制备的催化剂中形成了明显的具有三相反应界面的过渡区。最佳共掺杂样品在可见光区域表现出优异的光响应,最强的化学吸附活性和最活跃的位点。此外,在光照射下也会产生更多的原位额外氧缺陷。预计双重装饰催化剂在可见光照射下显示出高于0.76mmolgcal-1·h-1的显着氨产生速率,并且在420nm处具有1.08%的更高的表观量子效率,这是目前光催化固定N2最完整的性能之一。
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