Zhang Huaiwei, Bao Liang, Pan Ying, Du Jia, Wang Wei
College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, PR China.
College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, PR China.
J Colloid Interface Sci. 2024 Dec;675:130-138. doi: 10.1016/j.jcis.2024.07.008. Epub 2024 Jul 3.
Prospective photocatalytic ammonia synthesis process has received more attentions but quite challenging with the low visible light utilization and weak N molecule absorption ability around the photocatalysts. Herein, interface reconstruction of MXene-TiC/CeO 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 g·h 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 N fixation at present.
前瞻性光催化氨合成工艺受到了更多关注，但由于光催化剂周围可见光利用率低和对N分子吸收能力弱，该工艺颇具挑战性。在此，首次提出通过碳掺杂过程对具有高浓度活性位点的MXene-TiC/CeO复合材料进行界面重构，在制备的催化剂中形成了具有三相反应界面的明显过渡区。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多的活性位点。此外，在光照下还会产生更多的原位额外氧缺陷。预计这种双修饰催化剂在可见光照射下的产氨率显著高于0.76 mmol g·h，在420 nm处的表观量子效率更高，为1.08%，这是目前光催化固氮最具竞争力的性能之一。
