Ding Lan, Tang Yaoyao, Wang Siyang, Zhang Yuqi, Chen Xinyi, Zhou Hongjun
State Key Laboratory of Heavy Oil Processing Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum-Beijing, Beijing 102249, China.
College of Artificial Intelligence, China University of Petroleum-Beijing, Beijing 102249, China.
J Colloid Interface Sci. 2024 Jan;653(Pt B):1671-1682. doi: 10.1016/j.jcis.2023.09.145. Epub 2023 Sep 26.
Exploiting photocatalysts with high interfacial charge separation efficiency remains a huge challenge for converting solar energy into chemical energy. Herein, a novel 0D/2D heterojunction is successfully constructed by using bimetallic MoTiC MXene Quantum Dots (MoTiC QDs) firmly immobilized on the surface of g-CN nanosheet via an electrostatic self-assembly strategy. The MoTiC QDs/g-CN exhibits an efficient and stable photocatalytic hydrogen production performance up to 2809 µmol gh, which is 7.96 times higher than pure g-CN nanosheet, and prominently exceeding many reported photocatalysts. Besides, a prominent apparent quantum yield achieves 3.8% at 420 nm. The significant performance improvement derives from the giant interfacial electric field that formed between large interface contact areas, ensuring greatly efficient separation and transfer of the photogenerated carriers. Furthermore, the 0D/2D heterojunction possesses high-quality interfacial contact, which reduces the interfacial recombination of photoinduced electrons and holes, causing the quick electron transfer from the g-CN to electron acceptor MoTiC QDs, thus enhancing the charge utilization. Kelvin probe force microscopy (KPFM) measurements and density functional theory (DFT) calculation comprehensively demonstrate that g-CN modified by MoTiC QDs can modulate the electronic structure and prompt the establishment of the interfacial electric field, which consequently leads to efficient photocatalytic activity. This study adequately illustrates that constructing heterojunction interfacial electric fields based on MXene quantum dots is a prospective pathway to engineering high-performance photocatalytic platforms for solar energy conversion.
开发具有高界面电荷分离效率的光催化剂仍然是将太阳能转化为化学能的巨大挑战。在此,通过静电自组装策略,将双金属MoTiC MXene量子点(MoTiC QDs)牢固地固定在g-CN纳米片表面,成功构建了一种新型的0D/2D异质结。MoTiC QDs/g-CN表现出高效且稳定的光催化产氢性能,高达2809 μmol g⁻¹ h⁻¹,是纯g-CN纳米片的7.96倍,显著超过许多已报道的光催化剂。此外,在420 nm处的显著表观量子产率达到3.8%。显著的性能提升源于大界面接触区域之间形成的巨大界面电场,确保了光生载流子的高效分离和转移。此外,0D/2D异质结具有高质量的界面接触,减少了光致电子和空穴的界面复合,使电子从g-CN快速转移到电子受体MoTiC QDs,从而提高了电荷利用率。开尔文探针力显微镜(KPFM)测量和密度泛函理论(DFT)计算全面表明,经MoTiC QDs修饰的g-CN可以调节电子结构并促进界面电场的建立,进而导致高效的光催化活性。这项研究充分说明,基于MXene量子点构建异质结界面电场是设计用于太阳能转换的高性能光催化平台的一条有前景的途径。